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Sulfur doped iron-nitrogen-hard carbon nanosheets as efficient and robust noble metal-free catalysts for oxygen reduction reaction in PEMFC

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Journal of Energy Chemistry 2024年第2期89卷 422-433,I0010页

作者： Bin Liu Jiawang Li Bowen Yan Qi Wei Xingyu Wen Huarui Xie Huan He Pei Kang Shen Zhi Qun Tian Collaborative Innovation Center of Sustainable Energy materials School of Physical Science and TechnologyGuangxi UniversityGuangxi Key Laboratory of Electrochemical Energy MaterialsState Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite StructuresNanning 530004GuangxiChina

Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).To tackle the issue,herein,a new type of sulfur-doped ironnitrogen-hard carbon(S-Fe-N-HC)nanosheets with high activity and durability in acid media were developed by using a newly synthesized precursor of amide-based polymer with Fe ions based on copolymerizing two monomers of 2,5-thiophene dicarboxylic acid(TDA)as S source and 1.8-diaminonaphthalene(DAN)as N source via an amination *** as-synthesized S-Fe-N-HC features highly dispersed atomic Fe Nxmoieties embedded into rich thiophene-S doped hard carbon nanosheets filled with highly twisted graphite-like microcrystals,which is distinguished from the majority of M-N-C with soft or graphitic carbon *** unique characteristics endow S-Fe-N-HC with high ORR activity and outstanding durability in 0.5 M H_(2)SO_(4).Its initial half-wave potential is 0.80 V and the corresponding loss is only 21.m V after 30,000 ***,its practical PEMFC performance is a maximum power output of 628.0 mW cm^(-2)and a slight power density loss is 83.0 m W cm^(-2)after 200-cycle practical ***,theoretical calculation shows that the activity of Fe Nxmoieties on ORR can be further enhanced by sulfur doping at meta-site near FeN_(4)*** results evidently demonstrate that the dual effect of hard carbon substrate and S doping derived from the precursor platform of amid-polymers can effectively enhance the activity and durability of Fe-N-C catalysts,providing a new guidance for developing advanced M-N-C catalysts for ORR.

关键词： Transition metal-nitrogen-carbon Oxygen reduction reaction Hard carbon Amide based polymer reaction Proton exchange membrane cells

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Zeolite polymer membrane as protective interface for Mg battery

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Rare metals 2024年第9期43卷 4636-4638页

作者： Hai-Xia Wu Kai-Lu Guo College of Chemistry and Chemical Engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal UniversityLuoyang 471934China

Excessive electrolyte decomposition seriously determines the performance of high-voltage Mg batteries. In Nazar's work, the strategy using a zeolite polymer membrane as a protective interface was proposed to restrain the electrolyte decomposition. This strategy could boost Mg plating/stripping performance up to 6000 h in zeolite/Mg|zeolite/Mg symmetric cells and 91.capacity retention in zeolite/Mg||Mo_(3)S_(4)battery after 200 *** storage devices have been intensively explored because of their important roles in our daily lives [1.3].

关键词： zeolite interface electrolyte

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Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li Department of Chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University state {1. laboratory of Surface Physics and Department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous {1. oxide single crystals remains a formidable ***,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as *** key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon *** mesoporous Li2TiSiO5anode achieves a superior rate capability(1.8 mAh g-1.t5.0 A g-1. and outstanding long-term cycling stability(1.8 mAh g-1.fter 3000 cycles at 2.0 A g-1. for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-1. nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion *** method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous {1. micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

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Temperature-dependent self-trapped exciton emission in Cu(I) doped zinc-based metal halides from well-resolved excited {1. structures

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Nano Research 2024年第8期17卷 7768-7775页

作者： Yunlong Bai Shuai Zhang Nengneng Luo Bingsuo Zou Ruosheng Zeng state {1. laboratory of Featured metal materials and Life-cycle Safety for Composite Structures School of Physical Science and TechnologyGuangxi UniversityNanning 530004China

