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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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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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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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无机材料的“化学剪刀”结构编辑策略

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无机材料学报 2024年第2期39卷 115-128页

作者：丁浩明陈科李勉李友兵柴之芳黄庆中国科学院宁波材料技术与工程研究所先进能源材料工程实验室宁波315201 宁波杭州湾新材料研究院宁波315336 苏州大学苏州医学院放射医学与防护学院苏州215123

受到生物基因工程中“基因剪刀”的启发,“化学剪刀”作为一种重要的研究工具在材料结构编辑及应用研究中发挥着重要作用。本文对“化学剪刀”在材料结构编辑及应用方面的研究进展进行了评述。首先,介绍了“化学剪刀”的概念和基本原理... 详细信息

受到生物基因工程中“基因剪刀”的启发,“化学剪刀”作为一种重要的研究工具在材料结构编辑及应用研究中发挥着重要作用。本文对“化学剪刀”在材料结构编辑及应用方面的研究进展进行了评述。首先,介绍了“化学剪刀”的概念和基本原理,即指在保持初始材料主结构不变的条件下,通过化学反应敲除、置换、修复或重构目标原子或结构单元,从而定制化编辑材料晶格中的组成元素、晶体结构以及微观形貌,最终实现特定的材料结构与功能。随后,详细回顾了“化学剪刀”在材料结构编辑中的具体应用,即如何利用化学剪切、化学修饰、化学合成和化学刻蚀与化学插层等结构编辑方法对材料结构进行精确调控和功能设计。最后,对“化学剪刀”未来在材料结构编辑及应用的研究方向进行了展望。本评述详细介绍了“化学剪刀”在材料结构编辑及应用研究方面的研究进展和巨大潜力,为探索和开发“化学剪刀”在材料领域的应用提供了有力的理论和实验支撑,并有望推动相关材料领域的发展。

关键词：化学剪刀无机材料结构编辑专题评述

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利用假设检验方法开展物理实验误差分析

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物理通报 2024年第10期 112-116页

作者：柴志方华东师范大学物理与电子科学学院上海200241

误差分析是物理实验数据分析过程中的一个重要环节.基于统计学中假设检验的思想,利用统计学软件IBMSPSS,将T检验的方法运用到大学物理实验的误差分析中,运用概率来说明系统误差影响的大小,提出了物理实验的误差分析方法.最后,以圆柱体... 详细信息

误差分析是物理实验数据分析过程中的一个重要环节.基于统计学中假设检验的思想,利用统计学软件IBMSPSS,将T检验的方法运用到大学物理实验的误差分析中,运用概率来说明系统误差影响的大小,提出了物理实验的误差分析方法.最后,以圆柱体直径的测量实验为例,开展了误差分析,说明了利用假设检验开展误差分析的具体流程.

关键词：误差分析 t分布假设检验

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Influence of anions on the adsorption of uranyl on hydroxylated α-SiO_2(001):A first-principles study

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Green Energy & Environment 2017年第1期2卷 30-41页

作者： Hui Wang zhifang chai Dongqi Wang CAS Key Laboratory of Nuclear Radiation and Nuclear Energy Techniques and Multidisciplinary Initiative Center Institute of High Energy Physics Chinese Academy of Sciences CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and Technology School of Radiation Medicine and Interdisciplinary Sciences (RAD-X) Soochow University

The adsorption of uranyl on hydroxylated α-SiO_2(001) in the presence of a series of anionic ligands, i.e. OH^-, CO_3^(2-), NO_3^-, H_2PO_4^-, HPO_4^(2-),CH_3COO^-(Ac^-), C_6H_5COO^-(PhCO_2^-), C_6H_5O^-(PhO^-), was studied by the periodic density functional theory(DFT) implemented in the Vienna ab initio simulation package(VASP). For the ligands other than OH^-and PhO^-, only the bidentate coordination modes to the uranyl were considered. The excess charge effect of a charged system was first evaluated by constructing models with net charge as is or neutralized by creating defect at the bottom of silica, and the results show that a neutralized model, even with defects, is more realistic than the charged *** uranyl species prefer to bind with the deprotonated site(—O^-) rather than the protonated one(—O_H), which suggests that the increase of pH,which leads to the deprotonation of the surface, may enhance the uranyl adsorption. On the other hand, the anionic ligands, which are formed at higher pH, have negative effects. The weaker acidic ligands, such as H_2CO_3, H_3PO_4 and H_2O, whose speciation in solutions is sensitive to the fluctuation of pH, have more complex effect on the uranyl adsorption than strong acids or bases. Humic substances may coordinate with uranyl through carboxyl and phenolic groups, with the carboxyl group bound stronger. The ternary complexes with one bidentate(or monodentate)anion and one(or two) H20 as ligands, which leads to the uranyl penta-coordinated in its equatorial plane, are more favorable than other configurations when bound to the same anionic ligand. Both the charged nature and the coordination behavior of an anionic ligand are relevant to its ability to influence the adsorption of uranyl on the mineral surface. In addition, the uranyl species adsorbed at the surface functionalized by anionic ligands were also addressed, and the functionalized surfaces have weaker interaction with hydrated uranyl dication.

