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Chinese Chemical Letters 2024年第3期35卷 532-537页

作者： Meng-Juan Wang Bo Li Yong-Li Wei Shu-Na Zhao Shuang-Quan Zang henan Key Laboratory of crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China College of Chemistry and Pharmaceutical Engineering Nanyang Normal UniversityNanyang 473061China

It remains a big challenge to develop solid-state stimuli-responsive materials for time-dependent information encryption and inkless erasable printing with long retention ***,a 2D Cu_(2)I_(2)-based MOF with photoresponsive spiropyran(SP)groups orderly installed on its skeleton is *** structural isomerization from SP to colored merocyanine(MC)form can be triggered by removing the Ch_(3)CN ***,the degree of structural isomerization and the retention time can be adjusted by controlling the amount of Ch_(3)CN guests,exhibiting dynamic photochromic behavior with multicolor states and tunable retention *** on these advantages,time-dependent information encryption is successfully ***,the long retention time(>72 h)of the MC form under daylight conditions in the Ch_(3)CN-removed Cu_(2)I_(2)-based MOF and good repeatability make it promising in various applications,such as temporary calendars,price-cards,billboards,and reusable identity *** work provides a novel design strategy to fabricate multi-functional MOF-based smart materials for challenging applications of time-dependent information encryption and inkless erasable printing.

关键词： Stimuli-responsive materials Spiropyran Solid-state photochromism Time-dependent encryption Inkless erasable printing

Doping-driven dual heterogeneous interfacial structures boosting the durability of industry-compatible water splitting at high current density

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Science China Chemistry 2024年第10期67卷 3468-3481页

作者： Chunming Yang Lihai Zhou Zhijie Kong Xiang Li Wangchuan Zhu Guangqing Wang Yanzhong Zhen Feng Fu Yucang Liang Research Institute of Comprehensive Energy Industry Technology College of Chemistry & Chemical EngineeringYan'an University henan Key Laboratory of crystalline Molecular Functional Materials Green Catalysis CenterCollege of ChemistryZhengzhou University Institut für Anorganische Chemie Eberhard Karls Universit?t

Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm-2) in an anion-exchange membrane water electrolyzer（AEMWE） is an enormous challenge for water ***,based on the results of density function theory calculations,a dual heterogeneous interfacial structured NiSe/Fe-Ni（Oh）2catalyst was subtly designed and successfully prepared by electrodepositing Fe-doped Ni（Oh）2on NiSe-loaded nickel foam（NF）.Fe doping-driven heterogeneous structures in NiSe/Fe-Ni（Oh）2markedly boost catalytic activity and durability at industrially compatible current densities in single hydrogen and oxygen evolution reactions under alkaline *** particular,NiSe/Fe-Ni（Oh）2shows a negligible performance loss at 600 mA cm-2at least 1,000 h for overall water splitting,a distinguished long-term durability acting as AEMWE electrodes at 600 mA cm-2and 1 A cm-2at 85℃ for at least 95 *** to Fe doping-induced strong synergetic effect between Ni and Fe,dual heterostructure-promoted charge transfer and redistribution,abundant catalytic active sites,and improvement of stability and durability,a mechanism of Fe doping-driven heterogeneous interfacial structurepromoted catalytic performance was *** study provides a successful example of theory-directed catalyst preparation and pioneers a creative strategy for industry-compatible water splitting at high current density.

关键词： doping-induced heterojunction structure NiSe/Fe-Ni(Oh)2 large current density anion-exchange membrane industry-compatible water electrolysis

hydrothermal synthesis of polyimide-linked covalent organic frameworks towards ultrafast and stable cathodic sodium storage

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Science China Chemistry 2024年第4期67卷 1300-1310页

