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Actinoids in Biologic Systems and Catalysis
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Actinoids in Biologic Systems and Catalysis

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Physical Chemistry".

Deadline for manuscript submissions: closed (31 October 2022) | Viewed by 19891

Special Issue Editor

Prof. Dr. Dongqi Wang

E-Mail Website
Guest Editor
School of the Chemical Engineering, Dalian University of Technology, Dalian, China
Interests: computational actinoid chemistry; catalysis; computational biophysics

Special Issue Information

Dear Colleagues,

The past few decades witnessed the quick growth of our knowledge in actinoid chemistry, including their behaviors in catalysis and in biologic systems. Knowledge around these issues is important to the sustainable civil application of nuclear fission energy and contributes to an objective evaluation of potential influence to the environment and to health. Studies in these two issues have touched upon the fundamental nature of coordination chemistry of actinoids.

In the field of catalysis, low valent actinoid complexes have been reported to display intriguing reactivities to the activation of small molecules, e.g., CO2 and N2, which opened a new path to their activation and to the synthesis of more complex chemical compounds. These studies showed the potential to make use of isotopes with low radioactivity in catalysis that otherwise require geological disposal. This deserves extensive studies.

In the fields of bioinorganic chemistry and biophysics of actinoids, which have benefited from advanced experimental techniques and computational methodologies, an initial structure-based understanding of the interaction between in vivo actinoids and target proteins has been obtained, which has contributed to protein engineering by means of computer design and molecular biology to engineer proteins with improved binding affinities for actinoids. This knowledge also benefits the development of decorporation reagents.

These knowledges have shaped new views on the actinoids and will offer extensive influence on their civil application.

With this Special Issue, we hope to collect the recent research progress and opinions in the studies of actinoids in catalysis and in biological systems from both senior groups who have framed penetrating views and junior groups with active research interest in these issues. Submissions on the experimental techniques and methodologies that may be applied to study f-block chemistry and biophysics, and on the coordination chemistry of heavy metal systems which may stimulate a new understanding of f-block elements in catalysis and in biology, are also welcome. You are cordially invited to contribute to this Special Issue, in the form of either communications or articles or reviews, and share your opinions and your recent research to the community, through which we together learn from the past and look to the future.

Prof. Dr. Dongqi Wang
Guest Editor

Manuscript Submission Information

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Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Actinoids
  • f-block
  • electronic structure
  • biophysics
  • bioinorganic chemistry
  • catalysis
  • coordination chemistry

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Published Papers (11 papers)

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Editorial

Jump to: Research, Review

2 pages, 346 KiB  
Editorial
In Honor of Professor Zhifang Chai
by Dongqi Wang and Zhiyong Zhang
Molecules 2024, 29(19), 4627; https://doi.org/10.3390/molecules29194627 - 29 Sep 2024
Viewed by 343
Abstract
We are delighted to dedicate this Special Issue to a leading figure in actinoid chemistry, Prof [...] Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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2 pages, 118 KiB  
Editorial
An Editorial for the Special Issue “Actinoids in Biologic Systems and Catalysis”
by Dongqi Wang
Molecules 2024, 29(12), 2892; https://doi.org/10.3390/molecules29122892 - 18 Jun 2024
Viewed by 590
Abstract
The recent few decades witnessed a quick growth in our knowledge in actinoid chemistry, particularly in actinoids’ behaviors in catalysis and biologic systems [...] Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)

