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CO_(2) coordination-driven top-down synthesis of a 2D non-layered metal-organic framework

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Fundamental Research 2022年第5期2卷 674-681页

作者： Yannan Zhou Pengfei Yan Suoying Zhang Yunxiao Zhang Hongwei Chang Xiaoli Zheng Jingyun Jiang Qun Xu College of Materials Science and engineering Zhengzhou UniversityZhengzhou 450052China Henan Institute of advanced technology Zhengzhou UniversityZhengzhou 450052China Key Laboratory of Flexible Electronics&Institute of Advanced Materials Nanjing Tech University30 South Puzhu RoadNanjing 211816China

Combining the physical advantages of two-dimensional(2D)inorganic nanosheets and the modular design and programmed structure of metal-organic frameworks(MOFs),2D MOFs remain at the forefront of functional material *** tremendous efforts,precise control in the synthesis of 2D nonlayered MOFs with predesigned topology for desired applications remains *** in the bottom-up synthesis of 2D nonlayered MOFs via ligand exchange motivated us to incorporate partial BTC(BTC=1,3,5-benzenetricarboxylate)ligand dissociation and CO_(2) capped coordination into the top-down treatment of bulk Cu-BTC MOF,leading to successful conversion of a 3D nonlayered network to a 2D Cu-based topological ***,a supercritical CO_(2)-containing solvent mixture is employed to provide the desired defect and coordination ***,our work introduces a new top-down concept based on modulated synthesis to fabricate high-quality 2D nonlayered MOFs for the first time.

关键词： Top-down Metal-organic frameworks 2D nonlayered Cu-BTC CO_(2)coordination defect engineering

Threshold voltage modulation in monolayer MoS_(2) field-effect transistors via selective gallium ion beam irradiation

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Science China Materials 2022年第3期65卷 741-747页

作者： Baoshan Tang Yunshan Zhao Changjie Zhou Mingkun Zhang Huili Zhu Yida Li Jin Feng Leong Hao Shuai Hao Gong Weifeng Yang Department of Microelectronics and Integrated Circuit School of Electronic Science and EngineeringXiamen UniversityXiamen 361005China Department of Electrical and Computer engineering National University of SingaporeSingapore 117576Singapore NNU-SULI Thermal Energy Research Center(NSTER)&Center for Quantum Transport and Thermal Energy Science(CQTES) School of Physics and TechnologyNanjing Normal UniversityNanjing 210023China Department of Physics School of ScienceJimei UniversityXiamen 361021China engineering Research Center of Integrated Circuits for Next-Generation Communications Ministry of EducationSouthern University of Science and TechnologyShenzhen 518055China Department of Materials Science and engineering National University of SingaporeSingapore 117575Singapore

Electronic regulation of two-dimensional(2 D)transition metal dichalcogenides(TMDCs)is a crucial step towards next-generation optoelectronics and ***,we demonstrate controllable and selective-area defect engineering in 2D molybdenum disulfide(MoS_(2))using a focused ion beam with a low-energy gallium ion(Ga^(+))*** find that the surface defects of MoS_(2)can be tuned by the precise control of ion energy and ***,the fieldeffect transistors based on the monolayer MoS_(2)show a significant threshold voltage modulation over 70 V after Ga+***-principles calculations reveal that the Ga impurities in the monolayer MoS_(2)introduce a defect state near the Fermi level,leading to a shallow acceptor level of 0.25 eV above the valence band *** defect engineering strategy enables direct writing of complex pattern at the atomic length scale in a controlled and facile manner,tailoring the electronic properties of 2D TMDCs for novel devices.

