Studying carbon dioxide-reduction by Fe-Ni Sulfides with modern electronic structure methods:A case of multistate reactivity?

用现代电子结构方法研究铁镍硫化物还原二氧化碳：多态反应性案例？

• 批准号: 471174587
• 负责人: Professor Dr. Michael Roemelt
• 金额: --
• 依托单位: Arbeitsgruppe Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/471174587?language=en
• 关键词: Studying; carbon; dioxide; reduction; Fe

The transformation of CO2 into synthetically valuable products like formic acid, CO or methane has gained a lot of attraction in the field of chemistry in the last years for its obvious benefits. A particularly attractive approach to this goal is represented by electrocatalytic setups that utilize electricity from renewable sources like wind or photovoltaics. Recently, pentlandite electrodes have been introduced as viable materials for the evolution of dihydrogen and the reduction of CO2 with remarkable properties in terms of overpotentials, efficiencies and durability. However, at this point a systematic improvement of the pentlandite material is impeded by a lack of mechanistic insight. The work proposed in here aims at elucidating the mechanistic details of the CO2 reduction on an atomic scale by means of modern electronic structure methods. A central aspect of the proposed research concerns the exploration of the contribution of electronically excited states to the observed reactivity. On account of the structural and electronic properties of pentlandite such contributions are expected to be prominent.

近年来，将二氧化碳转化为甲酸、一氧化碳或甲烷等具有合成价值的产品因其明显的好处而在化学领域引起了广泛的关注。实现这一目标的一种特别有吸引力的方法是利用风能或光伏等可再生能源的电催化装置。最近，镍黄铁矿电极已被引入作为可行的材料，用于析出氢气和还原二氧化碳，在过电势、效率和耐用性方面具有卓越的性能。然而，在这一点上，由于缺乏机械洞察力，镍黄铁矿材料的系统改进受到阻碍。这里提出的工作旨在通过现代电子结构方法阐明原子尺度上二氧化碳还原的机制细节。拟议研究的一个核心方面涉及探索电子激发态对观察到的反应性的贡献。由于镍黄铁矿的结构和电子特性，预计这种贡献将是显着的。