Collaborative Research: SusChEM: Understanding Hydrogen Interactions with Metastable Surfaces for Tunable Catalysis Systems

合作研究：SusChEM：了解可调谐催化系统的氢与亚稳态表面的相互作用

• 批准号: 1665305
• 负责人: Jin Suntivich
• 金额: $ 43.73万
• 依托单位: Cornell University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-07-01 至 2021-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1665305&HistoricalAwards=false
• 关键词: Collaborative; Research; SusChEM; Understanding; Hydrogen

The ability to transform abundant resources, such as carbon dioxide and water, into energy-dense fuels and high-valued chemicals plays an important role in our pursuit of sustainable energy and chemical technologies. These processes often benefit from the presence of a heterogeneous catalyst, a solid substance that is able to direct the chemical reactions along faster, more efficient pathways. Designing catalyst materials with structure and compositions tailored to accelerate the desired chemical transformations is an important area of chemical research. In this project, a collaborative effort among Dr. Richard Hennig, Dr. Richard Robinson, and Dr. Jin Suntivich targets variation in composition and structure to create catalysts known as "metastable catalysts" since they fall outside of the normal solubility and structural ranges. The team is examining how to design and build metastable catalysts that efficiently and selectively convert carbon dioxide and water to hydrogen and high-valued compounds. Beyond creating new knowledge that can bring more sustainable energy and chemical technologies closer to reality, the investigators are actively engaged in outreach educational activities. These include a summer internship in the principle investigators' laboratories for undergraduate students and the creation of catalysis demonstration kits designed to disseminate the concepts of atomic building blocks and their role in catalysis technology. These activities are directed at improving student interest in chemical science and materials technology from the K-12 to undergraduate levels, and particularly target women and members of underrepresented minorities to build diversity in the STEM workforce.With support from the Chemical Catalysis program of the Chemistry Division, a collaborative project among Dr. Richard Hennig, Dr. Richard Robinson, and Dr. Jin Suntivich is examining how metastable surfaces can be structured to control the surface hydrogen interaction, and, consequently, the hydrogen evolution reaction and carbon dioxide reduction catalysis. The surface hydrogen interaction is believed to play an important role in stabilizing the intermediates of the hydrogen evolution reaction and the selectivity of the carbon dioxide reduction reaction. This project exploits metastable oxysulfide nanocrystals as model systems with expanded compositional ranges to enable a systematic analysis of composition, surface interaction and electrocatalytic performance. Combined theoretical and experimental studies are used in collaboration to verify the structure - activity connection at the atomic level and allows the PIs to determine how to design the surface structure and composition rationally to improve the catalysis performance. Broader impacts of the research result from an improved understanding of catalyst function and design in sustainable energy and chemical technologies. Broader impacts made through educational activities include graduate and undergraduate student trainings in chemical catalysis research from both theory and experiment sides in the principal investigators' laboratories. Additionally, catalysis demonstration kits are created to visually illustrate how to build catalytic nanomaterials from atomic building blocks and how each different building block can affect selected catalysis performance.

将二氧化碳和水等丰富资源转化为能量密集型燃料和高价值化学品的能力在我们追求可持续能源和化学技术的过程中发挥着重要作用。 这些过程通常受益于非均相催化剂的存在，这种固体物质能够引导化学反应沿着更快、更有效的途径进行。 设计具有适合加速所需化学转化的结构和成分的催化剂材料是化学研究的一个重要领域。 在该项目中，Richard Hennig 博士、Richard Robinson 博士和 Jin Suntivich 博士共同致力于改变成分和结构，以制造被称为“亚稳态催化剂”的催化剂，因为它们超出了正常的溶解度和结构范围。 该团队正在研究如何设计和构建亚稳态催化剂，以有效、选择性地将二氧化碳和水转化为氢气和高价值化合物。除了创造可以使更可持续的能源和化学技术更接近现实的新知识之外，研究人员还积极参与外展教育活动。其中包括为本科生在主要研究人员实验室进行暑期实习，以及创建催化演示套件，旨在传播原子构建单元的概念及其在催化技术中的作用。这些活动旨在提高从 K-12 到本科阶段的学生对化学科学和材料技术的兴趣，特别针对女性和代表性不足的少数族裔成员，以建立 STEM 劳动力队伍的多样性。在化学学院化学催化项目的支持下Division 是 Richard Hennig 博士、Richard Robinson 博士和 Jin Suntivich 博士之间的一个合作项目，正在研究如何构建亚稳态表面来控制表面氢相互作用，从而控制析氢反应和二氧化碳还原催化。表面氢相互作用被认为在稳定析氢反应的中间体和二氧化碳还原反应的选择性方面发挥着重要作用。该项目利用亚稳态硫氧化物纳米晶体作为具有扩展组成范围的模型系统，以实现对组成、表面相互作用和电催化性能的系统分析。理论与实验研究相结合，在原子水平上验证结构-活性联系，使PI能够确定如何合理设计表面结构和组成，以提高催化性能。该研究的更广泛影响源于对可持续能源和化学技术中催化剂功能和设计的更好理解。 通过教育活动产生的更广泛影响包括主要研究人员实验室的理论和实验方面的化学催化研究研究生和本科生培训。此外，还创建了催化演示套件，以直观地说明如何从原子构件构建催化纳米材料，以及每种不同的构件如何影响选定的催化性能。

项目成果

Iron and nitrogen-doped double gyroid mesoporous carbons for oxygen reduction in acidic environments

• DOI: 10.1088/2515-7655/abc31a
• 发表时间: 2020-11
• 期刊: Journal of Physics: Energy
• 作者: F. Matsuoka;Kevin E. Fritz;P. Beaucage;Fei Yu;Jin Suntivich;U. Wiesner

Tertiary Hierarchical Complexity in Assemblies of Sulfur-Bridged Metal Chiral Clusters

• DOI: 10.1021/jacs.0c04764
• 发表时间: 2020-08-26
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Han, Haixiang;Yao, Yuan;Robinson, Richard D.
• 通讯作者: Robinson, Richard D.

Multiscale hierarchical structures from a nanocluster mesophase

• DOI: 10.1038/s41563-022-01223-3
• 发表时间: 2022-04-14
• 期刊: NATURE MATERIALS
• 影响因子: 41.2
• 作者: Han, Haixiang;Kallakuri, Shantanu;Robinson, Richard D.
• 通讯作者: Robinson, Richard D.

Predicting the Electrochemical Synthesis of 2D Materials from First Principles

• DOI: 10.1021/acs.jpcc.8b10802
• 发表时间: 2019-02-07
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY C
• 影响因子: 3.7
• 作者: Ashton, Michael;Trometer, Nicole;Hennig, Richard G.
• 通讯作者: Hennig, Richard G.

Assessment of Soft Ligand Removal Strategies: Alkylation as a Promising Alternative to High-Temperature Treatments for Colloidal Nanoparticle Surfaces

• DOI: 10.1021/acsmaterialslett.9b00089
• 发表时间: 2019-06
• 期刊: ACS Materials Letters
• 影响因子: 11.4
• 作者: Andrew Nelson;Yixu Zong;Kevin E. Fritz;Jin Suntivich;R. D. Robinson