Premium
Electrocatalytic N 2 Fixation over Hollow VO 2 Microspheres at Ambient Conditions
Author(s) -
Zhang Rong,
Guo Haoran,
Yang Li,
Wang Yuan,
Niu Zhiguo,
Huang Hong,
Chen Hongyu,
Xia Li,
Li Tingshuai,
Shi Xifeng,
Sun Xuping,
Li Baihai,
Liu Qian
Publication year - 2019
Publication title -
chemelectrochem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.182
H-Index - 59
ISSN - 2196-0216
DOI - 10.1002/celc.201801484
Subject(s) - catalysis , faraday efficiency , electrochemistry , selectivity , reversible hydrogen electrode , chemistry , yield (engineering) , inorganic chemistry , nitrogen fixation , nitrogen , redox , metal , electrode , materials science , organic chemistry , working electrode , metallurgy
Electrochemical N 2 fixation has gained much attention as an environmentally friendly and sustainable process for NH 3 production at ambient conditions. Its efficiency depends greatly on identifying highly active electrocatalysts with good stability. In this work, we propose the use of VO 2 hollow microspheres as a robust non‐precious metal catalyst for the N 2 reduction reaction (NRR). The catalyst operates efficiently and stably at neutral pH to high Faradaic efficiency (3.97 %) and NH 3 yield (14.85 μg h −1 mg −1 cat. ) under an applied potential of −0.7 V (vs. the reversible hydrogen electrode). Note that this catalyst also presents a high selectivity for NH 3 synthesis without N 2 H 4 generation. Density functional theory reveals that the energetically favorable pathway for NRR is *N 2 →*NNH→*NHNH→*NHNH 2 →*NH 2 NH 2 →*NH 2 +NH 3 →*NH 3 +NH 3 →2NH 3 , where the first hydrogenation step to form *NNH is the potential‐determining step.