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engineering the axial coordination of cobalt single atom catalysts for efficient photocatalytic hydrogen evolution

Nano Research 2024年第6期17卷 5114-5121页

作者： Ning Kang Lingwen Liao Xue Zhang Zhen He Binlu Yu Jiahong Wang Yongquan Qu Paul KChu Seeram Ramakrishna Xue-Feng Yu Xin Wang Licheng Bai Materials Interfaces Center Shenzhen Institute of Advanced TechnologyChinese Academy of Sciences(CAS)Shenzhen 518055China Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsChinese Academy of SciencesHefei 230031China Department of Chemistry City University of Hong KongKowloonHong Kong 999077China Hong Kong Branch of National Precious Metals Material engineering Research Center(NPMM) City University of Hong KongKowloonHong Kong 999077China Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Department of Physics and Department of Materials Science and engineering City University of Hong KongKowloonHong Kong 999077China National University of Singapore(NUS)Centre for Nanofibers and Nanotechnology Department of Mechanical EngineeringNational University of SingaporeSingapore 117542Singapore

Improving the catalytic activity of non-noble metal single atom catalysts(SACs)has attracted considerable attention in materials *** optimizing the local electronic structure of single atom can greatly improve their catalytic activity,it often involves in-plane modulation and requires high ***,we report a novel strategy to manipulate the local electronic structure of SACs via the modulation of axial Co-S bond anchored onto graphitic carbon nitride(C_(3)N_(4))at room temperature(RT).Each Co atom is bonded to four N atoms and one S atom(Co-(N,S)/C_(3)N_(4)).Owing to the greater electronegativity of S in the Co-S bond,the local electronic structure of the Co atoms is available to be controlled at a relatively moderate ***,when employed for the photocatalytic hydrogen evolution reaction,the adsorption energy of intermediate hydrogen(H*)on the Co atoms is remarkably *** the presence of the Co-(N,S)/C_(3)N_(4)SACs,the hydrogen evolution rates reach up to 10 mmol/(g·h),which is nearly 10 and 2.5 times greater than the rates in the presence of previously reported transition metal/C_(3)N_(4)and noble platinum nanoparticles(PtNPs)/C_(3)N_(4)catalysts,*** to the tailorable axial Co-S bond in the SAC,the local electronic structure of the Co atoms can be further optimized for other photocatalytic *** axial coordination engineering strategy is universal in catalyst designing and can be used for a variety of photocatalytic applications.

关键词： transition metal single-atom local electronic structure photocatalytic hydrogen evolution graphitic carbon nitride axial coordination environment

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engineering the coordination structure of Cu for enhanced photocatalytic production of C_(1)chemicals from glucose

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Chinese Journal of Catalysis 2024年第8期63卷 234-243页

作者： Lulu Sun Shiyang Liu Taifeng Liu Dongqiang Lei Nengchao Luo Feng Wang State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China National&Local Joint engineering Research Center for Applied Technology of Hybrid Nanomaterials Collaborative Innovation Center of Nano Functional Materials and Applications of Henan Province Henan UniversityKaifeng 475004HenanChina Institute of Electrical engineering Chinese Academy of SciencesBeijing 100190China

Photocatalytic decomposition of sugars is a promising way of providing H_(2),CO,and HCOOH as sus-tainable energy ***,the production of C_(1)chemicals requires the cleavage of robust C−C bonds in sugars with concurrent production of H_(2),which remains ***,the photo-catalytic activity for glucose decomposition to HCOOH,CO(C_(1)chemicals),and H_(2)on Cu/TiO_(2)was enhanced by nitrogen *** to nitrogen doping,atomically dispersed and stable Cu sites resistant to light irradiation are formed on Cu/TiO_(2).The electronic interaction between Cu and nitrogen ions originates valence band structure and defect levels composed of N 2p orbit,distinct from undoped Cu/TiO_(2).Therefore,the lifetime of charge carriers is prolonged,resulting in the pro-duction of C_(1)chemicals and H_(2)with productivities 1.7 and 2.1 folds that of Cu/TiO_(2).This work pro-vides a strategy to design coordinatively stable Cu ions for photocatalytic biomass conversion.

