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Efficient and selective H_(2)O_(2)production through uranyl-assisted photocatalytic oxygen reduction reaction process in a uranium-organic framework

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Science China Chemistry 2024年第7期67卷 2274-2281页

作者： Jianxin Song Chao Liang Baoyu Li Xuemin wang Min Lei Lisha Jiang Zhenyu Li Yugang Zhang Jian Xie Zuju Ma Xing Dai Yanlong wang shuao wang Wei Liu School of Environmental and Materials Engineering Yantai UniversityYantai 264005China State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China School of Life and Environmental Sciences Shaoxing UniversityShaoxing 312000China School of Nuclear Science and Technology Xi’an Jiaotong UniversityXi’an 710049China

Harnessing solar energy by photocatalytically converting oxygen and water into high-value-added H_(2)O_(2)is a promising way of alleviating both environmental and energy issues.It is worth noting that suppressing detrimental side reactions,such as the generation of·O_(2)^(-),is a critical approach to enhancing H_(2)O_(2)production.Herein,a 2-fold interpenetrating 3D uranium-organic framework(YTU-W-1)was developed and introduced for photocatalytic H_(2)O_(2)production.The material demonstrates a different photocatalytic mechanism when employing uranyl as an initiator,as compared with the conventional semiconductor photocatalytic pathway involving photo-generated charge carriers.Benefiting from the strong hydrogen abstraction effect of the U≡O·and the direct one-step oxygen reduction pathway,YTU-W-1 exhibits enhanced photocatalytic performance for H_(2)O_(2)production with yield efficiency of 221μmol h-1g-1.Furthermore,YTU-W-1 displays a high H_(2)O_(2)selectivity of 68%,confirmed by rotating ring-disk electrode(RRDE)measurement.DFTcalculations were used to elucidate the critical role of uranyl in the photocatalytic oxygen reduction reaction for H_(2)O_(2)production.This research introduces an innovative approach to photo-driven H_(2)O_(2)production,underscoring the potential for heterogeneous catalysts to engage in photocatalytic reactions independently of photogenerated charge carriers.

关键词： uranyl metal-organic frameworks oxygen reduction reaction photocatalytic H_(2)O_(2)synthesis

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Flexible interdigitated layered framework with multiple accessible active sites for high-performance CH_(3)I capture

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Science China Chemistry 2024年第5期67卷 1569-1577页

作者： Bo Tai Baoyu Li Linwei He Zhonglin Ma Shujing Lin Mingxing Zhang Junchang Chen Fuqi Wu Long Chen Xing Dai Fuyin Ma Zhifang Chai shuao wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China

The development of adsorbent materials for effective capture of radioactive iodomethane(CH_(3)I) from the off-gas of used nuclear fuel reprocessing, remains a significant and challenging line of research because currently state-of-art adsorbents still suffer from low binding affinity with CH_(3)I. Here, we proposed a brand-new adsorption topological structure by developing a 2D interdigitated layered framework, named SCU-20, featuring slide-like channel with multiple active sites for CH_(3)I capture. The responsive rotating-adaptive aperture of SCU-20 enables the optimal utilization of all active sites within the pore for highly selective recognition and capture of CH_(3)I. A record-breaking CH_(3)I uptake capacity of 1.84 g/g was achieved under static sorption conditions with saturated CH_(3)I vapor. Both experimental and theoretical findings demonstrated that the exceptional uptake of SCU-20 towards CH_(3)I can be attributed to the confined physical electrostatic adsorption of F sites, coupled with the chemical nitrogen methylation reaction with uncoordinated N atoms of pyrazine. Moreover, dynamic CH_(3)I uptake capacity potentially allows for the capture of CH_(3)I in simulated real-world off gas reprocessing conditions. This study highlights the potential of SCU-20 as a promising candidate for efficient capture of iodine species and contributes to the development of effective solutions for radioactive iodine remediation.

关键词： 2D interdigitated layered framework iodomethane dual-sites electrostatic interaction physisorption and chemisorption

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Dinitrogen cleavage and hydrogenation to ammonia with a uranium complex

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National Science Review 2023年第2期10卷 165-173页

作者： Xiaoqing Xin Iskander Douair Yue Zhao shuao wang Laurent Maron Congqing Zhu State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical EngineeringNanjing University School of Medicine and Holistic Integrative Medicine Nanjing University of Chinese Medicine LPCNO CNRS and INSA Université Paul Sabatier State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow University

The Haber-Bosch process produces ammonia(NH3) from dinitrogen(N2) and dihydrogen(H2),but re quires high temperature and pressure.Before iron-based catalysts were exploited in the current industrial Haber-Bosch process,uranium-based materials served as effective catalysts for production of NH3from N2.Although some molecular uranium complexes are known to be capable of combining with N2,further hydrogenation with H2forming NH3has not been reported to date.Here,we describe the first example of N2cleavage and hydrogenation with H2to NH3with a molecular uranium complex.The N2cleavage product contains three uranium centers that are bridged by three imido μ2-NH ligands and one nitridoμ3-N ligand.Labeling experiments with15N demonstrate that the nitrido ligand in the product originates from N2.Reaction of the N2-cleaved complex with H2or H+forms NH3under mild conditions.A synthetic cycle has been established by the reaction of the N2-cleaved complex with trimethylsilyl chloride.The isolation of this trinuclear imido-nitrido product implies that a multi-metallic uranium assembly plays an important role in the activation of N2.

