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Metal-organic framework assisted synthesis of single-atom catalysts for energy applications

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National Science Review 2018年第5期5卷 626-627页

作者： Yao Zheng shi-zhang qiao School of Chemical Engineering The University of Adelaide School of Materials Science and Engineering Tianjin University

Metal single-atom catalysts (M-SACs)are emerging as a new research frontier because of their low-coordination metal atoms and uniform structures. As a representation of maximum atom utilization efficiency, M-SACs demonstrate unique properties in a wide variety of heterogeneous catalysis and electrocatalytic processes [1,2]. Metal-organic frameworks (MOFs) are composed of metal-

关键词： Co Metal-organic framework assisted synthesis of single-atom catalysts for energy applications ZIF Ni

Fe3O4 encapsulated mesoporous silica nanospheres with tunable size and large void pore

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Frontiers of Chemical Science and Engineering 2014年第1期8卷 114-122页

作者： Tingting LIU Lihong LIU Jian LIU Shaomin LIU shi zhang qiao Department of Chemical Engineering Curtin University Perth WA 6845 Australia School of Chemical Engineering The University of Adelaide SA5005 Australia

Magnetic Fe3O4 and mesoporous silica core- shell nanospheres with tunable size from 110-800 nm were synthesized via a one step self-assembly method. The morphological, structural, textural, and magnetic proper- ties were well-characterized by scanning electron micro- scopy, transmission electron microscopy, X-ray diffraction, N2 adsorption-desorption and magnetometer. These nanocomposites, which possess high surface area, large pore volume and well-defined pore size, exhibit two dimensional hexagonal （P6mm） mesostructures. Interest- ingly, magnetic core and mesoporous silica shell nano- composites with large void pore （20 nm） on the shell were generated by increasing the ratio of ethanol/water. Additionally, the obtained nanocomposites combined magnetization response and large void pore, implying the possibility of applications in drug/gene targeting delivery. The cell internalization capacity of NH2-functionalized nanocomposites in the case of cancer cells （HeLa cells） was exemplified to demonstrate their nano-medicine application.

关键词： mesoporous silicas magnetic nanoparticles,core-shell nanoparticles cell uptake

Metastable Two-Dimensional Materials for Electrocatalytic Energy Conversions

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Accounts of Materials Research 2021年第7期2卷 559-573页

作者： Huanyu Jin Taeseup Song Ungyu Paik shi-zhang qiao School of Chemical Engineering and Advanced Materials and Centre for Materials in Energy and Catalysis(CMEC) The University of AdelaideAdelaideSA 5005Australia Department of Energy Engineering Hanyang UniversitySeoul 04763Republic of Korea

CONSPECTUS:An urgent need for efficient energy conversion technologies is driving development of active and durable *** recent years,two-dimensional(2D)materials have emerged as practically promising electrocatalysts because of unique physical and chemical *** general,a significant proportion of 2D materials are polymorphous with diverse crystal structures or ***,pristine 2D materials found in nature are thermodynamically stable phases with inert catalytic *** phases,in contrast,are highly active for various electrocatalytic processes because of high-energy structures and high reactivity of nonequilibrium ***,the growth of metastable 2D materials requires higher formation energy compared with the thermodynamically stable phases,which are difficultly obtained in standard synthetic processes such as chemical vapor deposition and vapor transport *** destabilization of thermodynamically stable 2D materials via external forces facilitates the conversion of highentropy crystal structure into metastable *** date,a number of approaches,including confined growth,topotactic transformation,electron donating,and chemical exfoliation,have been demonstrated for the preparation of high-performance metastable 2D *** an atomic thin platform,metastable 2D materials represent an almost ideal prototype to achieve a comprehensive understanding of the fundamental principles and mechanisms of various electrocatalytic *** the design of metastable 2D electrocatalysts,a number of needs must be concomitantly considered,namely,(1)economic of synthesis methods,(2)product yield,(3)applicability of post-treatment for tuning electrocatalytic properties,(4)general synthesis protocols,and(5)the chemical and catalytic stabilities of metastable 2D *** this Account,we provide a critical and timely overview of metastable 2D materials for major electrocatalytic energy conversions

关键词： metastable catalytic stabilization

Customizing the microenvironment of CO_(2) electrocatalysis via three‐phase interface engineering

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SmartMat 2022年第1期3卷 111-129页

作者： Xianlong Zhou Hao Liu Bao Yu Xia Kostya(Ken)Ostrikov Yao Zheng shi‐zhang qiao School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSouth AustraliaAustralia Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureWuhanChina National Laboratory for Optoelectronics School of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)China School of Chemistry and Physics and Centre for Materials Science Queensland University of Technology(QUT)BrisbaneAustralia

Converting CO_(2) into high‐value fuels and chemicals by renewable‐electricitypowered electrochemical CO_(2) reduction reaction(CRR)is a viable approach toward carbon‐emissions‐neutral *** the thermocatalytic hydrogenation of CO_(2) at the solid‐gas interface,the CRR takes place at the three‐phase gas/solid/liquid interface near the electrode surface in aqueous solution,which leads to major challenges including the limited mass diffusion of CO_(2) reactant,competitive hydrogen evolution reaction,and poor product *** we critically examine the various methods of surface and interface engineering of the electrocatalysts to optimize the microenvironment for CRR,which can address the above *** effective modification strategies for the gas transport,electrolyte composition,controlling intermediate states,and catalyst engineering are *** key emphasis is made on the diverse atomic‐precision modifications to increase the local CO_(2) concentration,lower the energy barriers for CO_(2) activation,decrease the H2O coverage,and stabilize intermediates to effectively control the catalytic activity and *** perspectives on the challenges and outlook for the future applications of three‐phase interface engineering for CRR and other gasinvolving electrocatalytic reactions conclude the article.