关键词： Cu photocatalyst coordination structure Biomass C−C bond C_(1)chemicals

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engineering coordination Environment of Cobalt Center in Molecular Catalysts for Improved Photocatalytic CO_(2) Reduction

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Chinese Journal of Chemistry 2023年第23期41卷 3305-3310页

作者： Yuchen Wang Jihong Zhang Wei Yang Weixue Tao Keying Tao Jihua Deng Wenjie Shi Dichang Zhong Tongbu Lu MOE International Joint Laboratory of Materials Microstructure Institute for New Energy Materials & Low Carbon Technologies School of Material Science & EngineeringTianjin University of TechnologyTianjin300384 China Guangdong Provincial Key Laboratory of Fuel Cell Technology GuangzhouGuangdong510641 China

The creation of effective and inexpensive catalysts is essential for photocatalytic CO_(2) *** molecular catalysts,possessing definite crystal structures,are desirable to study the relationship between catalytic performance and coordination microenvironment around catalytic *** this report,we elaborately developed three Co(II)-based molecular catalysts with different coordination microenvironments for CO_(2) reduction,named[CoN_(3)O]ClO_(4),[CoN_(4)]ClO_(4),and[CoN_(3)S]ClO_(4),*** optimal[CoN_(3)O]ClO_(4) photocatalyst has a maximum TON of 5652 in photocatalytic reduced CO_(2) reduction,which is 1.28 and 1.65 times greater than that of[CoN_(4)]ClO_(4) and[CoN_(3)S]ClO_(4),*** high electronegativity of oxygen in L1(N,N-bis(2-pyridylmethyl)-N-(2-hydroxybenzyl)amine)provides the Co(II)catalytic centers with low reduction potentials and a more stable*COOH intermediate,which facilitates the CO_(2)-to-CO conversion and accounts for the high photocatalytic activity of[CoN_(3)O]ClO_(4).This work provides researchers new insights in development of catalysts for photocatalytic CO_(2) reduction.

关键词： Co(II)-based homogeneous catalysts coordination microenvironment Photocatalysis CO_(2)reduction Homogenous catalysis

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engineering the coordination Sphere of Isolated Active Sites to Explore the Intrinsic Activity in Single-Atom Catalysts

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Nano-Micro Letters 2021年第9期13卷 136-163页

作者： Xin Wu Huabin Zhang Shouwei Zuo Juncai Dong Yang Li Jian Zhang Yu Han State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China KAUST Catalysis Center Physical Sciences and Engineering DivisionKing Abdullah University of Science and TechnologyThuwal 23955-6900Saudi Arabia Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049People’s Republic of China Advanced Membranes and Porous Materials Center Physical Sciences and Engineering DivisionKing Abdullah University of Science and TechnologyThuwal 23955-6900Saudi Arabia

Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinct catalytic *** extensive research,it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic *** this review,we summarize a series of representative systems of single-atom catalysts,discussing their preparation,characterization,and structure-property relationship,with an emphasis on the correlation between the coordination spheres of isolated reactive centers and their intrinsic catalytic *** also share our perspectives on the current challenges and future research promises in the development of single-atom *** this article,we aim to highlight the possibility of finely tuning the catalytic performances by engineering the coordination spheres of single-atom sites and provide new insights into the further development for this emerging research field.

关键词： Isolated atoms coordination sphere Intrinsic activity Single-atom catalysts

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Unlocking high-efficiency oxygen evolution reaction through Co-N coordination engineering in Co@N-doped porous carbon core–shell nanoparticles

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Nano Research 2024年第8期17卷 7068-7076页

作者： Shucheng Liu Yu Shuai Xiaosi Qi Zhao Ding Yi Liu College of Big Data and Information engineering Guizhou UniversityGuiyang 550025China College of Physics Guizhou Province Key Laboratory for Photoelectrics Technology and ApplicationGuizhou UniversityGuiyang 550025China

