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Design of bifunctional single-atom catalysts NiSA/ZIF-300 for CO_(2) conversion by ligand regulation strategy

Nano Research 2024年第5期17卷 3827-3834页

作者： Wengang Fu Yapei Yun Hongting Sheng Xiaokang Liu Tao Ding Shuxian Hu Tao Yao Binghui Ge Yuanxin Du Didier Astruc Manzhou Zhu Department of Chemistry and Centre for Atomic Engineering of Advanced Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationCollege of Materials Science and EngineeringInstitutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefei 230601China Universitéde Bordeaux ISMUMR CNRS N°5255351 Cours de La Libération33405 Talence CedexFrance National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026China Department of Physics University of Science and Technology BeijingBeijing 100083China Anhui Tongyuan Environment Energy Saving Co. LtdHefei 230041China

Carbon-supported noble-metal-free single-atom catalysts(SACs)have aroused widespread interest due to their green chemistry aspects and excellent ***,we propose a“ligand regulation strategy”and achieve the successful fabrication of bifunctional SAC/MOF(MOF=metal-organic framework)nanocomposite(abbreviated NiSA/ZIF-300;ZIF=ZIF-8)with exceptional catalytic performance and *** designed NiSA/ZIF-300 has a planar interfacial structure with the Ni atom,involving one S and three N atoms bonded to Ni(Ⅱ),fabricated by controllable pyrolysis of volatile Ni-S *** CO_(2) cycloaddition to styrene epoxide,NiSA/ZIF-300 exhibits ultrahigh activity(turnover number(TON)=1.18×105;turnover frequency(TOF)=9830 molSC·mol_(Ni)^(-1)·h^(-1);SC=styrene carbonate)and durability at 70℃ under 1 atm CO_(2) pressure,which is much superior to Ni complex/ZIF,NiNP/ZIF-300,and most reported *** study offers a simple method of bifunctional SAC/MOF nanocomposite fabrication and usage,and provides guidance for the precise design of additional original SACs with unique catalytic properties.

关键词： single atom catalyst bifunctional CO_(2)conversion cycloaddition

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Symmetry breaking of highly symmetrical nanoclusters for triggering highly optical activity

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Fundamental Research 2024年第1期4卷 63-68页

作者： Xiao Wei Hao Li Honglei Shen Chuanjun Zhou Shuxin Wang Xi Kang Manzhou Zhu Department of Chemistry and Centre for Atomic Engineering of Advanced Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials.Anhui UniversityHefei 230601China

Developing new approaches to fulfill the enantioseparation of nanocluster racemates and construct cluster-based nanomaterials with optical activity remains highly desired in cluster science,because it is an essential prerequisite for fundamental research and extensive applications of these *** herein propose a strategy termed“active-site exposing and partly re-protecting”to trigger the symmetry breaking of highly symmetrical nanoclusters and to render cluster crystals optically *** vertex PPh_(3)of the symmetrical Ag_(29)(SSR)_(12)(PPh_(3))_(4)(SSR=1,3-benzenedithiol)nanocluster was firstly dissociated in the presence of counterions with large steric hindrance,and then the exposed Ag active sites of the obtained Ag_(29)(SSR)_(12)nanocluster were partly re-protected by Ag^(+),yielding an Ag_(29)(SSR)_(12)-Ag_(2)nanocluster with a symmetry-breaking ***_(29)(SSR)_(12)-Ag_(2)followed a chiral crystallization mode,and its crystal displayed strong optical activity,derived from CD and CPL ***,this work presents a new approach(i.e.,active-site exposing and partly re-protecting)for the symmetry breaking of highly symmetrical nanoclusters,the enantioseparation of nanocluster racemates,and the achievement of highly optical activity.

关键词： Atomically precise nanocluster Symmetry breaking Enantioseparation Circularly polarized luminescent Photoluminescence

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Stacking effects on magnetic, vibrational, and optical properties of CrSBr bilayers

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Physical Review B 2025年第12期111卷 125411-125411页

作者： Huicong Li Yali Yang Zhonghao Xia Yateng Wang Jiacheng Wei Beijing Key Laboratory for Magneto-Photoelectrical Composite and Interface Science The State Key Laboratory for Advanced Metals and Materials School of Mathematics and Physics University of Science and Technology Beijing Beijing 100083 China