Research

Jump to: Editorial, Review

11 pages, 8305 KiB  
Article
Effects of CeO2 Nanoparticles on Nutritional Quality of Two Crop Plants, Corn (Zea mays L.) and Soybean (Glycine max L.)
by Xin Gui, Chaonan Dong, Shixian Fan, Chunlei Jiao, Zhuda Song, Jiaqi Shen, Yong Zhao, Xuanzhen Li, Fawen Zhang, Yuhui Ma, Xiao He, Aijun Lin and Zhiyong Zhang
Molecules 2023, 28(4), 1798; https://doi.org/10.3390/molecules28041798 - 14 Feb 2023
Cited by 6 | Viewed by 1857
Abstract
With the widespread applications of manufactured nanoparticles (NPs), there are increasing concerns about their potential adverse effects on the environment and living systems. Many studies demonstrated that NPs could significantly affect the growth and development of crop plants. However, knowledge regarding the impacts [...] Read more.
With the widespread applications of manufactured nanoparticles (NPs), there are increasing concerns about their potential adverse effects on the environment and living systems. Many studies demonstrated that NPs could significantly affect the growth and development of crop plants. However, knowledge regarding the impacts of NPs on crop quality is rather limited. In this study, the effects of CeO2 NPs (25, 75, and 225 mg Ce/kg) and CeCl3 (25 mg Ce/kg) on the nutritional components of soil-cultivated corn and soybean plants were evaluated. Both treatments tended to decrease the dry weight of grain per plant, while only 225 mg/kg CeO2 NPs on soybean and CeCl3 on corn showed statistical significance compared with the respective control. CeO2 NPs at 225 mg/kg significantly decreased the content of starch in the corn kernels by 18.2% but increased total phenols in soybean seeds by 18.4%. Neither CeO2 NPs nor CeCl3 significantly affected the contents of minerals in corn kernels except for Zn. However, in the case of soybean, the two treatments tended to decrease the contents of P, Zn, Mn, and Mo but increase the content of S. Overall, the results suggest that CeO2 NPs and Ce3+ ions showed similar but not identical effects on corn and soybean plants. CeO2 NPs affect the nutritional quality of crop plants in a species-dependent manner. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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15 pages, 6963 KiB  
Article
Folding Dynamics of 3,4,3-LI(1,2-HOPO) in Its Free and Bound State with U4+ Implicated by MD Simulations
by Qin Wang, Ziyi Liu, Yu-Fei Song and Dongqi Wang
Molecules 2022, 27(23), 8151; https://doi.org/10.3390/molecules27238151 - 23 Nov 2022
Cited by 2 | Viewed by 1365
Abstract
The octadentate hydroxypyridonate ligand 3,4,3-LI(1,2-HOPO) (t-HOPO) shows strong binding affinity with actinide cations and is considered as a promising decorporation agent used to eliminate in vivo actinides, while its dynamics in its unbound and bound states in the condensed phase remain [...] Read more.
The octadentate hydroxypyridonate ligand 3,4,3-LI(1,2-HOPO) (t-HOPO) shows strong binding affinity with actinide cations and is considered as a promising decorporation agent used to eliminate in vivo actinides, while its dynamics in its unbound and bound states in the condensed phase remain unclear. In this work, by means of MD simulations, the folding dynamics of intact t-HOPO in its neutral (t-HOPO0) and in its deprotonated state (t-HOPO4−) were studied. The results indicated that the deprotonation of t-HOPO in the aqueous phase significantly narrowed the accessible conformational space under the simulated conditions, and it was prepared in a conformation that could conveniently clamp the cations. The simulation of UIV-t-HOPO showed that the tetravalent uranium ion was deca-coordinated with eight ligating O atoms from the t-HOPO4− ligand, and two from aqua ligands. The strong electrostatic interaction between the U4+ ion and t-HOPO4− further diminished the flexibility of t-HOPO4− and confined it in a limited conformational space. The strong interaction between the U4+ ion and t-HOPO4− was also implicated in the shortened residence time of water molecules. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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16 pages, 4762 KiB  
Article
Understanding the Role of the Lateral Dimensional Property of Graphene Oxide on Its Interactions with Renal Cells
by Wei Chen, Bing Wang, Shanshan Liang, Meng Wang, Lingna Zheng, Si Xu, Jiali Wang, Hao Fang, Pu Yang and Weiyue Feng
Molecules 2022, 27(22), 7956; https://doi.org/10.3390/molecules27227956 - 17 Nov 2022