Zero-dimensional metal halides are of unique structures and tunable photoluminescence properties,showing great potential applications such as light-emitting diodes(LEDs)and ***,we successfully synthesized Cu^(+)doped(MA)_(2)ZnCl_(4)metal halides by a slow evaporation solvent *** introduction of Cu^(+)results in sky-blue self-trapped exciton emission in(MA)_(2)ZnCl_(4) at 486 nm at room temperature,and a photoluminescence quantum yield is as high as 54.9%.Interestingly,at low temperatures,Cu^(+)-doped(MA)_(2)ZnCl_(4) exhibits two emission peaks located at 482 and 605 nm,*** temperaturedependent dual emission indicates two excited state structures that exist on the triplet excited-state potential energy *** addition,the temperature sensor we fitted has good performance(Sr=1.65%·K^(−1.),which is the first attempt in Cu^(+) doped Znbased metal *** work enriches the family of sky-blue metal halides and provides a promising strategy for building skyblue LEDs.

关键词： sky-blue emission self-trapped exciton metal halides excited state structures temperature sensor

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Exciting lattice oxygen of nickel–iron bi-metal alkoxide for efficient electrochemical oxygen evolution reaction

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Journal of Energy Chemistry 2024年第1期88卷 194-201,I0005页

作者： Saihang Zhang Senchuan Huang Fengzhan Sun Yinghui Li Li Ren Hao Xu Zhao Li Yifei Liu Wei Li Lina Chong Jianxin Zou National Engineering Research Center of Light Alloy Net Forming&state {1. laboratory of metal Matrix Composites Center of Hydrogen ScienceSchool of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Laboratory of Advanced MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsiChEM and State Key Laboratory of Molecular Engineering of PolymersCollege of Chemistry and MaterialsFudan UniversityShanghai 200433China

High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage *** electro-oxidation of water to oxygen plays a crucial role in such energy conversion ***,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 1. mA cm^(-2)at an overpotential of 21. mV in 0.1.M KOH *** catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in *** spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline ***-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide *** mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and *** findings provide promising strategies for the rational design of nonnoble metal OER catalysts.

关键词： Oxygen evolution reaction Nickel-iron bi-metal alkoxide Lattice oxygen-mediated reaction mechanism Alkaline electrolysis Electrocatalysts

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Improving high-field strain and temperature stability on KNN-based ceramics sintered in reducing atmosphere via defect engineering

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Journal of Materiomics 2024年第6期10卷 1165-1175页

作者： Zhenyong Cen Meiyi Feng Fuzhi Cao Yuqi Jiang Ze Xu Changrong Zhou Ke Wang Nengneng Luo state {1. laboratory of Featured metal materials and Life-cycle Safety for Composite Structures MOE Key Laboratory of New Proce sing Technology for Nonferrous Metals and MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi Univers ityNanning530004China Guangexi key {1. of Information materials Guilin University of Electronic TechnologyGuilin541004China state {1. laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua UniversityBeijing 100084China

High-field strain and its temperature stability of(1.x)K_(0.48)Na_(0.52)Nb_(0.96)Ta_(0.04)O_(3)-xBaZrO_(3)+8%MnO+3%ZrO_(2)(in mole,KNNT-xBZ+8Mn)ceramics sintered in reducing atmosphere are improved simultaneously via defect design in A and B *** is a conducting type transition from n-type to p-type at x=*** BaZrO_(3) dopant not only induces the increase of defects(Zr′_(Nb),Ba_(Na),Ba_(K))concentration,but also results in the increase of defect(Mn″_(Nb))concentration,because more Mn ions as+2 oxidation state in ceramics is triggered by BaZrO3 doping *** dipoles(Mn″_(Nb)-V_(o),Zr′_(Nb)-V_(o),Ba_(Na)-V′_(Na),Ba_(Na)-V′_(Na))in poled and aged ceramics enhance the reversibility of the non-1.0°domains switching,which increases the high-field strain of KNNT-xBZ+8Mn *** reversibility of non-1.0°domain switching can be preserved to high temperature due to stable defect dipoles(Ba_(Na)-V′_(Na),Ba_(K)-V′_(K))in *** KNNT-xBZ+8Mn ceramics at x=0.07 show the largest high-field strain coefficient(543 pm/V@20 kV/cm)and the highest temperature stability(1.5℃).The KNNT-xBZ+8Mn ceramic is a lead-free material with great potential to be applied in the fabrication of multilayer ceramic actuators with Ni inner electrodes in the future.