关键词： N

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The development of molecular and nano actinide decorporation agents

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Chinese Chemical Letters 2022年第7期33卷 3395-3404页

作者： Xiaomei wang Cen Shi Jingwen Guan Yemeng Chen Yigong Xu Juan Diwu shuao wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China

Internal contamination of actinides has led to significant health hazards to the public and workers in the context of nuclear power plant accidents,uranium ore mining,and reprocessing of the used fuel.An effective sequestering agent that is able to remove accidentally incorporated actinides in vivo with low toxicity is always in urgent need.The molecular decorporation ligands have been the most widely researched agents for the past few decades,while preliminary studies of functionalized nanoparticles have shown their clear advantages in metal binding selectivity,toxicity,and oxidative stress alleviation.Herein,the state-of-the-art of those two types of decorporation agents is presented with special attention being paid on the correlation between the solution and solid-state chemistry of those agents with actinides and the corresponding decorporation efficacies.

关键词： Actinides Chelator Binding selectivity Coordination mode Decorporation efficiency

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Fully conversing and highly selective oxidation of benzene to phenol based on MOFs-derived CuO@CN photocatalyst

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Chinese Chemical Letters 2023年第4期34卷 345-348页

作者： Longjiang Sun Dongxu wang Yuxin Li Baogang Wu Qi Li Cheng wang shuao wang Baojiang Jiang Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of ChinaSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China School of Pharmacy Jiamusi UniversityJiamusi 154007China State Key Laboratory of Radiation Medicine and Protection School for Radiological and interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions Soochow UniversitySuzhou 215123China Guangdong Laboratory of Chemitry and Fine Chemical Industry Jieyang Center Guangdong University of TechnologyJieyang 510006China

Developing highly efficient photocatalysts for selective oxidation of benzene to phenol is of great significance. However, it is still challenging to simultaneously achieve high conversion rate and selectivity.Herein, we demonstrate 99.9% of benzene photoconversion and 99.1% of phenol selectivity under the illumination of AM 1.5 for 12 h. For this purpose, an advanced CuO@CN photocatalyst has been fabricated by loading tubular carbon nitride(CN) with CuO nanoparticles thermally polymerized from Cu-based metal-organic frameworks(MOFs). The sluggish photocharge carrier recombination rate and the excellent stability indicate that the as-prepared nanocomposite is an ideal photocatalyst for benzene oxidation application. This work paves a new avenue for designing novel photocatalyst based on MOFs and carbon nitride materials.

关键词： Photocatalysis MOF CuO@CN Selectivity oxidation Highlyconversion rate

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A Trivalent Americium Organic Framework with Decent Structural Stability against Self-Irradiation

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Chinese Journal of Chemistry 2022年第7期40卷 801-805页

作者： Yugang Zhang Kai Li Sida Zhang Xia wang Hailong Zhang Yanlong wang Yaxing wang Zhifang Chai shuao wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySoochowJiangsu 215123China

We reported the synthesis,single crystal structure,and solid-state UV-Vis-NIR spectroscopy of a new transplutonium metal-organic framework(MOFs),Am(H_(2)O)[PO[(C6H4)COO]_(3)],denoted as AmTPO(TPO=tris(4-carboxylphenyl)-phosphineoxide).AmTPO forms a three-dimensional metal-organic framework structure with americium dimers as the secondary building unit.Clear 5f→5f transi-tions attributed to trivalent americium was observed in the absorption spectrum of AmTPO ranging from 300 to 1200 nm.Notably,AmTPO can maintain the crystallinity with no observable structural degradation within several months after being synthesized,re-vealing a long-term radiation resistance of this structure and the potential application of MOFs as a platform for nuclear waste dis-posal.

关键词： Metal-organic Frameworks Transplutonium Americium Radiochemistry Actinides

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ssDNA functionalized nanodiamonds for uranium decorporation

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Chinese Chemical Letters 2022年第7期33卷 3570-3572页

作者： Qinglong Yan Yu Miao Xiaomei wang Jifei Ma Juan Diwu Ying Zhu shuao wang Chunhai Fan Interdisciplinary Research Center Shanghai Synchrotron Radiation FacilityZhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesUniversity of Chinese Academy of SciencesShanghai 201210China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201800China State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules and National Center for Translational MedicineShanghai Jiao Tong UniversityShanghai 200240China

The hunt for agents that are suitable for actinide decorporation to reduce the whole-body load of actinide in accidental internal exposure is the ever-lasting goal in radiation protection and medical treatment in nuclear emergency.All current decorporation agents can be categorized as two groups,one is the molecular ligands,and the other is the nanoparticles decorated with molecular ligands.Here in this work,functional nanodiamonds(fN Ds)with ss DNA(the endogenous biomacromolecule rich in phosphate groups)loaded on the NDs is reported,which poses good uranyl adsorption selectivity,high cellular uptake,fast excretion,and effective decorporation of uranyl from rat renal proximal tubular epithelial cells(NRK-52E).All those results corroborate that f NDs can potentially serve as a brand new family of chelators for actinide decorporation.

