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Uranium: The Nuclear Fuel Cycle and Beyond

Associated data.

All data supporting the results of this work are presented in tables and figure of the manuscript.

This review summarizes the recent developments regarding the use of uranium as nuclear fuel, including recycling and health aspects, elucidated from a chemical point of view, i.e., emphasizing the rich uranium coordination chemistry, which has also raised interest in using uranium compounds in synthesis and catalysis. A number of novel uranium coordination features are addressed, such the emerging number of U(II) complexes and uranium nitride complexes as a promising class of materials for more efficient and safer nuclear fuels. The current discussion about uranium triple bonds is addressed by quantum chemical investigations using local vibrational mode force constants as quantitative bond strength descriptors based on vibrational spectroscopy. The local mode analysis of selected uranium nitrides, N≡U≡N, U≡N, N≡U=NH and N≡U=O, could confirm and quantify, for the first time, that these molecules exhibit a UN triple bond as hypothesized in the literature. We hope that this review will inspire the community interested in uranium chemistry and will serve as an incubator for fruitful collaborations between theory and experimentation in exploring the wealth of uranium chemistry.

1. Introduction

Uranium was discovered in 1789 by the German chemist Martin Heinrich Klaproth [ 1 ]. It is the most known and used actinide element mainly because of its usage in nuclear fuel processing; however, the application potential of uranium compounds is much broader, stretching, e.g., into the field of organometallic synthesis, catalysis and beyond, as sketched in Figure 1 [ 2 , 3 , 4 , 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 ]. Moreover, uranium is one of the few naturally occurring actinides [ 1 ], whereas the other members, with the exception of thorium, are considered to be human-made, despite their natural occurrence in traces as a result of uranium and thorium spontaneous fissions. In nature, uranium occurs as three main isotopes, where the non-fissile 238 U is the most abundant, encompassing over 99% of the available uranium resources.

An external file that holds a picture, illustration, etc.
Object name is ijms-23-04655-g001.jpg

Examples of the broad range of uranium use.

In the Earth’s crust, there are different types of uranium ores, such as uraninite or pitchblende ( x UO 2 · y UO 3 , with y / x < 2), carnotite (K 2 O·2UO 3 · V 2 O 5 · x H 2 O) and autunite (CaO·2UO 3 · P 2 O 5 · x H 2 O) [ 14 , 15 ]. In order to extract uranium from its ore, chemical processes utilizing acids and oxidizing agents are employed. Often, specific isotopic separation processes have to be applied in order to acquire the desired concentration of a given uranium isotope for energy generation purposes [ 1 ]. The most used isotopic separation process involves uranium conversion into the gaseous UF 6 followed by isotope separation due to mass differences [ 16 ].

A number of reviews have been previously published covering the industrial use of uranium, i.e., in energy supply and related fields [ 15 , 17 , 18 , 19 , 20 , 21 ]. Organouranium compounds, i.e., the uranium equivalent of organometallic complexes, have attracted considerable attention, including reviews on ( η 8 -C 8 H 8 ) 2 U and actinides cyclobutadienyl complexes, respectively [ 22 , 23 ].

Uranium coordination chemistry, in general, has been being widely investigated [ 9 , 24 , 25 , 26 ], especially with regard to possible applications in nuclear waste treatment [ 27 ], where the efficient extraction of uranium from the waste generated during the nuclear fuel cycle (so-called spent nuclear fuel), and its recycling into the nuclear fuel process is an important step to reduce long-term radioactive waste [ 28 , 29 , 30 , 31 , 32 ]. Uranium oxides have been used for a long time as nuclear fuel [ 33 , 34 ]. However, their handling in the spent nuclear fuel regeneration process is difficult [ 35 ].

N-substituted uranium amides, including uranyl nitrates with picolinamide-based ligands, uranyl di-amide complexes and uranyl Schiff-base complexes, have been found to be highly promising alternatives. They are fully combustable, show high hydrolytic and radiation stability and produce degradable products [ 11 , 36 , 37 , 38 ]. Furthermore, N-substituted uranium amides show diverse coordination behavior. They can bind through the carbonyl oxygen atom with the central metal atom or ion, and they can form bonds with a metal ion through the deprotonated N atom of the ligands.

It has been suggested that, in both cases, bonding can be strengthened in the presence of a preferable anchoring group that can form a five or six-membered chelate ring, as in picolinamide, which is an interesting aspect waiting to be further explored [ 11 ]. Some attempts have been made to estimate the uranium-oxygen (UO) and uranium-nitrogen (UN) bond strengths in these compounds via geometrical parameters, atomic charges or normal vibrational frequencies; however, a quantitative measure of the UO and UN bond strength allowing the strategic modulation of these uranyl complexes is missing, a problem that we will tackle in the last part of this review via a new tool for quantifying the strength of chemical bonds and/or weak chemical interactions based on vibrational spectroscopy [ 39 ].

Although the use of uranium amides appears to be an attractive alternative pathway, there is still the general concern about the effects of nuclear energy use on nature and human health, as documented in a number of reviews, such as [ 9 , 40 , 41 , 42 , 43 ].

Uuranium can adopt different oxidation states ranging from III to VI, thus, leading to a rich repertoire of uranium-ligand (UL) bonding with diverse covalency and 5f-/6d-orbital contributions, including δ and ϕ back-donation [ 44 ]. While, e.g., charge- and electron-loaded ligands favor U(VI), U(III) is mostly found in the presence of strong donor ligands engaging in ionic, lanthanide-like bonding [ 13 , 45 , 46 , 47 ]. Uranium multiple bonding has been discussed [ 48 , 49 ] and exhibited new opportunities in small-molecule activation [ 10 ].

In particular, uranium nitride linkages with a formal UN triple bond have attracted attention [ 38 ]. Recently, uranium mononitride was suggested as an attractive fuel for a range of reactors [ 50 ]. However, in order to explore these possibilities, there is a quest for further research to fully understand the nature of the UN triple bond. A powerful tool for the investigation of electronic structure and bonding in uranium compounds, the strategic investigation and fine-tuning of uranium-based catalysts and the discovery of novel and unusual U-catalytic transformations is provided by computational chemistry [ 51 ], which can also be helpful for the analysis of available experimental IR/Raman spectra of uranium complexes to identify normal mode vibrations with a high percentage of UL character [ 11 , 12 , 37 , 52 ].

However, the theoretical description of uranium complexes requires a careful treatment of relativistic effects [ 53 , 54 ], which make sizable or even dominate contributions to the molecular properties of uranium compounds—in particular, to UL bonding. In general, the s electrons of relativistic atoms are contracted as a direct consequence of their higher attraction to the heavy nucleus. This is also experienced by p orbitals, though in a smaller amount; d and f orbitals become shielded by the inner s and p .

As a consequence, outer electrons are less attracted to the nucleus and more available for chemical bonding [ 1 , 55 ], resulting in a larger variety of oxidation states, diverse coordination compounds [ 1 ] and a number of special properties, such as the color of gold [ 56 , 57 ].

