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Nano-Micro Letters 2022年第6期14卷 192-205页

作者： Wenhuan Huang Qiang Qiu Xiufang Yang shouwei zuo Jianan Bai Huabin Zhang Ke Pei Renchao Che Key Laboratory of Chemical Additives for China National Light Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and TechnologyXi’an 710021People’s Republic of China KAUST Catalysis Center King Abdullah University of Science and Technology23955-6900 ThuwalKingdom of Saudi Arabia Laboratory of Advanced Materials Shanghai Key Lab of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200438People’s Republic of China

Improving the atom utilization of metals and clarifying the M–M’interaction is both greatly significant in assembling high-performance ultra-light electromagnetic wave-absorbing materials.Herein,a high-temperature explosion strategy has been successfully applied to assemble the hierarchical porous carbon sponge with Co–Fe decoration via the pyrolysis of the energetic metal organic framework.The as-constructed hybrid displays a superior reflection loss(RL)value of-57.7 d B and a specific RL value of-192 d B mg-1 mm-1 at 12.08 GHz with a layer thickness of 2.0 mm(loading of 15 wt%).The off-axis electron hologram characterizes the highly distributed numerous polarized nanodomain variable capacitors,demonstrating the dipole and interfacial polarization along the edges of the nanopores.More importantly,the X-ray absorption spectroscopy analysis verifies the mutual interaction between the metal cluster and carbon matrix and the electronic coupling responsible for the greatly improved electromagnetic wave absorption.

关键词： Electromagnetic wave-absorbing materials Off-axis electron hologram M-M’interaction Hierarchical porous structure Energetic metal organic framework

Surface decorated Ni sites for superior photocatalytic hydrogen production

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SusMat 2022年第4期2卷 466-475页

作者： Wenhuan Huang Tingting Bo shouwei zuo Yunzhi Wang Jiamin Chen Samy Ould-Chikh Yang Li Wei Zhou Jing Zhang Huabin Zhang Key Laboratory of Chemical Additives for China National Light Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and TechnologyXi'anChina KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)ThuwalSaudi Arabia Department of Applied Physics Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing TechnologyFaculty of ScienceTianjin UniversityTianjinChina Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijingChina

Precise construction of isolated reactive centers on semiconductors with well-controlled configurations affords a great opportunity to investigate the reaction mechanisms in the photocatalytic process and realize the targeted conversion of solar energy to steer the charge kinetics for hydrogen evolution.In the current research,we decorated isolated Ni atoms on the surface of CdS nanowires for efficient photocatalytic hydrogen production.X-ray absorption fine structure investigations clearly demonstrate the atomical dispersion of Ni sites on the surface of CdS nanowires.Experimental investigations reveal that the isolated Ni atoms not only perform well as the real reactive centers but also greatly accelerate the electron transfer via direct Ni-S coordination.Theoretical simulation further documents that the hydrogen adsorption process has also been enhanced over the semi-coordinated Ni centers through electronic coupling at the atomic scale.

关键词： electron transfer hydrogen evolution molecular activation photocatalysis single atomcatalyst

Different mechanisms of improving CH_(3)NH_(3)PbI_(3) perovskite solar cells brought by fluorinated or nitrogen doped graphdiyne

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Nano Research 2022年第1期15卷 573-580页

作者： Huan Huang Bing Liu Dan Wang Rongli Cui Xihong Guo Ying Li shouwei zuo Zi Yin Huanhua Wang Jing Zhang Hui Yuan Lirong Zheng Baoyun Sun CAS Key Lab for Biomedical Effects of Nanomaterials&Nanosafety Institute of High Energy PhysicsChinese Academy of ScienceBeijing 100049China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China University of Chinese Academy of Sciences Beijing 100049China

Fluorinated and nitrogen-doped graphdiyne(F/N-GDY)have been used in the active layer of perovskite solar cells(PSCs)for the first time.The introduction of heteroatoms turns out to be an effective method for boosted solar cells performance,which increases by 32.8%and 33.0%,better than the pristine or GDY doped PSCs.The enhanced performance can be attributed firstly to the superiority of F/N-GDY originated from the unique structure and optoelectronic properties of GDY.Then,both can further reduce surface defects and improve surface and bulk crystallinity than pristine GDY.What's more,efficiency increase caused by F-GDY is mainly attributed to the improvement of fill factor(FF),while the higher short-circuit current(Jsc)plays more important role by N-GDY doping.Most importantly,the detailed mechanism brought about by doping of F-GDY or N-GDY is expounded by systematical characterizations,especially the synchrotron radiation technique.Doping of F-GDY causes Pb and forms new Pb-F bonds between F-GDY and Pb ions.Doping of N-GDY or GDY brings about Pb(N-GDY doping induces more deviation than that of GDY due to the participation of imine N),improving its electron density and conductivity.

