Journal
INORGANIC CHEMISTRY
Volume 58, Issue 15, Pages 10424-10431Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.9b01823
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Funding
- National Natural Science Foundation of China [51761024, 51671022]
- CAS Light of West China Program
- Feitian Scholar Program of Gansu Province
- Foundation of a Hundred Youth Talents Training Program of Lanzhou Jiaotong University
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The development of highly active and durable electrocatalysts toward the N(2 )reduction reaction (NRR) holds a key to ambient electrocatalytic NH3 synthesis. Herein, fluorine (F)-doped SnO2 mesoporous nanosheets on carbon cloth (F-SnO2/CC) were developed as an efficient NRR electrocatalyst. Benefiting from the combined structural advantages of mesoporous nanosheet structure and F-doping, the F-SnO2/CC exhibited high NRR activity with an NH3 yield of 19.3 mu g h(-1) mg(-1) and a Faradaic efficiency of 8.6% at -0.45 V (vs RHE) in 0.1 M Na2SO4, comparable or even superior to those of most reported NRR electrocatalysts. Density functional theory calculations revealed that the F-doping could readily tailor the electronic structure of SnO2 to render it with improved conductivity and increased positive charge on active Sn sites, leading to the lowered reaction energy barriers and boosted NRR activity.
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