Collaborative Research: High-resolution electrochemical and Correlated microscopic characterization of 2D electrocatalysts

合作研究：二维电催化剂的高分辨率电化学​​和相关微观表征

• 批准号: 1900463
• 负责人: Michael Mirkin
• 金额: $ 24万
• 依托单位: CUNY Queens College
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-07-01 至 2022-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1900463&HistoricalAwards=false
• 关键词: Collaborative; Research; resolution; electrochemical; Correlated

Professor Michael Mirkin of CUNY Queens College and Professor Huolin Xin of the University of California-Irvine are supported by the Chemical Catalysis Program of the Division of Chemistry to study two-dimensional materials, such as flat nanosheets of transition metal chalcogenides as electrocatalysts for speeding up the electrocatalytic production of hydrogen from water. The knowledge obtained is applicable to other important chemical reactions relevant to alternative energy production and storage technologies. The project seeks to develop a unique microscopy technique that allows for the high-resolution imaging of the reactive site. This imaging is conducted using two techniques: transmission electron microscopy (for atomic-scale structural information) and scanning electrochemical microscopy (for electrochemical information). Correlating the data of the two complementary techniques provides information on the nature of the catalytic nanosheet edges, defects and atomic steps. The information is needed to understand the catalytic activity of these materials. The project provides training for a diverse group of students in renewable energy related science and technology, including mathematical modeling and data processing and mining. Area middle school students are exposed to science research through hand-on experience in the investigators' laboratories. The overarching goal of this collaborative research is to visualize and quantify active sites on two-dimensional (2D) catalyst surfaces via high-resolution (i.e., equal or less than 10 nm) reactivity mapping by scanning electrochemical microscopy (SECM) in combination with scanning transmission electron microscopy (STEM) techniques. By using very small nanoelectrode probes and significantly increasing the SECM resolution the researchers map and quantitatively measure activities of the nanosheet edges, defects and atomic steps on 2D electrocatalysts and assess the effects of phase transformations and surface functionalization. The methodology is developed for multi-technique imaging of the same nanoscale portion of the catalytic surface to obtain spatially resolved mechanistic information about heterogeneous processes on 2D electrocatalysts. The nature of the active sites is elucidated by correlating the SECM activity maps with atomic scale structural and bonding information obtained by STEM and spatially resolved electron energy loss spectroscopy (STEM-EELS) with one-to-one correspondence. These approaches investigate two important classes of 2D materials - transition metal dichalcogenides and MXenes. The objective of the research project is to advance the understanding of factors influencing the activity/stability of 2D electrocatalysts and to help put forward new strategies for improving these properties.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

纽约州立大学皇后学院的迈克尔·米尔金教授和加州大学欧文分校的辛火林教授在化学系化学催化计划的支持下，研究二维材料，如平坦的过渡金属硫化物纳米片作为电催化剂，加速从水中电催化制氢。所获得的知识也适用于与替代能源生产和储存技术有关的其他重要化学反应。该项目寻求开发一种独特的显微镜技术，允许对反应部位进行高分辨率成像。这种成像使用两种技术：透射式电子显微镜(用于原子级结构信息)和扫描电化学显微镜(用于电化学信息)。将这两种互补技术的数据关联起来，可以提供关于催化纳米片边缘、缺陷和原子步骤的性质的信息。这些信息是理解这些材料的催化活性所必需的。该项目为不同群体的学生提供可再生能源相关科学和技术方面的培训，包括数学建模、数据处理和挖掘。该地区的中学生通过在研究人员的实验室中亲身体验科学研究。这项合作研究的主要目标是通过扫描电化学显微镜(SECM)和扫描透射电子显微镜(STEM)技术相结合的高分辨率(即等于或小于10 nm)反应性图谱，可视化和量化二维(2D)催化剂表面的活性中心。通过使用非常小的纳米电极探针并显著提高SECM分辨率，研究人员绘制并定量测量了2D电催化剂上纳米片状边缘、缺陷和原子步骤的活性，并评估了相变和表面功能化的影响。该方法用于对催化剂表面的同一纳米尺度部分进行多技术成像，以获得关于2D电催化剂上多相过程的空间分辨机理信息。通过将SECM活性图与STEM获得的原子尺度、结构和成键信息以及空间分辨电子能量损失谱(STEM-EELS)一一对应，阐明了活性中心的性质。这些方法研究了两类重要的2D材料--过渡金属二卤化物和MXenes。该研究项目的目的是促进对影响2D电催化剂活性/稳定性的因素的了解，并帮助提出改善这些性能的新策略。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Voltage-Driven Molecular Catalysis of Electrochemical Reactions

• DOI: 10.1021/jacs.1c07934
• 发表时间: 2021-10-13
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Barman, Koushik;Wang, Xiang;Mirkin, Michael, V
• 通讯作者: Mirkin, Michael, V

Direct high-resolution mapping of electrocatalytic activity of semi-two-dimensional catalysts with single-edge sensitivity

• DOI: 10.1073/pnas.1821091116
• 发表时间: 2019-06-11
• 期刊: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• 影响因子: 11.1
• 作者: Sun, Tong;Wang, Dengchao;Xin, Huolin L.
• 通讯作者: Xin, Huolin L.

Basal Plane Hydrogen Evolution Activity from Mixed Metal Nitride MXenes Measured by Scanning Electrochemical Microscopy

• DOI: 10.1002/adfm.202001136
• 发表时间: 2020-05-19
• 期刊: ADVANCED FUNCTIONAL MATERIALS
• 影响因子: 19
• 作者: Djire, Abdoulaye;Wang, Xiang;Neale, Nathan R.
• 通讯作者: Neale, Nathan R.