期刊
NATURE COMMUNICATIONS
卷 10, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-10888-5
关键词
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资金
- National Key Research and Development Program of China [2017YFA0206901, 2018YFA0209401]
- Natural Science Foundation of China [21773036, 21688102, 51761165012]
- Science and Technology Commission of Shanghai Municipality [17JC1400100, 19XD1420400]
- Innovation Program of Shanghai Municipal Education Commission [2019-01-07-00-07-E00045]
- Collaborative Innovation Center of Chemistry for Energy Materials (2011-iChem)
- Shanghai Synchrotron Radiation Facility (SSRF)
The electrochemical N-2 fixation to produce ammonia is attractive but significantly challenging with low yield and poor selectivity. Herein, we first used density function theory calculations to reveal adjacent bi-Ti3+ pairs formed on anatase TiO2 as the most active electrocatalytic centers for efficient N-2 lying-down chemisorption and activation. Then, by doping of anatase TiO2 with Zr4+ that has similar d-electron configuration and oxide structure but relatively larger ionic size, the adjacent bi-Ti3+ sites were induced and enriched via a strained effect, which in turn enhanced the formation of oxygen vacancies. The Zr4+-doped anatase TiO2 exhibited excellent electrocatalytic N-2 fixation performances, with an ammonia production rate (8.90 mu g.h(-1).cm(-2)) and a Faradaic efficiency of 17.3% at -0.45 V versus reversible hydrogen electrode under ambient aqueous conditions. Moreover, our work suggests a viewpoint to understand and apply the same-valance dopants in heterogeneous catalysis, which is generally useful but still poorly understood.
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