Regulation of Internal Electric Field via d Orbital Occupancy for Efficient CO<sub>2</sub> Photoreduction

doi:10.1002/adfm.202502686

IMR OpenIR

	Regulation of Internal Electric Field via d Orbital Occupancy for Efficient CO₂ Photoreduction
	Hou, Xiangyan 1; Shi, Jingyu 1; Jiang, Mengpei 3; Wu, Xiaofeng 1; Liang, Na 1; Shao, Zhiyu 4; Zhu, Qian 1; Zeng, Jianrong 5,6; Cong, Yingge 2; Huang, Keke 1
通讯作者	Zeng, Jianrong(zengjr@sari.ac.cn) ; Cong, Yingge(congyg@sibet.ac.cn) ; Huang, Keke(kkhuang@jlu.edu.cn)
	2025-03-16
发表期刊	ADVANCED FUNCTIONAL MATERIALS
ISSN	1616-301X
页码	9
摘要	Developing highly efficient CO2 photocatalysts is meaningful; however, the ultrafast recombination of photogenerated electrons and holes severely hinders the photocatalytic reaction. Herein, the internal electric field of ferroelectric KNbO3 is further enhanced by optimizing Nb 4d t(2)(g) orbital occupancy states through Nb-O-Fe charge transport channels regulated by different doped amounts of Fe as an electron donor, which further improves the separation efficiency of photogenerated electrons and holes. The optimal occupancy state of the Nb 4d t(2)(g) orbital effectively modulates its bonding interactions with neighboring oxygen atoms, achieving the maximum directional displacement of Nb along the [110] polarization axis of the NbO6 octahedron at the optimized t(2)(g) orbital occupancy, as evidenced by atomic pair distribution function (PDF) analysis and Raman spectroscopy. The photocatalytic performance revealed that KNbO3 with the strongest built-in electric field exhibited the highest CO yield (15.7 mu mol g(-)(1)h(-)(1)) and selectivity (92.3%). This work paves the way for tuning ferroelectric polarization via orbital regulation and lays a foundation for the rational design of energy-catalytic ferroelectric structures.
关键词	charge transfer CO2 photoreduction ferroelectric polarization KNbO3 orbital regulation
资助者	National Natural Science Foundation of China ; National Key R&D Program of China ; Jilin Province Science and Technology Development Plan
DOI	10.1002/adfm.202502686
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China ; National Key R&D Program of China[2021YFF0500502] ; National Key R&D Program of China[2023YFA1506304] ; Jilin Province Science and Technology Development Plan[20230101024JC] ; Jilin Province Science and Technology Development Plan[2021JGZ08] ; Jilin Province Science and Technology Development Plan[2022YJSJIP20] ; [22090044] ; [22171102] ; [22201298]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001446127100001
出版者	WILEY-V C H VERLAG GMBH
引用统计
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/192028
专题	中国科学院金属研究所
通讯作者	Zeng, Jianrong; Cong, Yingge; Huang, Keke
作者单位	1.Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China 2.Chinese Acad Sci, Suzhou Inst Biomed Engn & Technol, Dept Biomat & Stem Cells, Suzhou 215163, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 4.Jilin Univ, China Japan Union Hosp, Changchun 130061, Peoples R China 5.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China 6.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China
推荐引用方式 GB/T 7714	Hou, Xiangyan,Shi, Jingyu,Jiang, Mengpei,et al. Regulation of Internal Electric Field via d Orbital Occupancy for Efficient CO₂ Photoreduction[J]. ADVANCED FUNCTIONAL MATERIALS,2025:9.
APA	Hou, Xiangyan.,Shi, Jingyu.,Jiang, Mengpei.,Wu, Xiaofeng.,Liang, Na.,...&Huang, Keke.(2025).Regulation of Internal Electric Field via d Orbital Occupancy for Efficient CO₂ Photoreduction.ADVANCED FUNCTIONAL MATERIALS,9.
MLA	Hou, Xiangyan,et al."Regulation of Internal Electric Field via d Orbital Occupancy for Efficient CO₂ Photoreduction".ADVANCED FUNCTIONAL MATERIALS (2025):9.