Nanogap Electrochemistry of Adsorption-Coupled Electron Transfer

吸附耦合电子转移的纳米间隙电化学

• 批准号: 1904258
• 负责人: Shigeru Amemiya
• 金额: $ 43.35万
• 依托单位: University of Pittsburgh
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-06-15 至 2023-05-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1904258&HistoricalAwards=false
• 关键词: Nanogap; Electrochemistry; Adsorption; Coupled; Electron

In this project funded by the Chemical Measurement and Imaging Program, with co-funding from the Chemical Structure, Dynamics, and Mechanisms-A Program, of the Division of Chemistry, Professor Shigeru Amemiya of the University of Pittsburgh is developing new electrochemical methods that allow for the separate study of electron transfer and coupled adsorption events at novel nanometer-sized electrodes. This project focuses on gaining an advanced understanding of adsorption-coupled electron transfer, which plays a vital role in numerous electrochemical energy devices, such as fuel cells, batteries, solar cells, and supercapacitors. Reliable determination of rate and energy parameters is possible due to the creation of new research tools. Students from underrepresented groups gain interdisciplinary training in the research and undergraduate laboratory environments, as a result of their participating in cross-cutting research. This project is focused on the quantitative study of adsorption-coupled electron transfer as the key step of electrochemical technologies that span electrocatalysis, electrodeposition, and electroanalysis. New nanoelectrochemical methods developed in the Amemiya laboratory provide an opportunity to kinetically resolve adsorption-coupled electron transfer into its elementary steps. Specifically, nanogap voltammetry with a scanning electrochemical microscope affords a path to separately determine the dynamics of inner-sphere and outer-sphere electron transfer, surface adsorption, and even coupled chemical reactions. Reliable reaction parameters can be obtained by employing clean electrodes that maintain vacuum-level surface cleanliness in air and solution, as a result of new methods developed by Professor Amemiya's research group.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.

在这个由化学测量和成像计划资助的项目中，匹兹堡大学的Shigeru Amemiya教授正在开发新的电化学方法，该方法允许在新型纳米尺寸的电极上单独研究电子转移和耦合吸附事件。该项目的重点是获得对吸附耦合电子转移的深入了解，这在许多电化学能源设备中起着至关重要的作用，如燃料电池，电池，太阳能电池和超级电容器。由于新的研究工具的创建，速率和能量参数的可靠确定是可能的。来自代表性不足群体的学生在研究和本科实验室环境中获得跨学科培训，因为他们参与了跨学科研究。 本计画主要针对电化学技术中的吸附耦合电子转移进行定量研究，此电化学技术涵盖电催化、电沉积及电分析。Amemiya实验室开发的新纳米电化学方法提供了一个机会，将吸附耦合电子转移动力学分解为基本步骤。具体而言，纳米间隙伏安法与扫描电化学显微镜提供了一个路径，分别确定内球和外球的电子转移，表面吸附，甚至耦合的化学反应的动力学。雨宫教授的研究小组开发的新方法，通过使用在空气和溶液中保持真空级表面清洁度的清洁电极，可以获得可靠的反应参数。该奖项反映了NSF的法定使命，通过使用基金会的知识价值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

Perspective—Beyond the Century-Long Paradigm of Hydrogen Electrochemistry through the Laviron–Amatore Paradox

透视——通过拉维龙——阿马托悖论超越长达一个世纪的氢电化学范式

• DOI: 10.1149/1945-7111/abc840
• 发表时间: 2020
• 期刊: Journal of The Electrochemical Society
• 影响因子: 3.9
• 作者: Kurapati, Niraja;Buoro, Rafael Martos;Amemiya, Shigeru
• 通讯作者: Amemiya, Shigeru

Adsorption-Coupled Electron-Transfer Mode of Scanning Electrochemical Microscopy: Voltammetric Simulation

• DOI: 10.1016/j.electacta.2023.141973
• 发表时间: 2023-01
• 期刊: Electrochimica Acta
• 影响因子: 6.6
• 作者: Donald C. Janda;K. Barma;Moghitha Parandhaman;Xindi Sun;Kevin C. Leonard;S. Amemiya

Systematic assessment of adsorption-coupled electron transfer toward voltammetric discrimination between concerted and non-concerted mechanisms

吸附耦合电子转移对协同机制和非协同机制伏安区分的系统评估

• DOI: 10.1016/j.electacta.2022.140912
• 发表时间: 2022
• 期刊: Electrochimica Acta
• 影响因子: 6.6
• 作者: Janda, Donald C.;Barma, Kiran;Kurapati, Niraja;Klymenko, Oleksiy V.;Oleinick, Alexander;Svir, Irina;Amatore, Christian;Amemiya, Shigeru
• 通讯作者: Amemiya, Shigeru

Nanogap-Resolved Adsorption-Coupled Electron Transfer by Scanning Electrochemical Microscopy: Implications for Electrocatalysis

• DOI: 10.1021/acs.analchem.2c04008
• 发表时间: 2022-12-13
• 期刊: ANALYTICAL CHEMISTRY
• 影响因子: 7.4
• 作者: Kurapati, Niraja;Janda, Donald C.;Amemiya, Shigeru
• 通讯作者: Amemiya, Shigeru