Dithiocarbamate-Linked Phthalocyanine with CdSe QDs Enhancing Charge Transfer for Selective Photocatalytic CO2 Reduction

被引:0
作者
Qi, Yuanyuan [1 ]
Sun, Hai [1 ]
She, Ping [1 ,2 ]
Wu, Jiahui [1 ]
Han, Jingwei [1 ]
Xu, Qiang [1 ]
Qin, Jun-Sheng [1 ]
Rao, Heng [1 ]
机构
[1] Jilin Univ, Coll Chem, Int Ctr Future Sci, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China
[2] Jilin Univ, Coll Chem, State Key Lab Supramol Struct & Mat, Changchun 130012, Peoples R China
基金
中国国家自然科学基金;
关键词
cobalt phthalocyanine; covalent linking; photocatalytic CO2 reduction; semiconductor quantum dots; LIGHT-DRIVEN CO2; CARBON-DIOXIDE; QUANTUM DOTS; CATALYST; ELECTROREDUCTION; SEMICONDUCTORS; CHEMISTRY; METHANOL; WATER;
D O I
10.1002/adfm.202505021
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Photocatalytic CO2 reduction (PCR) to chemical fuels represents a promising solution to the energy crisis and global warming. The rational design of efficient photocatalysts is key to PCR. In this study, a molecular heterogeneous photocatalyst is constructed with cobalt (II) 2,9,16,23-tetraaminophthalocyanine (CoPc-NH2) covalently linked to CdSe quantum dots (QDs) via a dithiocarbamate group (& horbar;NHCS2). This covalent bond (& horbar;NHCS2) enables directional, efficient, and fast interfacial electron transfer, substantially improving the catalytic activity. The optimized CdSe@CoPc-NH2 heterojunction exhibits excellent activity for CO2 reduction, achieving an average CO generation rate of 3, 687 mu mol g(-1) h(-1) (TONCO = 2, 360), which is 31 times higher than that of pristine CdSe QDs. Furthermore, immobilizing CoPc-NH2 on CdSe QDs increases the selectivity for CO from 20% to 90%. The in situ formation of molecular heterogeneous photocatalysts features a covalently bonded interface, which can offer valuable insights for designing efficient photocatalysts for solar fuel generation.
引用
收藏
页数:11
相关论文
共 62 条
[1]   Photocatalytic Reduction of CO2 with N-Doped TiO2-Based Photocatalysts Obtained in One-Pot Supercritical Synthesis [J].
Andrade, Oscar R. ;
Rodriguez, Veronica ;
Camarillo, Rafael ;
Martinez, Fabiola ;
Jimenez, Carlos ;
Rincon, Jesusa .
NANOMATERIALS, 2022, 12 (11)
[2]   Quantum Dot-Sensitized Photoreduction of CO2 in Water with Turnover Number > 80,000 [J].
Arcudi, Francesca ;
Dordevic, Luka ;
Nagasing, Benjamin ;
Stupp, Samuel, I ;
Weiss, Emily A. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2021, 143 (43) :18131-18138
[3]   Selective Photocatalytic CO2 Reduction in Water by Electrostatic Assembly of CdS Nanocrystals with a Dinuclear Cobalt Catalyst [J].
Bi, Qian-Qian ;
Wang, Jia-Wei ;
Lv, Jia-Xin ;
Wang, Juan ;
Zhang, Wen ;
Lu, Tong-Bu .
ACS CATALYSIS, 2018, 8 (12) :11815-11821
[4]   Dimension-Matched Zinc Phthalocyanine/BiVO4 Ultrathin Nanocomposites for CO2 Reduction as Efficient Wide-Visible-Light-Driven Photocatalysts via a Cascade Charge Transfer [J].
Bian, Ji ;
Feng, Jiannan ;
Zhang, Ziqing ;
Li, Zhijun ;
Zhang, Yuhang ;
Liu, Yadi ;
Ali, Sharafat ;
Qu, Yang ;
Bai, Linlu ;
Xie, Jijia ;
Tang, Dongyan ;
Li, Xin ;
Bai, Fuquan ;
Tang, Junwang ;
Jing, Liqiang .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2019, 58 (32) :10873-10878
[5]   Alumina-Supported CoFe Alloy Catalysts Derived from Layered-Double-Hydroxide Nanosheets for Efficient Photothermal CO2 Hydrogenation to Hydrocarbons [J].
Chen, Guangbo ;
Gao, Rui ;
Zhao, Yufei ;
Li, Zhenhua ;
Waterhouse, Geoffrey I. N. ;
Shi, Run ;
Zhao, Jiaqing ;
Zhang, Mengtao ;
Shang, Lu ;
Sheng, Guiyang ;
Zhang, Xiangping ;
Wen, Xiaodong ;
Wu, Li-Zhu ;
Tung, Chen-Ho ;
Zhang, Tierui .
ADVANCED MATERIALS, 2018, 30 (03)
[6]   Synergizing Electron and Heat Flows in Photocatalyst for Direct Conversion of Captured CO2 [J].
Choi, Chungseok ;
Zhao, Fengyi ;
Hart, James L. ;
Gao, Yuanzuo ;
Menges, Fabian ;
Rooney, Conor L. ;
Harmon, Nia J. ;
Shang, Bo ;
Xu, Zihao ;
Suo, Sa ;
Sam, Quynh ;
Cha, Judy J. ;
Lian, Tianquan ;
Wang, Hailiang .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (23)
[7]   Conduction and valence band positions of Ta2O5, TaON, and Ta3N5 by UPS and electrochemical methods [J].
Chun, WJ ;
Ishikawa, A ;
Fujisawa, H ;
Takata, T ;
Kondo, JN ;
Hara, M ;
Kawai, M ;
Matsumoto, Y ;
Domen, K .
JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (08) :1798-1803
[8]   An infrared study of the intermediates of methanol synthesis from carbon dioxide over Pd/β-Ga2O3 [J].
Collins, SE ;
Baltanás, MA ;
Bonivardi, AL .
JOURNAL OF CATALYSIS, 2004, 226 (02) :410-421
[9]   The underestimated potential of solar energy to mitigate climate change [J].
Creutzig, Felix ;
Agoston, Peter ;
Goldschmidt, Jan Christoph ;
Luderer, Gunnar ;
Nemet, Gregory ;
Pietzcker, Robert C. .
NATURE ENERGY, 2017, 2 (09)
[10]   Hierarchical CeO2/Bi2MoO6 heterostructured nanocomposites for photoreduction of CO2 into hydrocarbons under visible light irradiation [J].
Dai, Weili ;
Hu, Xu ;
Wang, Tengyao ;
Xiong, Wuwan ;
Luo, Xubiao ;
Zou, Jianping .
APPLIED SURFACE SCIENCE, 2018, 434 :481-491