关键词： two-dimensional transition metal dichalcogenides field-effect transistors defect engineering Ga ion irradiation

Electronic structure regulation on layered double hydroxides for oxygen evolution reaction

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Chinese Journal of Catalysis 2019年第12期40卷 1822-1840页

作者： Liangliang Huang Yuqin Zou Dawei Chen Shuangyin Wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina College of Materials Science and engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province Shenzhen UniversityShenzhen 518060GuangdongChina Shenzhen Research Institute of Hunan University Shenzhen 518057GuangdongChina

Oxygen evolution reactions(OERs)as core components of energy conversion and storage technology systems,such as water splitting and rechargeable metal–air batteries,have attracted considerable attention in recent *** metal compounds,particularly layered double hydroxides(LDHs),are considered as the most promising electrocatalysts owing to their unique two-dimensional layer structures and tunable ***,heir poor intrinsic electrical conductivities and the limited number of active sites hinder their *** regulation of the electronic structure is an effective approach to improve the OER activity of LDHs,including cationic and anionic regulation,defect engineering,regulation of intercalated anions,and surface *** this review,we summarize recent advances in the regulation of the electronic structures of LDHs used as electrocatalysts in *** addition,we discuss the effects of each regulation type on OER *** review is expected to shed light on the development and design of effective OER electrocatalysts by summarizing various electronic structure regulation pathways and the effects on their catalytic performances.

关键词： Oxygen evolution reactions Layered double hydroxide Cationic/Anionic regulation defect engineering Electrocatalyst Electron Doping

High mass-specific reactivity of a defect-enriched Ru electrocatalyst for hydrogen evolution in harsh alkaline and acidic media

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Science China Materials 2021年第10期64卷 2467-2476页

作者： Yuanli Li Jingfu He Weiren Cheng Hui Su Changli Li Hui Zhang Meihuan Liu Wanlin Zhou Xin Chen Qinghua Liu National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Fundamental Science on Nuclear Wastes and Environmental Safety Laboratory Southwest University of Science and TechnologyMianyang 621010China School of Materials Sun Yat-sen UniversityGuangzhou 510275China Center for Computational Chemistry and Molecular Simulation College of Chemistry and Chemical EngineeringSouthwest Petroleum UniversityChengdu 610500China

A reasonable design strategy to improve the utilization of noble metal electrocatalysts for the hydrogen evolution reaction(HER)is crucial to simplify the process flow and accelerate the future renewable energy ***,abundant defects were created on 2.4-nm Ru nanoparticles to achieve unprecedently high mass-specific reactivity in harsh acidic and alkaline *** obtained defect-enriched Ru(DR-Ru)exhibits an ultrahigh HER turnover frequency of16.4 s^(-1)with a 100-mV overpotential in alkaline media,and it also retains an excellent value of 20.6 s^(-1)in acidic media;these results are superior to those reported for other Ru ***,a record-low loading of 2.5μg cm^(-2)for the DR-Ru catalysts and low overpotentials of 28.2 and 25.1 mV at10 mA cm^(-2)can be realized in alkaline and acidic media,***,the less coordinated Ru surface sites and partial lattice oxygen introduction weaken the bonding between H and DR-Ru catalysts,facilitate fast acidic HERkinetics and help dissociate the water molecule to overcome the major challenge of HER in alkaline electrolytes,leading to an activity comparable to that under acidic *** result provides a guideline for defect engineering on noble metal nanocatalysts to effectively improve the utilization of the catalysts and optimize reactivities.

关键词： defect engineering DR-Ru catalyst hydrogen evolution reaction electrocatalysis

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Research progress of defect-engineered UiO-66(Zr)MOFs for photocatalytic hydrogen production

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Frontiers in Energy 2021年第3期15卷 656-666页

作者： Yating WANG Chaosheng PENG Tao JIANG Xingang LI School of Chemical engineering and Material Science Tianjin University of Science and TechnologyTianjin 300457China School of Chemical engineering and Technology Tianjin UniversityTianjin 300072China

In recent years,defect-engineered Zr-based UiO-66 metal-organic frameworks(UiO-66(Zr)metalorganic frameworks(MOFs))have shown huge advantages in catalytic,functional materials,adsorption,and other fields due to their large surface areas,well-ordered porous structures,and flexible *** is extremely challenging to introduce defect sites in the synthesis of MOFs to regulate the physicochemical properties of materials such as(energy band structure,pore structure,etc.)to obtain an excellent *** paper reviews the recent research results of synthesis methods,characterization technologies,and application fields of defect-engineered UiO-66(Zr)MOFs materials in order to provide new insights to synthesize high-performance UiO-66(Zr)MOFs materials and promote the development of UiO-66(Zr)in various fields.

