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共价有机框架稳定单一CoN₄Cl₂ 站点增强光催化CO₂ 减少到可调节的合成气

Ping Fu¹, Cailing Chen², Chao Wu³

¹State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, 211816, P. R. China.

Angewandte Chemie (International ed. in English)

|August 28, 2024

概括

研究人员开发了一种使用共价有机框架 (COF) 的新型单原子催化剂,以有效地减少太阳能二氧化碳 (CO2). 这种催化剂实现了创纪录的二氧化碳生产率,为化学和燃料合成提供了可持续的途径.

科学领域:

材料科学材料科学材料科学
催化剂是一种催化剂.
可再生能源可再生能源是可再生能源.

背景情况:

太阳能二氧化碳 (CO2) 减少是可持续化学品和燃料的有希望的途径.
挑战包括光催化剂中的快速电荷重组和缓慢的二氧化碳减排动力学.
开发高活性和稳定的光催化剂对于高效的二氧化碳转化至关重要.

研究的目的:

设计和合成一种新的单原子催化剂,以提高太阳能二氧化碳的减少.
研究新材料的催化机制和性能.
在将二氧化碳转化为合成气等有价值产品方面实现高效率和选择性.

主要方法:

在含有三素的共价有机框架 (TPy-COF-Co) 中制造一个独特的Co-N4Cl2单位.
利用可见光辐射进行光催化二氧化碳减排.
采用了同步射线X射线吸收细结构 (XAFS) 和现场ATR-SEIRAS的操作操作,以及机械学研究的理论计算.

主要成果:

TPy-COF-Co催化剂实现了创纪录的426 mmol g−1 h−1.1的二氧化碳生产率.
证明的特殊营业额 (TON) 为2095和营业频率 (TOF) 为1607小时-1.
展示了稳定的回收性能和可调节的合成气 (CO/H2) 生产比率.

结论:

基于三的COF框架有效地促进了对单个Co-N4Cl2站点的电荷转移.
催化剂通过降低*COOH生成的能量障碍,显著增强了CO2激活.
分子工程衍生COF单原子催化剂具有很大的潜力,可以提高CO2光还原效率.

关键词:

减少二氧化碳减少二氧化碳协价有机框架协价有机框架光催化作用的光催化一个原子催化剂辛加斯天然气公司

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