SusChEM: Electrocatalysis with Butterfly [2Fe-2S] Clusters

SusChEM：蝴蝶 [2Fe-2S] 簇的电催化

基本信息

批准号：
1664745
负责人：
Dennis Lichtenberger
金额：
$ 55.09万
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：
2017
资助国家：
美国
起止时间：
2017-09-01 至 2021-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1664745&HistoricalAwards=false
关键词：
SusChEM Electrocatalysis Butterfly 2Fe 2S

项目摘要

SusChEM: Electrocatalysis with Butterfly [2Fe-2S] ClustersThe production of hydrogen, the simplest molecule, is a multi-billion dollar industry today that provides hydrogen primarily for combination with nitrogen to produce ammonia fertilizer needed to grow sufficient food for the world population, for removal of sulfur from fossil fuels, and for industrial applications needed to produce the materials for a modern society. Furthermore, one of the grand challenges facing the world today is the need for sustainable, clean, and cost-effective sources of energy and fuels. Hydrogen is a high energy fuel that on burning (or in fuel cells) simply has water as the exhaust product. Unfortunately 96% of the hydrogen produced today is obtained from the expensive action of extremely high temperature and pressure steam on hydrocarbons, a process that is wasteful of both energy and raw materials. Analysis shows that 2% of the world energy is used in these processes and half the world population would not be alive today without the process that uses hydrogen to produce fertilizer for food production. This research project, funded by the Catalysis Program of the Chemistry Division, is exploring the use of electricity to produce hydrogen directly from water in an efficient, clean and sustainable process. To effect the production of hydrogen from water at low temperature and pressure, an inexpensive, readily available catalyst is required. Professors Dennis L. Lichtenberger, Jeffrey Pyun and Richard S. Glass of the University of Arizona and Professor Dennis H. Evans of Purdue University are investigating the production of hydrogen from water using electricity and catalysts composed of inexpensive and plentiful iron and sulfur.The catalysts in this study are inspired by an enzyme found in anaerobic bacteria that produces hydrogen from a [2Fe-2S] cluster site that has a structure denoted as a ?butterfly? type. Although the enzyme generates hydrogen very rapidly, the organometallic butterfly [2Fe-2S] clusters prepared in this project are orders of magnitude faster. The high rates of hydrogen production observed in this project indicate different factors are at play compared to both the biological enzyme and to other inorganic catalysts. This project is exploring the synthesis of new organometallic [2Fe-2S] cluster catalysts and investigating (1) the mechanism that allows for such fast electrocatalytic hydrogen production, (2) the incorporation of the [2Fe-2S] clusters into metallopolymers for increased water solubility and durability of the catalysts, and (3) approaches to achieve high stability of the reactive catalysts in air. The project combines expertise in synthetic organometallic chemistry, polymer chemistry, electrochemistry, and computational chemistry directed toward the fundamental understanding needed to devise efficient electrocatalytic production of molecular hydrogen from water, and educates students in the multidisciplinary and team approaches needed to address complex scientific challenges in the future.

Suschem：用蝴蝶[2FE-2S]的电催化分析簇的产生，最简单的分子是当今数十亿美元的行业，它主要提供氢与氮与氮的结合，以生产为世界种植足够的食物，以生长足够的食物，以便为世界种植从化石燃料中除去硫，以及为现代社会生产材料所需的工业应用。此外，当今世界面临的巨大挑战之一是需要可持续，清洁和成本效益的能源和燃料来源。氢是一种高能燃料，在燃烧（或燃料电池中）仅将水作为排气产品。不幸的是，当今生产的氢中有96％是从碳氢化合物上极高的温度和压力蒸汽的昂贵作用中获得的，碳氢化合物的压力蒸汽是浪费能量和原材料的过程。分析表明，如果没有使用氢生产肥料进行粮食生产的过程，今天世界中有2％的世界能够在这些过程中使用。该研究项目由化学部催化计划资助，正在探索用电在有效，干净和可持续的过程中直接从水中产生氢的使用。为了在低温和压力下从水中产生氢的产生，需要廉价，随时可用的催化剂。亚利桑那大学的丹尼斯·L·利希滕伯格（Dennis L. Lichtenberger），杰弗里·皮恩（Jeffrey Pyun）和理查德·S·格拉斯（Richard S.在这项研究中，灵感来自在厌氧细菌中发现的酶，该酶从[2FE-2S]簇位点产生氢，该簇的结构表示为？蝴蝶？类型。尽管该酶产生的氢很快，但在该项目中制备的有机金属蝴蝶[2FE-2S]簇的速度更快。在该项目中观察到的高氢生产率表明，与生物学酶和其他无机催化剂相比，不同的因素在起作用。该项目正在探索新的有机金属[2FE-2S]簇催化剂的合成并研究（1）允许这种快速的电催化氢产生的机制，（2）将[2FE-2S]簇掺入金属聚合物中，以增加水的水催化剂的溶解度和耐用性，以及（3）实现空气中反应性催化剂的高稳定性的方法。该项目结合了合成有机金属化学，聚合物化学，电化学和计算化学方面的专业知识，该项目针对设计有效的电催化产生分子氢的基本理解，并教育学生在多学科和团队方法中教育学生，以应对多学科和团队的方法，以应对复杂的科学挑战。未来。

项目成果

期刊论文数量（7）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

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

Catalytic Metallopolymers from [2Fe‐2S] Clusters: Artificial Metalloenzymes for Hydrogen Production

[2Fe-2S] 簇催化金属聚合物：用于制氢的人工金属酶

DOI：
10.1002/ange.201813776
发表时间：
2019
期刊：
Angewandte Chemie
影响因子：
0
作者：
Karayilan, Metin;Brezinski, William P.;Clary, Kayla E.;Lichtenberger, Dennis L.;Glass, Richard S.;Pyun, Jeffrey
通讯作者：
Pyun, Jeffrey

Water-soluble and air-stable [2Fe-2S]-metallopolymers: A new class of electrocatalysts for H 2 production via water splitting

水溶性且空气稳定的[2Fe-2S]金属聚合物：通过水分解生产H 2 的新型电催化剂

DOI：
10.1080/10426507.2019.1603705
发表时间：
2019
期刊：
and Silicon and the Related Elements
影响因子：
0
作者：
Glass, Richard S.;Pyun, Jeffrey;Lichtenberger, Dennis L.;Brezinski, William P.;Karayilan, Metin;Clary, Kayla E.;Pavlopoulos, Nicholas G.;Evans, Dennis H.
通讯作者：
Evans, Dennis H.

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.