Layer stacking presents a promising avenue for manipulating the physical properties of two-dimensional materials. The van der Waals layered semiconductor CrSBr, which exhibits A-type antiferromagnetism and a relatively high Néel temperature, has been successfully exfoliated into atomically thin sheets. In this paper, we investigate the structural, lattice dynamical, electronic, magnetic, and optical properties of four distinct stacking structures of CrSBr bilayers using first-principles calculations and Monte Carlo simulations. Our findings show that, though the most energetically favorable bilayer structure retains the stacking pattern of the bulk counterpart, three other high-symmetry stacking structures can be achieved by sliding one of the layers along three distinct directions, with energy cost comparable to that observed in MoS2 bilayer. All these four bilayers exhibit semiconductor behavior with A-type antiferromagnetic ordering, similar to the bulk material, and demonstrate closely aligned Néel temperatures. Moreover, these bilayers exhibit relatively low lattice thermal conductivities, pronounced anisotropy, and a strong dependence on stacking patterns. This behavior is attributed to significant phonon-phonon scattering arising from avoided crossings between acoustic and optical phonons, as well as the presence of flat optical phonon bands in the low-frequency region. While the electronic structures and optical properties of these bilayers show weak dependence on the stacking pattern for antiferromagnetic ordering, they undergo significant changes for ferromagnetic ordering, influencing the band gap, valence and conduction band splitting, and effective mass. Furthermore, we found that antiferromagnetic ordering can transition to ferromagnetic under intense light illumination. Thus, the integration of layer stacking and light illumination offers an effective means to control the heat transfer, magnetic, and optical properties of CrSBr bilayers.

关键词： Layered semiconductors

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Interfacial behavior of a thermoelectric film bonded to a graded substrate

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Applied Mathematics and Mechanics(English Edition) 2023年第11期44卷 1853-1870页

作者： Juan PENG Dengke LI Zaixing HUANG Guangjian PENG Peijian CHEN Shaohua CHEN School of Materials Science and Physics State Key Laboratory for Geomechanics and Deep Underground EngineeringSchool of Mechanics and Civil EngineeringChina University of Mining and TechnologyXuzhou 221116Jiangsu ProvinceChina State Key Laboratory of Mechanics and Control of Mechanical Structures Nanjing University of Aeronautics and AstronauticsNanjing 210016China College of Mechanical Engineering Zhejiang University of TechnologyHangzhou 310014China State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Institute of Advanced Structure Technology Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Lightweight Multi-functional Composite Materials and Structures Beijing Institute of TechnologyBeijing 100081China Collaborative Innovation Center of Electric Vehicles in Beijing Beijing Institute of TechnologyBeijing 100081China

To improve the thermoelectric converting performance in applications such as power generation,reutilization of heat energy,refrigeration,and ultrasensitive sensors in scramjet engines,a thermoelectric film/substrate system is widely designed and applied,whose interfacial behavior dominates the strength and service life of thermoelectric ***,a theoretical model of a thermoelectric film bonded to a graded substrate is *** interfacial shear stress,the normal stress in the thermoelectric film,and the stress intensity factors affected by various material and geometric parameters are comprehensively *** is found that adjusting the inhomogeneity parameter of the graded substrate,thermal conductivity,and current density of the thermoelectric film can reduce the risk of interfacial failure of the thermoelectric film/graded substrate *** a stiffer and thicker thermoelectric film is advantageous to the reliability of the thermoelectric film/graded substrate *** results should be of great guiding significance for the present and upcoming applications of thermoelectric materials in various fields.

关键词： thermoelectric film graded substrate interfacial behavior singular integral equation shear stress intensity factor

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Trimeric carbazole phosphonic acid hole-transporting molecules with robust processability enhance the efficiency of organic solar cells to 20%

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science China Chemistry 2025年

作者： Tianqi Chen Yunxin Zhang Wenkai Zhao Yanyi Zhong Wanying Feng Baofa Lan Xuehang Dong Jingwen Yang Jiangbin Zhang Kai Han Guankui Long Bin Kan Yongsheng Chen School of Materials Science and Engineering National Institute for Advanced Materials Nankai University State Key Laboratory and Institute of Elemento-Organic Chemistry Frontiers Science Center for New Organic Matter The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials Renewable Energy Conversion and Storage Center(RECAST) College of Chemistry Nankai University College of Advanced Interdisciplinary Studies National University of Defense Technology Nanhu Laser Laboratory National University of Defense Technology Hunan Provincial Key Laboratory of High Energy Laser Technology National University of Defense Technology

Carbazole-based self-assembled molecules have been widely adopted as hole-transporting layers（HTLs） in high-performance organic solar cells（OSCs）. However, their practical implementation has been constrained by their limited concentration in solutions and poor solvent tolerance. Herein, to address these limitations, we designed two novel trimeric molecules（TPACz-1and TPACz-2） that synergistically integrate the structural merits of small molecules with the processing advantages of ***, TPACz-2 showed exceptional hole-transporting capacity with uniform coverage on indium tin oxide（ITO） substrates,coupled with robust processability characterized by an extended concentration tolerance range(0.2–1.0 mg mL-1) and compatibility with a broad range of solvents. Binary OSCs based on TPACz-2 showed an excellent power conversion efficiency（PCE） of 19.65% with a short-circuit current density of 27.49 mA cm-2and a fill factor of 80.9%. At the same time, the corresponding ternary devices exhibited a high PCE exceeding 20%. Furthermore, the TPACz-based devices demonstrated superior ambient stability, retaining ～80% of their initial PCE after 680 h at 25% relative humidity, substantially outperforming conventional PEDOT:PSS-based counterparts. This work offers valuable guidance and highlights the crucial role of oligomeric molecular design as a pivotal strategy for the development of innovative HTLs in OSCs.