In order to capture the relativistic effects, one has to go beyond the non-relativistic Schrödinger equation and instead refer to the far more complex Dirac Equation [ 58 ], thus, leading to relativistic Dirac-exact wave functions and associated molecular properties [ 59 , 60 , 61 ]. The most rigorous way to include relativity in the calculation of molecular systems is to use Dirac’s full four-component (4c) formalism, leading to wave functions as vectors of four complex numbers (known as bispinors) [ 62 ].

A large variety of approximate methods have been derived over the years [ 39 , 63 ], motivated by the assumption that the full 4c approach is computationally too demanding and cannot be applied to larger molecules [ 64 , 65 , 66 , 67 , 68 , 69 , 70 , 71 ]. Quasi-four component and two-component forms [ 63 ] have been developed to make these calculations more practical, such as the Douglas–Kroll–Hess approach [ 72 , 73 ], Regular Approximations [ 74 ] and the Normalized Elimination of the Small Component (NESC) [ 75 ].

Over the years, our group has developed a powerful two-component (2c)-NESC method [ 55 , 76 ] that allows the accurate calculation of first- and second-order response properties, including vibrational frequencies [ 77 , 78 , 79 , 80 , 81 , 82 , 83 , 84 ], for a variety of density functional and correlation-corrected wave function methods, thus, guaranteeing a broad application range [ 55 , 85 ].

A recent review on this topic, in particular with regard to the description of actinides can be found in reference [ 39 ], which also addresses the popular use of effective core potentials to describe relativistic effects using a non-relativistic platform, which are a cheap alternative to complex Dirac-based methods [ 86 ]. However, these seriously fail in the case of uranium, leading to calculated molecular properties with errors as large as 20% [ 87 ]. Recently, we adopted a new version of NESC using the atomic approximation (NESCau), which substantially increases the efficiency of relativistic calculations [ 39 , 64 ] even for larger systems.

The review is structured in the following way. In Section 2 , we focus on the use of uranium as nuclear fuel, followed by brief summary of the uranium cycle. In Section 3 , case studies of human and environmental injuries caused by accidents and disasters occurred in power plants are presented. Section 4 approaches the main challenges with respect to nuclear waste treatment, targeting recent suggestions. Finally, in Section 5 , we discuss uranium nitrides and their potential as novel nuclear fuels. We present a new effective way to quantitatively determine the strength of a chemical bond based on the local vibrational mode analysis (LMA), originally suggested by Konkoli and Cremer [ 88 , 89 , 90 , 91 , 92 ], and apply LMA to tackle the currently controversy about the U-O and U-N bond strengths in uranium nitrides. In Section 6 , a final outlook is given.

2. Role of Uranium in the Nuclear Fuel Cycle

Uranium is mainly used in the nuclear fuel cycle sketched in Figure 2 , an industrial process involving various activities to produce electricity from uranium in nuclear power reactors, i.e., the progression of nuclear fuel from creation to disposal. Typically, uranium is employed in the form of UO 2 . During uranium decay, fissile plutonium is produced. As spent fuel can be reprocessed and recycled, this explains the presence of a plutonium admixture with uranium in the subsequent fuel cycle [ 14 , 93 ].

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Object name is ijms-23-04655-g002.jpg

Nuclear fuel cycle. Source: Pennsylvania State University Radiation Science and Engineering Center (public domain).

Uranium is a relatively common element that is found throughout the world and mined in a number of countries. After mining, uranium ore is crushed in a mill and grounded to a fine slurry, which is leached in sulfuric acid (or sometimes a strong alkaline solution) to allow the separation of uranium from the waste rock. It is then recovered from solution and precipitated as uranium oxide concentrate, mostly U 3 O 8 , which is sometimes referred to as yellowcake uranium (caused by its khaki color). U 3 O 8 concentrate typically contains more than 80% uranium. The original ore, by comparison, may contain as little as 0.1% uranium [ 14 , 93 ].

Often, the yellowcake needs to be highly purified, due to impurities originated from the ore that remain, a process that is highly specific and depends on the ore quality [ 94 ]. Alternate processes have been proposed, such as supercritical carbon dioxide extraction, in particular for phosphate ores [ 95 , 96 ]. Purified U 3 O 8 is the product that is sold. About 200 tonnes are required to keep a large (1000 MWe) nuclear power reactor generating electricity for a year.

The uranium oxide obtained after uranium milling is not directly usable as fuel for a nuclear reactor—additional processing is required. Only 0.7% of natural uranium is fissile—capable of undergoing fission, the process by which energy is produced in a nuclear reactor. The form (or isotope) of uranium that is fissile is 235 U, whereas the remainder is 238 U. About 3.5–5% of the fissile isotope 235 U is required to maintain the chain reaction. Therefore, a physical process commonly called uranium enrichment has to be invoked to increase (or ‘enrich’) the 235 U concentration, which requires uranium to be in a gaseous form [ 1 ]. U 3 O 8 is first refined to uranium dioxide UO 2 , which can be directly used as fuel for those types of reactors that do not require enriched uranium. For reactors requiring enriched uranium, UO 2 is converted into uranium hexafluoride, which is a gas at relatively low temperatures. In order to produce UF 6 , UO 2 is first converted into the solid UF 4 , followed by oxidation with F 2 , yielding UF 6 (g).

This route is often preferable instead of the direct conversion of the oxide into the fluoride, due to the lower fluorine demand. Solid state reactions often lead to byproducts, which also have to be taken into account [ 94 , 97 , 98 , 99 ]. A gas-phase mechanism for such reactions was previously studied theoretically [ 100 ]. Currently, centrifuges are used for U-enrichment processes. Nonetheless, there are alternative techniques, such as gaseous diffusion, which was widely used in the past, and laser-based processes, which are still in development [ 101 ].

Subsequently, uranium has to be re-converted to its oxide form. There are several processes available, including wet conversions employing aqueous ammonia, for example, which hydrolyses UF 6 , followed by calcination. An alternative process is dry conversion, which is known to be less injurious for the environment. Independent of the method used, it is important that the final product—the actual reactor fuel—has the correct oxygen to uranium ratio [ 93 ]. In order to increase the stability and strength, nuclear fuel can be alloyed with zirconium [ 14 , 93 , 102 ], which has also drawn attention due to its potential use in spent fuel reprocessing [ 103 , 104 ].

The fission process transforms U (and Pu) into lighter elements, denoted as fissile products , which are often also radioactive. Thus, there are safety concerns regarding nuclear waste. Spent fuel still contains large amounts of uranium, known as depleted uranium and, therefore, can be recycled and reused from nuclear waste [ 14 ]; however, the often highly radioactive fissile products have to be safely stored [ 14 , 105 ].

As alternative to uranium oxides, uranium nitrides are discussed as novel nuclear fuel as they display higher values for thermal conductivity and melting point [ 106 ]. The species N≡U≡N was first obtained in an argon matrix through a molecular nitrogen reaction with atomic uranium. Clearly, uranium has the potential to break the triple bond in N 2 [ 107 ]. A recent investigation of N≡U≡N in both neutral and negatively charged states has led to new insights into the properties of this molecule in both the ground and excited states [ 108 ].