作者： Xiya Yang Lei Gong Zhixin Liu Qianjun Zhi Baoqiu Yu Xin Chen Kang Wang Xiaofeng Li Dongdong Qi Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Redox-active organic materials are capturing growing attention as cathode materials for sustainable alkaline metal ion ***,the storage of Na+in most organic materials-based cathodes is plagued by low capacity and unsatisfying rate performance due to their low active site densities and limited exposed active ***,two polyimide-linked covalent organic frameworks(COFs),namely hATN-PD-COF and hATN-TAB-COF,were fabricated from hydrothermal synthesis with redoxactive triphenylene-2,3,6,7,10,11-hexacarboxylic acid and aromatic amines as starting *** X-ray diffraction and electron microscopy analysis indicate the high crystalline nature of these COFs with AA stacking configuration and orderly mesoporous tunnel.N_(2) sorption measurement discloses the permanent porosity of these two COFs with a Brunauer-EmmettTeller surface area of 1,065-1,200 m^(2)g^(-1)and a large pore size of 2.0-3.1 *** intermittent titration technique and density functional theory calculations reveal the facile Na+ion diffusion along the mesoporous tunnel of these COFs with a small energy barrier of 0.13-0.40 e *** particular,the as-prepared COFs based-cathodes show ultrafast and stable Na+storage associated with their conjugated electronic structure,highly ordered mesoporous tunnel,robust structure,and redox-active C=N/C=O-rich framework as exemplified by the high reversible capacity of 210 m A h g^(-1)at 200 m A g^(-1),record-high rate performance(195 m A h g^(-1)at a high current density of 10,000 m A g^(-1))among organic electrodes and the capacity retention of nearly 91%at 10,000 m A g^(-1)after 7,000 cycles for hATN-PD-COF.

关键词： covalent organic framework sodium ion battery cathode high rate organic electrode

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Technology for the next gravitational wave detectors

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Science China(Physics,Mechanics & Astronomy) 2015年第12期58卷 65-90页

作者： MITROFANOV Valery P. ChAO Shiuh PAN huang-Wei KUO Ling-Chi COLE Garrett DEGALLAIX Jerome WILLKE Benno Faculty of Physics Moscow State University Institute of Photonics Technologies "National" Tsing Hua University crystalline mirror solutions LLC crystalline mirror solutions gmb h Seestadtstr Vienna Center for Quantum Science and Technology(VCQ) Faculty of Physics University of Vienna Laboratoire des Mat'eriaux Avanc'es 7 Avenue Pierre de Coubertin Max Planck Institute for Gravitational Physics(Albert Einstein Institute) and Leibniz Universitt hannover

This paper reviews some of the key enabling technologies for advanced and future laser interferometer gravitational wave detectors, which must combine test masses with the lowest possible optical and acoustic losses, with high stability lasers and various techniques for suppressing noise. Sect. 1 of this paper presents a review of the acoustic properties of test masses. Sect. 2 reviews the technology of the amorphous dielectric coatings which are currently universally used for the mirrors in advanced laser interferometers, but for which lower acoustic loss would be very advantageous. In sect. 3 a new generation of crystalline optical coatings that offer a substantial reduction in thermal noise is reviewed. The optical properties of test masses are reviewed in sect. 4, with special focus on the properties of silicon, an important candidate material for future detectors. Sect. 5 of this paper presents the very low noise, high stability laser technology that underpins all advanced and next generation laser interferometers.

关键词： gravitational waves advanced techniques thermal noise coating laser

高效光催化二氧化碳还原钻单原子催化剂的多尺度结构工程

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Science China Materials 2024年第4期67卷 1292-1300页

作者：王榆惠郑天宇金昱丞孙婷婷丁旭王萧徐清梅李彤轩张少龙姜建壮 Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China

人工光合作用将二氧化碳转化为增值化学品和燃料,在克服全球环境能源危机方面具有巨大潜力.然而,由于CO_(2)的热力学稳定性和动力学滞后性,开发高效的CO_(2)RR光催化剂是一个巨大的挑战.本文在微介孔氮掺杂碳(0.8-Co-ISAS/MMNC-900)上... 详细信息

人工光合作用将二氧化碳转化为增值化学品和燃料,在克服全球环境能源危机方面具有巨大潜力.然而,由于CO_(2)的热力学稳定性和动力学滞后性,开发高效的CO_(2)RR光催化剂是一个巨大的挑战.本文在微介孔氮掺杂碳(0.8-Co-ISAS/MMNC-900)上制备了一种具有高度分散Co单原子位的分级多孔钴单原子光催化剂,该催化剂显著促进了CO_(2)-to-CO的光还原.0.8-Co-ISAS/MMNC-900催化剂的CO生成速率高达7261μmol g^(-1)h^(-1),CO选择性高达90.1%,并且在四次循环测试中表现出良好的稳定性.实验数据和理论结果表明,分层多孔结构可以促进电荷分离引起的外部局部电场的形成,Co隔离的单原子位和微介孔构型协同作用,促进光激发电子积累、CO_(2)吸附活化和*COOh中间体的形成.本研究通过多尺度多孔结构工程,提出了一种合成CO_(2)还原光催化剂的新策略.