Modulation of metal sites coordination can significantly refine the electronic architecture of catalysts,thereby improving their catalytic *** work successfully developed a core–shell Co@N-doped porous carbon(Co@NC)catalyst by pyrolyzing the COF/MOF(IISERP-COF3/ZIF-67)composite in an inert *** Co@NC catalyst exhibited impressive oxygen evolution reaction(OER)performance,with a small overpotential of 304 mV and a modest Tafel slope of 88.6 mV·dec^(−1) in a 1 M KOH,alongside remarkable stability,maintaining 98.5%of its activity over 13 *** role of IISERP-COF3 was pivotal in preventing Co atom aggregation during the ZIF-67 pyrolysis,which facilitated the creation of mesopores for enhanced mass transport and ***,it effectively modulated the Co-N coordination to fine-tune the electronic structure,thereby optimizing the catalyst's capacity for adsorption of intermediates and boosting its intrinsic *** functional theory(DFT)studies corroborate that the exceptional OER efficiency of Co@NC can be linked to the enhanced Co-N coordination,optimizing the localized electronic structure at the Co active *** study not only proposes an innovative approach for optimizing COF/MOF as effective electrocatalysts but also clears the path for the emergence of affordable,high-performance alternatives to precious metal-based catalysts,marking a significant advancement in sustainable energy technologies.

关键词： covalent organic framework(COF) metal-organic framework(MOF) core-shell structure catalysts oxygen evolution reaction

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Simplified p-i-n Perovskite Solar Cells with a Multifunctional Polyfullerene Electron Transporter

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Chinese Journal of Polymer Science 2024年第8期42卷 1060-1066页

作者： Fei-Fei Wang Tian-Xiao Liu Ze-Wei Cui Ling-Yuan Wang Yun-Jie Dou Xiao-Yu Shi Si-Wei Luo Xiao-Dong Hu Zhi-Jun Ren Yang-Yang Liu Yu Zhao Shang-Shang Chen State Key Laboratory of coordination Chemistry MOE Key Laboratory of High Performance Polymer Materials&TechnologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 21003China

In prevailing p-i-n perovskite solar cells(PSCs),solution-processible fullerene molecules are widely used as electron-transporting layers(ETLs)but they typically suffer from poor uniformity and undesirable stability ***,a separate bathocuproine(BCP)layer is needed to block hole tran sfer,increasing fabrication complexity and ***,we address these limitations by develo ping a novel polymeric ETL(named PF BCP)synthesized by polymerizing C_(60)with *** innovative material achieves both efficient electron transport and hole blocking,while its excellent uniformity minimizes interface recombination and enhances ***,our blade-coated PSCs utilizing PFBCP achieve a high power conversion efficiency exceeding 22%and retain 91%of initial efficiency after 1200 h of light *** development not only paves the way for commercially viable PSCs but also opens avenues for future ETL design to realize even more efficient and stable PSCs.

关键词： Polyfullerene Perovskite solar cells Electron transporter Stability

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Acylfluorination of enynes via phosphine and silver catalysis

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Chinese Chemical Letters 2024年第8期35卷 260-264页

作者： Yu Mao Yilin Liu Xiaochen Wang Shengyang Ni Yi Pan Yi Wang State Key Laboratory of coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

This work describes intermolecular acylfluorination of gem-difluoroenynes using acyl fluorides as both acyl source and fluorine ***-substituted allenones or furans could be selectively achieved via phosphine and silve... 详细信息

关键词： Phosphine catalysis Silver catalysis Difunctionalization Allenone Furan Trifluoromethyl

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A Self-Healing Elastomer with Extremely High Toughness Achieved by Acylsemicarbazide Hydrogen Bonding and Cu^(2+)-Neocuproine coordination Interactions

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Chinese Journal of Polymer Science 2024年第10期42卷 1425-1434,I0007页

作者： Xiao-Ming An Yi-Ping Wang Tang-Song Zhu Chong Xing Xu-Dong Jia Qiu-Hong Zhang Key Laboratory of High Performance Polymer Material and Technology of MOE Department of Polymer Science and EngineeringSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210093China State Key Laboratory of coordination Chemistry Nanjing UniversityNanjing210093China