关键词： Nanodiamond ssDNA Uranium Decorporation

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Radiation-induced one-pot synthesis of grafted covalent organic frameworks

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Science China Chemistry 2023年第6期66卷 1781-1787页

作者： Mingxing Zhang Mengjia Yuan Xiaofang Zhao Junchang Chen Linwei He Qianhong Gao Jiangtao Hu Guozhong Wu Zhifang Chai shuao wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201800China School of Environmental and Biological Engineering Nanjing University of Science&TechnologyNanjing 210094China

Post-synthetic functionalization of covalent organic frameworks(COFs)is an alternative way to enhance and broaden their properties and potential applications.However,the chemical functionalization of COFs is a great challenge because traditional procedures are often time-and energy-consuming,while the crystallinity of COFs can be damaged under harsh conditions.Here we report the in-situ introduction of functional graft chains onto the skeleton of COFs during the synthesis process through the combination of radiation-induced synthesis and graft polymerization techniques under ^(60)Co gamma-ray radiation.The synthesis and functionalization of COFs are simultaneously accomplished in a chemical system under ambient conditions yielding a large number of different functionalized COFs.The obtained carboxyl-functionalized COFs exhibit excellent radioactive uranium removal capabilities from aqueous solution with fast uptake dynamics,high adsorption capacity,and excellent selectivity over other competing metal ions.

关键词： covalent organic frameworks gamma ray radiation one-pot synthesis grafting functionalization uranium adsorption

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Improving in vivo Uranyl Removal Efficacy of a Nano-Metal Organic Framework by Interior Functionalization with 3-Hydroxy-2-pyridinone

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Chinese Journal of Chemistry 2022年第17期40卷 2054-2060页

作者： Mengping Chen Lang Lang Lei Chen Xiaomei wang Cen Shi Qiwen Sun Yigong Xu Juan Diwu shuao wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhouJiangsu215123 China

The environmental contamination of uranium will occur in scenarios such as nuclear accidents and leakage from nuclear waste storage sites,which eventually leads to the internal uranium exposure of people,causing consequential injuries of renal failure,osteosarcoma,etc.The development of uranyl specific chelating agents that could sequester uranium in vivo is in urgent need and is important for the safe and efficient development of nuclear industry.Metal organic frameworks(MOFs)already serve as efficient uranium depletion materials in solutions of a wide range of pH and ionic strength for nuclear fuel recycling,uranium extraction from seawater,as well as environmental decontamination.Herein,a chromium-based nano-metal organic framework(nano-MOF)functionalized interiorly with 3,2-HOPO ligands,MIL-101-HOPO,is rationally synthesized.In vitro adsorption experiments show that MIL-101-HOPO exhibits high adsorption selectivity and fast adsorption kinetics for uranyl.The results of in vivo uranyl decorporation assays reveal that MIL-101-HOPO with the decoration of HOPO ligands on the interior wall exhibits significantly increased uranyl removal ratio in kidneys comparing to the pristine nMOFs,and is more effective than the clinically used ZnNa_(3)-DTPA.All those results corroborate the interior functionalization of MOFs as an efficient strategy to develop promising uranyl decorporation agents.

关键词： Metal-organic frameworks Uranium 3,2-HOPO Adsorption Sequestration

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A Tetravalent Plutonium Organic Framework Containing[Pu_(2)O_(16)]Dimers as Secondary Building Units:Synthesis,Structure,and Radiation Stability

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中国化学:英文版 2023年第13期41卷 1552-1556页

作者： Yugang Zhang Yingzhe Du Lili Li Ye Tao Kai Li Hailong Zhang Yanlong wang Lanhua Chen Yaxing wang Zhifang Chai shuao wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhouJiangsu215123 China China Nuclear Power Technology Research Institute Co. Ltd.ShenzhenGuangdong518028 China

The second example of tetravalent plutonium carboxyl-based organic framework,^(242)Pu(OH)[PO[(C_(6)H_(4))COO]_(3)]·H_(2)O,termed as PuTPO(TPO=tris(4-carboxylphenyl)-phosphineoxide),was reported in this work.A series of characterizations of PuTPO,such as X-ray crystallography and solid-state UV-Vis-NIR spectroscopy,were carried out to expatiate its structure and physicochemical properties.PuTPO is constructed by dimers of the plutonium-oxygen subunit of[Pu_(2)O_(16)].Characteristic peaks located at approximately 1100 nm can be considered to be the fingerprint peaks of tetravalent plutonium.While PuTPO can maintain high crystallinity within several months after synthesis,it exhibits a radiation-induced swelling effect probed by the expansion of cell parameter of b axis after self-irradiation fromα-decay of ^(242)Pu.This result enriches the inventory of tetravalent plutonium compounds and provides an insight into the irradiation resistance of metal-organic frameworks.

关键词： Metal-organic frameworks Plutonium Actinides Crystal structure Coordination chemistry

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