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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 *** 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)***,a 2-fold interpenetrating 3D uranium-organic framework(YTU-W-1)was developed and introduced for photocatalytic H_(2)O_(2)*** material demonstrates a different photocatalytic mechanism when employing uranyl as an initiator,as compared with the conventional semiconductor photocatalytic pathway involving photo-generated charge *** 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^(-1)g^(-1).Furthermore,YTU-W-1 displays a high H_(2)O_(2)selectivity of 68%,confirmed by rotating ring-disk electrode(RRDE)*** were used to elucidate the critical role of uranyl in the photocatalytic oxygen reduction reaction for H_(2)O_(2)*** 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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Recent progress of radionuclides separation by porous materials

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Science China Chemistry 2024年第11期67卷 3515-3577页

作者： Yinghui Xie Long Yu Long Chen Cheng Chen Li wang Fenglei Liu Yun Liao Peng Zhang Tao Chen Yihui Yuan Yuexiang Lu Boyang Huang Hui Yang Suhua wang shuao wang Lijian Ma Feng Luo Yunhai Liu Baowei Hu Hongqing wang Duoqiang Pan Wenkun Zhu Ning wang Zhe wang Liang Mao Shengqian Ma Xiangke wang Guangdong Provincial Key Laboratory for Green Agricultural Production and Intelligent Equipment School of Environmental Science and Engineering Guangdong University of Petrochemical Technology School of Life Science Shaoxing University College of Environmental Science and Engineering North China Electric Power University 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 University College of Chemistry Sichuan University School of Chemistry and Materials Science East China University of Technology School of Chemistry and Chemical Engineering University of South China Frontiers Science Center for Rare Isotopes Lanzhou University State Key Laboratory of Environment-friendly Energy Materials National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety Sichuan Civil-military Integration Institute School of National Defence & Nuclear Science and TechnologySouthwest University of Science and Technology State Key Laboratory of Marine Resource Utilization in South China Sea Collaborative Innovation Center of Marine Science and Technology Hainan University Institute of Nuclear and New Energy Technology Tsinghua University State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Department of Chemistry University of North Texas

The separation of radionuclides is critical for the sustainable development of nuclear energy. It is urgent to design and prepare functionalized materials for efficient radionuclides separation. Porous materials are considered excellent candidates for the separation of radionuclides under complex conditions due to their high specific surface areas, tunable pore structures and controllable functionalities. In this review, we summarized the design, preparation and functionalization of porous materials and their application for separation of radionuclides in the past five years, discussed the separation performance and analyzed the structure-activity relationship between various radionuclides and porous materials, and systematically clarified their characterization and mechanism of different type porous materials. We also introduced the detection, irradiation and chemical toxicity of different reflective radionuclides.

关键词： porous materials radionuclides detection separation radiotoxicity interaction mechanism

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Metal-Organic Framework-Derived Metallic Carbon with Record High Radon Gas Capture Performance

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CCS Chemistry 2024年第7期6卷 1789-1797页

作者： Shicheng Gong Yi Tao Lixi Chen Qiuting Xu Junhao Lu Fuyin Ma Xia wang Guodong Li Jun Wan Guoxun Ji Linfeng He Xiaohui Yu Duo Zhang Xuhui Sun 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 215123 Institute of Functional Nano&Soft Materials Laboratory(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123 School of Environment and Material Engineering Yantai UniversityYantai 264005 Xi’an Research Institute of Hi-Technology Hong Qing TownXi’an 710025 Shanghai Institute of Measurement and Testing Technology Shanghai 201203 Engineering Institute of Advanced Manufacturing and Modern Equipment Technology Jiangsu UniversityZhenjiang 212013

Developing efficient adsorbents for radon(Rn)capture from the ambient environment is of paramount importance for public ***,it poses a great challenge due to the chemical inertness and extremely low molar concentration of Rn in ***,we report a zeolite imidazolate frameworkderived metallic carbon adsorbent(Zn@NPC)with record high Rn removal performance under ambient *** one-step pyrolysis,the prepared Zn@NPC possesses pores with a preference for Rn and atomically dispersed Zn sites,achieving a high Rn removal efficiency that doubles in adsorption coefficient(9.47 L·g^(−1))and triples in adsorption kinetic coefficient(20.25 mL·g^(−1)·min^(−1))over the benchmark Rn adsorbent coconut activated *** functional theory calculations elucidate the important role of the metal polarization effect,which cooperates with the pore size confinement effect to boost the overall Rn adsorption *** work launches a promising alternative for practical Rn capture.

