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Highly Efficient Visible-Light-Driven CO2-to-CO Conversion by Coordinatively Unsaturated Co-Salen Complexes in a Water-Containing System
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-11-23 , DOI: 10.1021/acs.inorgchem.2c02515
Chao Su 1 , Zilu Chen 1 , Qin Feng 1 , Fangsha Wei 1 , Mingling Zhang 1 , Anna Mo 1 , Hai-Hua Huang 1 , Huancheng Hu 1 , Dongcheng Liu 1
Affiliation  

The development of cost-effective catalysts for CO2 reduction is highly desired but remains a significant challenge. The unsaturated coordination metal center in a catalyst is favorable for the process of catalytic CO2 reduction. In this paper, two asymmetric salen ligands were used to synthesize two coordinatively unsaturated Co-salen complexes. The two Co-salen complexes exhibit an unsaturated coordination pattern and display high activity and CO selectivity for visible-light-driven CO2 reduction in a water-containing system. The photocatalytic performance of 2 is higher than that of 1 because the reduction potential of the catalytic CoII center and the energy barrier of the catalytic transition states of 2 are lower than those of 1, with turnover numbers (TONCO), turnover frequencies (TOF), and CO selectivity values of 8640, 0.24 s–1, and 97% for 2, respectively. The photocatalytic reduction of CO2 to CO for 2 is well supported by control experiments and density functional theory (DFT) calculations.

中文翻译:

在含水系统中通过配位不饱和 Co-Salen 配合物实现高效可见光驱动的 CO2 到 CO 转化

非常需要开发具有成本效益的 CO 2还原催化剂,但仍然是一项重大挑战。催化剂中的不饱和配位金属中心有利于催化CO 2还原过程。在本文中,两个不对称的 salen 配体被用来合成两个配位不饱和的 Co-salen 配合物。这两种 Co-salen 配合物表现出不饱和配位模式,并且在可见光驱动的含水系统中还原CO 2时表现出高活性和 CO 选择性。2的光催化性能高于1 ,因为催化Co II的还原电位2的催化过渡态的中心和能垒低于1,转换数(TON CO)、转换频率(TOF)和CO选择性值分别为8640、0.24 s –12的97% , 分别。控制实验和密度泛函理论 (DFT) 计算很好地支持了CO 2光催化还原为 CO 2
更新日期:2022-11-23
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