Other uranium nitrides followed, such as the related NUO, that was first observed in solid argon as a product of the reaction between U and NO, and density functional theory calculations predicted a duplet spin state [ 109 ]. NUO was also synthesized in solid neon by Zhou and Andrews [ 110 ]. A related species, NUNH, was observed as a product of the N≡U≡N reaction with hydrogen atoms, suggesting that NUNH features both double and triple uranium-nitrogen bonds [ 111 ].

3. Spent Fuel Recycling

The spent fuel contains uranium (about 96%), plutonium (about 1%) and high level radioactive waste products (about 3%). In order to recycle the spent fuel, uranium and plutonium have to be extracted from the nuclear waste. Current reprocessing plants dissolve the spent fuel and chemically separate it into those three components: uranium, plutonium and high level waste in most cases by dissolution in concentrated nitric acid, followed by extraction with tributyl phosphate (TBP) in kerosene. This leads to the complexation of uranium and plutonium, whereas the other fission products remain in the aqueous phase [ 112 , 113 , 114 ].

TBP, in turn, may undergo degradation, thus, requiring the removal of potential degradation products [ 94 ]. Therefore, alternative solvents have been proposed and successfully applied, such as Aliquat 336 [ 115 ] and Alamine 336 [ 116 ]. There are different ways to extract the left-over fission products. Alkali and alkaline earth metals can be removed through pH adjustments, followed by ion exchange [ 94 ]. The separation of lanthanides and actinides contained in spent fuel is a challenge for the nuclear industry due to their chemical similarities [ 117 , 118 , 119 ].

A number of complexation methods using different ligands and coordination patterns have been suggested [ 27 ]. In general, coordination chemistry has been successfully applied to extract depleted uranium from waste water for re-use. Apart from that, uranium complexes have shown to be potentially useful in catalysis [ 9 , 120 ]. Therefore, in the next section, the coordination chemistry of uranium will be further elucidated.

4. Coordination Chemistry of Uranium

The coordination chemistry of uranium dates back to at least the early 1800s. It has become an increasingly popular topic in the last 15–20 years, mostly because of the development of easy-to-synthesize, stable starting materials for, e.g., organometallic synthesis and catalysis. There is tremendous diversity in the type of ligands that have been found to form stable complexes with uranium [ 121 ]. Uranium atoms can adopt different oxidation states ranging from III to VI, leading to a rich repertoire of UL bonding with diverse covalency and 5f-/6d-orbital contributions. While, e.g., charge- and electron-loaded ligands favor U(VI), U(III) is mostly found in the presence of strong donor ligands engaging in ionic, lanthanide-like bonding [ 13 , 45 , 46 , 47 ].

The majority of uranium coordination compounds display either IV or VI oxidation states. In general, U(IV) molecules are more difficult to synthesize, as specific experimental conditions are required [ 122 , 123 ]. U(V) compounds tend to disproportionate into IV and VI oxidation states [ 14 , 99 ]. Nonetheless, procedures have been suggested for how to stabilize U(V) molecules while taking into consideration that the apparent U(V) instability could be a result of experimental limitations [ 124 ].

Uranium complexes with a UO 2 group and are often called uranyl compounds [ 99 ]. High-level coupled-cluster calculations have predicted that UO 2 + hydrolysis leads to an intermediate adduct and UO(OH) 2 + as the final product (see Figure 3 , molecule 1 ). The corresponding U(VI) complex, i.e., UO 2 2 + undergoes a similar reaction, as experimentally confirmed; however, it was found that the reaction barrier is slightly higher than that of the corresponding U(V) complex [ 125 , 126 ]. Many other reactions involving the uranyl cation have been studied thus far [ 127 ].

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Object name is ijms-23-04655-g003.jpg

Representative uranium complexes; the numbers refer to the discussion in the text.

For some time, it was believed that the lowest oxidation of uranium was III [ 1 , 128 ]. However, in 2013, the first stable U(II) complex was synthesized in the form of [Cp 3 ′ U] − , in which Cp ′ accounts for the group C 5 H 3 (SiMe 3 ) [ 129 ] (see Figure 3 , complex 2a ). After that, other stable U(II) molecules were isolated, e.g., using sodium as a reducing agent in the synthesis of U(II) compounds [ 128 ]. In addition to U(IV) and U(III) metallocenes with a bent structure [ 3 , 5 ], recently, the first stable U(II) [ η 5 -C 5 i Pr 5 ) 2 U] sandwich complex (see Figure 3 , complex 2b ) was synthesized in the reduction of U(III) by potassium graphite, and this has an unusual linear Cp-U-Cp angle [ 4 ].

Electronic structure calculations exhibit a mixing between 6d z 2 and 7s orbitals, which, according to the authors, is the main reason for the linear arrangement found in this complex. Recently, our group conducted a NESCau study on actinides sandwich complexes, including uranium; an example can be found in Figure 3 , complex 3 [ 39 ]. A theoretical study on a set of ( η 5 -C 5 i Pr 5 ) 2 U-derived complexes is currently under investigation in our group.

It has been hypothesized that bulky substituents are necessary to isolate this stable U(II) uranocene with substantial covalent U- π character, caused by uranium 5f and 6d orbital participation. Negatively charged U(II) metallocenes have been widely investigated computationally [ 130 ]. Confirmed by both experiment and theory, the (SiMe 3 ) group can serve as a stabilizing substituent due to its electron withdrawing character; however, stable U(II) complexes with electron-donating ligands have been reported as well, such as [Cp ′ ( C 5 Me 4 H) 3 U] − [ 131 ]. According to these studies, the high-spin quintet state is the most stable in these U(II) compounds, where uranium adopts a valence configuration of 5f 3 6d 1 .

Thus far, no U(I) complexes have been observed, except a divalent uranium, which behaves in 2- or 3-electron reductions, such as a U(I) species and, therefore, was named U(I) synthon [ 132 ] (see Figure 3 , complex 4 ). As discussed above, N-substituted uranium amide complexes (see Figure 3 ; complex 5a : uranyl nitrates, including picolinamide-based ligands [ 11 ]; complex 5b : uranyl diamide complexes [ 36 ]; complex 5c : uranyl Schiff-base coordination complexes [ 37 ]) have been recently discussed as attractive candidates for the next generation of reactors with regard to both the actual nuclear fuel cycle, spent fuel reprocessing and recycling [ 11 , 36 , 37 ], as well as complexes with uranium multiple bonding, including uranium nitrides [ 10 , 48 , 49 , 50 ] (see Figure 3 , complex 6 ).

The [UN 2 ] isoelectronic nitrogen analogue of the well know uranyl cation [UO 2 ] 2 + [ 127 ] has been suggested as future player for ceramic fuel in nuclear reactors [ 48 , 108 ]. Recent X-ray structures of the triuranium complexes, isolated in an argon matrix, supported by Raman spectra suggest a central U(VI) [UN 2 ] core with U≡N triple bonding [ 48 ]. Photoelectron spectroscopy predicts that electron attachment and electronic excitation significantly bends the [UN 2 ] unit and elongates the U≡N bond [ 108 ]. Since excited-state uranium nitrides may be prevalent in nuclear reactors, it will be interesting to systematically investigate the strength of the interaction between the pentagonal bipyramidal [UN 2 R 2 R’ 3 ] core and the two flanking uranium cations as well as their influence on the strength of the U≡N triple bond in both the ground and excited state.

