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Recent progress on photoactive nonprecious transition-metal complexes

Science China Chemistry 2025年第1期68卷 46-95页

作者： Zhong-Liang Gong Hong-Jie Zhang Yan Cheng Jianxun Liu Yuhan Ai Yaqin Li Zhihui Feng Qiong Zhang Shaolong Gong Yong Chen Chang-Jiang Yao Yuan-Yuan Zhu Liang-Jin Xu Yu-Wu Zhong CAS Key laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences State Key laboratory of Structural Cemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences School of Chemistry and Chemical Engineering Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of Technology State Key laboratory of Explosion Science and Safety Protection School of Mechatronical Engineering Beijing Institute of Technology College of Chemistry and Molecular Sciences Hubei Key Lab on Organic and Polymeric Optoelectronic Materials Wuhan University School of Chemistry and Chemical Engineering Anhui University Key laboratory of Photochemical Conversion and Optoelectronic Materials & CAS-HKU Joint laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Photoactive complexes of nonprecious transition metals, mainly including those in the first-row and partially the second-row of the Periodic table of elements, have received increasing attention in view of their low cost and long-term sustainability. They are recognized as promising alternatives to noble transition metal complex congeners that have been extensively studied in optoelectronic devices, artificial photosynthesis, photocatalysis, biodiagnostics, and therapeutics, etc. This review is devoted to a comprehensive summary on the classical and recent advances on photoactive nonprecious transition metal complexes, including photoactive Zr, V, Cr, Mo, and W complexes, Mn complexes and hybrids, Fe, Co, Ni, and Cu complexes, and Zn and Cd complexes and hybrids. A particular focus is given on the molecular design, modulation of photophysical and photochemical properties, and applications of the representative and lately-developed nonprecious metal complexes. In addition, a perspective on the future development in this field is provided at the end of this review.

关键词： photoactive metal complexes earth-abundant metals nonprecious metal complexes luminescence photochemistry

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Effects of CRAC Channel on Spatiotemporal Ca2＋ Patterns in T Cells

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Chinese Physics Letters 2010年第2期27卷 311-314页

作者：李丛鑫陈晓芳王鹏业王渭池 Chinese Acad Sci Inst Phys Beijing Natl Lab Condensed Matter Phys Lab Soft Matter Phys Beijing 100190 Peoples R China

A reaction-diffusion model is built to investigate the temporal and spatial patterns of cytoplasmic Ca2＋ dynamics under the effects of Ca2＋-release activated Ca2＋（CRAC） channels in T cells. Simulation results show a strong dependence of the modulation mode of Ca2＋ oscillation and dynamic patterns of Ca2＋ wave on the influx rate through the CRAC channel （ksoc）. When ksoc is small, cytoplasmic Ca2＋ is modulated as a frequency-modulation （FM） signal, whereas it shows an amplitude modulation （AM） mode after ksoc passes through a critical value. The heterogeneity in spatial Ca2＋ distribution is mostly arising from the influx through CRAC channels in both FM and AM modes. During each Ca2＋ spike, a more sustained cytoplasmic Ca2＋ gradient is maintained in the AM mode rather than in the FM mode.

关键词： Biological physics

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Intermetallic PdCd Core Promoting CO Tolerance of Pd Shell for Electrocatalytic Formic Acid Oxidation

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Chinese Journal of Chemistry 2022年第18期40卷 2161-2168页

作者： Ming-Xi Chen Yue Liu Tian-Wei Song Rui-Lin Wei Xiao-Dong Zhuang Yao-Yue Yang Hai-Wei Liang Hefei National Research Center for Physical Sciences at the Microscale Department of ChemistryUniversity of Science and Technology of ChinaHefeiAnhui230026 China Key laboratory of Fundamental Chemistry of the State Ethnic Commission School of Chemistry and EnvironmentSouthwest Minzu UniversityChengduSichuan610041 China the meso-entropy matter lab State Key Laboratory of Metal Matrix CompositesShanghai Key Laboratory of Electrical Insulation and Thermal AgingSchool of Chemistry and Chemical EngineeringFrontiers Science Center for Transformative MoleculesShanghai Jiao Tong University800 Dongchuan RDShanghai200240 China

