CAS-Climate: Electroadsorption Kinetics on Transition Metals: Measurement and Mechanism

CAS-Climate：过渡金属的电吸附动力学：测量和机理

• 批准号: 2155157
• 负责人: Jin Suntivich
• 金额: $ 54.2万
• 依托单位: Cornell University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-07-01 至 2025-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2155157&HistoricalAwards=false
• 关键词: CAS; Climate; Electroadsorption; Kinetics; Transition

With support from the Chemical Structure, Dynamics, and Mechanism A (CSDM-A) Program in the Division of Chemistry, Drs. Jin Suntivich and Héctor Abruña of Cornell University are investigating the mechanism of surface hydrogen formation on transition metals with well-defined structure and orientation. Electrochemical and non-linear spectroscopic measurements facilitate the formation of a conceptual framework for proton and electron transfers across the metal-water interface. Drs. Suntivich and Abruña and their students examine the electrode potential-dependent formation of surface hydrogen on metal single crystals because this reaction represents the first step in the evolution/production of hydrogen and involves only one electron and one proton. The team also investigates the influence of local variables such as interfacial electric field and surface chemistry on proton and electron-transfer kinetics. Non-linear spectroscopy is used to provide local electric field information at the metal-water interface. By advancing the mechanistic knowledge of electrochemical reactions, future catalysts that efficiently generate or evolve hydrogen from water could be designed. The team also translates concepts in electrochemical and optical sciences to outreach activities through the New York Stat 4-H Youth Development program. The team is developing new curricular materials on chemical circularity for first year students at Cornell University. This project investigates the proton-coupled electron transfer (PCET) mechanism on well-defined single-crystal metal surfaces such as platinum and palladium. These heterogeneous electrochemical reactions are common in electrocatalysis; however, they are complex because most PCET reactions involve the transfer of multiple protons and electrons. The research team applies a time-dependent electro-analytical method and non-linear spectroscopy to probe surface hydrogen formation, which involves only one proton and one electron. These studies examine the surface hydrogen formation kinetics on single-crystal metal surfaces as a function of proton donor and metal chemistries as well as local electric field and surface oxide. Phase-sensitive second harmonic generation measurements are employed to characterize the local electric field during the electrochemical reaction. These investigations foster a deep understanding of the molecular picture during the heterogeneous PCET electrocatalysis mechanism.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.

在化学系化学结构、动力学和机理 A (CSDM-A) 项目的支持下，康奈尔大学的 Jin Suntivich 和 Héctor Abruña 博士正在研究结构明确的过渡金属表面氢形成的机制。电化学和非线性光谱测量促进了质子和电子在金属-水界面转移的概念框架的形成。该团队还研究了金属单晶上表面氢依赖于电极电势的形成，因为该反应代表氢的演化/产生的第一步，并且仅涉及一个电子和一个质子。质子和电子转移动力学的表面化学用于提供金属-水界面的局部电场信息，通过推进电化学反应的机理知识，未来可以有效地从水中产生或释放氢气的催化剂。设计的。该团队还通过纽约统计局 4-H 青年发展计划将电化学和光学科学的概念转化为外展活动。该团队为康奈尔大学一年级学生提供了有关化学循环的新课程材料。该项目开发了质子耦合电子转移。 (PCET) 机制在明确的单晶金属表面，如铂和钯，这些非均相电化学反应在电催化中很常见；然而，它们很复杂，因为大多数 PCET 反应都涉及转移。研究小组应用一种随时间变化的电分析方法和非线性光谱来探测表面氢的形成，这些研究仅涉及一个质子和一个电子，研究了单晶上的表面氢形成动力学。金属表面作为质子供体和金属化学的函数以及局部电场和表面氧化物测量被用来表征电化学反应过程中的局部电场。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力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

Reactive Crystallization via Metal–Organic-Framework Formation Enables Separation of Terephthalic Acid from Textile Impurities

通过金属有机骨架形成的反应结晶能够从纺织品杂质中分离对苯二甲酸

• DOI: 10.1021/acssuschemeng.2c05496
• 发表时间: 2023
• 期刊: ACS Sustainable Chemistry & Engineering
• 影响因子: 8.4
• 作者: Nason, Abigail K.;Jerozal, Ronald T.;Milner, Phillip J.;Suntivich, Jin
• 通讯作者: Suntivich, Jin