Dual Active Sites with Charge-asymmetry in Organic Semiconductors Promoting C-C Coupling for Highly Efficient CO<sub>2</sub> Photoreduction to Ethanol

doi:10.1002/anie.202416684

IMR OpenIR

	Dual Active Sites with Charge-asymmetry in Organic Semiconductors Promoting C-C Coupling for Highly Efficient CO₂ Photoreduction to Ethanol
	Tan, Haotian 1; Si, Wenping 2; Zhang, Rongao 3; Peng, Wei 1; Liu, Xiaoqing 1; Zheng, Xusheng 3; Hou, Feng 1; Yin, Lichang 4; Liang, Ji 1
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)
	2024-11-12
发表期刊	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN	1433-7851
页码	10
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 COCO 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.
关键词	charge-asymmetry organic-semiconductor C-C coupling dual active sites photocatalyst
资助者	National Natural Science Foundation of China
DOI	10.1002/anie.202416684
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China ; [22379111] ; [22179093] ; [22002107]
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001357036400001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：2[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/191547
专题	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.