Highly Efficient Visible-Light-Driven CO2-to-CO Conversion by Coordinatively Unsaturated Co-Salen Complexes in a Water- Containing System

被引:7
作者
Su, Chao [1 ]
Chen, Zilu [1 ]
Feng, Qin [1 ]
Wei, Fangsha [1 ]
Zhang, Mingling [1 ]
Mo, Anna [1 ]
Huang, Hai-Hua [1 ]
Hu, Huancheng [1 ]
Liu, Dongcheng [1 ]
机构
[1] Guangxi Normal Univ, Collaborat Innovat Ctr Guangxi Ethn Med, Sch Chem & Pharmaceut Sci, State Key Lab Chem & Mol Engn Med Resources, Guilin 541004, Peoples R China
基金
中国国家自然科学基金;
关键词
METAL-ORGANIC FRAMEWORKS; COBALT COMPLEXES; ELECTROCHEMICAL REDUCTION; PHOTOCATALYTIC REDUCTION; CARBON-DIOXIDE; AQUEOUS CO2; PHOTOREDUCTION; ELECTRON; IRON; MACROCYCLES;
D O I
10.1021/acs.inorgchem.2c02515
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
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 Cosalen 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.
引用
收藏
页码:19748 / 19755
页数:8
相关论文
共 62 条
[1]   Coupling of a new porphyrin photosensitizer and cobaloxime cocatalyst for highly efficient photocatalytic H2 evolution [J].
Bodedla, Govardhana Babu ;
Wong, Wai-Yeung ;
Zhu, Xunjin .
JOURNAL OF MATERIALS CHEMISTRY A, 2021, 9 (36) :20645-20652
[2]   Molecular catalysis of the electrochemical and photochemical reduction of CO2 with Fe and Co metal based complexes. Recent advances [J].
Bonin, Julien ;
Maurin, Antoine ;
Robert, Marc .
COORDINATION CHEMISTRY REVIEWS, 2017, 334 :184-198
[3]   Selective and Efficient Photocatalytic CO2 Reduction to CO Using Visible Light and an Iron-Based Homogeneous Catalyst [J].
Bonin, Julien ;
Robert, Marc ;
Routier, Mathilde .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (48) :16768-16771
[4]   Highly Efficient and Selective Photocatalytic CO2 Reduction to CO in Water by a Cobalt Porphyrin Molecular Catalyst [J].
Call, Arnau ;
Cibian, Mihaela ;
Yamamoto, Keiya ;
Nakazono, Takashi ;
Yamauchi, Kosei ;
Sakai, Ken .
ACS CATALYSIS, 2019, 9 (06) :4867-4874
[5]   A robust and efficient cobalt molecular catalyst for CO2 reduction [J].
Chan, Sharon Lai-Fung ;
Lam, Tsz Lung ;
Yang, Chen ;
Yan, Siu-Cheong ;
Cheng, Nga Man .
CHEMICAL COMMUNICATIONS, 2015, 51 (37) :7799-7801
[6]   CO2 photo-reduction: insights into CO2 activation and reaction on surfaces of photocatalysts [J].
Chang, Xiaoxia ;
Wang, Tuo ;
Gong, Jinlong .
ENERGY & ENVIRONMENTAL SCIENCE, 2016, 9 (07) :2177-2196
[7]   Two novel nickel cluster substituted polyoxometalates: syntheses, structures and their photocatalytic activities, magnetic behaviors, and proton conduction properties [J].
Chen, Yi ;
Guo, Zheng-Wei ;
Chen, Ya-Peng ;
Zhuang, Zan-Yong ;
Wang, Guo-Qiang ;
Li, Xin-Xiong ;
Zheng, Shou-Tian ;
Yang, Guo-Yu .
INORGANIC CHEMISTRY FRONTIERS, 2021, 8 (05) :1303-1311
[8]   Boosting Photocatalytic CO2 Reduction on CsPbBr3 Perovskite Nanocrystals by Immobilizing Metal Complexes [J].
Chen, Zhoujie ;
Hu, Yangguang ;
Wang, Jin ;
Shen, Qing ;
Zhang, Yaohong ;
Ding, Chao ;
Bai, Yu ;
Jiang, Guocan ;
Li, Zhengquan ;
Gaponik, Nikolai .
CHEMISTRY OF MATERIALS, 2020, 32 (04) :1517-1525
[9]   Selective photocatalytic reduction of CO2 to CO mediated by a [FeFe]-hydrogenase model with a 1,2-phenylene S-to-S bridge [J].
Cheng, Minglun ;
Zhang, Xiongfei ;
Zhu, Yong ;
Wang, Mei .
CHINESE JOURNAL OF CATALYSIS, 2021, 42 (02) :310-319
[10]   ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE MEDIATED BY MOLECULAR CATALYSTS [J].
COLLIN, JP ;
SAUVAGE, JP .
COORDINATION CHEMISTRY REVIEWS, 1989, 93 (02) :245-268