电子顺磁共振
氧气
表面光电压
可见光谱
离域电子
光化学
材料科学
吸收光谱法
载流子
谱线
光谱学
吸收(声学)
吸收边
化学
光电子学
分析化学(期刊)
带隙
核磁共振
光学
量子力学
物理
复合材料
有机化学
色谱法
天文
作者
Ju Wu,Xiaodong Li,Wen Shi,Peiquan Ling,Yongfu Sun,Xingchen Jiao,Shan Gao,Liang Liang,Jiaqi Xu,Wensheng Yan,Chengming Wang,Yi Xie
标识
DOI:10.1002/anie.201803514
摘要
Abstract Solar CO 2 reduction efficiency is largely limited by poor photoabsorption, sluggish electron–hole separation, and a high CO 2 activation barrier. Defect engineering was employed to optimize these crucial processes. As a prototype, BiOBr atomic layers were fabricated and abundant oxygen vacancies were deliberately created on their surfaces. X‐ray absorption near‐edge structure and electron paramagnetic resonance spectra confirm the formation of oxygen vacancies. Theoretical calculations reveal the creation of new defect levels resulting from the oxygen vacancies, which extends the photoresponse into the visible‐light region. The charge delocalization around the oxygen vacancies contributes to CO 2 conversion into COOH* intermediate, which was confirmed by in situ Fourier‐transform infrared spectroscopy. Surface photovoltage spectra and time‐resolved fluorescence emission decay spectra indicate that the introduced oxygen vacancies promote the separation of carriers. As a result, the oxygen‐deficient BiOBr atomic layers achieve visible‐light‐driven CO 2 reduction with a CO formation rate of 87.4 μmol g −1 h −1 , which was not only 20 and 24 times higher than that of BiOBr atomic layers and bulk BiOBr, respectively, but also outperformed most previously reported single photocatalysts under comparable conditions.
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