Cited by 2 | Viewed by 1697
Abstract
Renal excretion is expected to be the major route for the elimination of biomedically applied nanoparticles from the body. Hence, understanding the nanomedicine–kidney interaction is crucially required, but it is still far from being understood. Herein, we explored the lateral dimension- (~70 nm [...] Read more.
Renal excretion is expected to be the major route for the elimination of biomedically applied nanoparticles from the body. Hence, understanding the nanomedicine–kidney interaction is crucially required, but it is still far from being understood. Herein, we explored the lateral dimension- (~70 nm and ~300 nm), dose- (1, 5, and 15 mg/kg in vivo and 0.1~250 μg/mL in vitro), and time-dependent (48 h and 7 d in vivo) deposition and injury of PEGylated graphene oxide sheets (GOs) in the kidney after i.v. injection in mice. We specially investigated the cytotoxic effects on three typical kidney cell types with which GO renal excretion is related: human renal glomerular endothelial cells (HRGECs) and human podocytes, and human proximal tubular epithelial cells (HK-2). By using in vivo fluorescence imaging and in situ Raman imaging and spectroscopic analysis, we revealed that GOs could gradually be eliminated from the kidneys, where the glomeruli and renal tubules are their target deposition sites, but only the high dose of GO injection induced obvious renal histological and ultrastructural changes. We showed that the high-dose GO-induced cytotoxicity included a cell viability decrease and cellular apoptosis increase. GO uptake by renal cells triggered cellular membrane damage (intracellular LDH release) and increased levels of oxidative stress (ROS level elevation and a decrease in the balance of the GSH/GSSG ratio) accompanied by a mitochondrial membrane potential decrease and up-regulation of the expression of pro-inflammatory cytokines TNF-α and IL-18, resulting in cellular apoptosis. GO treatments activated Keap1/Nrf2 signaling; however, the antioxidant function of Nrf2 could be inhibited by apoptotic engagement. GO-induced cytotoxicity was demonstrated to be associated with oxidative stress and an inflammation reaction. Generally, the l-GOs presented more pronounced cytotoxicity and more severe cellular injury than s-GOs did, demonstrating lateral size-dependent toxicity to the renal cells. More importantly, GO-induced cytotoxicity was independent of renal cell type. The results suggest that the dosage of GOs in biomedical applications should be considered and that more attention should be paid to the ability of a high dose of GO to cause renal deposition and potential nephrotoxicity. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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11 pages, 2555 KiB  
Article
Nano-WSe2 Is Absorbable and Transformable by Rice Plants
by Xue Tian, Hongxin Xie, Jincheng Li, Liwei Cui, Yong-Liang Yu, Bai Li and Yu-Feng Li
Molecules 2022, 27(22), 7826; https://doi.org/10.3390/molecules27227826 - 13 Nov 2022
Viewed by 1688
Abstract
As typical transition metal dichalcogenides (TMDC), tungsten selenide (WSe2) nanosheets (nano-WSe2) are widely used in various fields due to their layered structures and highly tunable electronic and magnetic properties, which results in the unwanted release of tungsten (W) and [...] Read more.
As typical transition metal dichalcogenides (TMDC), tungsten selenide (WSe2) nanosheets (nano-WSe2) are widely used in various fields due to their layered structures and highly tunable electronic and magnetic properties, which results in the unwanted release of tungsten (W) and selenium (Se) into the environment. However, the environmental effects of nano-WSe2 in plants are still unclear. Herein, we evaluated the impacts and fate of nano-WSe2 and micro-WSe2 in rice plants (Oryza sativa L.). It was found that both nano-WSe2 and micro-WSe2 did not affect the germination of rice seeds up to 5000 mg/L but nano-WSe2 affected the growth of rice seedlings with shortened root lengths. The uptake and transportation of WSe2 was found to be size-dependent. Moreover, W in WSe2 was oxidized to tungstate while Se was transformed to selenocysteine, selenomethionine, SeIV and SeVI in the roots of rice when exposed to nano-WSe2, suggesting the transformation of nano-WSe2 in rice plants. The exposure to nano-WSe2 brought lipid peroxidative damage to rice seedlings. However, Se in nano-WSe2 did not contribute to the synthesis of glutathione peroxidase (GSH-Px) since the latter did not change when exposed to nano-WSe2. This is the first report on the impacts and fate of nano-WSe2 in rice plants, which has raised environmental safety concerns about the wide application of TMDCs, such as WSe2 nanosheets. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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12 pages, 2485 KiB  