Liquid fed fuel cells such as direct formic acid fuel cells(DFAFCs)are considered to be promising power sources for portable electronic ***,the poison of CO intermediates on the state-of-the-art platinum and palladium-based electrocatalysts for the formic acid oxidation reaction(FAOR)at the anode hampers the implementation of DFAFCs ***,we report a core/shell catalyst consisting of intermetallic PdCd core and Pd shell(i-PdCd@Pd)with promoted CO anti-poison ability and thus FAOR *** optimal i-PdCd@Pd catalyst exhibits a high mass activity and specific activity at peak potential,which are 24 and 4 times greater than that of commercial Pd/C catalyst,*** understand by in-situ surface-enhanced infrared absorption spectroscopy(ATR-SEIRA)and X-ray photoelectron spectroscopy(XPS)that in i-PdCd@Pd,the intermetallic PdCd under-layers can induce the downshift of d-band center of surface Pd atoms,which would improve the CO tolerance and thus promote the FAOR performance.

关键词： Electrochemistry Intermetallicphases PdCd Supported catalysts IR spectroscopy

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A Reproducible Approach of Preparing High-Quality Overdoped Bi_2Sr_2CaCu_2O_(8+δ) Single Crystals by Oxygen Annealing and Quenching Method

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Chinese Physics Letters 2016年第6期33卷 132-136页

作者：张玉晓赵林顾根大周兴江 National lab for Superconductivity Beijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of Sciences Condensed matter Physics and Materials Science Department Brookhaven National Laboratory Collaborative Innovation Center of Quantum matter

We report a reproducible approach in preparing high-quality overdoped Bi2 Sr2 CaCu2 08＋δ （Bi2212） single crystals by annealing Bi2212 crystals in high oxygen pressure followed by a fast quenching. In this way, high-quality overdoped and heavily overdoped Bi2212 single crystals are obtained by controlling the annealing oxygen pressure. We find that, beyond a limit of oxygen pressure that can achieve most heavily overdoped Bi2212 with a Tc N63 K, the annealed Bi2212 begins to decompose. This accounts for the existence of the hole-doping limit and thus the Tc limit in the heavily overdoped region of Bi2212 by the oxygen annealing process. These results provide a reliable way in preparing high-quality overdoped and heavily overdoped Bi2212 crystals that are important for studies of the physical properties, electronic structure and superconductivity mechanism of the cuprate superconductors.

关键词： Bi is it of A Reproducible Approach of Preparing High-Quality Overdoped Bi2Sr2CaCu2O Single Crystals by Oxygen Annealing and Quenching Method in high that by Sr

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Decrypting the Influence of Axial Coordination on the Electronic Microenvironment of Co-N_(5)Site for Enhanced Electrocatalytic Reaction

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CCS Chemistry 2023年第8期5卷 1876-1887页

作者： Bingyu Huang Senhe Huang Chenbao Lu Longbin Li Judan Chen Ting Hu Dirk Lützenkirchen-Hecht Kai Yuan Xiaodong Zhuang Yiwang Chen Institute of Polymers and Energy Chemistry(IPEC) College of Chemistry and Chemical EngineeringNanchang UniversityNanchang 330031 the meso-entropy matter lab School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240 School of Materials Science and Engineering Nanchang UniversityNanchang 330031 Faculty of Mathematics and Natural Sciences-Physics Department Bergische Universität WuppertalWuppertal D-42119 Institute of Advanced Scientific Research(iASR) Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022

