A Photochemical CO2 Reduction Over Supported Single Atom Catalyst: A Knowledge Driven Approach From Molecular to Heterogeneous Catalysis

负载单原子催化剂上的光化学二氧化碳还原：从分子催化到多相催化的知识驱动方法

• 批准号: EP/X024822/1
• 负责人: Erwin Reisner
• 金额: $ 24.26万
• 依托单位: University of Cambridge
• 依托单位国家: 英国
• 项目类别: Fellowship
• 财政年份: 2023
• 资助国家: 英国
• 起止时间: 2023 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FX024822%2F1
• 关键词: Photochemical; CO2; Reduction; Over; Supported

Mitigating CO2 to minimize the steady rise in global temperature is a pressing topic and the scientific community is putting every effort to reduce CO2 emissions from major point sources such as steel or cement industries. This research proposal investigates the photochemical reduction of CO2 with single-atom catalysts (SACs) of 1st-row transition metals incorporated in light-absorbing host matrices like C3N4 or porphyrinic materials. A knowledge-driven interdisciplinary approach from a molecular catalyst to a supported catalyst will systematically address issues like (a) how an efficient SAC can be synthesized, (b) the mechanism of CO2 reduction over SACs, (c) the dynamic behavior of atoms via tracking the active center (change in oxidation state, symmetry, and bond distances) with operando spectroscopic investigations such as FTIR and X-Ray absorption spectroscopy. 1st-row transition metal complexes are active for the photochemical reduction of CO2; this research proposal investigates the synthesis of heterogeneous analogs of these metals (Mn, Fe, Co, Ni, and Cu) as SACs. After a successful grant application, Dr. Bidyut Bikash Sarma (researcher) will be able to explore a new field of research in the group of Prof. Erwin Reisner (host). A two-way knowledge transfer between the host group (expertise in photocatalysis and artificial photosynthesis) and the researcher (expertise in surface science and operando spectroscopy) will bring new ideas that will benefit both parties.

减少二氧化碳排放以尽量减少全球气温的稳步上升是一个紧迫的话题，科学界正在尽一切努力减少钢铁或水泥行业等主要点源的二氧化碳排放。这项研究计划研究了CO2的光化学还原与单原子催化剂（SAC）的第一行过渡金属纳入光吸收主体矩阵，如C3 N4或卟啉材料。从分子催化剂到负载型催化剂的知识驱动的跨学科方法将系统地解决以下问题：（a）如何合成有效的SAC，（B）SAC上的CO2还原机制，（c）通过跟踪活性中心（氧化态，对称性和键距的变化）与操作光谱研究（如FTIR和X射线吸收光谱）来跟踪原子的动态行为。第一行过渡金属络合物对CO2的光化学还原具有活性;本研究提案研究了这些金属（Mn，Fe，Co，Ni和Cu）作为SAC的非均相类似物的合成。在成功申请资助后，Bidyut Bikash Sarma博士（研究员）将能够在Erwin Reisner教授（主持人）的团队中探索新的研究领域。宿主组（在光合作用和人工光合作用方面的专业知识）和研究人员（在表面科学和操作光谱学方面的专业知识）之间的双向知识转移将带来对双方都有利的新想法。