Accelerating Electron-Transfer Dynamics by TiO2-Immobilized Reversible Single-Atom Copper for Enhanced Artificial Photosynthesis of Urea

被引：82

作者：

Li, Dong ^{[1
,2
]}

Zhao, Yunxuan ^{[1
]}

Miao, Yingxuan ^{[1
,2
]}

Zhou, Chao ^{[1
]}

Zhang, Li-Ping ^{[1
,3
]}

Wu, Li-Zhu ^{[1
]}

Zhang, Tierui ^{[1
,2
]}

机构：

[1] Chinese Acad Sci, Tech Inst Phys & Chem, Key Lab Photochem Convers & Optoelect Mat, Beijing 100190, Peoples R China

[2] Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China

[3] Univ Chinese Acad Sci, Sch Future Technol, Beijing 100049, Peoples R China

来源：

ADVANCED MATERIALS | 2022年 / 34卷 / 51期

基金：

中国博士后科学基金; 北京市自然科学基金; 中国国家自然科学基金;

关键词：

electron-transfer dynamics; photocatalysis; reversible variation; single-atom copper; urea synthesis; NITROGEN; CONVERSION; REDUCTION; EVOLUTION; CATALYSTS; G-C3N4;

D O I：

10.1002/adma.202207793

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Photocatalysis as a sustainable technology is expected to provide a novel sight for the green synthesis of urea directly using N-2, CO2, and H2O under mild conditions. However, the fundamental issue of inefficient electron transfer in photocatalysis strongly hinders its feasibility, especially for the above multi-electron-demanding urea synthesis. Herein, an effective strategy of accelerating electron-transfer dynamics is reported by TiO2-immobilized reversible single-atom copper (denoted as Cu SA-TiO2) to enhance the performance for photosynthesis of urea from N-2, CO2, and H2O. As revealed by a series of quasi-in-situ characterizations (e.g., electron paramagnetic resonance, and wavelength-resolved and femtosecond time-resolved spectroscopies), the expedited dynamics behaviors originating from reversible single-atom copper in as-designed Cu SA-TiO2 (electron extraction rate: over 30 times faster than the reference photocatalysts) allow the assurance of abundant and continual photogenerated electrons for multi-electron-demanding co-photoactivation of N-2 and CO2, resulting in considerable rates of urea production. The strategy above for improving the photoelectron-extraction ability of photocatalysts will offer a high-efficiency and promising route for artificial urea photosynthesis and other multi-electron-demanding photocatalytic reactions.

引用

页数：7