Article
Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study
by Shuang Li, Yu-Chang Hou, Yuan-Ru Guo and Qing-Jiang Pan
Molecules 2022, 27(18), 6094; https://doi.org/10.3390/molecules27186094 - 18 Sep 2022
Cited by 3 | Viewed by 1812
Abstract
Transition metal oxides (TMOs) and actinide ones (AnOs) have been widely applied in catalytic reactions due to their excellent physicochemical properties. However, the reaction pathway and mechanism, especially involving TM–An heterometallic centers, remain underexplored. In this respect, relativistic density functional theory (DFT) was [...] Read more.
Transition metal oxides (TMOs) and actinide ones (AnOs) have been widely applied in catalytic reactions due to their excellent physicochemical properties. However, the reaction pathway and mechanism, especially involving TM–An heterometallic centers, remain underexplored. In this respect, relativistic density functional theory (DFT) was used to examine uranium-doped zinc, copper, and nickel oxides for their catalytic activity toward the conversion of furfural to furfuryl alcohol. A comparison was made with their undoped TMOs. It was found that the three TMOs were capable of catalyzing the reaction, where the free energies of adsorption, hydrogenation, and desorption fell between −33.93 and 45.00 kJ/mol. The uranium doping extremely strengthened the adsorption of CuO-U and NiO-U toward furfural, making hydrogenation or desorption much harder. Intriguingly, ZnO-U showed the best catalytic performance among all six catalyst candidates, as its three reaction energies were very small (−10.54–8.12 kJ/mol). The reaction process and mechanism were further addressed in terms of the geometrical, bonding, charge, and electronic properties. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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11 pages, 2448 KiB  
Article
Light Promotes the Immobilization of U(VI) by Ferrihydrite
by Yun Wang, Jingjing Wang, Zhe Ding, Wei Wang, Jiayu Song, Ping Li, Jianjun Liang and Qiaohui Fan
Molecules 2022, 27(6), 1859; https://doi.org/10.3390/molecules27061859 - 13 Mar 2022
Cited by 11 | Viewed by 2188
Abstract
The environmental behaviors of uranium closely depend on its interaction with natural minerals. Ferrihydrite widely distributed in nature is considered as one main natural media that is able to change the geochemical behaviors of various elements. However, the semiconductor properties of ferrihydrite and [...] Read more.
The environmental behaviors of uranium closely depend on its interaction with natural minerals. Ferrihydrite widely distributed in nature is considered as one main natural media that is able to change the geochemical behaviors of various elements. However, the semiconductor properties of ferrihydrite and its impacts on the environmental fate of elements are sometimes ignored. The present study systematically clarified the photocatalysis of U(VI) on ferrihydrite under anaerobic and aerobic conditions, respectively. Ferrihydrite showed excellent photoelectric response. Under anaerobic conditions, U(VI) was converted to U(IV) by light-irradiated ferrihydrite, in the form of UO2+x (x < 0.25), where •O2− was the dominant reactive reductive species. At pH 5.0, ~50% of U(VI) was removed after light irradiation for 2 h, while 100% U(VI) was eliminated at pH 6.0. The presence of methanol accelerated the reduction of U(VI). Under aerobic conditions, the light illumination on ferrihydrite also led to an obvious but slower removal of U(VI). The removal of U(VI) increased from ~25% to 70% as the pH increased from 5.0 to 6.0. The generation of H2O2 under aerobic conditions led to the formation of UO4•xH2O precipitates on ferrihydrite. Therefore, it is proved that light irradiation on ferrihydrite significantly changed the species of U(VI) and promoted the removal of uranium both under anaerobic and aerobic conditions. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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Review