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Exploring the Multi-Scale Evolution Mechanism of the Ultra-High-Temperature Mechanical Behaviour of Carbon/Carbon composites

SSRN

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SSRN 2024年

作者： Song, Lichao Meng, Songhe Zhang, Ying Yang, Fan Xie, Weihua National Key Laboratory of Science and Technology on Advanced Composites in Special Environments Harbin Institute of Technology Harbin150080 China Key Laboratory of Advanced Functional Composite Materials Aerospace Research Institute of Materials & Processing Technology Beijing100076 China

The microstructure and mechanical properties of Carbon/Carbon (C/C) composites were investigated after ultra-high-temperature heat treatment (HTT) in the range of 30 – 2950 °C. The effect mechanism of high temperatures on the mechanical behaviour of C/C composites was proposed for three scales, i.e., graphene sheets, carbon fibre (CF) monofilaments, and C/C composites. The results displayed that the tensile strength of CF monofilaments decreases monotonically as the HTT increases in the range of 2000 – 2950 °C, while C/C composites present a tendency to decrease and then increase, demonstrating that CF/matrix interfacial properties play a decisive role in the tensile properties. The compression and flexural properties showed a trend opposite to the tensile properties, Young’s modulus of both CF monofilaments and C/C composites increases. A turning point in the microstructure of C/C composites was observed after HTT at 2700 °C, in which the graphitisation degree decreases and the size of graphene sheets becomes fluctuating, while the high-temperature mechanical properties began to be superior to room temperature (RT). The high-temperature mechanical properties of C/C composites were regulated by the competing mechanisms of the graphite crystallite structure and the skin-core structure of CF monofilament, the CF/matrix interfacial strength and the porosity of C/C composites. © 2024, The Authors. All rights reserved.

关键词： Carbon fibers

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Construction of ZnO@CDs@Co_(3)O_(4) sandwich heterostructure with multi-interfacial electron-transfer toward enhanced photocatalytic CO_(2) reduction

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Chinese Chemical Letters 2024年第4期35卷 147-152页

作者： Xiuzheng Deng Yi Ke Jiawen Ding Yingtang Zhou Hui Huang Qian Liang Zhenhui Kang Advanced Catalysis and Green Manufacturing Collaborative Innovation Center CNPC-CZU Innovation AllianceSchool of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316004China

Photocatalytic conversion of CO_(2) into small-molecule chemical feedstocks can meet the growing demand for energy and alleviate the global warming. Herein, a p-n ZnO@CDs@Co_(3)O_(4) heterojunction with sandwich structure was constructed by calcination method of self-assembled ZIF-8@CDs@ZIF-67. The ZnO@CDs@Co_(3)O_(4) with well-defined interfacial structure exhibited the significantly enhanced photocatalytic CO_(2) reduction activity, and the optimal catalyst indicated the(CO + CH_(4)) evolution rate of 214.53μmol g^(-1)h^(-1) under simulated solar light, which was superior to ZnO, Co_(3)O_(4) and binary ZnO@Co_(3)O_(4).The internal cavity, exposed active sites, multiple interfaces and constructed p-n heterojunction can facilitate the light harvesting and photoexcited electron transfer. Besides, after introduction of CDs placed in the middle layer between ZnO and Co_(3)O_(4), CDs with excellent photoelectric property further promoted charge separation and migration. This work represents an appealing strategy to construct well-defined photocatalysts for boosting CO_(2) photoreduction.

关键词： Metal-organic framework Photocatalytic CO_(2) reduction Carbon dots p-n heterojunction Sandwich heterostructure

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Secondary ligand engineering of nanoclusters:Effects on molecular structures,supramolecular aggregates,and optical properties

Aggregate

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Aggregate 2023年第1期4卷 277-284页

作者： Xiao Wei Ying Lv Honglei Shen Hao Li Xi Kang Haizhu Yu Manzhou Zhu Department of Chemistry and Centre for Atomic Engineering of Advanced Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefeiChina

