Hexanuclear ring cobalt complex for photochemical CO_(2) to CO conversion

作     者：Xiangyu Meng Rui Li Junyi Yang Shiming Xu Chenchen Zhang Kejia You Baochun Ma Hongxia Guan Yong Ding 孟翔宇;李睿;杨峻懿;许世明;张辰晨;尤可嘉;马宝春;管红霞;丁勇

作者机构：State Key Laboratory of Applied Organic ChemistryKey Laboratory of Advanced Catalysis of Gansu ProvinceCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000GansuChina State Key Laboratory for Oxo Synthesis and Selective OxidationLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000GansuChina School of Science and TechnologyGeorgia Gwinnett College1000 University Center LaneLawrencevilleGA 30043USA 

出 版 物：《Chinese Journal of Catalysis》 (催化学报（英文）)

年 卷 期：2022年第43卷第9期

页      面：2414-2424页

核心收录：

学科分类：081704[工学-应用化学] 081705[工学-工业催化] 07[理学] 0817[工学-化学工程与技术] 08[工学] 070304[理学-物理化学(含∶化学物理)] 0703[理学-化学] 

基　　金：国家自然科学基金(22075119) 甘肃省自然科学基金(21JR7RA440) 中央高校基本科研业务费专项资金优秀研究生项目(lzujbky-2021-it13) 

主　　题：Photosynthesis Homogeneous catalysis CO_(2)reduction reaction Density functional theory Hexanuclear ring cobalt complex 

摘      要：Photosynthesis in nature has been deemed as the most significant biochemical reaction,which maintains a relatively stable content of O_(2) and CO_(2) in the ***,for a deeper comprehension of natural photosynthesis,an artificial photosynthesis model reaction of photochemical CO_(2) to CO conversion(CO_(2)+2 H^(+)+2e^(-)→CO+H_(2)O)catalyzed by a homogeneous hexanuclear ring cobalt complex{K_(2)[CoO_(3)PCH_(2)N(CH_(2)CO_(2))_(2)]}_(6)(Co6 complex)is *** the[Ru(bpy)_(3)]^(2+)as a photosensitizer and TEOA as a sacrificial electron donor,an optimal turnover frequency of 503.3 h^(‒1) and an apparent quantum efficiency of 0.81%are *** good photocatalytic CO_(2) reduction performance is attributed to the efficient electron transfer between Co6 complex and[Ru(bpy)_(3)]^(2+),which boosts the photogenerated carriers separation of the *** is confirmed by the j‐V curves,light‐assisted UV‐vis curves,steady‐state photoluminescence spectra and real‐time laser flash photolysis *** addition,the proposed catalytic mechanism for CO_(2) reduction reaction catalyzed by the Co6 complex is explored by the potassium thiocyanate poison experiment,Pourbaix diagram and density functional theory calculations.