关键词： Lead-free ceramics Piezoelectric materials Reducing atmosphere Defects

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Realizing efficient emission and triple-mode photoluminescence switching in air-stable tin(IV)-based metal halides via antimony doping and rational structural modulation

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Aggregate 2024年第1期5卷 257-269页

作者： Xuefei He Hui Peng Qilin Wei Zhijie Zhou Guolun Zhang Zhentao Du Jialong Zhao Bingsuo Zou Department of materials Physics and Chemistry State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite StructuresMOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materialsand School of ResourcesEnvironment and MaterialsGuangxi UniversityNanningChina

Recently,many lead-free metal halides with diverse structures and highly efficient emission have been ***,their poor stability and single-mode emission color severely limit their ***,three homologous Sb^(3+)-doped zero-dimensional(0D)air-stable Sn(IV)-based metal halides with different crystal structures were developed by inserting a single organic ligand into SnCl_(4)lattice,which brings different optical *** photoexcitation,(C_(25)H_(22)P)SnC_(l5)@Sb⋅CH_(4O)(Sb^(3+)−1.does not emit light,(C_(25)H_(22)P)_(2)SnC_(l6)@Sb-α(Sb^(3+)−2α)shines bright yellow emission with a photoluminescence quantum yield(PLQY)of 92%,and(C_(25)H_(22)P)_(2)SnC_(l6)@Sb-β(Sb^(3+)−2β)exhibits intense red emission with a PLQY of 78%.The above three compounds show quite different optical properties should be due to their different crystal structures and the lattice ***,Sb^(3+)−1.can be successfully converted into Sb^(3+)−2αunder the treatment of C_(25)H_(22)PCl solution,accompanied by a transition from nonemission to efficient yellow emission,serving as a“turn-on”photoluminescence(PL)***,a reversible structure conversion between Sb^(3+)−2αand Sb^(3+)−2βwas witnessed after dichloromethane or volatilization treatment,accompanied by yellow and red emission ***,a triple-mode tunable PL switching of off-onI-onII can be constructed in Sb^(3+)-doped Sn(IV)-based ***,we demonstrated the as-synthesized compounds in fluorescent anticounterfeiting,information encryption,and optical logic gates.

关键词： information encryption Sb^(3+)-doping Sn(IV)-based metal halides structural modulation triple-mode

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Filling the gaps in icosahedral superatomic metal clusters

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National Science Review 2024年第7期11卷 168-176页

作者： Wei-Miao He Jia-Hua Hu Yu-Jia Cui Jing Li Yu-Bing Si Shuai-Bo Wang Yu-Jing Zhao Zhan Zhou Lu-Fang Ma Shuang-Quan Zang College of Chemistry Zhengzhou University School of Science Xuchang University College of Chemistry and Chemical Engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal University

Chemically modified superatoms have emerged as promising candidates in the new periodic table, in which Au1.and its doped M_nAu1.-nhave been widely studied. However, their important counterpart, Ag1.artificial element, has not yet been synthesized. In this work, we report the synthesis of Ag1.nanoclusters using strong chelating ability and rigid ligands, that fills the gaps in the icosahedral superatomic metal clusters. After further doping Ag1.template with different degrees of Au atoms, we gained insight into the evolution of their optical properties. Theoretical calculations show that the kernel metal doping can modulate the transition of the excited-state electronic structure, and the electron transfer process changes from local excitation（LE） to charge transfer（CT） to LE. This study not only enriches the families of artificial superatoms, but also contributes to the understanding of the electronic states of superatomic clusters.

