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Dramatically Enhanced Ambient Ammonia Electrosynthesis Performance by In‐Operando Created Li–S Interactions on MoS 2 Electrocatalyst
Author(s) -
Liu Yanyan,
Han Miaomiao,
Xiong Qizhong,
Zhang Shengbo,
Zhao Cuijiao,
Gong Wanbing,
Wang Guozhong,
Zhang Haimin,
Zhao Huijun
Publication year - 2019
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201803935
Subject(s) - electrocatalyst , faraday efficiency , catalysis , electrosynthesis , adsorption , materials science , ammonia production , electrochemistry , reversible hydrogen electrode , redox , chemical engineering , inorganic chemistry , nanotechnology , chemistry , electrode , organic chemistry , reference electrode , engineering
The Haber‐Bosch process can be replaced by the ambient electrocatalytic N 2 reduction reaction (NRR) to produce NH 3 if suitable electrocatalysts can be developed. However, to develop high performance N 2 fixation electrocatalysts, a key issue to be resolved is to achieve efficient hydrogenation of N 2 without interference by the thermodynamically favored hydrogen evolution reaction (HER). Herein, in‐operando created strong Li–S interactions are reported to empower the S‐rich MoS 2 nanosheets with superior NRR catalytic activity and HER suppression ability. The Li + interactions with S‐edge sites of MoS 2 can effectively suppress hydrogen evolution reaction by reducing H* adsorption free energy from 0.03 to 0.47 eV, facilitate N 2 adsorption by increasing N 2 adsorption free energy from –0.32 to –0.70 eV and enhance electrocatalytic N 2 reduction activity by decreasing the activation energy barrier of the reaction control step (*N 2 → *N 2 H) from 0.84 to 0.42 eV. A NH 3 yield rate of 43.4 μg h −1 mg −1 MoS 2 with a faradaic efficiency (FE) of 9.81% can be achieved in presence of strong Li–S interactions, more than 8 and 18 times by the same electrocatalyst in the absence of Li–S interactions. This report opens a new way to design and develop catalysts and catalysis systems.