关键词： radon removal metal-organic frameworks microporous carbon synergistic effect dynamic adsorption

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Tumor Imaging by a^(99m)TcO_(4)^(−)-Labeled Cationic Polymeric Network

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CCS Chemistry 2024年第8期6卷 1868-1875页

作者： Jie Li Rongzhen Xie Baoyu Li Lixi Chen Wenhao Shen Yuting Zhao Qi Guo Long Chen Boqi Xu Xijian Chen Jingwen Guan Lei Chen Kai Yang 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 215123 Department of General Surgery The First Affiliated Hospital of Soochow UniversitySuzhou 215000

Technetium-99m(99mTc)is the most used(>80%)radionuclide in the clinical nuclear diagnostic imaging *** traditional approach to preparing 99mTc-based imaging agents utilizes stannous chloride(SnCl_(2))for the reduction of noncomplexing pertechnetate(^(99m)TcO_(4)^(−))to low-valent Tc[e.g.,Tc(IV)].This process,however,is difficult to control precisely and usually results in toxic SnCl_(2) residue and remaining 99mTc(VII),both of which are destructive to ***,we report a new strategy for preparing^(99m)TcO_(4)^(−)-labeled agents without adding any *** deliberately designed nanoscale cationic polymeric network(SCU-CPN-3)shows excellent affinity for^(99m)TcO_(4)^(−)even at trace levels originating from the strong p-πinteraction with^(99m)TcO_(4)^(−).Impressively,record-fast labeling kinetics are observed,where almost quantitative labeling efficacy(>96%)can be achieved within 1 min,giving rise to a short labeling time and simple operation using a clinical *** single-photon emission computed tomography(SPECT)images and ex vivo biodistribution of different tumor model analyses verify the potential feasibility of this strategy for tumor imaging.

关键词： ^(99m)TcO_(4)^(−)-based agent tumor imaging fast-labeling kinetics high labeling efficiency no reductant

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三价超铀元素镅冠醚包合物的合成与表征

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科学通报 2024年第23期69卷 3404-3411页

作者：李凯王俊人代星程丽葳张海龙林健王亚星王殳凹苏州大学放射医学与辐射防护国家重点实验室苏州215123 西安交通大学核科学与技术学院西安710049

本文报道了95号元素镅(Am)的冠醚包合物[Am(NO_(3))_(2)(18-crown-6)]_(3)·[Am(NO_(3))_(6)](简写为Am-18C6)合成、单晶结构和固体紫外-可见-近红外光谱.X射线单晶衍射表明,Am-18C6晶体属于单斜晶系中的C2/m空间群,非对称单元由[Am(NO_(3))_(6)]^(3-)、[Am(NO_(3))_(2)(18C6)]^(+)和二重无序的[Am(NO_(3))_(2)(18C6)]^(+)孤立离子对组装而成.我们系统比较了Am-O键长与镧系同构晶体中Nd-O键长的差异,并将其与密度泛函理论(density function theory,DFT)计算的理论键长进行了对比.结果表明,Am^(3+)和Nd^(3+)的电子密度变化截然不同,Am^(3+)表现出明显地失去5f电子密度,这意味着Am^(3+)的5f电子在向着O–Am配位键中心延展和极化,而Nd^(3+)并未表现出此特性.本工作对加深三价超铀元素和大环配体之间主客体相互作用理解提供了帮助,为设计新型镧锕分离萃取剂提供了结构模型与理论基础.

关键词：超铀元素镅配合物密度泛函理论

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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 *** iron-based catalysts were exploited in the current industrial Haber-Bosch process,uranium-based materials served as effective catalysts for production of NH3from *** some molecular uranium complexes are known to be capable of combining with N2,further hydrogenation with H2forming NH3has not been reported to ***,we describe the first example of N2cleavage and hydrogenation with H2to NH3with a molecular uranium *** N2cleavage product contains three uranium centers that are bridged by three imido μ2-NH ligands and one nitridoμ3-N *** experiments with15N demonstrate that the nitrido ligand in the product originates from *** 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 *** 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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UranyI Phosphonates with Multiple UranyI Coordination Geometries and Low Temperature Phase Transition

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Chinese Journal of Chemistry 2021年第3期39卷 597-604页

作者： Lanhua Chen Yugang Zhang Zhehui Weng Zhiyong Liu Jiarong Zhang Yaxing wang shuao wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collabora-tive Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhouJiangsu 215123China Department of Chemical Science and Technology Kunming UniversityYunnanKunming 650214China

Main observation and conclusion Two new uranium(VI)phosphonate compounds,namely K_(8)[N(C_(2)H_(5))_(4)]_(2)(UO_(2))_(17)(H_(2)O)_(4)[CH_(2)(PO_(3))_(2)]_(8)[CH_(2)(PO_(3))(PO_(3)H)]_(4)·16(H_(2)O)(1)and[N(C_(2)H_(5))_(4)]_(4)(H_(3)O)_(2)(UO_(2))_(10)[CH_(2)(PO_(3))_(2)]_(5)[CH_(2)(PO_(3))(PO_(3)H)]_(2)·10H_(2)O(2),have been synthesized under mild hydro/solvothermal *** structural analysis of the two compounds reveals that they both contain all three typical coordination geometries of the U(VI)ions,including UO;tetragonal,UO,pentagonal,and UOg hexagonal ***,compound 1 displays a tempera-ture-induced single crystal to single crystal phase transformation as confirmed by the Single-crystal X-ray diffraction data collected at different ***-dependent fluorescence spectra presented herein illustrate the perturbation of the electronic structure of uranyl centers.

关键词： Uranium(VI)Phosphonate compounds Multiple coordination geometries Low temperature phase transition Coordination chemistry Fluorescence spectroscopy

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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 *** effective sequestering agent that is able to remove accidentally incorporated actinides in vivo with low toxicity is always in urgent *** 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 ***,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 ***, 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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