5. Uranium and Human Health

Despite all safety efforts, disasters involving nuclear power plants have occurred, and serious consequences have arisen [ 133 , 134 , 135 ]. The Chernobyl disaster, which took place in the Ukraine in 1986, is an appalling example. A fire that broke out during a safety test led to an explosion and the release of radioactive material into the environment with catastrophic human and nature impacts [ 136 ]. Melted material (so-called lava ) is a signature of such an accident, causing the spread of radio-nuclides and an emerging risk of secondary explosions [ 134 , 135 ].

People in the surrounding area (workers and inhabitants) were exposed to high levels of radiation, and an increased risk of cancer, mainly leukemia, was observed [ 137 ], as well as congenital malformations, as a consequence of the exposure to radiation [ 138 ]. In 2011, following an Earthquake, a horrible accident occurred at Fukushima Dai-ichi Nuclear Power Plant in Japan [ 133 , 139 ]. Although the power plant was immediately shut down after the earthquake, the following tsunami led to power outages, which interrupted the reactor cooling system [ 135 ]. Similarly to Chernobyl, nuclear meltdowns and radiation leakage arose. The Fukushima disaster also caused the release of contaminated material into the ocean as a direct consequence of the flooding; a portion of the contaminated seawater was later recycled into the environment [ 133 , 135 ].

In both cases, many people lost their lives, and regions close to the plant had to be evacuated and remain inhabitable up to date [ 140 ]. Both accidents initiated vivid debates on nuclear energy, including the problem of how to best store nuclear waste on a long-term basis and how to make these plants more efficient while maintaining all possible safety standards. A serious health problem is connected with depleted Uranium (DU), a byproduct of natural uranium after the enrichment and extraction of 235 U that is used to provide fuel for nuclear power plants and/or to charge nuclear weapons [ 141 , 142 ].

Aerosol inhalation is considered the primary route of DU exposure. Although laboratory tests have confirmed that inhalation of DU aerosol can cause lung, kidney and other organ damage, epidemiological studies have found no conclusive evidence that persons in areas with prolonged exposure to DU-containing bombs are affected. Apart from that, DU can induce multiple other health effects, such as renal tubular necrosis and bone malignancies [ 143 ].

Uranium contamination is a global health concern. Regarding natural or anthropogenic uranium contamination, the major sources of concern are groundwater, mining, phosphate fertilizers, nuclear facilities and military activities. Apart from radioactivity, uranium shows the typical chemotoxicity of a heavy metal [ 144 ]. The consumption of water or food contaminated with uranium can lead to chronic kidney diseases and failure [ 145 , 146 ].

According to the World Health Organization (WHO), uranium intake from food or air is relatively low and, according to the region’s soil, water consumption might be a source of contamination. A guideline of 30 mg/L has been established; however, thus far, there is not sufficient evidence regarding cancer risks and other health issues [ 147 ]. Nonetheless, despite its lower overall chemical toxicity, as discussed above, a number of uranium isotopes are highly radioactive, including γ ray emissions. These isotopes are highly carcinogenic and dangerous for humans and wildlife.

In nuclear medicine, radionuclides are widely used in both diagnostics and treatment. Uranium is not directly employed for this to date; however, it is used to provide radioisotopes to be used in nuclear medicine. The most known example is 99 Mo/ 99 m Tc, which is used in imaging diagnostics. Another example of a radionuclide obtained from uranium is 229 Th/ 225 Ac. It is used in Targeted Alpha Therapy , a class of radionuclide therapy [ 148 , 149 ]. 235 U is used to produce 99 Mo through a fission reaction.

Its daughter 99 m Tc is widely used in diagnostics. The majority of 99 Mo/ 99 m Tc is produced in research reactors; nonetheless, there are other routes, such as cyclotrons, which have the disadvantage of a lower production yield [ 150 ]. 229 Th results from 233 U decay. Its decay leads to 225 Ac, which has been used in the treatment of several types of cancer, including prostate cancer. A high level of purity is needed due to the fact that radionuclide impurities may be potentially toxic [ 149 ].

6. UN Bond Strength in Uranium Nitrides

Given the increasing interest in uranium nitrides, in this section, we introduce an efficient tool to quantitatively assess the strength of a chemical bond/weak chemical interaction based on vibrational spectroscopy and showcase its application for some selected uranium nitrides, N≡U≡N, U≡N, N≡U=NH and N≡U=O, clarifying if these molecules exhibit a UN triple bond, as hypothesized in the literature.

LMA has been extensively described in a recent review [ 151 ]; therefore, in the following, only highlights are summarized. The idea of characterizing a chemical bond via the normal mode stretching force constant has its roots in the 1920s and 1930s and is based on the famous Badger rule , an inverse power relationship between the bond length and stretching force constant [ 152 ]. While this rule works perfectly fine for diatomic molecules, its extension to polyatomic molecules has been a major obstacle [ 151 , 153 ] because normal vibrational modes tend to delocalize over the molecule rather than being localized in a specific bond [ 154 , 155 ].

As of that important fact, the related normal mode stretching force constants cannot serve as a suitable bond strength measure. LMA, originally suggested by Konkoli and Cremer [ 88 , 89 , 90 , 91 , 92 ], solved this problem, which led to a new measure of the intrinsic strength of a chemical bond or weak chemical interactions and a generalized Badger rule [ 153 ] based on local mode force constants k a . A comprehensive discussion of the underlying theory of LMA, following two independent routes to derive local vibrational modes, is given in Ref. [ 151 ].

Local mode force constants, contrary to normal mode force constants are independent of the choice of the coordinates used to describe the molecule in question [ 153 , 156 , 157 ]. They are sensitive to differences in the electronic structure (e.g., caused by changing a substituent), and because they are, in contrast to frequencies, independent of the atomic masses, they capture pure electronic effects. In their landmark paper, Zou and Cremer [ 158 ] proved that the local stretching force constant k n a (AB) reflects the intrinsic strength of the bond/interaction between two atoms A and B, which is described by an internal coordinate q n .

In essence, LMA has advanced as a powerful analytical tool, extensively applied to a broad range of chemical systems from simple molecular systems to systems in solution [ 159 , 160 ] to proteins [ 161 , 162 ], accounting for both covalent bonds [ 153 , 158 , 163 , 164 , 165 , 166 , 167 , 168 , 169 , 170 , 171 , 172 , 173 , 174 , 175 ] and non-covalent interactions [ 172 , 176 , 177 , 178 , 179 , 180 , 181 , 182 , 183 , 184 , 185 , 186 , 187 , 188 , 189 , 190 ], including hydrogen bonds [ 191 , 192 , 193 , 194 , 195 , 196 , 197 , 198 , 199 , 200 , 201 ]. Recently, LMA theory has been extended to periodic systems, a large step forward to the quantitative description of bonding in crystals and solids [ 190 , 202 , 203 ].

