期刊
CHEMICAL ENGINEERING JOURNAL
卷 362, 期 -, 页码 349-356出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.01.051
关键词
Photoelectrochemical (PEC) N-2 fixation; Oxygen vacancies; BiOI; Lewis-base; Active sites
资金
- National Natural Science Foundation of China [21671083, 21401082]
- Open Project of State Key Laboratory of Rare Earth Resource Utilizations [RERU2018011]
- Jiangsu Provincial Six Talent Peaks [XCL-019]
- Jiangsu Province Natural Science Foundation [BK20170526]
- Youth Backbone Teacher Training Engineering of Jiangsu University
The adsorption and activation of N-2 on the catalyst surface is a major problem in the process of photoelectrochemical (PEC) N-2 reduction. Herein, we report a strategy to fabricate intrinsic BiOI (I-BiOI) photocathode with oxygen vacancies (OVs) (R-BiOI) by a facile in-situ method, and the R-BiOI was successfully selected as the model matrix for understanding the role of OVs in the PEC N-2 reduction system for the first time. The correlation between carrier concentration/Lewis-base/active sites and OVs was in-depth demonstrated by Mott-Schottky plots and photoelectrochemical impedance spectroscopy (PEIS) results, meanwhile the Linear-sweep-voltammetry (LSV) data further confirmed the selectivity for active N-2 over R-BiOI photocathode. The tandem built from BiVO4 photoanode and R-BiOI photocathode presented the desirable production rate of ammonia at about 1.4 mmol/m(2)/h, which is 1.3 and 2.9 times than that of I-BiOI (1.1 mmol/m(2)/h) and Pt (0.48 mmol/m(2)/h). Our findings have initially developed the proposed mechanism for the behavior of solar-electron-ammonia conversion and offered an alternative potential route for green N-2 fixation.
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