Developing new templates to evaluate the ligand engineering effect in manipulating nanoclusters from both molecular and supramolecular aspects remains highly desired in cluster science because it allows for an in-depth understanding of structure-property *** herein presented the secondary ligand(i.e.,the phosphine ligand)engineering based on an Ag_(29) nanocluster template and its dual effects on intracluster structures and intercluster ***“dissociationcombination equilibrium”of phosphine ligands on the nanocluster surface was controlled by tailoring the C-H…πinteractions within the ligand shell,which led to the fabrication of a family of[Ag_(29)(BDT)_(12)(PR_(3))_(x)]^(3-)*** the molecular level,the dissociation of phosphine ligands contracted the nanocluster framework,while the overall configuration of[Ag_(29)(BDT)_(12)]^(3-)was *** the supramolecular level,the complete dissociation of phosphine ligands yielded a bare nanocluster,which followed a chiral crystallization mode,and its crystals displayed high optical activity,derived from circular dichroism and circularly polarized luminescence ***,this work presents the peripheral ligand effects in directionally controlling intracluster configurations and intercluster aggregations,which hopefully benefit future design and preparation of new nanoclusters or cluster-based nanomaterials with customized structures and performances.

关键词： precise nanocluster ligand engineering molecular structure supramolecular aggregate optical property

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Promoting effect of d-band center and in-situ precipitation strategy on sulfur evolution reaction

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Journal of Energy Chemistry 2025年第5期104卷 740-748页

作者： Jun Pu Yun Tan Jiasen Yin Zihan Shen Shoujie Liu Kai Zhang Lei Zhou Yagang Yao Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Provincial Engineering Laboratory for New-Energy Vehicle Battery Energy-Storage MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002AnhuiChina National Laboratory of Solid State Microstructures College of Engineering and Applied SciencesJiangsu Key Laboratory of Artificial Functional MaterialsCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093JiangsuChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Materials Science and Engineering Anhui UniversityHefei 230601AnhuiChina School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina Department of Electrical Engineering Eindhoven University of TechnologyEindhoven MB 5600the Netherlands

The slow conversion of polyphase in lithium-sulfur(Li-S)batteries not only intensifies the shuttle effect of lithium polysulfides(LiPSs),but also causes the continuous accumulation of inactive sulfur species,resulting in rapid capacity attenuation and sluggish dynamic ***,the promoting effect of atomic interface stress on sulfur reaction was investigated via CoFe-CoFe_(2)O_(4)heterogeneous nanosheets with a cavity *** strain force induced by the in-situ precipitation of Co Fe bimetallic alloy in oxide matrix increased the d-band center,which was conducive to the interaction between catalyst and Li *** sulfur cathode based on this two-dimensional(2D)nanosheet design showed an extremely high capacity of 751 mAh g^(-1)at 4 *** with a sulfur loading of 5.55 mg cm^(-2),its area capacity was still as high as 7.15 mAh cm^(-2).Meanwhile,the enhanced stability greatly improved the practical potential of Li-S batteries.

关键词： 2D nanosheets In-situ precipitation Strain effect D-band center Li-S batteries

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One-step synthesis of hierarchical Ni_(3)Se_(2)nanosheet-on-nanorods/Ni foam electrodes for hybrid supercapacitors

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Chinese Chemical Letters 2022年第1期33卷 475-479页

作者： Fangshuai Chen Yanan Chen Qing Han Liangti Qu Key Laboratory of Cluster Science Ministry of Education of China Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China The Key Laboratory of Organic Optoelectronics&Molecular Engineering of Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin 300072China

Transitional metal selenides have high conductivity,even metal quality,which makes them great for using as electrode materials for fabricating ***,hierarchical Ni_(3)Se_(2)nanosheet-on-nanorods on Ni foam(NSR-Ni_(3)Se_(2)/Ni)was fabricated by a facile three-dimensional(3D)substrate-assisted confinement assembly method,and used as a freestanding electrode material for hybrid supercapacitors(HSCs).In this design,metallic Ni_(3)Se_(2)with hybrid 1D/2D architecture could effectively enhance the active specific surface area of electrode and improve space utilization,as well as significantly facilitate electrons transport,while Ni foam served as the Ni source of Ni_(3)Se_(2)and provided 3D multi-electron transport channels,thus boosting the specific *** constructed hierarchical NSR-Ni_(3)Se_(2)electrode delivered a superior areal specific capacity of 1.068 mAh/cm^(2)(7.69 F/cm^(2))at 2 mA/cm^(2)and retained 68.2%of the initial capacity when the current density increases by 15 ***,the as-assembled NSR-Ni_(3)Se_(2)device exhibited an ultrahigh energy density of 56.4 Wh/kg and high power density of 4640.3 W/kg,and a capacity retention of 92.6%even after 6000 cycles.

关键词： Hybrid supercapacitors Hierarchical Ni_(3)Se_(2)nanosheet-on-nanorods Freestanding electrode Ni foam-assisted confinement assembly Microstructure

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