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 in | Chemical communications (Cambridge, England) Vol. 55; no. 21; pp. 3152 - 3155 |
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Main Authors | , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
Cambridge
Royal Society of Chemistry
07.03.2019
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Subjects | |
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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. |
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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 |
Author_xml | – sequence: 1 givenname: Hongyu surname: Chen fullname: Chen, Hongyu – sequence: 2 givenname: Xiaojuan surname: Zhu fullname: Zhu, Xiaojuan – sequence: 3 givenname: Hong surname: Huang fullname: Huang, Hong – sequence: 4 givenname: Huanbo surname: Wang fullname: Wang, Huanbo – sequence: 5 givenname: Ting surname: Wang fullname: Wang, Ting – sequence: 6 givenname: Runbo surname: Zhao fullname: Zhao, Runbo – sequence: 7 givenname: Hongguo surname: Zheng fullname: Zheng, Hongguo – sequence: 8 givenname: Abdullah surname: Asiri middlename: M fullname: Asiri, Abdullah M – sequence: 9 givenname: Yonglan surname: Luo fullname: Luo, Yonglan – sequence: 10 givenname: Xuping surname: Sun fullname: Sun, Xuping |
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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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