Jump to: Editorial, Research

13 pages, 2029 KiB  
Review
Recent Advances in the Study of Trivalent Lanthanides and Actinides by Phosphinic and Thiophosphinic Ligands in Condensed Phases
by Qin Wang, Ziyi Liu, Yu-Fei Song and Dongqi Wang
Molecules 2023, 28(17), 6425; https://doi.org/10.3390/molecules28176425 - 4 Sep 2023
Cited by 1 | Viewed by 1898
Abstract
The separation of trivalent actinides and lanthanides is a key step in the sustainable development of nuclear energy, and it is currently mainly realized via liquid–liquid extraction techniques. The underlying mechanism is complicated and remains ambiguous, which hinders the further development of extraction. [...] Read more.
The separation of trivalent actinides and lanthanides is a key step in the sustainable development of nuclear energy, and it is currently mainly realized via liquid–liquid extraction techniques. The underlying mechanism is complicated and remains ambiguous, which hinders the further development of extraction. Herein, to better understand the mechanism of the extraction, the contributing factors for the extraction are discussed (specifically, the sulfur-donating ligand, Cyanex301) by combing molecular dynamics simulations and experiments. This work is expected to contribute to improve our systematic understanding on a molecular scale of the extraction of lanthanides and actinides, and to assist in the extensive studies on the design and optimization of novel ligands with improved performance. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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15 pages, 691 KiB  
Review
Analytical Methods for the Determination of 90Sr and 239,240Pu in Environmental Samples
by Ningjie Zhong, Lili Li, Xiaofan Yang and Yonggang Zhao
Molecules 2022, 27(6), 1912; https://doi.org/10.3390/molecules27061912 - 15 Mar 2022
Cited by 2 | Viewed by 2852
Abstract
Artificial long-lived radionuclides such as 90Sr and 239,240Pu have been long released into the environment by human nuclear activities, which have a profound impact on the ecological environment. It is of great significance to monitor the concentration of these radionuclides for [...] Read more.
Artificial long-lived radionuclides such as 90Sr and 239,240Pu have been long released into the environment by human nuclear activities, which have a profound impact on the ecological environment. It is of great significance to monitor the concentration of these radionuclides for environmental safety. This paper summarizes and critically discusses the separation and measurement methods for ultra-trace determination of 90Sr, 239Pu, and 240Pu in the environment. After selecting the measurement method, it is necessary to consider the decontamination of the interference from matrix elements and the key elements, and this involves the choice of the separation method. Measurement methods include both radiometric methods and non-radiometric methods. Radiometric methods, including alpha spectroscopy, liquid scintillation spectrometry, etc., are commonly used methods for measuring 239+240Pu and 90Sr. Mass spectrometry, as the representative of non-radiometric measurement methods, has been regarded as the most promising analytical method due to its high absolute sensitivity, low detection limit, and relatively short sample-analysis time. Through the comparison of various measurement methods, the future development trend of radionuclide measurement is prospected in this review. The fully automatic and rapid analysis method is a highlight. The new mass spectrometer with ultra-high sensitivity shows strong analytical capabilities for extremely low concentrations of 90Sr, 239Pu, and 240Pu, and it is expected to develop determination methods with higher sensitivity and lower detection limit. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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17 pages, 6256 KiB  
Review
High Sorption and Selective Extraction of Actinides from Aqueous Solutions
by Linfa Bao, Yawen Cai, Zhixin Liu, Bingfeng Li, Qi Bian, Baowei Hu and Xiangke Wang
Molecules 2021, 26(23), 7101; https://doi.org/10.3390/molecules26237101 - 24 Nov 2021
Cited by 4 | Viewed by 2438
Abstract
The selective elimination of long-lived radioactive actinides from complicated solutions is crucial for pollution management of the environment. Knowledge about the species, structures and interaction mechanism of actinides at solid–water interfaces is helpful to understand and to evaluate physicochemical behavior in the natural [...] Read more.
The selective elimination of long-lived radioactive actinides from complicated solutions is crucial for pollution management of the environment. Knowledge about the species, structures and interaction mechanism of actinides at solid–water interfaces is helpful to understand and to evaluate physicochemical behavior in the natural environment. In this review, we summarize recent works about the sorption and interaction mechanism of actinides (using U, Np, Pu, Cm and Am as representative actinides) on natural clay minerals and man-made nanomaterials. The species and microstructures of actinides on solid particles were investigated by advanced spectroscopy techniques and computational theoretical calculations. The reduction and solidification of actinides on solid particles is the most effective way to immobilize actinides in the natural environment. The contents of this review may be helpful in evaluating the migration of actinides in near-field nuclear waste repositories and the mobilization properties of radionuclides in the environment. Full article
(This article belongs to the Special Issue Actinoids in Biologic Systems and Catalysis)
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