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Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Zscheme heterojunctions with enhanced photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 5002-5010页

作者： Qingtao Zhu Honglei Shen Chao Han Liu Huang Yanting Zhou Yuanxin Du Xi Kang Manzhou Zhu Department of materials Science and Engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic performance.Herein,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and CoP.The enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional migration.This work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.

关键词： atomically precise metal nanocluster Z-scheme heterojunction interfacial charge transfer build-in electric field photocatalytic hydrogen production

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Topological magnetoelectric response in ferromagnetic axion insulators

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National Science Review 2024年第2期11卷 8-14页

作者： Yuhao Wan Jiayu Li Qihang Liu Department of Physics and Shenzhen Institute for Quantum Science and Engineering(SIQSE) Southern University of Science and Technology Shenzhen Key laboratory of advanced Quantum functional materials and Devices Southern University of Science and Technology Guangdong Provincial Key laboratory for Computational Science and material Design Southern University of Science and Technology

The topological magnetoelectric effect （TME） is a hallmark response of the topological field theory,which provides a paradigm shift in the study of emergent topological phenomena.However,its direct observation is yet to be realized due to the demanding magnetic configuration required to gap all surface states.Here,we theoretically propose that axion insulators with a simple ferromagnetic configuration,such as the MnBi2Te4/（Bi2Te3）nfamily,provide an ideal playground to realize the TME.In the designed triangular prism geometry,all the surface states are magnetically gapped.Under a vertical electric field,the surface Hall currents give rise to a nearly half-quantized orbital moment,accompanied by a gapless chiral hinge mode circulating in parallel.Thus,the orbital magnetization from the two topological origins can be easily distinguished by reversing the electric field.Our work paves the way for direct observation of the TME in realistic axion-insulator materials.

关键词： topological magnetoelectric effect axion insulator magnetic topological materials

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Progress and prospect of Pt-based catalysts for electrocatalytic hydrogen oxidation reactions

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Nano Research 2024年第3期17卷 960-981页

作者： Xu Zhang Ying Xie Lei Wang Key laboratory of functional Inorganic material Chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

To achieve the goals of the peak carbon dioxide emissions and carbon neutral,the development and utilization of sustainable clean energy are extremely important.Hydrogen fuel cells are an important system for converting hydrogen energy into electrical energy.However,the slow hydrogen oxidation reaction(HOR)kinetics under alkaline conditions has limited its development.Therefore,elucidating the catalytic mechanism of HOR in acidic and alkaline media is of great significance for the construction of highly active and stable catalysts.In terms of practicality,Pt is still the primary choice for commercialization of fuel cells.On the above basis,we first introduced the hydrogen binding energy theory and bifunctional theory used to describe the HOR activity,as well as the pH dependence.After that,the rational design strategies of Pt-based HOR catalysts were systematically classified and summarized from the perspective of activity descriptors.In addition,we further emphasized the importance of theoretical simulations and in situ characterization in revealing the HOR mechanism,which is crucial for the rational design of catalysts.Moreover,the practical application of Pt-based HOR catalysts in fuel cells was also presented.In closing,the current challenges and future development directions of HOR catalysts were discussed.This review will provide a deep understanding for exploring the mechanism of highly efficient HOR catalysts and the development of fuel cells.

关键词： Pt-based catalysts hydrogen oxidation reaction(HOR) electrocatalytic mechanism hydrogen binding energy theory bifunctional theory

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Recent progress of cobalt-based electrocatalysts for water splitting: Electron modulation, surface reconstitution, and applications

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Nano Research 2024年第4期17卷 2234-2269页

作者： Zhijian Liang Di Shen Lei Wang Honggang Fu Key laboratory of functional Inorganic material Chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

Electrocatalytic water splitting is an essential and effective means to produce green hydrogen energy structures,so it is necessary to develop non-precious metal catalysts to replace precious metals.Cobalt-based catalysts present effective alternatives due to the diverse valence states,adjustable electronic structures,and plentiful components.In this review,the catalytic mechanisms of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)for electrocatalytic water splitting are described.Then,the synthesis strategies of various cobalt-based catalysts are systematically summarized,followed by the relationships between the structure and performance clarified.Subsequently,the effects of d-band center and spin regulation for cobalt-based catalysts are also discussed.Furthermore,the dynamic electronic and structural devolution of cobalt-based catalysts are elucidated by combining a series of in-situ characterizations.Finally,we highlight the challenges and future developed directions of cobalt-based catalysts for electrocatalytic water splitting.

关键词： cobalt-based electrocatalysts water splitting electron modulation surface reconfiguration

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β-C(sp^(3))−H chlorination of amide derivatives via photoinduced copper charge transfer catalysis

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Chinese Chemical Letters 2024年第2期35卷 361-365页

作者： Yuhang He Chao Tian Guanghui An Guangming Li Key laboratory of functional Inorganic material Chemistry (MOE) School of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China

An atom economicβ-C(sp^(3))−H chlorination of amide derivatives has been developed.This mild protocol employs CuCl_(2) instead of palladium catalysts with atom-economic HCl as chlorine sources and enables the late-stage functionalization of medicine derivatives.Mechanism studies suggest a plausible visible light triggered ligand-to-metal charge transfer(LMCT)/1,4-hydrogen atom transfer(HAT)cascade.