关键词： icosahedral superatomic metal clusters analog clusters photoluminescence alloying near-infrared quantum yield

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Size-controlled synthesis and near-infrared photothermal response of Cp^(*)Rh-based metalla[2]catenanes and rectangular metallamacrocycles

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Chinese Chemical Letters 2024年第6期35卷 337-343页

作者： Ying Zhao Yin-Hang Chai Tian Chen Jie Zheng Ting-Ting Li Francisco Aznarez Li-Long Dang Lu-Fang Ma College of Chemistry and Chemical Engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal UniversityLuoyang 471934China College of Chemistry Zhengzhou UniversityZhengzhou 450001China Shanghai key {1. of Molecular Catalysis and Innovative materials State Key Laboratory of Molecular Engineering of PolymersDepartment of ChemistryFudan UniversityShanghai 200438China

A variety of research reports on novel supramolecular topologies have been published over the last ***,it is still a great challenge to tap into the inner functional properties of these ***,two tetranuclear metallamacrocycles 1.and 2 and four octonuclear[2]catenanes 3-6 were constructed successfully via a coordination-driven self-assembly strategy,by conscious design and use of the tetramethyl bidentate pyridine ligand L1.and the appropriate selection of six binuclear half-sandwich rhodium building units with different longitudinal *** complexes have been fully characterized by single crystal X-ray diffraction analysis and NMR ***,near-infrared photothermal studies of the obtained[2]catenanes reveal different photothermal response in solid and solution {1.s,which may be attributed to a strong fluorescence quenching effect of the half-sandwich organometallic fragment and different conjugated effect of Cp^(*)Rh based building blocks in the interlocking *** photothermal conversion efficiencies of[2]catenanes 4-6 fall in the range 30.5%-1..5% *** contribution aims to play a key role in the experimental development of Cp^(*)-based photothermal materials.

关键词： Catenanes Photothermal materials Supramolecular topologies Half-sandwich fragment 3,3'-N-donor analogues

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3D‑Printed Carbon‑Based Conformal Electromagnetic Interference Shielding Module for Integrated Electronics

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Nano-Micro Letters 2024年第5期16卷 87-101页

作者： Shaohong Shi Yuheng Jiang Hao Ren Siwen Deng Jianping Sun Fangchao Cheng Jingjing Jing Yinghong Chen state {1. laboratory of Featured metal materials and Life‑Cycle Safety for Composite Structures School of ResourcesEnvironment and MaterialsGuangxi UniversityNo.100Daxuedong RoadNanning 530004People’s Republic of China state {1. laboratory of Polymer materials Engineering Polymer Research Institute of Sichuan UniversitySichuan UniversityNo.24 South Section 1Yihuan RoadChengdu 610065People’s Republic of China

Electromagnetic interference shielding(EMI SE)modules are the core com-ponent of modern ***,the tra-ditional metal-based SE modules always take up indispensable three-dimensional space inside electronics,posing a major obstacle to the integra-tion of *** innovation of integrating 3D-printed conformal shielding(c-SE)modules with packaging {1. onto core electronics offers infinite possibilities to satisfy ideal SE func-tion without occupying additional ***,the 3D printable carbon-based inks with various proportions of graphene and carbon nanotube nanoparticles are well-formulated by manipulating their rheological ***,the free-constructed architectures with arbitrarily-customized structure and multifunctionality are created via 3D *** particular,the SE performance of 3D-printed frame is up to 61.4 dB,simultaneously accompanied with an ultralight architecture of 0.076 g cm^(-3) and a superhigh specific shielding of 802.4 dB cm3 g^(-1..Moreover,as a proof-of-concept,the 3D-printed c-SE module is in situ integrated into core electronics,successfully replacing the traditional metal-based module to afford multiple functions for electromagnetic compatibility and thermal ***,this scientific innovation completely makes up the blank for assembling carbon-based c-SE modules and sheds a brilliant light on developing the next generation of high-performance shielding {1. with arbitrarily-customized structure for integrated electronics.

关键词： 3D printing Carbon-based nanoparticles Conformal electromagnetic interference shielding Integrated electronics

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