Collaborative Research: Dinuclear Heterogeneous Catalysts (DHCs) as a new Platform for Selective Oxidation of Carbon Monoxide (CO) and Methane (CH4)

合作研究：双核多相催化剂（DHC）作为一氧化碳（CO）和甲烷（CH4）选择性氧化的新平台

• 批准号: 1955786
• 负责人: Xiaoqing Pan
• 金额: $ 15万
• 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: 2020
• 资助国家: 美国
• 起止时间: 2020-06-01 至 2024-05-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1955786&HistoricalAwards=false
• 关键词: Collaborative; Research; Dinuclear; Heterogeneous; Catalysts

Catalysts, substances that increase the speed of chemical reactions without themselves being consumed, play critical roles in large-scale chemical processes that underpin our economy. One example is found in the reforming of natural gas, where catalysts convert methane to hydrogen and carbon monoxide (CO). Hydrogen can be readily used as a source of clean energy. CO can serve as a starting material for the synthesis of valuable chemicals such as methanol and acetic acid. A critical challenge presented by the current natural gas reforming processes, however, is that they are often energy intensive. The key to addressing this inefficiency is through novel catalyst designs. With funding from the Chemical Catalysis Program of the Division of Chemistry, Dr. Wang of Boston College, Drs. Batista and Brudvig of Yale University, and Dr. Pan of the University of California, Irvine are investigating a new type of catalyst that has the potential to meet this challenge. Featuring precisely designed and defined structures, the catalysts are being studied for two prototypical reactions, carbon monoxide oxidation and methane activation. In an effort to broaden the impacts of the project, concerted educational and outreach activities are being carried out. These programs involve participants from diverse backgrounds, especially those of underrepresented minorities. With funding from the Chemical Catalysis Program of the Division of Chemistry, this project studies new class of catalysts, dinuclear heterogeneous catalysts (DHCs), for selective oxidation of CO and methane (CH4). DHCs belong to the emerging class of heterogeneous catalysts featuring atomically dispersed motifs. They offer new properties for chemical transformations. Dr. Wang from Boston College, Drs. Batista and Brudvig from Yale University, and Dr. Pan from the University of California, Irvine leverage their complementary expertise in catalyst design, synthesis, characterization, and reaction mechanisms. They collaborate to test the hypothesis that DHCs are more effective toward reactions such as selective CO oxidation and CH4 activation, than conventional catalysts or the recently characterized single-atom catalysts. The study is unique as it examines the involvement of heterogeneous catalysts with dinuclear active centers whose catalytic core is well defined. The research activities are complemented by educational efforts aimed at promoting scientific research by underrepresented groups, K-12 students, and the general public as well as undergraduate researchers.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.

催化剂是一种能够提高化学反应速度而不消耗自身的物质，在支撑我们经济的大规模化学过程中发挥着关键作用。天然气重整就是一个例子，其中催化剂将甲烷转化为氢气和一氧化碳 (CO)。氢可以很容易地用作清洁能源。 CO可以作为合成有价值化学品（例如甲醇和乙酸）的起始材料。然而，当前天然气重整过程提出的一个关键挑战是它们通常是能源密集型的。解决这种低效率问题的关键是通过新颖的催化剂设计。在化学系化学催化项目的资助下，波士顿学院王博士、Drs.耶鲁大学的巴蒂斯塔和布鲁德维格以及加州大学欧文分校的潘博士正在研究一种有潜力应对这一挑战的新型催化剂。该催化剂具有精确设计和定义的结构，正在研究一氧化碳氧化和甲烷活化这两种典型反应。为了扩大该项目的影响，正在开展协调一致的教育和推广活动。这些计划涉及来自不同背景的参与者，尤其是代表性不足的少数群体。在化学系化学催化项目的资助下，该项目研究新型催化剂，即双核多相催化剂（DHC），用于选择性氧化CO和甲烷（CH4）。 DHC 属于新兴的多相催化剂，具有原子分散的基序。它们为化学转化提供了新的特性。波士顿学院王博士耶鲁大学的巴蒂斯塔和布鲁德维格以及加州大学欧文分校的潘博士利用他们在催化剂设计、合成、表征和反应机制方面的互补专业知识。他们合作测试了这样的假设：与传统催化剂或最近表征的单原子催化剂相比，DHC 对选择性 CO 氧化和 CH4 活化等反应更有效。这项研究是独一无二的，因为它研究了具有明确催化核心的双核活性中心的多相催化剂的参与。这些研究活动得到了教育工作的补充，旨在促进代表性不足的群体、K-12 学生、公众以及本科研究人员的科学研究。该奖项反映了 NSF 的法定使命，并通过使用基金会的评估进行评估，认为值得支持。智力价值和更广泛的影响审查标准。

项目成果

Directly Probing the Local Coordination, Charge State, and Stability of Single Atom Catalysts by Advanced Electron Microscopy: A Review

通过先进电子显微镜直接探测单原子催化剂的局域配位、电荷状态和稳定性：综述

• DOI: 10.1002/smll.202006482
• 发表时间: 2021-02
• 期刊: Small
• 影响因子: 13.3
• 作者: Tieu, Peter;Yan, Xingxu;Xu, Mingjie;Christopher, Phillip;Pan, Xiaoqing
• 通讯作者: Pan, Xiaoqing

Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts

双核多相催化剂高度稳定的一氧化碳优先氧化

• DOI: 10.1073/pnas.2206850120
• 发表时间: 2023-01-03
• 期刊: Proceedings of the National Academy of Sciences
• 作者: Zhao, Yanyan;Dai, Sheng;Yang, Ke R.;Cao, Sufeng;Materna, Kelly L.;Lant, Hannah M.;Kao, Li Cheng;Feng, Xuefei;Guo, Jinghua;Brudvig, Gary W.;et al
• 通讯作者: et al