CAS: Enhanced Electrocatalytic Hydrogen Production with Polymer-Supported [2Fe-2S] Clusters

CAS：利用聚合物支撑的 [2Fe-2S] 簇增强电催化产氢

• 批准号: 1954641
• 负责人: Dennis Lichtenberger
• 金额: $ 52万
• 依托单位: University of Arizona
• 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: 2020-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1954641&HistoricalAwards=false
• 关键词: CAS; Enhanced; Electrocatalytic; Hydrogen; Production

With support from the Chemical Catalysis Program of the Division of Chemistry at the National Science Foundation, the research team headed by Professors Dennis Lichtenberger, Jeffrey Pyun, and Richard Glass at the University of Arizona are developing new approaches for producing hydrogen gas from water using electricity. This research is relevant to the U.S. economy because hydrogen gas is used to make many industrial products, including fertilizers and fuels. The team is developing catalysts to speed up the product formation and notably, the catalysts made by this team are made of earth-abundant iron and sulfur. Similar iron-sulfur catalysts are found in nature, but they are fragile. The new catalysts, after being modified with special polymers, are rugged. The goal of this research is to learn how the polymer enhances the catalyst reactivity and to optimize the system's performance so more fuel is produced in less time. One specific project involves changing the structure of the polymer and the way it is attached to the catalyst. This award also provides students with hands-on experience in the areas of catalysis and energy science. Once engaged in a collaborative project, the students are exposed to a variety of disciplines and technical cultures, which makes them better leaders. An integral part of the project is outreach to the community with emphasis on women in STEM and K-12 students and teachers. With support from the Chemical Catalysis (CAT) Program in NSF's Division of Chemistry, the research team headed by Professors Dennis Lichtenberger, Jeffrey Pyun, and Richard Glass at The University of Arizona are developing new catalysts for the production of hydrogen (H2). The research promises to contribute to a clean and sustainable energy economy using intermittent energy sources such as solar and wind as the electricity generated from these sources can be directly stored in the two-electron chemical bond of H2. This same energy can be easily recovered by burning the hydrogen or by converting the energy back to electricity with a fuel cell, both of which cycle the hydrogen back to water. Typically, the most effective materials for converting electricity and water to hydrogen are platinum and other expensive metals that are too rare to employ on a large scale for a broad energy economy. Nature has solved this problem with hydrogenase enzymes, which feature iron sulfides embedded in the structure of the enzyme to efficiently produce hydrogen. With this inspiration from nature, the first-generation system of iron and sulfur embedded in a metallopolymer created by the team at the University of Arizona produces hydrogen 25 times faster than the natural enzyme and approaches platinum in efficiency. The research prepares students for the technical workforce that will support the U.S. economy.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.

在国家科学基金会化学系化学催化计划的支持下，由丹尼斯·利希滕贝格（Dennis Lichtenberger）教授，杰弗里·皮恩（Jeffrey Pyun）和亚利桑那大学的理查德·格拉斯（Richard Glass）领导的研究小组正在开发新的方法，用于使用电力从水中生产氢气。这项研究与美国经济有关，因为氢气被用来制造许多工业产品，包括肥料和燃料。该团队正在开发催化剂来加快产品形成，尤其是，该团队制造的催化剂是由富含地球的铁和硫制成的。 在自然界中也发现了类似的铁硫催化剂，但它们很脆弱。 通过特殊聚合物修饰后，新的催化剂变得坚固。 这项研究的目的是了解聚合物如何增强催化剂的反应性并优化系统的性能，从而在更少的时间内产生更多的燃料。 一个特定的项目涉及更改聚合物的结构及其连接到催化剂的方式。该奖项还为学生提供了催化和能源科学领域的动手经验。 一旦参与了一个协作项目，学生就会接触到各种学科和技术文化，这使他们成为更好的领导者。 该项目不可或缺的一部分是向社区推广，重点是STEM和K-12学生和老师的女性。在NSF化学部的化学催化计划（CAT）计划的支持下，由丹尼斯·利希滕贝格（Dennis Lichtenberger），杰弗里·皮尤（Jeffrey Pyun）教授，杰弗里·皮恩（Jeffrey Pyun）和亚利桑那大学（University of Arizona）的理查德·格拉斯（Richard Glass）领导的研究小组正在开发用于生产氢的新催化剂（H2）。该研究有望使用间歇性的能源（例如太阳能和风能）为清洁和可持续的能源经济做出贡献，因为这些来源产生的电力可以直接存储在H2的两电子化学键中。 通过燃烧氢或将能量转换回电池，可以轻松回收相同的能量，这两者都将氢循环回水。通常，将电和水转换为氢的最有效的材料是铂金和其他昂贵的金属，这些金属太罕见了，无法大规模利用广泛的能源经济。大自然已经用氢化酶解决了这个问题，氢酶酶具有嵌合在酶结构中以有效产生氢的结构中的硫化物。凭借自然的灵感，亚利桑那大学团队创建的铁和硫的第一代系统嵌入了金属聚合物中，其氢比天然酶快25倍，并在效率方面接近铂金。该研究为学生提供了支持美国经济的技术劳动力的准备。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子优点和更广泛影响的评论标准来评估值得支持的。

项目成果

Synthesis of Metallopolymers via Atom Transfer Radical Polymerization from a [2Fe‐2S] Metalloinitiator: Molecular Weight Effects on Electrocatalytic Hydrogen Production

[2Fe-2S] 金属引发剂通过原子转移自由基聚合合成金属聚合物：分子量对电催化产氢的影响

• DOI: 10.1002/marc.201900424
• 发表时间: 2019
• 期刊: Macromolecular Rapid Communications
• 影响因子: 4.6
• 作者: Karayilan, Metin;McCleary‐Petersen, Keelee Cathleen;Hamilton, Meghan O'Brien;Fu, Liye;Matyjaszewski, Krzysztof;Glass, Richard S.;Lichtenberger, Dennis L.;Pyun, Jeffrey
• 通讯作者: Pyun, Jeffrey

Natural Assembly of Electroactive Metallopolymers on the Electrode Surface: Enhanced Electrocatalytic Production of Hydrogen by [2Fe–2S] Metallopolymers in Neutral Water

电极表面电活性金属聚合物的自然组装：[2Fe-2S]金属聚合物在中性水中增强电催化产氢

• DOI: 10.1021/jacs.3c03379
• 发表时间: 2023
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Clary, Kayla E.;Gibson, Arthur C.;Glass, Richard S.;Pyun, Jeffrey;Lichtenberger, Dennis L.
• 通讯作者: Lichtenberger, Dennis L.

Increasing the rate of the hydrogen evolution reaction in neutral water with protic buffer electrolytes

• DOI: 10.1073/pnas.2012085117
• 发表时间: 2020-12-29
• 期刊: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• 影响因子: 11.1
• 作者: Clary, Kayla E.;Karayilan, Metin;Lichtenberger, Dennis L.
• 通讯作者: Lichtenberger, Dennis L.