关键词： Density functional theory Adsorption α-SiO2(001) Uranyl Anionic ligands

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Towards understanding the correlation between UO_2^(2+) extraction and substitute groups in 2,9-diamide-1,10-phenanthroline

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Science China Chemistry 2018年第10期61卷 1285-1292页

作者： Xinrui Zhang Liyong Yuan zhifang chai Weiqun Shi Laboratory of Nuclear Energy Chemistry Institute of High Energy Physics Chinese Academy of Sciences School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions Soochow University

2,9-Diamide-1,10-phenanthroline(DAPhen)ligands represent a new family of tetradentate extractants given their strong affinity to actinides and the CHON *** this family,N,N′-diethyl-N,N′-ditolyl-2,9-diamide-1,10-phenanthroline(Et-TolDAPhen),initially reported by us,exhibits excellent selectivity towards actinides(U,Th,Am,Pu)over lanthanides and thus can be potentially applied in the group actinide extraction(GANEX)process for the group separation of *** this article,by tailoring the lengths of alkyl chains,we synthesized other four DAPhen ligands with different substitute groups in the diamide moieties,and characterized the relationship between properties and substitute groups of DAPhen *** extraction results show that three of the ligands exhibit high performance in UO_2^(2+)extraction from an acidic solution and the extracted UO_2^(2+)can be easily stripped by only using ultrapure *** titration confirms that UO_2^(2+)combined with all the four ligands in 1:1 *** extended X-ray absorption finestructure(EXAFS)study shows that six donor atoms comprise the first equatorial shell of the UO_2^(2+)ions bonded by the DAPhen ligands,among which two nitrogen and two oxygen atoms are from the DAPhen ligand,while other two oxygen atoms are from one nitrate *** article promises to provide basic data for assessing the feasibility of this kind of DAPhen ligands applied in actinides separation from nuclear wastes.

关键词： 2,9-diamide-1,10-phenanthroline UO2^2+ extraction UV-Vis titration EXAFS

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Probing the interaction at nano-bio interface using synchrotron radiation-based analytical techniques

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Science China Chemistry 2015年第5期58卷 768-779页

作者： Bing Wang Weiyue Feng zhifang chai Yuliang Zhao CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety CAS Key Laboratory of Nuclear Radiation and Nuclear Energy Technology Institute of High Energy Physics Chinese Academy of Sciences

Understanding the interactions of nanomaterials(NMs) with biomolecules, organelles, cells, and organic tissues at the nano-bio interface can offer important information for their uptake, distribution, translocation, metabolism and degradation in vitro and in vivo, which can help to precisely tune and design "smart" NMs for biomedical applications. However, probing the interactions at the nano-bio interface, which generally requires dedicated analytical methods and tools, is remarkably complicated due to the dynamically changed nature of the nano-bio interface. Because of the advantages of high spatial resolution, high sensitivity, excellent accuracy, low matrix effects and non-destructiveness, synchrotron radiation(SR)-based analytical techniques have become extremely valuable tools. Herein, we present a comprehensive overview of SR-based techniques for the visualized study of NMs at cellular and subcellular interfaces and their transformation in vitro; the exploration of biodistribution, translocation, metabolism and degradation of NMs in vivo; and clarification of the molecular mechanisms of NMs' reactions with biomolecules. Rapid development of advanced light source means that in situ, real-time analysis of NMs at the nano-bio interface will be achieved.

关键词： nano-bio interface synchrotron-radiation-based analytical techniques interaction

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Heterostructure engineering of MoS_(2)/Mo_(2)CT_(x) nanoarray via molten salt synthesis for enhanced hydrogen evolution reaction

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Journal of Materiomics 2023年第6期9卷 1122-1128页

作者： Yanze Wu Lin Wang zhifang chai Weiqun Shi Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing100049China

Two-dimensional layered transition metal carbides(MXenes),have huge potential advantage for applications in hydrogen evolution reaction(HER).However,the hindered hydrogen evolution at large current densities and the instability of MXenes during HER remains major ***,we report the MoS_(2)/Mo_(2)CT_(x) nanoarray with aerophobic structure via molten salt *** situ vertical distribution of MoS_(2)nanoarray on the surface of Mo_(2)CT_(x) accelerates hydrogen gas release from the electrode,exhibiting significantly enhanced catalytic activity and stability to bare MoS_(2)and Mo_(2)CT_(x).The MoS_(2)/Mo_(2)CT_(x) nanoarray possesses excellent stability at100 mA/cm^(2)for 100 h with only 3%overpotential *** work provides guidance for developing high-stability MXene-based catalysts by virtue of in situ bonding between nanoarray and MXene.

关键词： Molten salt Aerophobic structure Nanoarray Hydrogen evolution reaction

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Applications of radiotracer techniques for the pharmacology and toxicology studies of nanomaterials

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Chinese Science Bulletin 2009年第2期54卷 173-182页

作者： ZHANG ZhiYong ZHAO YuLiang chai zhifang Key Laboratory of Nuclear Analytical Techniques and Laboratory for Biological Effects of Nanomaterials and Nanosafety Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China

With the rapid development of nanosciences and nanotechnology, a wide variety of manufactured nanomaterials are now used in commodities, pharmaceutics, cosmetics, biomedical products, and industries. While nanomaterials possess more novel and unique physicochemical properties than bulk materials, they also have an unpredictable impact on human health. In the pharmacology and toxicology studies of nanomaterials, it is essential to know the basic behavior in vivo, i.e. absorption, distribution, metabolism, and excretion (ADME) of these newly designed materials. Radiotracer techniques are especially well suited to such studies and have got the chance to demonstrate their enchantment. In this paper, radiolabeling methods for carbon nanomaterials, metallic and metal oxide nanoparticles, etc. are summarized and the applications of the radiolabeled nanomaterials in pharmacology and toxicology studies are outlined.

关键词：放射性示踪剂毒物学药理学数量分析

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