Development of Hybrid Solid Materials for Stable Molecular Oxygen Anodes

稳定分子氧阳极混合固体材料的开发

• 批准号: 1805022
• 负责人: Thomas Gunnoe
• 金额: $ 70万
• 依托单位: University of Virginia Main Campus
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2022-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1805022&HistoricalAwards=false
• 关键词: Development; Hybrid; Solid; Materials; Stable

Electrocatalysts are materials that make electrically-driven chemical reactions proceed faster, more efficiently, and/or with less input of electricity. This project will involve discovery of new catalytic materials for efficient electrochemical oxidation of water to produce hydrogen and oxygen, where the hydrogen can be used directly as a fuel to produce electricity in hydrogen fuel cells, or as a reactant to upgrade low-grade carbon-containing compounds to high-value fuels and chemicals. The project will address a critical step in a sustainable process for converting solar energy to chemical energy, thus alleviating dependence on fossil resources. This is a collaborative effort that brings together Professors Thomas Gunnoe and Sen Zhang from the University of Virginia with Professor William Goddard from the California Institute of Technology and scientists from the Max Planck Institute for Chemical Energy Conversion, working under the MAXNET Energy consortium. The international collaboration will enhance U.S. research eminence in the science and engineering of sustainable energy. The project will also involve educational outreach to primarily undergraduate institutions (PUIs) to increase interest among students from diverse backgrounds in careers as scientists and engineers. This project represents a cross-disciplinary effort to develop, understand and test new carbon-supported copper and cobalt materials for electrocatalytic water oxidation. It incorporates groups with expertise in molecular catalysis, nanomaterials, computational modeling, and carbon materials and catalyst characterization. The primary foundation is to develop and optimize multi-nuclear molecular catalysts and then integrate these units into carbon-based materials. Participation in the MAXNET Energy consortium will provide assessment of new catalyst materials under a standardized set of protocols to provide rigorous comparison and benchmarking to other heterogeneous catalytic materials. To achieve these goals, three objectives will be pursued: 1) prepare a series of multi-nuclear cobalt and copper complexes with variable molecular and electronic structure - as guided by computational modeling - to provide an understanding of structure-activity relationships; 2) support multi-nuclear molecular complexes on conductive carbonaceous materials; 3) study the OER activity and stability of carbon-supported catalysts. Educational outreach will involve visits by graduate students to the PUIs to deliver short courses based on their research, combined with participation of undergraduate students in summer research internships in the PIs' laboratories.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.

电催化剂是一种材料，它可以使电驱动的化学反应进行得更快，更有效，和/或更少的电力输入。该项目将涉及发现新的催化材料，用于水的有效电化学氧化产生氢和氧，其中氢可以直接用作氢燃料电池中发电的燃料，或作为将低品位含碳化合物升级为高价值燃料和化学品的反应物。该项目将处理将太阳能转化为化学能的可持续进程中的一个关键步骤，从而减轻对矿物资源的依赖。这是一项由弗吉尼亚大学的Thomas Gunnoe教授和Sen Zhang教授、加州理工学院的William Goddard教授和马克斯普朗克化学能转换研究所的科学家共同合作的成果，他们在MAXNET能源联盟下工作。这项国际合作将提高美国在可持续能源科学和工程方面的研究地位。该项目还将涉及向主要的本科院校（PUIs）进行教育推广，以增加来自不同背景的学生对科学家和工程师职业的兴趣。该项目代表了跨学科的努力，以开发、理解和测试用于电催化水氧化的新型碳支撑铜和钴材料。它整合了分子催化，纳米材料，计算建模，碳材料和催化剂表征方面的专业知识。主要的基础是开发和优化多核分子催化剂，然后将这些单元整合到碳基材料中。参与MAXNET能源联盟将根据一套标准化的协议对新催化剂材料进行评估，从而对其他多相催化材料进行严格的比较和基准测试。为了实现这些目标，将追求三个目标：1)在计算建模的指导下，制备一系列具有可变分子和电子结构的多核钴和铜配合物，以提供对结构-活性关系的理解；2)在导电碳质材料上支持多核分子配合物；3)研究碳负载催化剂的OER活性和稳定性。教育拓展将包括研究生访问公共关系学院，根据他们的研究提供短期课程，同时本科生参加公共关系学院实验室的暑期研究实习。该奖项反映了美国国家科学基金会的法定使命，并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

Atomistic Explanation of the Dramatically Improved Oxygen Reduction Reaction of Jagged Platinum Nanowires, 50 Times Better than Pt

• DOI: 10.1021/jacs.9b13218
• 发表时间: 2020-05-13
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Chen, Yalu;Cheng, Tao;Goddard, William A., III
• 通讯作者: Goddard, William A., III

Electrocatalytic Water Oxidation by a Trinuclear Copper(II) Complex

• DOI: 10.1021/acscatal.1c01395
• 发表时间: 2021-06-04
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Geer, Ana M.;Musgrave, Charles, III;Gunnoe, T. Brent
• 通讯作者: Gunnoe, T. Brent

Stabilizing Highly Active Ru Sites by Suppressing Lattice Oxygen Participation in Acidic Water Oxidation

通过抑制晶格氧参与酸性水氧化来稳定高活性 Ru 位点

• DOI: 10.1021/jacs.1c00384
• 发表时间: 2021
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Wen Yun Zhou;Chen Pei Ning;Wang Lu;Li Shang Yu;Wang Zi Yun;Abed Jehad;Mao Xin Nan;Min Yi Meng;Dinh Cao Thang;De Luna Phil;Huang Rui;Zhang Long Sheng;Wang Lie;Wang Li Ping;Nielsen Robert J.;Li Hui Hui;Zhuang Tao Tao;Ke Chang Chun;Voznyy Oleks;r;Hu Yong F
• 通讯作者: Hu Yong F

New Quantum Mechanics Based Methods for Multiscale Simulations with Applications to Reaction Mechanisms for Electrocatalysis

• DOI: 10.1007/s11244-020-01369-x
• 发表时间: 2020-09
• 期刊: Topics in Catalysis
• 影响因子: 3.6
• 作者: W. Goddard

Development of the ReaxFF Reactive Force Field for Cu/Si Systems with Application to Copper Cluster Formation during Cu Diffusion Inside Silicon

• DOI: 10.1021/acs.jpcc.1c04178
• 发表时间: 2021-08
• 期刊: The Journal of Physical Chemistry C
• 作者: Kamyar Akbari Roshan;Mahdi Khajeh Talkhoncheh;J. Mueller;W. Goddard;A. V. van Duin