For the comparison of larger sets of k a values, the use of a relative bond strength order (BSO) is more convenient. According to the generalized Badger rule derived by Cremer, Kraka and co-workers [ 153 , 169 ], both are connected via a power relationship of the form

where the parameters u and v are obtained from two reference molecules with known BSO and k a values and the request that, for a zero force constant, the BSO value is also zero. For example, for CC bonds, suitable references are ethane and ethylene with bond orders n = 1 and n = 2, respectively, [ 163 , 174 , 204 ]. In the case of more complex bonding situations, e.g., metal–ligand bonding, guidance by Mayer bond orders [ 205 , 206 , 207 ] can be utilized [ 208 ]. It is important to note that the reference molecules have to be calculated with the same model chemistry as the set of molecules under investigation.

In this work, H 2 N-UH and HN=UH 2 were used as reference molecules for uranium-nitrogen single and double bonds with k a values of 2.253 and 4.865 mDyn/Å, respectively. Optimized UN bond lengths of 2.166 and 1.872 Å, respectively, obtained in this work are in excellent agreement with previously reported bond lengths [ 209 ]. The corresponding Mayer bond orders for the UN single and double bonds were 1.150 and 2.265. Scaling the Mayer bond order of the UN single bond to the value 1.0, the corresponding bond order of the UN double bond is 1.97, which led to u and v values of 0.4894 and 0.8803, respectively, as used in this work.

For the uranium-oxygen bonds, uranyl hydroxide, UO 2 (OH) 2 (complex 1 in Figure 3 ) was used as a single reference molecule, because it has both single and double uranium-oxygen bonds. We obtained k a values for the UO single and double bonds of 2.791 and 7.114 mDyn/Å, respectively, and optimized UO bond lengths of 2.100 and 1.762 Å, respectively. The corresponding Mayer bond orders for the UO single and double bonds were 1.175 and 2.270. Scaling the Mayer bond order of the UO single bond to the value 1.0, the corresponding bond order of the UO double bond is 1.932, which led to u and v values of 0.4855 and 0.7041, respectively, as used in this work.

The quantum theory of atoms-in-molecules (QTAIM), developed by Bader [ 210 , 211 , 212 , 213 ], identifies, analyzes and characterizes chemical bonds via the topological features of the total electron density ρ ( r ) . In this work, we used QTAIM as a complementary tool to LMA to determine the covalent character of the UN and UO bonds via the Cremer–Kraka criterion [ 214 , 215 , 216 ] of covalent bonding. The Cremer–Kraka criterion is composed of two conditions: (i) a necessary condition: the existence of a bond path and bond critical point r b , i.e., the (3,−1) saddle point of electron density ρ ( r ) between the two atoms under consideration; and (ii) a sufficient condition: the energy density H ( r b ) at that point is smaller than zero. H ( r ) is defined as:

where G ( r ) is the kinetic energy density and V ( r ) is the potential energy density. The negative V ( r ) corresponds to a stabilizing accumulation of density whereas the positive G ( r ) corresponds to depletion of the electron density [ 215 ]. As a result, the sign of H ( r b ) indicates which term is dominant [ 216 ]. If H ( r b ) < 0, the interaction is considered to be covalent in nature, whereas H ( r b ) > 0 is indicative of electrostatic interactions.

All geometry and frequency calculations were performed in the is work with the PBE0 density functional [ 217 , 218 , 219 ] combined with the cc-pwCVTZ-X2C basis set for uranium and the corresponding cc-pVTZ basis set for the non-relativistic atoms [ 220 , 221 , 222 , 223 , 224 ]. Relativistic effects were included through the NESCau Hamiltonian [ 64 ] (recently applied to a larger set of actinide sandwich complexes [ 39 ]) using the COLOGNE2020 program package [ 225 ]. LMA properties were calculated with the LmodeA program [ 226 ], and the energy density at the bond critical points was obtained using the AIMALL software [ 227 ].

In Table 1 , LMA and QTAIM results for N≡U≡N, U≡N, N≡U=NH, N≡U=O and UO 2 are summarized. Figure 4 shows the BSO values obtained from the local stretching force constants k a , Figure 5 correlates H ( r b ) and k a . The BSO values (see Table 1 and Figure 4 ) clearly show that, in all four compounds, U≡N bonds are of triple bond character, thus quantifying, for the first time, previous speculations and suggestions [ 109 , 110 , 111 ]. The lowest value of 2.976 was found for U≡N, comparable values of 3.081 and 3.087 for N≡U≡N and N≡U=NH, respectively, and the strongest triple bond for N≡U=O with BSO = 3.238.

An external file that holds a picture, illustration, etc.
Object name is ijms-23-04655-g004.jpg

BSO values of UN bonds for the selected uranium nitrides derived from k a values via the power relationship described above. NESCau/PBE0//cc-pwCVTZ-X2C (uranium) and NESCau/PBE0//cc-pVTZ (N,O,H) level of theory.

An external file that holds a picture, illustration, etc.
Object name is ijms-23-04655-g005.jpg

Correlation between H( r b ) and k a for UN and UO bonds. NESCau/PBE0//cc-pwCVTZ-X2C (uranium) and NESCau/PBE0//cc-pVTZ (N,O,H) level of theory.

Bond lengths in Å, k a in mDyn/Å, BSO and H( r b ), in Hartree/Å 3 , spin multiplicity and oxidation number of uranium for N≡U≡N, U≡N, N≡U=NH, N≡U=O and UO 2 ( a ) calculated at the NESCau/PBE0//cc-pwCVTZ-X2C (uranium) and NESCau/PBE0//cc-pVTZ (N,O,H) level of theory.

( a ) 3 Φ u is the ground state of UO 2 being 40.0 kcal·mol −1 more stable than the singlet 1 Φ u state.

The U=NH bond in U≡N, N≡U=NH can be identified as double bond with BSO = 1.989, and the U=O bond in N≡U=O and UO 2 is a slightly stronger double bond with BSO = 2.066 and 1.966, respectively. The U=O double bond of the UO 2 triplet 3 Φ u ground state mirrors with a bond length of r = 1.775 Å and BSO of 1.966 the U=O bond in N≡U=O (r = 1.761 Å, BSO = 2.066), whereas the U=O bond in the excited UO 2 1 Φ u singlet state is considerably longer and weaker (r = 1.836 Å, BSO = 1.689).

As is depicted in Table 1 and Figure 5 , all UN and UO bonds investigated are of covalent character showing the general trend that a stronger bond is also more covalent. There is no perfect correlation between these two properties, which is the result of the fact that whereas local force constants reflect the electronic environment, the energy density is taken at only one point on the bond path [ 39 ].

7. Conclusions and Future Perspectives

This review summarizes the recent research on the use of uranium as nuclear fuel, including recycling and health aspects elucidated from a chemical point of view, i.e., emphasizing the rich uranium coordination chemistry, which has also raised interest in using uranium compounds in synthesis and catalysis. A number of novel uranium coordination features are addressed, such as the emerging number of U(II) complexes and uranium nitrides as a promising class of materials for more efficient and safer nuclear fuels. The current discussion about uranium triple bonds was addressed by quantum chemical investigations using local vibrational mode force constants as a quantitative bond strength descriptor based on vibrational spectroscopy.

