Dramatically Enhanced Ambient Ammonia Electrosynthesis Performance by In-Operando Created Li-S Interactions on MoS2 Electrocatalyst
Author(s)
Liu, Yanyan
Han, Miaomiao
Xiong, Qizhong
Zhang, Shengbo
Zhao, Cuijiao
Gong, Wanbing
Wang, Guozhong
Zhang, Haimin
Zhao, Huijun
Griffith University Author(s)
Year published
2019
Metadata
Show full item recordAbstract
The Haber‐Bosch process can be replaced by the ambient electrocatalytic N2 reduction reaction (NRR) to produce NH3 if suitable electrocatalysts can be developed. However, to develop high performance N2 fixation electrocatalysts, a key issue to be resolved is to achieve efficient hydrogenation of N2 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 MoS2 nanosheets with superior NRR catalytic activity and HER suppression ability. The Li+ interactions with S‐edge sites of MoS2 can effectively suppress ...
View more >The Haber‐Bosch process can be replaced by the ambient electrocatalytic N2 reduction reaction (NRR) to produce NH3 if suitable electrocatalysts can be developed. However, to develop high performance N2 fixation electrocatalysts, a key issue to be resolved is to achieve efficient hydrogenation of N2 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 MoS2 nanosheets with superior NRR catalytic activity and HER suppression ability. The Li+ interactions with S‐edge sites of MoS2 can effectively suppress hydrogen evolution reaction by reducing H* adsorption free energy from 0.03 to 0.47 eV, facilitate N2 adsorption by increasing N2 adsorption free energy from –0.32 to –0.70 eV and enhance electrocatalytic N2 reduction activity by decreasing the activation energy barrier of the reaction control step (*N2 → *N2H) from 0.84 to 0.42 eV. A NH3 yield rate of 43.4 μg h−1 mg−1 MoS2 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.
View less >
View more >The Haber‐Bosch process can be replaced by the ambient electrocatalytic N2 reduction reaction (NRR) to produce NH3 if suitable electrocatalysts can be developed. However, to develop high performance N2 fixation electrocatalysts, a key issue to be resolved is to achieve efficient hydrogenation of N2 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 MoS2 nanosheets with superior NRR catalytic activity and HER suppression ability. The Li+ interactions with S‐edge sites of MoS2 can effectively suppress hydrogen evolution reaction by reducing H* adsorption free energy from 0.03 to 0.47 eV, facilitate N2 adsorption by increasing N2 adsorption free energy from –0.32 to –0.70 eV and enhance electrocatalytic N2 reduction activity by decreasing the activation energy barrier of the reaction control step (*N2 → *N2H) from 0.84 to 0.42 eV. A NH3 yield rate of 43.4 μg h−1 mg−1 MoS2 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.
View less >
Journal Title
Advanced Energy Materials
Volume
9
Issue
14
Subject
Macromolecular and materials chemistry
Materials engineering
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Energy & Fuels