关键词：单原子热力学稳定性激发电子光还原多尺度结构人工光合作用多孔结构电荷分离

heterogeneous Catalysis with Metal-Containing crystalline Porous Materials:Element-and Site-Specific Insights

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CCS Chemistry 2024年第5期6卷 1110-1129页

作者： Yan Li Andrew G.Walsh Peng Zhang Tianjun Zhang State Key Laboratory of New Pharmaceutical Preparations and Excipients College of Chemistry and Materials ScienceHebei UniversityBaoding 071002 Department of Chemistry Dalhousie UniversityHalifaxNova Scotia B3H 4R2

Metal-containing crystalline porous materials(CPMs)are gaining popularity in heterogeneous catalysis because of their highly crystalline and porous systems,and their excellent chemical *** of the metal species and framework structure permits them to have greater activity,selectivity,and stability over other *** in-depth understanding of the complex nature of metal active sites in CPMs is essential for revealing the structure-performance relationships and directing the rational design of such *** to conventional characterization techniques,the rapid development of X-ray absorption spectroscopy(XAS)has provided element-and site-specific deep insights into the electronic and structural information of metal species in *** such,this review begins by summarizing novel XAS techniques and analysis methods in accurately obtaining such ***,the combination of XAS with other high-level characterization methods into disclosing the configuration of active sites in metalcontaining CPMs is ***,the utilization of theory-assisted XAS data analysis in examining complex metal-containing CPM catalysts is ***,advanced in-situ/operando XAS studies into revealing the working sites in metal-containing CPMs under catalytic conditions are *** conclude by outlining the future challenges and prospects of XAS measurements,data analyses,and in-situ/operando setups in advancing the study of metal-in-CPM catalysts.

关键词： X-ray absorption spectroscopy in-situ metal species crystalline porous materials heterogeneous catalysis

Uniform zinc deposition on O,N-dual functionalized carbon cloth current collector

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Journal of Energy Chemistry 2022年第6期31卷 76-83,I0003页

作者： Mengqi Zhou Guoqiang Sun Shuang-Quan Zang henan Key Laboratory of crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis CenterCollege of ChemistryZhengzhou UniversityZhengzhou 450001HenanChina

The society’s urgent demand for environmentally friendly, safe and low-cost energy storage devices has promoted the research of aqueous zinc-ion batteries. however, the uneven deposition of Zn ions on anodes will lead to the growth of the dendrite and reduce the Coulombic efficiency as well as the lifespan of the devices. herein, we construct an O,N-dual functionalized carbon cloth current collector via a simple hydrothermal strategy, in which the oxygen-containing functional groups and the N heteroatoms can regulate the transmission and deposition of Zn ions, respectively. The proposed synergistic strategy ensures the uniform distribution of Zn ions on the surface of the Zn anode and inhibits the formation of dendrites. The symmetric cell based on the O,N-dual doped carbon cloth presents superior cycling stability(318 h) with a low voltage hysteresis(11.2 mV) at an areal capacity of 1 m Ah cm^(-2)(20% depth of diacharge). Meanwhile, the appreciably low overpotential(16 m V) and high Columbic efficiency(98.2%)also demonstrate that the O,N-dual functionalized carbon cloth can be worked as a promising host for Zn ions deposition.

关键词： O N-dual functionalized carbon cloth Synergistic strategy Long cycle life Low overpotential Dendrite-free Zn anode

Two-dimensional conjugated N-rich covalent organic frameworks for superior sodium storage

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Science China Chemistry 2022年第7期65卷 1291-1298页

作者： Xiya Yang Yucheng Jin Baoqiu Yu Lei Gong Wenbo Liu Xiaolin Liu Xin Chen Kang Wang Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and TechnologyBeijing 100083China