The local mode analysis for selected uranium nitrides, N≡U≡N, U≡N, N≡U=NH and N≡U=O, could confirm and quantify, for the first time, that these molecules exhibit a UN triple bond as has been hypothesized in the literature. After this proof of concept, we are currently expanding our investigation to a larger series of molecules with potential UN triple bonds.

Future work in our group will also include (i) a comprehensive study of the intrinsic strength of UL bonds—in particular, their covalent or non-covalent character as well as the role of the f orbitals for UL bonding, including δ and ϕ back-donation [ 44 ], which is a necessary prerequisite for the strategic fine-tuning of uranium-based catalysts and the discovery of novel and unusual U-catalytic transformations; (ii) a systematic analysis of available experimental IR/Raman spectra of uranium complexes with LMA to identify normal mode vibrations with a high percentage of UL character [ 11 , 12 , 37 , 52 ]; (iii) following the procedure determined for actinide sandwich compounds [ 39 ], we will derive valuable guidelines for the fine-tuning of these U(II) sandwich compounds in their role as powerful reducing agents, including the evaluation of current suggestions that bulky substituents are necessary to isolate this stable U(II) uranocene with substantial covalent U- π character, caused by uranium 5f and 6d orbital participation; and (iv) the investigation of a series of uranyl nitrates with and without picolinamide-based ligands, uranyl diamide and uranyl Schiff-base coordination complexes and the compilation of a comprehensive list of U-O and U-N local force constants together with electron density data quantifying the covalent character of these bonds.

Based on our results, we will determine a design protocol to increase the U-ligand bond strength towards an improved remediation of nuclear waste from reactor fuels. We hope that this review will inspire the community interested in uranium chemistry and will serve as an incubator for fruitful collaborations between theory and experimentation to explore the wealth of uranium chemistry.

Author Contributions

Conceptualization, E.K. and B.M.T.C.P.; methodology, B.M.T.C.P. and E.K.; validation, E.K. and B.M.T.C.P.; investigation, B.M.T.C.P. and E.K.; resources, E.K.; data curation, B.M.T.C.P.; writing—original draft preparation, B.M.T.C.P. and E.K.; writing—review and editing, E.K. and B.M.T.C.P.; visualization, B.M.T.C.P. and E.K.; supervision, E.K.; project administration, E.K.; funding acquisition, E.K. All authors have read and agreed to the published version of the manuscript.

This research was funded by the National Science Foundation grant number CHE 2102461. The authors thank Southern Methodist University and SMU’s Center for Research Computing for providing excellent computational resources.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Data availability statement, conflicts of interest.

The authors declare no conflict of interest.

Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in published maps and institutional affiliations.

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Introduction to Nuclear Chemistry

Heino nitsche, publication history.

  • Published online 13 February 2013
  • Published in issue 13 February 2013

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SPECIAL ISSUE

This article is part of the 2013 Nuclear Chemistry special issue.

  Disclosure Statement

Views expressed in this editorial are those of the author and not necessarily the views of the ACS.

Nuclear chemistry has its origin in the research of Marie and Pierre Curie, who isolated the first radioactive elements, polonium and radium, from several tons of uranium ore in 1898. With the increased understanding of the atom stemming from the research of Rutherford, Bohr, and many other scientists in the beginning of the last century, the phenomenon of radioactivity was recognized as a nuclear process. During the ensuing years of the twentieth century, the field has grown and matured to a highly diverse discipline. In addition to frontier research, nuclear chemistry has found essential uses and applications in a broad variety of applied disciplines, such as nuclear medicine and isotope production, radio-pharmaceutical preparation, nuclear stockpile stewardship and security, surveillance of clandestine nuclear activities, nuclear power, separation science, nuclear waste processing and minimization, waste isolation and remediation of nuclear-contaminated sites, and prediction and monitoring of behavior of actinides in the environment, to name only a few. This thematic issue of Chemical Reviews , although far from comprehensive, covers a selected variety of applications as well as fundamental nuclear research themes.

Cutler and co-workers discuss the application of radioactive isotopes in medicine for diagnostics, imaging, and radiotherapy. Medical isotopes are used in more than 10,000 hospitals worldwide, and 80% of all nuclear medicine applications apply technetium-99, resulting in about 30 million uses per year. The authors review the nuclear and chemical properties of radionuclides currently used in nuclear imaging and therapy, together with their production methods and preclinical and clinical trials.

Mayer et al. present an overview of nuclear forensic science. Nuclear forensics is a relatively new branch of nuclear chemistry that combines radiochemistry, nuclear physics, and material science to identify the origin of clandestine nuclear materials. The review concentrates on the nuclear forensics of uranium and plutonium, as both elements have fissionable isotopes, and their origin, history, and intended use may be of interest for national security.

The next four articles review selected fundamental nuclear chemistry research areas that provide indispensable data necessary for an improved understanding of radionuclide transport in contaminated surface and subsurface environments. This information is vital for conducting performance assessment of potential geologic high-level nuclear waste repositories. The worst-case scenario for risk assessment is the intrusion of ground or surface water into a nuclear waste repository. This can corrode the waste forms and thus potentially transport radionuclides to the accessible environment. The release rate is then controlled by a variety of different processes: dissolution of the waste form, radionuclide solubility, redox and complexation interactions, as well as precipitation reactions with inorganic and natural and anthropogenic organic water components, and finally by the various geochemical and physical reactions with the host rock and its components. Actinides are the main contributors to the radiation dose of a nuclear repository, as short-lived fission products have decayed after several hundreds of years. The earlier actinides (U, Np, Pu, Am, and Cm) display a very rich redox chemistry. They can exist in a variety of oxidation states, ranging from +3 to +7 for neptunium and plutonium, from +3 to +6 for americium, and from +3 and +4 for curium. It is noteworthy that Pu(IV), Pu(V), and Pu(VI) can coexist in oxic aqueous solutions due to their similar redox potentials.

Geochemical transport models require, as input, accurate thermodynamic data of solid and solution radionuclide species that may form via chemical reactions with groundwater components and the surrounding geomedia. Altmaier and colleagues summarize the advances of aqueous actinide chemistry and thermodynamics. Results of these studies are important contributors to thermodynamic databases assessing the risk of migration of radionuclides in potential waste repositories and contaminated environments. Furthermore, data need to be available for elevated temperatures because the decay heat of nuclear waste stored in an underground repository can generate temperatures up to several hundred degrees.

Knope and Soderholm discuss experimental studies of actinide hydrates and their hydrolysis and condensation products that provide direct structural information of metal–ligand coordination numbers and bonding distances in solution. Recent refinements of existing techniques, such as intensity increases and spatial resolution improvements for synchrotron-based X-ray absorption fine structure (EXAFS) studies, and the application of X-ray scattering techniques to solution species, especially high-energy X-ray scattering (HEXS), have been instrumental to significant advances of the field. Such studies provide tangible metrics for an improved interpretation of thermodynamic solution measurements and are essential for calibration and refinement of theoretical molecular modeling calculations.