关键词： catalytic selectivity electrochemical CO_(2)reduction intermediates microenvironment three‐phase interface

Hybrid working mechanism enables highly reversible Zn electrodes

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eScience 2023年第2期3卷 83-92页

作者： Libei Yuan Junnan Hao Bernt Johannessen Chao Ye Fuhua Yang Chao Wu shi-Xue Dou Hua-Kun Liu shi-zhang qiao Institute for Superconducting and Electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongWollongongNew South Wales2522 Australia School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSouth Australia5005 Australia Australian Synchrotron 800 Blackburn RdClaytonVIC3168 Australia

Zn dendrite growth and water-related side reactions have been criticized to hinder actual applications of aqueous Zn-ion *** address these issues,a series of Zn interfacial modifications of building solid/electrolyte interphase(SEI)and nucleation layers have been widely proposed,however,their effectiveness remains debat***,we report a boron nitride(BN)/Nafion layer on the Zn surface to efficiently solve Zn problems through combining the hybrid working mechanisms of SEI and nucleation *** our protective layer,Nafion exhibits the SEI mechanism by blocking water from the Zn surface and providing abundant channels for rapid Zn^(2+)þtransmission,whilst BN nanosheets induce Zn deposition underneath with a preferred(002)***,dendrite-free and side-reaction-free Zn electrode with(002)deposition under the protective layer is realized for the first time,as reflected by its high reversibility with average Coulombic efficiency of 99.2%for>3000 *** protected Zn electrode also shows excellent performance in full cells when coupling with polyaniline cathode under the strict condition of lean electrolyte *** work highlights insights for designing highly reversible metal electrodes towards practical applications.

关键词： Aqueous Zn-ion batteries Hybrid working mechanism Boron nitride Nafion

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纳米尺度富集效应促进二氧化碳电还原

物理化学学报 2020年第11期36卷 7-8页

作者：乔世璋 School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaide SA 5005Australia

电催化二氧化碳还原具有可在常温常压下进行,能够实现人为闭合碳循环等优点,为当前可再生能源的利用和化学燃料合成提供了一种极具应用前景的方法1。当前,更高效催化剂的设计合成与催化机制理解,从而推动二氧化碳电还原技术走向工业化... 详细信息

电催化二氧化碳还原具有可在常温常压下进行,能够实现人为闭合碳循环等优点,为当前可再生能源的利用和化学燃料合成提供了一种极具应用前景的方法1。当前,更高效催化剂的设计合成与催化机制理解,从而推动二氧化碳电还原技术走向工业化应用成为研究重点与难点^2–4。

关键词：二氧化碳还原可再生能源电还原催化机制高效催化剂常温常压富集效应设计合成

在亚稳态MoS_(2)上高负载Pt单原子催化剂应用于高效析氢反应

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Science Bulletin 2023年第23期68卷 2896-2897页

作者：凌涛乔世璋 School of Materials Science and Engineering Tianjin UniversityTianjin 300072China School of Chemical Engineering The University of AdelaideAdelaide SA 5005Australia

Electrocatalysts play a key role in sustainable energy storage and conversion devices,such as water electrolysers[1],fuel cells[2],*** controllable and uniform dispersion of electrocatalysts on suitable support materials has received increasing attentions in academia and *** is because the supports[3]can greatly enhance the catalytic activity and stability of the electrocatalysts through the atomic and electronic interactions between the support and catalytic sites,thus improving the catalytic efficiency of the catalysts,especially for precious metals.

关键词：单原子催化剂析氢反应亚稳态高负载

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外悬挑花架梁支模施工技术分析

建筑技术开发 2017年第8X期44卷 37-38页

作者：张世桥河南省第一建筑工程集团有限责任公司郑州450000

针对高空外悬挑花架梁的结构特点,设计由斜拉圆钢与工字钢组成的型钢平台,保证了外挑结构主体施工模板支撑脚手架和外防护架的搭设安全,可为同行提供借鉴和参考。

关键词：外悬挑花架梁斜拉圆钢工字钢支撑平台

Co/Co_(7)Fe_(3)heterostructures with controllable alloying degree on carbon spheres as bifunctional electrocatalyst forrechargeable zinc-air batteries

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 476-487页

作者： Junkang Chen Yongyue Zhuang Yanxin qiao Yu zhang Aihua Yuan Hu Zhou School of Materials Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China

Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree control strategy was employed to fabricate nitrogen-doped carbon sphere(NCS)decorated with dual-phase Co/Co_(7)Fe_(3)heterojunctions(CoFe@NCS).The phase composition of materials has been adjusted by controlling the alloying *** optimal CoFe_(0.08)@NCS electrocatalyst displays a half-wave potential of 0.80 V for ORR and an overpotential of 283 mV at 10 mA·cm^(-2)for OER in an alkaline *** intriguing bifunctional electrocatalytic activity and durability is attributed to the hierarchically porous structure and interfacial electron coupling of highly-active Co_(7)Fe_(3)alloy and metallic Co *** the CoFe_(0.08)@NCS material is used as air-cathode catalyst of rechargeable liquid-state zinc-air battery(ZAB),the device shows a high peak power-density(157 mW·cm^(-2))and maintains a stable voltage gap over 150 h,outperforming those of the benchmark(Pt/C+RuO_(2))-based *** particular,the as-fabricated solid-state flexible ZAB delivers a reliable compatibility under different bending *** work provides a promising strategy to develop metal/alloy-based electrocatalysts for the application in renewable energy conversion technologies.

关键词： bifunctional electrocatalysts oxygen reduction reaction oxygen evolution reaction zinc-air battery metal/alloy carbon sphere