Metal porphyrins are star molecules that possess welldefined coordination metal centers for versatile catalytic ***,most previous work has focused on the correlations between in-plane symmetric configuration of metal-N_(4)sites and their catalytic *** the catalytic contribution of additional axial coordination to such symmetric configuration remains a *** calculations revealed that axially anchoring an extra pyridine on the tetra-coordinated cobalt porphyrin(Co-N4)to construct penta-coordinated cobalt porphyrin(Co-N_(5))renders cobalt a higher electron density,thereby favoring the rate-determining O_(2)adsorption/activation and reducing the oxygen electroreduction ***,a well-defined Co-N_(5)site is rationally introduced into the azo-linked polymer framework for a fundamental structure-catalytic performance correlation ***-prepared Co-N_(5)catalyst exhibits a 26 mV positive shift in half-wave potential compared with the pyridine-free Co-N_(4)counterpart,discloses a markedly higher power density(141.4 mW cm^(−2)),and possesses better long-term durability(over 160 h cycles)in a Zn-air ***,such a Co-N_(5)catalyst also showcases potential applications for CO_(2)reduction with high CO_(2)-to-CO conversion faradic efficiency and better selectivity than the Co-N_(4)counterpart because coordination of the fifth pyridine evokes electronic localization that suppresses a competitive side *** work proves the positive electrocatalytic contribution of axial penta-coordination on well-defined metalporphyrin-based catalysts and offers atomic understanding of the structure-performance correlation on single atom catalysts for future catalyst design.

关键词： porphyrin axial coordination pentacoordination structureactivity correlation oxygen reduction reaction

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Diluted ferromagnetic semiconductor(LaCa)(ZnMn)SbO isostructural to “1111” type iron pnictide superconductors

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Science China(Physics,Mechanics & Astronomy) 2013年第11期56卷 2026-2030页

作者： HAN Wei ZHAO Kan WANG XianCheng LIU QingQing NING FanLong DENG Zheng LIU Ying ZHU JinLong DING Cui MAN HuiYuan JIN ChangQing National lab for Condensed matter Physics Institute of PhysicsChinese Academy of Sciences Department of Physics Zhejiang University

We report discovery of ferromagnetism in(LaCa)(ZnMn)SbO isostructural to the well-studied iron-based superconductor LaFeAs(O1 xFx).Spin is induced by partial substitution of Mn2+for Zn2+,while charge is induced by substitution of Ca2+for La3+within the parent compound *** with Curie temperature(TC)is observed up to 40 K at the spin doping 0.15 by introducing Mn2+into the Zn2+sites for(La0.95Ca0.05)(Zn1 xMnx)*** Hall coefficient measurement indicates p-type carrier for(La0.95Ca0.05)(Zn0.9Mn0.1)SbO with concentration of n^1020cm 3showing anomalous Hall effect below TC.

关键词： semiconductor "1111" type structure diluted magnetism

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Catalyst-Free Growth of Nanographene Films on Various Substrates

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Nano Research 2011年第3期4卷 315-321页

作者： Lianchang Zhang Zhiwen Shi Yi Wang Rong Yang Dongxia Shi Guangyu Zhang Nanoscale Physics and Device lab Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences Beijing 100190 China Surface Physics lab Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences Beijing 100190 China

We have developed a new method to grow uniform graphene films directly on various substrates, such as insulators, semiconductors, and even metals, without using any catalyst. The growth was carried out using a remote plasma enhancement chemical vapor deposition （r-PECVD） system at relatively low temperatures, enabling the deposition of graphene films up to 4-inch wafer scale. Scanning tunneling microscopy （STM） confirmed that the films are made up of nanocrystalline graphene particles of tens of nanometers in lateral size. The growth mechanism for the nanographene is analogous to that for diamond grown by PECVD methods, in spite of sp2 carbon atoms being formed in the case of graphene rather than sp3 carbon atoms as in diamond. This growth approach is simple, low-cost, and scalable, and might have potential applications in fields such as thin film resistors, gas sensors, electrode materials, and transparent conductive films.