Elastomers with high mechanical toughness can guarantee their durability during service ***-healing ability,as well as recyclability,can also extend the life of materials and save the consuming cost of the *** efforts have been dedicated to promoting the mechanical toughness as well as the self-healing capability of elastomers at the same time,while it remains a challenge to balance the trade-off between the above properties in one *** we proposed a molecular design driven by dual interactions of acylsemicarbazide hydrogen bonding and Cu^(2+)-neocuproine coordination *** introducing the reversible multiple hydrogen bonds and strong coordination bonds,we successfully fabricated an extremely tough and self-healing *** elastomer can achieve an impressive top-notch toughness of 491 MJ/m^(3).Furthermore,it boasted rapid elastic restorability within 10 min and outstanding crack tolerance with high fracture energy(152.6kJ/m^(2)).Benefiting from the combination of dynamic interactions,the material was able to self-repair under 80℃conveniently and could be reprocessed to restore the exceptional mechanical properties.

关键词： Metal-ligand coordination Hydrogen bond Ultra-tough elastomer Self-healing

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Chiral thermally activated delayed fluorescence materials for circularly polarized organic light-emitting diodes

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Science China Chemistry 2024年第4期67卷 1097-1116页

作者： Li Yuan Yi-Pin Zhang You-Xuan Zheng State Key Laboratory of coordination Chemistry Collaborative Innovation Center of Advanced MicrostructuresJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Chirality is an important natural characteristic of organic molecules,and chiral organic molecules have shown extensive application in areas such as pharmaceutical development and material *** from the ability to achieve circularly polarized luminescence(CPL),chiral luminescent materials have shown potential applications in anti-glare display,optical communication and,3D display,*** to the ability to harvest both singlet and triplet excitons by a fast reverse intersystem crossing process without involving noble metals,chiral thermally activated delayed fluorescence(TADF)materials with point chirality,axial chirality,planar chirality and helical chirality are regarded as the state-of-the-art materials for circularly polarized organic light-emitting diodes(CP-OLEDs).In recent years,the chiral TADF materials and CP-OLEDs have rapidly developed,but unfortunately,the dissymmetry factors(g)are far from the requirement of practical *** ideal emitters and devices should have both high efficiency and a g factor,or at least a balance between these two *** review gives an overview of recent progress in chiral TADF materials,with a particular focus on the chiral skeleton,CPL property and device ***,the molecular design concept,device structure and methods to improve the g factors of chiral materials and CP-OLEDs are also discussed.

关键词： chiral thermally activated delayed fluorescence material chiral skeleton circularly polarized luminescence circularly polarized organic light-emitting diodes dissymmetry factor

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A color image encryption scheme based on a 2D coupled chaotic system and diagonal scrambling algorithm

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Chinese Physics B 2024年第7期33卷 233-243页

作者：苏静明方士辉洪炎温言 Anhui Mining Machinery and Electrical Equipment coordination Innovation Center Anhui University of Science and TechnologyHuainan 232001China School of Computer Science and Information engineering Hefei University of TechnologyHefei 230009China

A novel color image encryption scheme is developed to enhance the security of encryption without increasing the complexity. Firstly, the plain color image is decomposed into three grayscale plain images, which are converted into the frequency domain coefficient matrices(FDCM) with discrete cosine transform(DCT) operation. After that, a twodimensional(2D) coupled chaotic system is developed and used to generate one group of embedded matrices and another group of encryption matrices, respectively. The embedded matrices are integrated with the FDCM to fulfill the frequency domain encryption, and then the inverse DCT processing is implemented to recover the spatial domain signal. Eventually,under the function of the encryption matrices and the proposed diagonal scrambling algorithm, the final color ciphertext is obtained. The experimental results show that the proposed method can not only ensure efficient encryption but also satisfy various sizes of image encryption. Besides, it has better performance than other similar techniques in statistical feature analysis, such as key space, key sensitivity, anti-differential attack, information entropy, noise attack, etc.

关键词： color image encryption discrete cosine transform two-dimensional(2D)coupled chaotic system diagonal scrambling

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