To continue the theme of actinide speciation in the environment, Walther and Denecke present a review of the origin, distribution, and analysis of natural and anthropogenic actinide colloids and particles generated from thorium and uranium minerals, reactor accidents in Chernobyl and Fukushima, above-ground nuclear testing, accidents during the transport of nuclear devices, and depleted uranium ammunition and shielding.

These colloids are considered important species for the transport of specific radionuclides in aqueous media. Tetravalent plutonium ions can form or become associated with colloidal sized particles. This represents another vector for transporting actinides through the geosphere. Plutonium in this form will not behave like a dissolved species and may exhibit considerably different migration behavior than the dissolved species. Depending on their size and charge relative to the surrounding porous media, colloids can move more rapidly or more slowly than the average groundwater velocity. During the last fifty years, Pu(IV) colloid, often also called Pu(IV) polymer, as well as Pu(IV) real or eigen colloids, was considered an amorphous noncrystalline solid that is closely related to tetravalent Pu(IV) amorphous hydrous oxide, PuO 2 (am, hyd). Recent studies suggest that Pu(IV) colloid exists in solution in the form of nanocrystalline PuO 2 that can grow in size due to cluster formation. Amorphous, hydrous plutonium dioxide, PuO 2 (am, hyd), may be X-ray diffraction-amorphous material because the correlation distances between the nanocrystals are too small to be sensitive to X-ray diffraction. PuO 2 (am, hyd) may indeed be nanocrystalline material. This dichotomy is illustrated in the papers by Knope and Soderholm, and Walther and Denecke. Future studies of this subject will hopefully contribute to an even more advanced understanding of the formation, nature, and stability of Pu(IV) colloid.

In the fourth and last paper related to the understanding of actinides in the environment, Geckeis and coauthors summarize the current status of actinide reactions at the interface between aqueous solution and minerals. Different types of interaction mechanisms, outer-sphere and inner-sphere actinide surface coordination, and actinide incorporation mechanisms are discussed together with theoretical and geochemical actinide sorption modeling.

Wen et al. survey theoretical methods and their computational approximations to predict the electronic structure and physical properties of actinide oxides ranging from Th to Cm. Their paper, titled “Density Functional Theory Studies of the Electronic Structure of Solid State Actinide Oxides”, focuses on theoretical predictions of lattice constants, electronic densities of states, band gaps, and magnetic and optical properties.

Qiu and Burns report on “Clusters of Actinides with Oxide, Peroxide, or Hydroxide Bridges”. Whereas there are an abundance of studies on thorium and uranium clusters reported in the literature, only a few corresponding studies on neptunium and plutonium exist. This may be due to increased experimental challenges when working with α-radiation, including the production of toxic materials and their limited availability in only small quantities at an ever increasing expense. A better understanding of actinide clusters on a fundamental level at the nanoscale may improve processing of nuclear materials as well as spent nuclear fuel separation methods. The paper by Andrews and Cahill, titled “Uranyl Bearing Hybrid Materials: Synthesis, Speciation, and Solid State Structures”, focuses on the underlying design principles of the synthesis of hexavalent uranyl hybrid materials. The authors discuss the influence of hydrolysis, pH variation, building unit selectivity, and efforts to incorporate supramolecular tools.

Fundamental actinide coordination chemistry in nonaqueous solutions is a rapidly growing field. Jones and Gaunt discuss the “Recent Developments in Synthesis and Structural Chemistry of Nonaqueous Actinide Complexes” to establish an increased understanding of bonding principles and electronic structure changes of actinides with a wide range of ligands relevant to industrial nuclear processes and environmental management. New fuel cycles for fourth generation fast neutron reactors (GEN IV) require a new approach to reprocessing. New strategies for high-level spent nuclear fuel management propose sophisticated separation schemes that separate long-lived waste radionuclides from short-lived ones. The separated radionuclides can be either conditioned for underground disposal or transmuted to shorter-lived radionuclides via neutron capture in nuclear reactors or accelerators. These reactions transmute long-lived actinides into higher actinides. Some of these will also undergo neutron-induced fission. This separation is essential for a successful transmutation of these actinides because the lanthanides would interfere, as they are strong neutron absorbers. Important radionuclides for removal are the fission products strontium-90, technetium-99, iodine-129, and cesium-135 to reduce the heat load on the nuclear waste form, and the trivalent actinides americium and curium. In their paper titled “Complexation and Extraction of Trivalent Actinides and Lanthanides by Triazinylpyridine N Donor Ligands”, Panak and Geist summarize the newest developments for the separation of trivalent americium and curium from fission lanthanides.

Lastly, Türler and Pershina report on the “Advances in the Production and Chemistry of the Heaviest Elements”. During the last three decades, eight new elements have been synthesized, independently confirmed, and named with approval from IUPAC. Since 1999, a collaboration between scientists from the Joint Institute for Nuclear Research (JINR), Russia, and the Lawrence Livermore National Laboratory (LLNL), USA, synthesized elements 112 through 118 at previously unknown high reaction cross sections. This was accomplished via a new reaction route using a high-intensity calcium-48 beam on neutron-rich actinide targets from uranium to californium. These experiments resulted in six new elements (113–118) and more than 50 previously unknown isotopes. In 2012, elements 114 and 116 were named flerovium (Fl) and livermorium (Lv), respectively. Elements 113, 115, 117, and 118 are still awaiting independent confirmation. Recently one-atom-at-a-time gas-phase volatility studies placed element 112, copernicium (Cn), as a d-metal in group 12 in the Periodic Table, which is in agreement with theoretical predictions. The first experiments for studying the chemical behavior of Fl are in progress.

I would like to thank all the authors for providing the outstanding review articles for this thematic issue of Chemical Reviews . I truly appreciate their tremendous efforts to help showcase the exciting field and the vibrancy of nuclear chemistry. I also thank the editorial staff and the editor Dr. Guy Bertrand for their hard work in publishing this issue on nuclear chemistry in Chemical Reviews . I very much hope that this publication provides a welcome reference to the experts as well as interesting information about the diversity of the field to the curious reader.

