Sulfur dots–graphene nanohybrid: a metal-free electrocatalyst for efficient N2-to-NH3 fixation under ambient conditions

NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber–Bosch process with huge CO2 emission. Electrochemical N2 reduction offers a carbon-neutral process to convert N2 to NH3 under ambient conditions, but it requires efficient and stable...

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Published inChemical communications (Cambridge, England) Vol. 55; no. 21; pp. 3152 - 3155
Main Authors Chen, Hongyu, Zhu, Xiaojuan, Huang, Hong, Wang, Huanbo, Wang, Ting, Zhao, Runbo, Zheng, Hongguo, Asiri, Abdullah M, Luo, Yonglan, Sun, Xuping
Format Journal Article
LanguageEnglish
Published Cambridge Royal Society of Chemistry 07.03.2019
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Abstract NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber–Bosch process with huge CO2 emission. Electrochemical N2 reduction offers a carbon-neutral process to convert N2 to NH3 under ambient conditions, but it requires efficient and stable catalysts to drive the N2 reduction reaction. Herein, we report that a sulfur dots–graphene nanohybrid acts as a metal-free electrocatalyst for ambient N2-to-NH3 conversion with excellent selectivity. When operated in 0.5 M LiClO4, this electrocatalyst achieves a large NH3 yield of 28.56 μg h−1 mgcat.−1 and a high Faradaic efficiency of 7.07% at −0.85 V vs. reversible hydrogen electrode. Notably, it also shows good electrochemical stability.
AbstractList NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber–Bosch process with huge CO2 emission. Electrochemical N2 reduction offers a carbon-neutral process to convert N2 to NH3 under ambient conditions, but it requires efficient and stable catalysts to drive the N2 reduction reaction. Herein, we report that a sulfur dots–graphene nanohybrid acts as a metal-free electrocatalyst for ambient N2-to-NH3 conversion with excellent selectivity. When operated in 0.5 M LiClO4, this electrocatalyst achieves a large NH3 yield of 28.56 μg h−1 mgcat.−1 and a high Faradaic efficiency of 7.07% at −0.85 V vs. reversible hydrogen electrode. Notably, it also shows good electrochemical stability.
NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber-Bosch process with huge CO2 emission. Electrochemical N2 reduction offers a carbon-neutral process to convert N2 to NH3 under ambient conditions, but it requires efficient and stable catalysts to drive the N2 reduction reaction. Herein, we report that a sulfur dots-graphene nanohybrid acts as a metal-free electrocatalyst for ambient N2-to-NH3 conversion with excellent selectivity. When operated in 0.5 M LiClO4, this electrocatalyst achieves a large NH3 yield of 28.56 μg h-1 mgcat.-1 and a high Faradaic efficiency of 7.07% at -0.85 V vs. reversible hydrogen electrode. Notably, it also shows good electrochemical stability.NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber-Bosch process with huge CO2 emission. Electrochemical N2 reduction offers a carbon-neutral process to convert N2 to NH3 under ambient conditions, but it requires efficient and stable catalysts to drive the N2 reduction reaction. Herein, we report that a sulfur dots-graphene nanohybrid acts as a metal-free electrocatalyst for ambient N2-to-NH3 conversion with excellent selectivity. When operated in 0.5 M LiClO4, this electrocatalyst achieves a large NH3 yield of 28.56 μg h-1 mgcat.-1 and a high Faradaic efficiency of 7.07% at -0.85 V vs. reversible hydrogen electrode. Notably, it also shows good electrochemical stability.
NH₃ is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber-Bosch process with huge CO₂ emission. Electrochemical N₂ reduction offers a carbon-neutral process to convert N₂ to NH₃ under ambient conditions, but it requires efficient and stable catalysts to drive the N₂ reduction reaction. Herein, we report that a sulfur dots-graphene nanohybrid acts as a metal-free electrocatalyst for ambient N₂-to-NH₃ conversion with excellent selectivity. When operated in 0.5 M LiClO₄, this electrocatalyst achieves a large NH₃ yield of 28.56 μg h⁻¹ mgcₐₜ.⁻¹ and a high Faradaic efficiency of 7.07% at −0.85 V vs. reversible hydrogen electrode. Notably, it also shows good electrochemical stability.
Author Asiri, Abdullah M
Zheng, Hongguo
Wang, Ting
Luo, Yonglan
Sun, Xuping
Zhu, Xiaojuan
Wang, Huanbo
Zhao, Runbo
Chen, Hongyu
Huang, Hong
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Snippet NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber–Bosch process with huge CO2 emission....
NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber-Bosch process with huge CO2 emission....
NH₃ is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber-Bosch process with huge CO₂ emission....
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SubjectTerms Ammonia
carbon dioxide
catalysts
chemical reactions
Chemical reduction
Chemical synthesis
electrochemistry
electrodes
Emissions control
Graphene
greenhouse gas emissions
hydrogen
nanohybrids
nitrogen
Organic chemistry
Selectivity
Sulfur
Title Sulfur dots–graphene nanohybrid: a metal-free electrocatalyst for efficient N2-to-NH3 fixation under ambient conditions
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