关键词： defect engineering metal-organic frameworks UiO-66 photocatalysis

Oxygen vacancies in metal oxides: recent progresstowards advanced catalyst design

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Science China Materials 2020年第11期63卷 2089-2118页

作者： Guoxin Zhuang Yawen Chen Zanyong Zhuang Yan Yu Jiaguo Yu College of Materials Science and engineering Fuzhou UniversityFuzhou 350108China Key Laboratory of Advanced Materials Technologies(Fuzhou University) Fujian Province UniversityFuzhou 350108China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Energy crisis and environmental problems urgently drive the proposal of new strategies to improve human wellbeing and assist sustainable *** this end,scientists have explored many metal oxides-based photocatalysts with high stability,low cost,earth abundance,and potentially high catalytic activity relevant for key applications such as H2O splitting,CO2 reduction,N2 fixation,and advanced oxidation of *** these metal oxides,oxygen vacancies(OVs)are ubiquitous and intrinsic defects with pronounced impacts on the physicochemical properties of the catalysts,which may open new opportunities for obtaining efficient metal *** thorough understanding of the structural and electronic nature of OVs is necessary to determine how they serve as catalytically active *** this review,we summarize the origin of OVs,the strategies to introduce OVs,as well as the fundamental structure-activity relationships to relate these crystal defects to catalyst properties including light absorption,charge separation,*** emphasize the mechanism of OVs formation and their effects on the intrinsic catalytic characteristics of the metal *** also present some multicomponent catalytic platforms where OVs contribute to catalysis via ***,opportunities and challenges on engineering defects in photocatalysts are summarized to highlight the future directions of this research field.

关键词： oxygen vacancy catalysis defect engineering energy and environment metal oxide

Ultrafast micro/nano-manufacturing of metastable materials for energy

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National Science Review 2024年第4期11卷 283-298页

作者： Xiaoya Cui Yanchang Liu Yanan Chen School of Materials Science and engineering Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education) and Tianjin Key Laboratory of Composite and Functional MaterialsTianjin University Ministry of Education Key Laboratory of Protein Sciences School of Life SciencesTsinghua University

The structural engineering of metastable nanomaterials with abundant defects has attracted much attention in energy-related fields. The high-temperature shock(HTS) technique, as a rapidly developing and advanced synthesis strategy, offers significant potential for the rational design and fabrication of high-quality nanocatalysts in an ultrafast, scalable, controllable and eco-friendly way. In this review, we provide an overview of various metastable micro-and nanomaterials synthesized via HTS, including single metallic and bimetallic nanostructures, high entropy alloys, metal compounds(e.g. metal oxides) and carbon nanomaterials. Note that HTS provides a new research dimension for nanostructures, i.e. kinetic modulation. Furthermore, we summarize the application of HTS—as supporting films for transmission electron microscopy grids—in the structural engineering of 2D materials, which is vital for the direct imaging of metastable materials. Finally, we discuss the potential future applications of high-throughput and liquid-phase HTS strategies for non-equilibrium micro/nano-manufacturing beyond energy-related *** is believed that this emerging research field will bring new opportunities to the development of nanoscience and nanotechnology in both fundamental and practical aspects.

