Dual Active Sites with Charge-asymmetry in Organic Semiconductors Promoting C-C Coupling for Highly Efficient CO2 Photoreduction to Ethanol
文献类型：期刊论文
| 作者 | Tan, Haotian1; Si, Wenping2; Zhang, Rongao3; Peng, Wei1; Liu, Xiaoqing1; Zheng, Xusheng3; Hou, Feng1; Yin, Lichang4; Liang, Ji1 |
| 刊名 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
 |
| 出版日期 | 2024-11-12 |
| 页码 | 10 |
| 关键词 | charge-asymmetry organic-semiconductor C-C coupling dual active sites photocatalyst |
| ISSN号 | 1433-7851 |
| DOI | 10.1002/anie.202416684 |
| 通讯作者 | Si, Wenping(siwp@hebut.edu.cn) ; Zheng, Xusheng(zxs@ustc.edu.cn) ; Hou, Feng(houf@tju.edu.cn) ; Liang, Ji(liangji@tju.edu.cn) |
| 英文摘要 | Selective CO2 photoreduction into high-energy-density and high-value-added C2 products is an ideal strategy to achieve carbon neutrality and energy shortage, but it is still highly challenging due to the large energy barrier of the C-C coupling step and severe exciton annihilation in photocatalysts. Herein, strong and localized charge polarization is successfully induced on the surface of melon-based organic semiconductors by creating dual active sites with a large charge asymmetry. Confirmed by multiscale characterization and theoretical simulations, such asymmetric charge distribution, originated from the oxygen dopants and nitrogen vacancies over melon-based organic semiconductors, reduces exciton binding energy and boosts exciton dissociation. The as-formed charge polarization sites not only donate electrons to CO2 molecules but also accelerate the coupling of asymmetric *CO*CO intermediates for CO2 photoreduction into ethanol by lowering the energy barrier of this process. Consequently, an exceptionally high selectivity of up to 97 % for C2H5OH and C2H5OH yield of 0.80 mmol g-1 h-1 have been achieved on this dual active sites organic semiconductor. This work, with its potential applicability to a variety of non-metal multi-site catalysts, represents a versatile strategy for the development of advanced catalysts tailored for CO2 photoreduction reactions. |
| 资助项目 | National Natural Science Foundation of China ; [22379111] ; [22179093] ; [22002107] |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:001357036400001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 资助机构 | National Natural Science Foundation of China |
| 源URL |  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Si, Wenping; Zheng, Xusheng; Hou, Feng; Liang, Ji |
| 作者单位 | 1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300072, Peoples R China 2.Hebei Univ Technol, Sch Mat Sci & Engn, Dingzigu Rd 1, Tianjin 300130, Peoples R China 3.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China 4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China |
| 推荐引用方式 GB/T 7714 | Tan, Haotian,Si, Wenping,Zhang, Rongao,et al. Dual Active Sites with Charge-asymmetry in Organic Semiconductors Promoting C-C Coupling for Highly Efficient CO2 Photoreduction to Ethanol[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2024:10. |
| APA | Tan, Haotian.,Si, Wenping.,Zhang, Rongao.,Peng, Wei.,Liu, Xiaoqing.,...&Liang, Ji.(2024).Dual Active Sites with Charge-asymmetry in Organic Semiconductors Promoting C-C Coupling for Highly Efficient CO2 Photoreduction to Ethanol.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,10. |
| MLA | Tan, Haotian,et al."Dual Active Sites with Charge-asymmetry in Organic Semiconductors Promoting C-C Coupling for Highly Efficient CO2 Photoreduction to Ethanol".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024):10. |
入库方式： OAI收割
来源：金属研究所
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