Interparticle Metal-Metal Interactions in Electrocatalytic Carbon Dioxide Reduction Reactions

电催化二氧化碳还原反应中的颗粒间金属-金属相互作用

• 批准号: 2028351
• 负责人: Hailiang Wang
• 金额: $ 44.47万
• 依托单位: Yale University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-10-01 至 2023-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2028351&HistoricalAwards=false
• 关键词: Interparticle; Metal; Interactions; Electrocatalytic; Carbon

A major challenge in the transition to clean energy is reducing emissions of carbon dioxide from fuel combustion. Using renewable electricity to convert carbon dioxide to value-added fuels and chemical products is a promising way of turning carbon emissions into a resource. Palladium is a unique metal that can catalyze the electrochemical conversion of carbon dioxide to formate ion (HCOO-). Formate is a building-block compound that can be used to produce industrially important chemicals such as formaldehyde and methanol. The catalytic performance of palladium, however, is severely limited by rapid deactivation of the catalyst active site, and it is difficult to design improved systems without further understanding of both the reaction and deactivation mechanisms. This research project will study novel catalysts composed of palladium and a secondary metal. The aim is to stabilize the catalyst active site and thereby develop catalysts can perform the sustained, efficient conversion of carbon dioxide into formate. This research project also will foster new teaching and learning opportunities for a large and diverse body of students.The aim of this research project is to investigate how nanoscale interparticle metal-metal interactions influence the catalytic mechanisms of carbon dioxide electroreduction on palladium. The goals are to limit catalyst deactivation during the production of formate and to enable the synthesis of new products such as formaldehyde or methanol. Metal nanoparticles will be used as “electronic ligands” and modify the binding strength of palladium with reaction intermediates. The nanoparticles also can act as “collaborative ligands” that directly participate in catalysis by providing a secondary type of surface site. The electronic and collaborative interactions between palladium and a variety of other metals will be studied. Additionally, experiments will be performed to learn how these interactions change the binding energetics of palladium with the reaction intermediates and the potential-dependent reduction reaction pathways. Ultimately, the knowledge gained from these studies will be used to develop electrocatalysts that are stable for efficient conversion of carbon dioxide to formate and then on to more complex products.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.

过渡到清洁能源的主要挑战是从燃料组成中减少二氧化碳的排放。使用可再生电力将二氧化碳转换为增值燃料和化学产品是将碳排放转化为资源的有希望的方法。钯是一种独特的金属，可以催化二氧化碳形成离子（HCOO-）的电化学转化。格式是一种建筑块化合物，可用于生产工业重要的化学物质，例如甲醛和甲醇。然而，钯的催化性能受到催化剂活性位点的快速失活的严重限制，并且在不进一步了解反应和失活机制的情况下，很难设计改进的系统。该研究项目将研究由钯和二级金属组成的新型催化剂。目的是稳定催化剂活性位点，从而开发催化剂可以执行二氧化碳持续，有效地转化为形式。该研究项目还将为大量学生提供新的教学机会。该研究项目的目的是调查纳米级粒子间金属 - 金属相互作用如何影响二氧化碳电动量的催化机制对钯的催化机制。目标是限制在形式生产过程中催化剂停用，并能够合成诸如甲醛或甲醇之类的新产品。金属纳米颗粒将用作“电子配体”，并改变钯与反应中间体的结合强度。纳米颗粒也可以用作“协作配体”，通过提供次要的表面位点直接参与催化。钯与其他各种金属之间的电子和协作相互作用将研究。此外，将进行实验，以了解这些相互作用如何改变钯的结合能源与反应中间体和潜在的依赖性还原反应途径。最终，从这些研究中获得的知识将用于开发电催化剂，这些电催化剂稳定，以有效地转化二氧化碳形成，然后再呈更复杂的产品。这项奖项反映了NSF的法定任务，并被认为是通过基金会的知识分子优点和更广泛的影响审查标准来通过评估而被认为是珍贵的支持。

项目成果

Cascade electrocatalytic reduction of carbon dioxide and nitrate to ethylamine

• DOI: 10.1016/j.jechem.2021.06.007
• 期刊: Journal of Energy Chemistry
• 影响因子: 13.1
• 作者: Zixu Tao;Yueshen Wu;Zishan Wu;Bo Shang;Conor L. Rooney;Hailiang Wang

Intrinsic Catalytic Activity of Carbon Nanotubes for Electrochemical Nitrate Reduction

• DOI: 10.1021/acscatal.2c01144
• 发表时间: 2022-08-05
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Harmon, Nia J.;Rooney, Conor L.;Wang, Hailiang
• 通讯作者: Wang, Hailiang