关键词： high-temperature shock technique defect engineering metastable phase kinetic modulation non-equilibrium micro/nano-manufacturing

双缺陷工程RuO_(2)/D-Co_(3)O_(4)/CC复合材料作为引发酸性介质中氧析出反应的高效电催化剂

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Science China Materials 2024年第3期67卷 771-779页

作者：刘玉洁袁兆朔宋琪徐同广何刚孙海晓乔倩管学峰徐焘代小平张鑫 State Key Laboratory of Heavy Oil Processing College of Chemical EngineeringChina University of PetroleumBeijing 102249China Beijing Third Class Tobacco Supervision Station Beijing 101121China

缺陷工程被认为是提高催化剂性能的有效方法,因为它能使催化剂具有丰富的活性位点和合适的结合能,从而提高催化性能.本文采用简单的电沉积和酸蚀刻方法制备了双缺陷工程RuO_(2)/D-Co_(3)O_(4)/CC(低Ru负载2.42 wt%)复合材料,用于增强酸... 详细信息

缺陷工程被认为是提高催化剂性能的有效方法,因为它能使催化剂具有丰富的活性位点和合适的结合能,从而提高催化性能.本文采用简单的电沉积和酸蚀刻方法制备了双缺陷工程RuO_(2)/D-Co_(3)O_(4)/CC(低Ru负载2.42 wt%)复合材料,用于增强酸性介质中的氧析出反应(OER).所制备的RuO_(2)/D-Co_(3)O_(4)/CC催化剂采用物理化学技术进行了深入表征,结果表明催化剂中存在明显的阴离子和阳离子缺陷.实验研究表明具有双重缺陷的优化RuO_(2)/D-Co_(3)O_(4)/CC催化剂暴露了更多的电化学活性位点,有效降低了催化反应对电解质中质子浓度的依赖性,从而触发了高性能的OER.只需要181 mV的过电位就能驱动10 mA cm^(-2)的电流密度,并能在此电流密度下保持连续电解120 ***_(2)/D-Co_(3)O_(4)/CC是一种很有前途的酸性OER电催化剂.

关键词： oxygen evolution reaction defect engineering anion defects and cation defects

Reduced CoNi2S4 nanosheets decorated by sulfur vacancies with enhanced electrochemical performance for asymmetric supercapacitors

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Science China Materials 2020年第7期63卷 1216-1226页

作者： Yanpeng Liu Yuxiang Wen Yanan Zhang Xiaogang Wu Haoqian Li Hangda Chen Juanjuan Huang Guohan Liu Shanglong Peng National&Local Joint engineering Laboratory for Optical Conversion Materials and Technology School of Physical Science and TechnologyLanzhou UniversityLanzhou 730000China Shenzhen Key Laboratory of Nanobiomechanics Shenzhen Institutes of Advanced Technology Chinese Academy of SciencesShenzhen 518055China Institute of Sensor Technology Gansu Academy of SciencesLanzhou 730000China

Nowadays,it is a matter of great concern to design electrode materials with excellent electrochemical performance for supercapacitors by a safe,efficient and simple *** these characteristics are usually related to the vacancies and impurities in the *** investigate the effect of the vacancies on the electrochemical properties of the supercapacitor cathode material,the uniform reduced CoNi2S4(r-CoNi2S4)nanosheets with sulfur vacancies have been successfully prepared by a one-step hydrothermal *** the formation of sulfur vacancies are characterized by Raman,X-ray photoelectron spectroscopy and other *** the electrode for supercapacitor,the r-CoNi2S4 nanosheet electrode delivers a high capacity of 1918.9 Fg-1 at a current density of 1 A g-1,superior rate capability(87.9%retention at a current density of 20 A g-1)and extraordinary cycling *** with the original CoNi2S4 nanosheet electrode(1226 F g-1at current density of 1 A g-1),the r-CoNi2S4 nanosheet electrode shows a great *** asymmetric supercapacitor based on the r-CoNi2S4 positive electrode and activated carbon negative electrode exhibits a high energy density of 30.3 Wh kg-1 at a power density of 802.1 W kg-1,as well as excellent long-term cycling *** feasibility and great potential of the device in practical applications have been successfully proved by lightening the light emitting diodes of three different colors.

关键词： defect engineering sulfur vacancies electrochemical performance asymmetric supercapacitors