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Study of Hydrogen Evolution by a Series of Metal-Mabiq complexes

一系列金属-Mabiq配合物析氢的研究

基本信息

批准号：
319960088
负责人：
Professor Dr. Hubert A. Gasteiger
金额：
--
依托单位：
Institut für Anorganische Chemie
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2016
资助国家：
德国
起止时间：
2015-12-31 至 2019-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/319960088?language=en
关键词：
Study Hydrogen Evolution Series Metal

项目摘要

The project focuses on a family of macrocyclic metal complexes, and their ability to act as catalysts for hydrogen production. Hydrogen is a promising fuel alternative. However, the realization of hydrogen as an alternate fuel demands the development of efficient, economical catalysts for its production. Significant advances have been made toward the development of late first-row transition metal electrocatalysts for this reaction. Yet aspects of the reaction mechanism remain unresolved, and catalyst features still need to be optimized, warranting further research and new catalyst platforms. We herein describe studies to examine, in detail, electrocatalytic hydrogen evolution by a series of metal compounds coordinated by a unique redox-active macrocyclic ligand, Mabiq. The project consists of in-depth mechanistic and structure-function studies, with the following key objectives:1. to examine the catalytic performance of cobalt-Mabiq complexes;2. to identify the available pathway(s) for hydrogen evolution by the Co-Mabiq complexes, and associated reaction intermediates;3. to investigate structural contributions to catalyst reactivity, by additionally examining complexes containing Fe and Ni, and modified ligands;4. to explore the coordination chemistry of an available second metal binding site of our ligand, including an initial examination of its influence on catalysis.The project will employ a combination of synthetic, electrochemical and spectroscopic methods, and reactivity studies.The research aims to address unsettled aspects of the hydrogen evolution reaction mechanism, and to contribute to the design of enhanced catalysts.

该项目的重点是一系列大环金属络合物，以及它们作为氢气生产催化剂的能力。氢气是一种很有前途的燃料替代品。然而，实现氢气作为替代燃料需要开发高效、经济的催化剂来生产氢气。用于该反应的晚期第一排过渡金属电催化剂的开发已经取得了重大进展。然而，反应机理的一些方面仍然没有解决，催化剂的性能仍然需要优化，需要进一步的研究和新的催化剂平台。在这里，我们描述了一系列由独特的氧化还原活性大环配体Mabiq配位的一系列金属化合物电催化放氢的研究。该项目包括深入的机理和结构-功能研究，主要目标如下：1.考察Co-Mabiq络合物的催化性能；2.确定Co-Mabiq络合物及其相关反应中间体析氢的有效途径(S)；3.通过考察含Fe、Ni的络合物和修饰配体，考察结构对催化剂反应活性的贡献；4.探索配体的第二金属结合部位的配位化学，包括初步考察其对催化剂的影响。该项目将采用合成、电化学和光谱方法相结合的方法，并进行反应性研究。研究旨在解决析氢反应机理中尚未解决的方面，并为增强型催化剂的设计做出贡献。