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原位透射电子显微镜中MoS2纳米片的生长、掺杂与析氢反应机理研究

项目来源

国家自然科学基金(NSFC)

项目主持人

刘培植

项目受资助机构

太原理工大学

项目编号

52001222

立项年度

2020

立项时间

未公开

研究期限

未知 / 未知

项目级别

国家级

受资助金额

24.00万元

学科

工程与材料科学-金属材料-金属材料设计、计算与表征

学科代码

E-E01-E0101

基金类别

青年科学基金项目

关键词

电催化活性位 ; 电子结构 ; 亚埃尺度 ; 原位电子显微学 ; 原子结构调控 ;

参与者

未公开

参与机构

未公开

项目标书摘要：析氢反应(HER)电催化剂是实现将太阳能等可再生能源转换为高能量密度清洁氢能的关键材料之一，二维MoS2纳米片是一种具有良好应用前景的新型非贵金属HER催化剂。目前MoS2纳米片因生长机制、催化活性位和电催化机理等有待深入研究，还未实现可控制备与应用。本研究:1)拟在原位加热透射电子显微镜(TEM)中生长MoS2纳米片，从原子尺度上研究其生长过程，调控其基面生长模式、层数、及尺寸等。2)原位研究Ag在MoS2纳米片中掺杂的位点，阐明MoS2的生长与掺杂调控机制，实现MoS2纳米片催化剂的可控制备。3)构建原位TEM电化学纳米反应器，研究MoS2纳米片在电催化HER中的活性位及其演化过程，再结合第一性原理计算，阐明电催化反应过程中的电荷转移路径和电催化机理。MoS2纳米片的生长机制、活性位与催化性能的构效关系研究，将为新型二维电催化剂的结构优化与可控制备提供坚实的实验数据和理论指导。

Application Abstract: Hydrogen evolution reaction(HER)electrocatalyst is a key in energy conversions from the renewable energy sources,such as solar energy,to hydrogen,which is a clean energy with high power density.2D MoS2 nanosheet is one of the new non-noble metal HER electrocatalysts with high application potentials.The controllable synthesis and application of MoS2 electrocatalyst are unsuccessful so far,since the growth mechanism,electrocatalytic active sites,and electrocatalytic mechanism are calling for further study.In this proposal,we will:1)grow MoS2 nanosheets via in situ heating in transmission electron microscope(TEM),study the growth process in atomic scale,and tuning the growth mode of basal planes,number of layers,and crystal size.2)observe the doping sites of Ag in MoS2 nanosheets in in situ TEM atom by atom and explore the tuning mechanisms of growth and doping.3)construct an electrochemical nano-cell for in situ TEM to investigate the active sites of MoS2 nanosheets and their evolutions during the electrocatalytic HER process.Combine the first principle calculations to interpret the reaction pathways and mechanism of electrocatalysis.The growth mechanism and the structure-activity relationship study will provide a reliable experiment data and theoretic guidance for the structure optimizing and controllable preparation of novel 2D electrocatalysts.

项目受资助省

山西省

项目结题报告(全文)

析氢反应(HER)、析氧反应(ORR)、氧还原反应(ORR)等氢能转化电催化剂是实现绿色氢能应用的关键材料。MoS2、PtSe2等过渡金属硫族化合物(TMDCs)二维纳米片是一类具有良好应用前景的新型非贵金属氢能转化电催化剂。本项目从电催化活性晶面晶体学取向调控、掺杂与修饰、载体选配等三个方面，系统研究了TMDCs基氢能转化电催化剂的制备，以及活性位原子构型和电催化性能之间的构效关系。本项目分别以泡沫镍(NF)和碳布(CC)为基体，制备了Au/MoS2/Ni3S2@NF双功能全水解电催化剂、Ru掺杂1T-MoS2@CC的HER电催化剂和PtCo/PtSe2多孔异质结纳米片HER电催化剂。在500 mA/cm2的高电流密度下,MoS2基催化剂的活性优于商用Pt/C、RuO2催化剂。催化剂系统的结构表征和构效关系研究表明,HER活性位源于TMDCs纳米片，而OER电催化活性位源于NF基体硫化后的产物Ni2S3,且电极的高稳定是实现大电流密度下高效电解水催化剂应用的关键。项目还研究了石墨烯基和金属(氢)氧化物基氢能转化电催化剂的制备、性能和活性位原子构型，发展了先进电子显微学在纳米功能材料结构解析中的应用，在活性位的原子构型解析、构效关系分析与活性位设计等方面取得了重要进展，研究结果为进一步开发高性能TMDCs电催化剂和电极奠定了坚实基础，并将推进电解水和燃料电池等氢能转化装置的应用。

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  • 1.Atomic-scale investigation of carbon-based materials by gentle transmission electron microscopy

    • 关键词：
    • Transmission electron microscopy; Beam sensitive carbon-based materials;Atomic resolution; Low voltage; Low dose;RADIATION-DAMAGE; GRAPHENE; PHASE; PERFORMANCE; CATALYSTS; CRYSTAL; TEM

    Although carbon-based materials, such as graphene, metal-organic frameworks (MOFs), polymers and biomolecules, have aroused increasing scientific interest in the fields of physics, chemistry, materials science and molecular biology, their atomic-scale observation is still a challenge due to their structural instability under the electron beam. Ambiguous atomic arrangements have critically limited the fundamental understanding on these materials and their potential applications in electronics, mechanics, thermodynamics, catalysis, bioscience and medicine. Very recently, revolutionary sub-Angstrom resolution achievements of transmission electron microscopy (TEM) using a low voltage, a low electron dose, or a cryogenic environment have greatly facilitated the atomic-scale structural and chemical examination of electron beam sensitive materials. In particular, the ability to image light elements atom by atom gives unprecedented insight into the structures and properties of novel carbon-based materials. In this review, the recent developments in advanced TEM combined with various imaging and spectroscopy techniques, and their use in examining graphene-based materials, MOFs, polymers, and biomacromolecules are summarized and discussed. The current challenges in materials research and trends for the future design of TEM equipment are outlined, which is expected to provide a deeper understanding of structure-performance relationships and the discovery of new carbon materials.

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