关键词： Nanographene catalyst-free plasma enhancement chemical vapor deposition (PECVD) transparent and conductive film

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General Formulations of Finite-field Method Classifiedby Symmetry for Molecular Linear and Nonlinear Polarizabilities

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Chinese Journal of Structural Chemistry 2001年第5期20卷 369-380页

作者：陈锡华林晨升等 Chinese Acad Sci Fujian Inst Res Struct Matter State Key Lab Struct Chem Fujian 350002 Peoples R China

The formulations of the finite-field approach to calculate the linear and non-linear optical coefficients (i, (ij, (ijk and (ijkl of a molecular system with different symmetries have been deduced and summarized. The possible choices of the energy sets of the 48 frequent point groups have been optimized and categorized into 11 classes. With the restriction of symmetry operators, a minimum of 9, no more than 21 energy points have to be calculated in order to determine the coefficients, except in the case of the first class to which C1 point group belongs and in which the 34 non-relative energy points selected in our uniform and general scheme are all needed. The symmetric operators that cause some of the tensor components to vanish have been demonstrated as well.

关键词： nonlinear optical polarizability finite-field approach point group symmetry

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The Spatial Correlation between Crystalline and Amorphous Orientations of Isotactic Polypropylene during Plastic Deformation:An in situ Observation with FTIR Imaging

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Chinese Journal of Polymer Science 2015年第4期33卷 613-620页

作者： Wei Chen Xiang-yang Li Yan-ping Liu Jing Li Wei-ming Zhou 陈亮李良彬 National Synchrotron Radiation lab and College of Nuclear Science and Technology CAS Key Laboratory of Soft Matter ChemistryUniversity of Science and Technology of China

On the basis of research method in FTIR imaging, we made a heterogeneous thin film of isotactic polypropylene （iPP） that contains a few large spherulites （-150 μm） which are surrounded by small spherulites （-15 μm） for tensile testing. The evolution processes of crystalline and amorphous orientations of iPP are monitored with its characteristic peaks at 998 and 973 cm^-1, respectively. By introducing the correlation images, the analysis demonstrates the relationships between the orientation evolutions of crystalline and amorphous phases in a space of 250 μm × 250 μm detecting area. During the plastic deformation, crystalline orientation is higher than amorphous orientation outside the large spherulite, while that is opposite inside the region. In addition, the evolutions of crystalline and amorphous orientations almost keep a positive correlation.

关键词： lsotactic polypropylene FTIR imaging Deformation Orientation evolution.

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A Universal Equipment for Biaxial Stretching of Polymer Films

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Chinese Journal of Polymer Science 2015年第5期33卷 754-762页

作者： Ling-pu Meng Yuan-fei Lin Jia-li Xu Xiao-wei Chen Xue-yu Li Qian-lei Zhang Rui Zhang Nan Tian 李良彬 National Synchrotron Radiation lab and College of Nuclear Science and Technology CAS Key Laboratory of Soft Matter ChemistryUniversity of Science and Technology of China

A biaxial stretching equipment was designed and constructed to enable fundamental studies of the relationship between film processing conditions and structures of oriented film products. With programmable drive motors and scissorlike mechanism, all stretching modes, including uniaxial stretching with constant and free width, simultaneous and sequential biaxial stretching, can be applied to a square-shaped sheet. Parameters related to film stretching manufacturing, such as temperature, draw ratio and stretching speed can be set independently to meet the requirement of different polymers. The force information during stretching is recorded by two miniature tension sensors in two directions independently, which can monitor the mechanical stimulus and stress response. Using this equipment, experiments are conducted to investigate the influence of stretching parameters on the structure of polypropylene films, which provides an effective method to tailor the processing conditions to obtain the films with desired properties.

关键词： Biaxial stretching Processing/structure relationship Dynamics of stretching

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