关键词： Photoinduced copper catalysis Ligand-to-metal charge transfer 1,4-Hydrogen atom transfer β-Halogenated amide Late-stage functionalization

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Tuning interface mechanism of FeCo alloy embedded N,S-codoped carbon substrate for rechargeable Zn-air battery

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Journal of Energy Chemistry 2024年第6期93卷 400-410,I0010页

作者： Hui Chang Lulu Zhao Shan Zhao Zong-Lin Liu Peng-Fei Wang Ying Xie Ting-Feng Yi School of materials Science and Engineering Northeastern UniversityShenyang 110819LiaoningChina Key laboratory of functional Inorganic material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080HeilongjiangChina Key laboratory of Dielectric and Electrolyte functional material Hebei Province School of Resources and MaterialsNortheastern University at QinhuangdaoQinhuangdao 066004HebeiChina

The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple one-step pyrolysis strategy.The experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of S atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon material.The FeCo/SNC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/S-NC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for OER.In addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/S-NC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle performance.These results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.

关键词： FeCo alloy N S co-doped carbon DFT calculation Zn-air batteries Interfacial interaction

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Recent Progress in Fabrication and Structural Design of Thermal Conductive Polymer Composites

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Chinese Journal of Polymer Science 2024年第3期42卷 277-291,I0004页

作者： Yuan-Kai Du Zheng-Xue Shi Shan Dong Hui Jin Xue Ke Pei Zhao Bing-Bing Jiang Feng You Hubei Key laboratory of Plasma Chemistry and advanced materials School of Material Science and EngineeringWuhan Institute of TechnologyWuhan 430205China Key laboratory of Green Preparation and Application of functional materials Ministry of EducationHubei UniversityWuhan 430062China Institute of Molecular Aggregation Science Tianjin UniversityTianjin 300072China

In recent years, the demand direction for electronic equipment has expanded into embedded and miniaturized devices. The heat radiation problem has become one of the most significant factors for hindering the development of electronic devices. Since heat radiation material is one of the important components in electronic devices, the demand for enhancing thermal conductivity is also increasingly urgent. Research on thermal conductive polymer composites has become a major direction for developing functional composites. This work reviewed the recent progress in the fabrication of thermal conductive polymer composites. Five different structures are presented, including the using of single fillers,hybrid fillers, double threshold percolation structure, segregated structure and other complex multiphase structures. Specifically, the preparation of high-performance thermal conductive polymer composites was introduced through the combination of various thermal conductive fillers.Finally, the development direction of high thermal conductive polymer composites was briefly explored.

关键词： Thermal conductive polymer Hybrid fillers Polymer composite Thermal resistance

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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China Chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao Key laboratory of advanced Energy material Chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,etc.Major studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali co-catalysts.Therefore,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction conditions.Herein,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1-x(x=1,2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,respectively.Cu NPs@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild conditions.The corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale experiments.Additionally,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air conditions.Importantly,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@1-3.Mechanism investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal centers.More importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

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Hollow Ni Mo-based nitride heterojunction with super-hydrophilic/aerophobic surface for efficient urea-assisted hydrogen production

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Journal of Energy Chemistry 2024年第8期95卷 428-439页

作者： Yuying Fan Ying Gu Dongxu Wang Yanqing Jiao Aiping Wu Chungui Tian Key laboratory of functional Inorganic material Chemistry Ministry of Education of the People's Republic of China Heilongjiang University College of Chemistry Chemical Engineering and Resource Utilization Northeast Forestry University

Hydrogen evolution reaction（HER） and urea oxidation reaction（UOR） are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional（3D） hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07° and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm-2.The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm-2,which is approximately 209 mV lower than water electrolysis.

关键词： Hollow heterojunctions Hydrogen evolution Super hydrophilic/aerophobic Transition metal nitrides Urea electrooxidation

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C_(60) as a metal-free catalyst for lithium-oxygen batteries

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Nano Research 2024年第5期17卷 3982-3987页

作者： Xinxin Zhang Jiaming Tian Yu Wang Shaohua Guo Yafei Li Jiangsu Collaborative Innovation Centre of Biomedical functional materials School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional MaterialsNational Laboratory of Solid State MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresFrontiers Science Center for Critical Earth Material CyclingNanjing UniversityNanjing 210023China

Carbon materials have shown significant potential as catalysts for lithium-oxygen batteries(LOBs).However,the intrinsic carbon sites are typically inert,necessitating extensive modifications and resulting in a limited density of active sites.Here we present C_(60) as a metal-free cathode catalyst for LOBs,using density functional theory calculations and experimental verifications.The lithiation reactions on the pristine carbon sites of C_(60) are energetically favorable due to its curvedπ-conjugation over the pentagon-hexagon networks.The kinetic analysis specifically reveals low energy barriers for Li_(2)O_(2) decomposition and Li diffusion on C_(60).Consequently,C_(60) exhibits significantly higher catalytic activity than typical carbon materials such as graphene and carbon nanotubes.Our electrochemical measurements validate the predictions,notably demonstrating that the intrinsic activity of C_(60) is comparable to that of noble metals.

关键词： lithium-oxygen batteries C_(60) density functional theory(DFT)calculations metal-free cathode

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