Author Information

  • Heino Nitsche ,  University of California, Berkeley

Heino Nitsche was born in Munich, Germany, in 1949. He received his B.S. (Dipl. Chem.) in 1976 and his Ph.D. (Dr. rer. nat.) in 1980 from the Freie Universität Berlin (West). He joined Lawrence Berkeley National Laboratory (LBNL) as a staff scientist in September 1980 and became principal investigator and leader of the radionuclide group in 1984. In 1993, he returned to Germany to become a chaired Professor of Radiochemistry at the Technische Universität Dresden, Germany. Additionally, he was appointed director of the Institute of Radiochemistry in the newly founded Forschungszentrum Rossendorf in Dresden. Nitsche is a professor in the Department of Chemistry at the University of California, Berkeley, and a Faculty Senior Scientist at LBNL since 1998. He is the founding director of the Glenn T. Seaborg Center at LBNL and served in this position until 2002. He has served on the advisory boards of the National Academy of Sciences, the International Atomic Energy Agency, the OECD Nuclear Energy Agency, and the Joint Research Centre of the European Union. He was Chair of the Nuclear Chemistry Section of the German Chemical Society and 2007 Chair of the Division of Nuclear Chemistry and Technology (DNCT) of the American Chemical Society (ACS). He was selected as a member of the 2011 class of ACS Fellows. He leads the Heavy Element Nuclear and Radiochemistry Group. Nitsche’s research interests include nuclear chemistry and physics of the heaviest elements, fundamental molecular-level understanding of actinides at metal-oxide and biological interfaces, the thermodynamics and kinetics of actinides in solution, and their relationship to nuclear waste disposal, environmental contamination, and separation science. He is also a member of an international team that first studied the chemistry of the heaviest elements, bohrium (107) and hassium (108), and he independently verified the discovery of element 114 in 2009 with his Berkeley team. Recently, his group discovered six new isotopes, reaching in an unbroken α decay chain from element 114 down to 104, rutherfordium. This is a major step toward better understanding how to explore the region of enhanced stability thought to lie in the vicinity of element 114—and possibly beyond.

This article is cited by 8 publications.

  • Robert Polly, Nicolas Finck, Tim Platte, Nikoleta Morelova, Frank Heberling, Bernd Schimmelpfennig, Horst Geckeis . First Principle Investigation of the Incorporation of Trivalent Lanthanides and Actinides in Hydroxycarbonate and Hydroxychloride Green Rust. The Journal of Physical Chemistry C 2022 , 126 (18) , 8016-8028. https://doi.org/10.1021/acs.jpcc.1c10814
  • Robert Polly, Bianca Schacherl, Jörg Rothe, Tonya Vitova . Relativistic Multiconfigurational Ab Initio Calculation of Uranyl 3d4f Resonant Inelastic X-ray Scattering. Inorganic Chemistry 2021 , 60 (24) , 18764-18776. https://doi.org/10.1021/acs.inorgchem.1c02364
  • Jagriti Singh, Dolly Yadav, Jai Deo Singh . En Route Activity of Hydration Water Allied with Uranyl (UO22+) Salts Amid Complexation Reactions with an Organothio-Based (O, N, S) Donor Base. Inorganic Chemistry 2019 , 58 (8) , 4972-4978. https://doi.org/10.1021/acs.inorgchem.8b03622
  • Ning Jiang , W. H. Eugen Schwarz , and Jun Li . Theoretical Studies on Hexanuclear Oxometalates [M6L19]q− (M = Cr, Mo, W, Sg, Nd, U). Electronic Structures, Oxidation States, Aromaticity, and Stability. Inorganic Chemistry 2015 , 54 (15) , 7171-7180. https://doi.org/10.1021/acs.inorgchem.5b00372
  • Matthieu Virot , Thomas Dumas , Manon Cot-Auriol , Philippe Moisy , Sergey I. Nikitenko . Synthesis and multi-scale properties of PuO 2 nanoparticles: recent advances and open questions. Nanoscale Advances 2022 , 4 (23) , 4938-4971. https://doi.org/10.1039/D2NA00306F
  • Xiang Liu , Jean-René Hamon . Recent developments in penta-, hexa- and heptadentate Schiff base ligands and their metal complexes. Coordination Chemistry Reviews 2019 , 389 , 94-118. https://doi.org/10.1016/j.ccr.2019.03.010
  • Hui Wang , Zhifang Chai , Dongqi Wang . Adsorption of uranyl on hydroxylated α-SiO 2 (001): a first-principle study. Dalton Transactions 2015 , 44 (4) , 1646-1654. https://doi.org/10.1039/C4DT02872D
  • Jean-Pierre Dognon . Theoretical insights into the chemical bonding in actinide complexes. Coordination Chemistry Reviews 2014 , 266-267 , 110-122. https://doi.org/10.1016/j.ccr.2013.11.018
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  • Feiqing Liu

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China conducts nationwide audit of research misconduct after thousands of papers retracted last year

Zahra Khan

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The Chinese government has launched a nationwide review of research misconduct in response to Hindawi retracting thousands of papers by Chinese authors. China has the highest retraction rate globally, including conference papers, exceeding 20 per 10,000 articles. Hindawi, a subsidiary of Wiley, retracted over 8000 articles involving a Chinese co-author in 2023, a record-breaking year for retractions that resulted in Wiley announcing that it would stop using the Hindawi brand and fold the journals into the rest of its portfolio.

As part of the review, China’s education ministry will require universities to declare all retractions and report any misconduct. Universities will have to compile a comprehensive list detailing all academic articles from English and Chinese language journals in the past three years and why they were retracted. ‘It seems to me a good move to investigate retraction and scientific misconduct. This will certainly do good to improve the scientific environment,’ says Shu-Li You  at the Shanghai Institute of Organic Chemistry.

The Chinese government is worried that the high number of retractions is damaging its academic reputation. In 2022, China was the world leader in scientific research output and ‘high impact’ studies, accounting for 23.4% of the world’s research output, according to a report published by Japan’s science and technology ministry. However, analysis conducted by Nature revealed that there were almost 17,000 retraction notices on papers with China-affiliated authors since January 2021.

Paper mills – illicit businesses that put together poor or fake journal papers that resemble genuine research and then sell authorship to them – pose a real threat to research integrity and the reliability of the scientific record. China is a major market for these fake papers and much of the mass retractions that have affected the scientific literature are the result of the discovery of paper mills. The Chinese government’s policies that see authors rewarded with promotions or financial incentives for the number of papers they publish have been cited as part of the problem . Publishers can struggle to weed out all the fraudulent articles and so the number of these papers is often underreported.

Largest investigation ever

While there have been investigations into batches of retracted papers in China before, this is the first time that such an investigation will be carried out at scale, and simultaneously by all institutions. ‘We recognise this effort by the Chinese government to address this issue at scale, and we encourage all stakeholders to scrutinise the motivations underpinning these research integrity challenges,’ a spokesperson for Wiley tells Chemistry World . However, the timing is a concern as the tight deadline, especially after the lunar new year and the winter break, makes it hard for the universities to submit their findings, having only been given slightly less than three months to complete this self-review.

‘The monetary incentive makes it worse. Indeed, it is a systematic problem that the purpose of research is not to advance knowledge but to gain promotion and money,’ adds Fei Shu , a research consultant at Hangzhou Dianzi University. The ministry has emphasised the seriousness of this measure with penalties for researchers failing to declare retracted papers with an explanation, such as image manipulation or honest mistakes. While the punishment for non-compliance has not been announced, prior consequences for misconduct have included salary cuts, withdrawal of bonuses and demotions. Shu is sceptical on the effectiveness of these deterrents saying that ‘the only solution is to build a new research assessment system on the basis of merit itself rather than counting the number of publications’.

The ministry has not said what it will do with the findings. ‘If no further action is required by the [education ministry], it will be forgotten after the Chinese new year break,’ adds Shu. ‘I really hope such a move will promote the scientific community worldwide to pay more attention on the scientific misconduct and to take actions too,’ says You.

Zahra Khan

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