关键词： perovskite solar cells graphdiyne grazing incidence X-ray diffraction(GIXRD) X-ray absorption fine structure(XAFS) synchrotron radiation technique

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 performance.Through extensive research,it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic behaviors.In 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 activities.We also share our perspectives on the current challenges and future research promises in the development of single-atom catalysis.With 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

Stable Metal–Halide Perovskite Colloids in Protic Ionic Liquid

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CCS Chemistry 2022年第10期4卷 3264-3274页

作者： Hao Gu Tingting Niu shouwei zuo Yongqing Cai Lingfeng Chao Peter Müller-Buschbaum Yingdong Xia Jing Zhang Guichuan Xing Yonghua Chen Key Laboratory of Flexible Electronics(KLOFE) Institution of Advanced Materials(IAM)Nanjing Tech University(NanjingTech)Nanjing 211816Jiangsu Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoTaipa 999078Macao Frontiers Science Center for Flexible Electronics Xi’an Institute of Flexible Electronics(IFE)Xi’an Institute of Biomedical Materials&EngineeringNorthwestern Polytechnical UniversityXi’an 710072 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049 University of Chinese Academy of Sciences Beijing 100049 Lehrstuhl für Funktionelle Materialien Physik DepartmentTechnische Universität MünchenGarching 85748 Heinz Maier-Leibnitz Zentrum(MLZ) Technische Universität MünchenGarching 85748

Obtaining long-term stable and robust perovskite colloids solution remains an important scientific challenge due to the limited interaction between solvent and perovskite solutes.Here,we unveil the formation mechanism of chemically robust perovskite precursor solutions under ambient conditions using methylammonium acetate(CH3NH3•CH3COO,MAAc)protic ionic liquid(PIL)solvent.Tens of nanometers colloids are assembled on the molecular level via regular oriented gel-like lamellae with a mean thickness of 34.69 nm,width of 56.81 nm,and distance of 91.05 nm.

关键词： perovskite colloids protic ionic liquid X-ray absorption fine structure spectroscopy coordination interaction

Si Doping-Induced Electronic Structure Regulation of Single-Atom Fe Sites for Boosted CO_(2) Electroreduction at Low Overpotentials

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Research 2023年第4期2023卷 307-319页

作者： Changsheng Cao Shenghua Zhou shouwei zuo Huabin Zhang Bo Chen Junheng Huang Xin-Tao Wu Qiang Xu Qi-Long Zhu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of Chinese Academy of Science Beijing100049China KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)Thuwal23955-6900Saudi Arabia Department of Chemistry City University of Hong KongHong Kong999077China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsFujianInstitute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China Institute for Integrated CellMaterial Sciences(iCeMS) Kyoto UniversityKyoto 606-8501Japan Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials(SKLPM) SUSTech-Kyoto University Advanced Energy Materials Joint Innovation Laboratory(SKAEM-JIL)and Department of Materials Science and EngineeringSouthern University of Science and Technology(SUSTech)Shenzhen518055China

Transition metal-based single-atom catalysts(TM-SACs)are promising alternatives to Au-and Ag-based electrocatalysts for CO production through CO_(2)reduction reaction.However,developing TM-SACs with high activity and selectivity at low overpotentials is challenging.Herein,a novel Fe-based SAC with Si doping(Fe-N-C-Si)was prepared,which shows a record-high electrocatalytic performance toward the CO_(2)-to-CO conversion with exceptional current density(>350.0 mA cm^(−2))and~100%Faradaic efficiency(FE)at the overpotential of90%)for CO production.Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulate the electronic structure of the atomic Fe sites in Fe-N-C-Si to markedly accelerate the key pathway involving^(*)CO intermediate desorption,inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO_(2)RR performance.This work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on singleatom sites to improve their electrocatalytic performance.

关键词： desorption bonds exceptional

Origin of High Efficiency and Long-Term Stability in Ionic Liquid Perovskite Photovoltaic

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Research 2020年第1期2020卷 391-403页

作者： Lingfeng Chao Tingting Niu Hao Gu Yingguo Yang Qi Wei Yingdong Xia Wei Hui shouwei zuo Zhaohua Zhu Chengjie Pei Xiaodong Li Jing Zhang Junfeng Fang Guichuan Xing Hai Li Xiao Huang Xingyu Gao Chenxin Ran Lin Song Li Fu Yonghua Chen Wei Huang Frontiers Science Center for Flexible Electronics Xi’an Institute of Flexible Electronics(IFE)and Xi’an Institute of Biomedical Materials&EngineeringNorthwestern Polytechnical University127 West Youyi RoadXi’an 710072China Key Laboratory of Flexible Electronics(KLOFE)&Institution of Advanced Materials(IAM) Nanjing Tech University(Nanjing Tech)Nanjing211816 JiangsuChina Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201204China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China School of Physics and Electronic Science Ministry of EducationNanophotonics&Advanced Instrument Engineering Research CenterEast China Normal UniversityShanghai 200062China Institute of Applied Physics and Materials Engineering University of MacaoMacaoMacao SAR 999078China Key Laboratory for Organic Electronics&Information Displays(KLOEID)and Institute of Advanced Materials(IAM) Nanjing University of Posts and TelecommunicationsNanjing210023 JiangsuChina

Environment-friendly protic amine carboxylic acid ionic liquids(ILs)as solvents is a significant breakthrough with respect to traditional highly coordinating and toxic solvents in achieving efficient and stable perovskite solar cells(PSCs)with a simple one-step air processing and without an antisolvent treatment approach.However,it remains mysterious for the improved efficiency and stability of PSCs without any passivation strategy.Here,we unambiguously demonstrate that the three functions of solvents,additive,and passivation are present for protic amine carboxylic acid ILs.We found that the ILs have the capability to dissolve a series of perovskite precursors,induce oriented crystallization,and chemically passivate the grain boundaries.This is attributed to the unique molecular structure of ILs with carbonyl and amine groups,allowing for strong interaction with perovskite precursors by forming C=O…Pb chelate bonds and N-H…I hydrogen bonds in both solution and film.This finding is generic in nature with extension to a wide range of IL-based perovskite optoelectronics.

关键词： perovskite bonds breakthrough