期刊
ELECTROCHIMICA ACTA
卷 435, 期 -, 页码 -出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2022.141333
关键词
Electrochemical nitrogen oxidation; N2 fixation; Nitrate synthesis; Mo-doped TiO2; Self-supported electrode
资金
- National Natural Science Foundation of China
- Ministry of Science and Technology of the People?s Republic of China
- China Postdoctoral Science Foundation
- Ministry of Education of the People?s Republic of China
- [22102076]
- [22121005]
- [21925503]
- [21871149]
- [2017YFA0206700]
- [2020M670621]
- [B12015]
Mo-doped TiO2 electrode enhances nitrogen adsorption and activation for efficient nitrate synthesis, providing experimental and theoretical evidence for promoting stable Ti-based oxide towards NOR.
Electrocatalytic nitrogen oxidation reaction (NOR) provides an eco-friendly pathway for ambient N2 fixation and nitrate/nitric acid synthesis but is plagued by sluggish kinetics due to the weak adsorption of N2 molecules and cleavage of N---N triple bonds. Herein, a self-supported Mo-doped TiO2 electrode prepared by one-step hydro -thermal method is reported for efficient nitrogen oxidation. Electrochemical measurements and spectroscopy investigations reveal that the inert TiO2 is effectively triggered by Mo substitution in terms of enhanced N2 adsorption and activation. As further confirmed by density function theory calculations, the incorporation of Mo reduces the barrier of the rate-determining step and provides an energetically favorable NOR pathway compared to pristine rutile TiO2. Electrochemical results show that Mo-doped TiO2 electrode achieves a nitrate yield of 5.44 mu g h-1 mgcat- 1 (or 8.77 +/- 0.39 nmol h-1 cm-2) with a Faradaic efficiency of 2.88%. The formation of nitrate from N2 under positive bias is further demonstrated by in situ ultraviolet-visible spectrophotometry. This work provides experimental and theoretical evidences that Mo doping can stimulate the stable yet electrocatalytically inert Ti-based oxide toward NOR via promoting active sites formation and lowering activation energy barriers.
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