期刊
SMALL METHODS
卷 3, 期 6, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smtd.201800386
关键词
electrocatalysts; faradaic efficiency; NbO2; nitrogen reduction reaction
资金
- National Key Research and Development Program of China [2017YFA0206901, 2018YFA0209401]
- Natural Science Foundation of China [21773036, 21473038, 21471034]
- Science and Technology Commission of Shanghai Municipality [17JC1402000]
- International Scientific Partnership Program ISPP at King Saud University [ISPP-0017]
The electrocatalytic N-2 reduction reaction (NRR) to produce ammonia is an attractive but highly challenging approach, due to the extreme inertness of N-2 molecules and significantly lower N-2 concentration compared to the surrounding water molecules. Herein, NbO2 nanoparticles are demonstrated as an efficient NRR electrocatalyst with significantly improved electrochemical performances. Compared to Nb2O5 with a similar crystal structure unit but different linkage, the Nb4+ cation not only provides empty d-orbitals for strong N-2 adsorption, but also a single d-electron to further enable back donation to activate the N N triple bond. As a result, the NbO2 nanoparticles present an outstanding ammonia production rate of 11.6 mu g h(-1) mg(cat.)(-1) at -0.65 V versus reversible hydrogen electrode (RHE) and an excellent electrochemical stability, significantly higher than those of the Nb2O5 nanorods under similar conditions. More importantly, a peak faradaic efficiency of ammonia production of 32% is obtained for NbO2 at -0.60 V versus RHE, which is one of the highest reported NRR faradaic efficiencies to date.
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