CAS: Innovating New Strategies for Selective Electrocatalytic Reduction

CAS：创新选择性电催化还原新策略

• 批准号: 2102589
• 负责人: Jenny Yang
• 金额: $ 47.5万
• 依托单位: University of California-Irvine
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-04-01 至 2024-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102589&HistoricalAwards=false
• 关键词: CAS; Innovating; New; Strategies; Selective

With the support of the Chemical Catalysis program in the Division of Chemistry, Dr. Jenny Y. Yang of the University of California, Irvine is studying new methods to improve the performance of catalysts that use electrical energy for chemical transformations. Electricity-driven catalysts have many potential economic and environmental advantages over conventional thermal catalysts. They often function under milder conditions, are more energy efficient, and generate less chemical waste. They also have a smaller carbon footprint if operated using renewable electricity. However, some catalysts often convert water to hydrogen as an undesirable side reaction that wastes energy. The proposed study seeks to develop and test catalyst design strategies to inhibit hydrogen evolution while achieving higher yields of the desired products. The concepts will be applied to catalysts that can recycle CO2 into useful products. However, these design strategies are general, and the studies have broader potential to improve the performance of all electricity-driven catalysts. These studies will also provide excellent training for undergraduate and graduate researchers and postdoctoral associates in multiple topics directly relevant to training the next-generation scientific work force. In addition to building expertise in state-of-the-art experimental techniques, they will also develop skills in critical thinking, hypothesis-driven experimental design, and written and oral communication. Additionally, the researchers will work in a highly collaborative team atmosphere that works towards common goals. With the support of the Chemical Catalysis program in the Division of Chemistry, Dr. Jenny Y. Yang of the University of California, Irvine is studying new strategies for selective electrocatalytic reduction. Electrochemical methods for reduction have several advantages over the use of stoichiometric reductants. These include the ability to dial in a redox potential to elicit greater reaction selectivity, fewer operational hazards and reduced chemical waste. However, electrochemical and electrocatalytic reduction reactions that require protons often suffer from low Faradaic yields due to direct proton reduction to hydrogen. The challenge of product selectivity over hydrogen evolution is pervasive throughout electrochemical reduction reactions. The studies will pursue catalyst design strategies to kinetically suppress proton reduction while not inhibiting the reduction of desired substrates. The strategies will be tested on complexes designed to have CO2 reduction activity. Electrocatalytic CO2 reduction toward fuels is important as a mechanism for renewable energy storage and transport. Thus, the proposed research will concurrently develop guidelines for mediating electrochemical reduction and result in new catalysts and mechanistic insights into CO2 reduction to fuels. However, the design strategies are generalizable to a broad range of catalysts, from electro-organic reduction to other feedstock-to-fuel reductions.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.

在化学系化学催化项目的支持下，Jenny Y.加州大学欧文分校的Yang正在研究新的方法来提高利用电能进行化学转化的催化剂的性能。与传统的热催化剂相比，电驱动催化剂具有许多潜在的经济和环境优势。它们通常在温和的条件下工作，更节能，产生的化学废物更少。如果使用可再生电力，它们的碳足迹也会更小。然而，一些催化剂通常将水转化为氢气，这是浪费能量的不期望的副反应。拟议的研究旨在开发和测试催化剂设计策略，以抑制析氢，同时实现所需产品的更高收率。这些概念将应用于可以将CO2回收为有用产品的催化剂。然而，这些设计策略是通用的，并且这些研究具有更广泛的潜力来改善所有电驱动催化剂的性能。这些研究还将为本科生和研究生研究人员以及博士后研究人员提供与培训下一代科学工作者直接相关的多个主题的优秀培训。除了建立国家的最先进的实验技术的专业知识，他们还将开发批判性思维，假设驱动的实验设计，以及书面和口头沟通的技能。此外，研究人员将在高度协作的团队氛围中工作，为共同的目标而努力。在化学系化学催化项目的支持下，Jenny Y.加州大学欧文分校的Yang正在研究选择性电催化还原的新策略。还原的电化学方法与使用化学计量的还原剂相比具有若干优点。这些包括在氧化还原电位拨号的能力，以引起更大的反应选择性，更少的操作危险和减少化学废物。然而，需要质子的电化学和电催化还原反应由于直接质子还原成氢而经常遭受低法拉第产率。产物选择性相对于析氢的挑战在整个电化学还原反应中是普遍存在的。这些研究将追求催化剂设计策略，以动力学抑制质子还原，同时不抑制所需底物的还原。这些策略将在旨在具有CO2减排活性的复合物上进行测试。电催化CO2还原为燃料作为可再生能源储存和运输的机制是重要的。因此，拟议的研究将同时制定介导电化学还原的指南，并产生新的催化剂和将二氧化碳还原为燃料的机理见解。然而，设计策略可推广到广泛的催化剂，从电有机还原到其他原料到燃料的还原。该奖项反映了NSF的法定使命，并被认为值得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。

项目成果

Inhibiting the Hydrogen Evolution Reaction (HER) with Proximal Cations: A Strategy for Promoting Selective Electrocatalytic Reduction

• DOI: 10.1021/acscatal.1c01527
• 发表时间: 2021-06-18
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Barlow, Jeffrey M.;Ziller, Joseph W.;Yang, Jenny Y.
• 通讯作者: Yang, Jenny Y.

Uniting biological and chemical strategies for selective CO2 reduction

• DOI: 10.1038/s41929-021-00683-1
• 发表时间: 2021-11-01
• 期刊: NATURE CATALYSIS
• 影响因子: 37.8
• 作者: Shafaat, Hannah S.;Yang, Jenny Y.
• 通讯作者: Yang, Jenny Y.

Thermochemical Studies of Nickel Hydride Complexes with Cationic Ligands in Aqueous and Organic Solvents

氢化镍与阳离子配体在水和有机溶剂中配合物的热化学研究

• DOI: 10.1021/acs.organomet.2c00319
• 发表时间: 2022
• 期刊: Organometallics
• 影响因子: 2.8
• 作者: Cypcar, Andrew D.;Kerr, Tyler A.;Yang, Jenny Y.
• 通讯作者: Yang, Jenny Y.