Engineering the electron localization of metal sites on nanosheets assembled periodic macropores for CO2 photoreduction

被引:2
作者
Lyu, Wenyuan [1 ]
Liu, Yang [2 ]
Chen, Datong [1 ]
Wang, Fengliang [1 ]
Li, Yingwei [1 ]
机构
[1] South China Univ Technol, Sch Chem & Chem Engn, Guangzhou 510640, Peoples R China
[2] Guangdong Univ Petrochem Technol, Sch Environm Sci & Engn, Guangdong Prov Key Lab Petrochem Pollut Proc & Con, Maoming 525000, Guangdong, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
ORGANIC FRAMEWORKS; REDUCTION; CENTERS; STATE; WATER;
D O I
10.1038/s41467-024-54988-3
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Photocatalytic conversion of CO2 into syngas is highly appealing, yet still suffers from the undesirable product yield due to the sluggish carrier transfer and the uncontrollable affinity between catalytic sites and intermediates. Here we report the fabrication of Co sites with tunable electron localization capability on two dimensional (2D) nanosheets assembled three dimensional (3D) ordered macroporous framework (3DOM-NS). The as-prepared Co-based 3DOM-NS catalysts exhibit attractive photocatalytic performances toward CO2 reduction, among which the cobalt sulfide one (3DOM Co-SNS) shows the highest syngas generation rate up to 347.3 mu mol h-1 under the irradiation of visible light and delivers a remarkable catalytic activity (1150.7 mu mol h-1) in a flow reaction system under natural sunlight. Mechanism studies reveal that the high electron localization of metal sites in 3DOM Co-SNS strengthens the interaction between Co and HCOO* via the orbital interactions of dyz/dxz-p and s-s, thus facilitating the cleaving process of C-O bond. Additionally, the ordered macroporous framework with nanosheet subunits elevates the transfer efficiency of photoexcited electrons, which contributes to its high activity.
引用
收藏
页数:12
相关论文
共 50 条
  • [41] Metal halide perovskites as an emergent catalyst for CO2 photoreduction: a minireview
    Mendez-Galvan, Melissa
    Alcantar-Vazquez, Brenda
    Diaz, Gabriela
    Ibarra, Ilich A.
    Lara-Garcia, Hugo A.
    [J]. REACTION CHEMISTRY & ENGINEERING, 2021, 6 (05) : 828 - 838
  • [42] Metal-Organic-Framework-Based Catalysts for Photoreduction of CO2
    Li, Rui
    Zhang, Wang
    Zhou, Kun
    [J]. ADVANCED MATERIALS, 2018, 30 (35)
  • [43] Energy Band Alignment and Redox-Active Sites in Metalloporphyrin-Spaced Metal-Catechol Frameworks for Enhanced CO2 Photoreduction
    Chen, Er-Xia
    Qiu, Mei
    Zhang, Yong-Fan
    He, Liang
    Sun, Ya-Yong
    Zheng, Hui-Li
    Wu, Xin
    Zhang, Jian
    Lin, Qipu
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (01)
  • [44] Metal Vacancies in CoAl-Layered Double Hydroxide Nanosheets Enabling Boosted Visible Light Driven CO2 Photoreduction
    Yang, Lan
    Yu, Pengfei
    Liu, Jiandang
    Li, Xiaohong
    Li, Huiyi
    Liu, Chengyuan
    Pan, Yang
    Ye, Bangjiao
    Pan, Bicai
    Xiao, Chong
    Xie, Yi
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2023, 127 (15) : 7172 - 7183
  • [45] Efficient Photoreduction of CO2 to CO with 100% Selectivity by Slowing Down Electron Transport
    Chen, Cheng
    Wu, Mingge
    Xu, Yifan
    Ma, Chunyan
    Song, Maoyong
    Jiang, Guibin
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2024, 146 (13) : 9163 - 9171
  • [46] MOF-based ternary nanocomposites for better CO2 photoreduction: roles of heterojunctions and coordinatively unsaturated metal sites
    He, Xiang
    Wang, Wei-Ning
    [J]. JOURNAL OF MATERIALS CHEMISTRY A, 2018, 6 (03) : 932 - 940
  • [47] Relative Local Electron Density Tuning in Metal-Covalent Organic Frameworks for Boosting CO2 Photoreduction
    Zhang, Mi
    Huang, Pei
    Liao, Jia-Peng
    Yang, Ming-Yi
    Zhang, Shuai-Bing
    Liu, Yu-Fei
    Lu, Meng
    Li, Shun-Li
    Cai, Yue-Peng
    Lan, Ya-Qian
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (44)
  • [48] Bandgap engineering of covalent triazine frameworks for highly efficient and selective photoreduction of CO2 to CO
    Shi, Yan
    Qi, Guangdong
    Liao, Fudong
    Gao, Min
    Tao, Engang
    Wei, Dong
    Zheng, Jinyang
    Huang, Yulin
    Yang, Chengyu
    Gong, Fang
    Zhao, Jun
    [J]. JOURNAL OF SOLID STATE CHEMISTRY, 2025, 343
  • [49] Preparation of thickness-tunable BiOCl nanosheets with high photocatalytic activity for photoreduction of CO2
    Jin, Jiarui
    Wang, Yanjie
    He, Tao
    [J]. RSC ADVANCES, 2015, 5 (121): : 100244 - 100250
  • [50] Optimizing the Oxygen Vacancies Concentration of Thin NiO Nanosheets for Efficient Selective CO2 Photoreduction
    Xiang, Junxiang
    Zhang, Tingshi
    Cao, Ruodan
    Lin, Mingxiong
    Yang, Bixia
    Wen, Yonglin
    Zhuang, Zanyong
    Yu, Yan
    [J]. SOLAR RRL, 2021, 5 (12)