Sodium-ion batteries(SIBs) are considered as a promising next-generation energy storage system. To achieve the large-scale application of SIBs, it is crucial to develop cost-effective anode materials with high Na-ion storage capacity. herein twodimensional(2D) conjugated covalent organic frameworks(c COFs) with N-rich phthalocyanine(Pc) units fused via benzene moieties(named MPc-2D-c COFs) were explored as the SIBs anode materials. Electrochemical tests reveal their high reversible capacities of 538 and 342 m A h g^(-1) at 50 and 1000 m A g^(-1), respectively, good rate performance, and excellent stability,comparable to the state-of-the-art anode materials of SIBs, indicating their outstanding Na-ion storage performance. Ex situ Xray photoelectron and Fourier transform infrared spectroscopies together with theoretical calculations disclose the N atoms at the pore channels and conjugated pyrrole moieties of MPc-2D-c COFs provide abundant Na-ion storage sites. This, in cooperation with the enhanced electrical conductivity owing to the 2D conjugated structure, contributes to the outstanding Na-ion storage capacity of MPc-2D-c COFs. The present result is surely helpful for developing high-performance and cost-effective COFs as electroactive materials for SIBs.

关键词： covalent organic frameworks sodium-ion batteries phthalocyanine anode materials π-conjugated 2D COFs

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一种原位还原策略用于构筑无枝晶锌负极

Science China Materials 2023年第5期66卷 1757-1766页

作者：周梦奇吴周王锐孙国强臧双全 henan Key Laboratory of crystalline Molecular Functional Materials Green Catalysis CenterCollege of ChemistryZhengzhou UniversityZhengzhou 450001China

结合了三维结构和亲锌物种的集流体构筑策略被认为是构建高稳定锌金属负极的有效方法.然而,高昂的成本和复杂的制备工艺阻碍了其实际应用.本文通过在有均匀Cu^(2+)锚定的碳布集流体(ACC-600@Cu^(2+))上沉积锌,合理设计了一种稳定的三维... 详细信息

结合了三维结构和亲锌物种的集流体构筑策略被认为是构建高稳定锌金属负极的有效方法.然而,高昂的成本和复杂的制备工艺阻碍了其实际应用.本文通过在有均匀Cu^(2+)锚定的碳布集流体(ACC-600@Cu^(2+))上沉积锌,合理设计了一种稳定的三维锌金属复合阳极(Zn@ACC-600@Cu^(2+)).在锌成核过程中,Cu^(2+)原位还原为金属Cu,然后随着锌的进一步沉积,碳布表面逐渐形成均匀的亲锌的Cu-Zn合金界面层.密度泛函理论计算和实验观察表明,Cu-Zn合金界面不仅可以作为锌离子的亲锌沉积点,而且可以提高导电率,使电场和锌离子通量均匀化.因此,ACC-600@Cu^(2+)集流体可以实现高的镀锌/剥离可逆性,并在15.8 mV的极化电压下稳定循环410 h以上.作为概念验证,我们组装的Zn@ACC-600@Cu^(2+)‖MnO_(2)全电池具有良好的电池倍率性能,与原始碳布相比,其比容量显著提高至110 mA h g^(-1).本文提出的原位还原策略为三维锌金属复合负极的设计提供了一种简便且低成本的方法,促进了无枝晶和高稳定锌金属电池的发展.

关键词： in situ reduction strategy zincophilic species 3D composite Zn anode Cu-Zn alloy

Role of the surface chemistry of activated carbons in dye removal from aqueous solution

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International Journal of Minerals,Metallurgy and Materials 2015年第7期22卷 770-776页

作者： hua-lei Zhou Wen-juan Zhen Qian Zhu Xiao-bin Wu Zhi-dong Chang Wen-jun Li Beijing Key Laboratory for Science and Application of Functional Molecular and crystalline Materials School of Chemistry and Biological Engineering University of Science and Technology Beijing

Commercial activated carbons were modified by a series of chemical or physical treatments using h202, Nh3, and heating under N2 flow without notably changing their pore structures. The resultant carbons were characterized by N2 adsorption and Bohem titration and then used to remove Ponceau 4R, methyl orange and brilliant blue from aqueous solutions. Surface chemistry was found to play a signifi- cantly different role in removing these three compounds. The removal of anionic Ponceau 4R increases with increasing carbon surface ba- sicity due to the predominant dispersive interaction mechanism. In contrast, surface chemistry has little effect on the removal of anionic methyl orange, which can be explained by two parallel mechanisms involving electrostatic and dispersive interactions due to the basic amine group in a dye molecule. The influence of surface chemistry on the removal of amphoteric brilliant blue dye can also be ignored due to a weak interaction between the carbons and dye molecules, which is resulted from strong cohesive energy from electrostatic forces inside amphoteric dye molecules.

关键词： activated carbon decolorization dyes modification surface chemistry