Toward enhanced activity of a graphitic carbon nitride-based electrocatalyst in oxygen reduction and hydrogen evolution reactions via atomic sulfur doping
Atomic doping has always been demonstrated as a feasible way to effectively alter the catalytic properties of metal-free electrocatalysts. Herein, we report the first experimental and theoretical investigation regarding the influence of sulfur doping on the activity of a carbon nitride (C 3 N 4 )-ba...
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| Published in | Journal of materials chemistry. A, Materials for energy and sustainability Vol. 4; no. 31; pp. 12205 - 12211 |
|---|---|
| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
2016
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Atomic doping has always been demonstrated as a feasible way to effectively alter the catalytic properties of metal-free electrocatalysts. Herein, we report the first experimental and theoretical investigation regarding the influence of sulfur doping on the activity of a carbon nitride (C
3
N
4
)-based electrocatalyst in the oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). It is found that the sulfur dopant within the mesoporous carbon-supported C
3
N
4
motif can remarkably boost its ORR activity, which rivals that of commercial Pt/C yet with better cross-over tolerance and durability, while the HER performance of the composite catalyst is superior than most other reported metal-free electrocatalysts and is even comparable to the most active non-noble metal-based HER materials. Theoretical calculations further reveal that the excellent activity of the doped composite stems from the high charge and spin densities in the C
3
N
4
motif as well as altered competent adsorption energies of reaction intermediates
via
the atomic sulfur doping. The results in this work feature a facile and effective approach for engineering a high performance C
3
N
4
-based electrocatalyst, which may also enlighten the designing and fabrication of other metal-free materials as next-generation electrocatalysts. |
|---|---|
| AbstractList | Atomic doping has always been demonstrated as a feasible way to effectively alter the catalytic properties of metal-free electrocatalysts. Herein, we report the first experimental and theoretical investigation regarding the influence of sulfur doping on the activity of a carbon nitride (C3N4)-based electrocatalyst in the oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). It is found that the sulfur dopant within the mesoporous carbon-supported C3N4 motif can remarkably boost its ORR activity, which rivals that of commercial Pt/C yet with better cross-over tolerance and durability, while the HER performance of the composite catalyst is superior than most other reported metal-free electrocatalysts and is even comparable to the most active non-noble metal-based HER materials. Theoretical calculations further reveal that the excellent activity of the doped composite stems from the high charge and spin densities in the C3N4 motif as well as altered competent adsorption energies of reaction intermediates via the atomic sulfur doping. The results in this work feature a facile and effective approach for engineering a high performance C3N4-based electrocatalyst, which may also enlighten the designing and fabrication of other metal-free materials as next-generation electrocatalysts. Atomic doping has always been demonstrated as a feasible way to effectively alter the catalytic properties of metal-free electrocatalysts. Herein, we report the first experimental and theoretical investigation regarding the influence of sulfur doping on the activity of a carbon nitride (C 3 N 4 )-based electrocatalyst in the oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). It is found that the sulfur dopant within the mesoporous carbon-supported C 3 N 4 motif can remarkably boost its ORR activity, which rivals that of commercial Pt/C yet with better cross-over tolerance and durability, while the HER performance of the composite catalyst is superior than most other reported metal-free electrocatalysts and is even comparable to the most active non-noble metal-based HER materials. Theoretical calculations further reveal that the excellent activity of the doped composite stems from the high charge and spin densities in the C 3 N 4 motif as well as altered competent adsorption energies of reaction intermediates via the atomic sulfur doping. The results in this work feature a facile and effective approach for engineering a high performance C 3 N 4 -based electrocatalyst, which may also enlighten the designing and fabrication of other metal-free materials as next-generation electrocatalysts. Atomic doping has always been demonstrated as a feasible way to effectively alter the catalytic properties of metal-free electrocatalysts. Herein, we report the first experimental and theoretical investigation regarding the influence of sulfur doping on the activity of a carbon nitride (C₃N₄)-based electrocatalyst in the oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). It is found that the sulfur dopant within the mesoporous carbon-supported C₃N₄ motif can remarkably boost its ORR activity, which rivals that of commercial Pt/C yet with better cross-over tolerance and durability, while the HER performance of the composite catalyst is superior than most other reported metal-free electrocatalysts and is even comparable to the most active non-noble metal-based HER materials. Theoretical calculations further reveal that the excellent activity of the doped composite stems from the high charge and spin densities in the C₃N₄ motif as well as altered competent adsorption energies of reaction intermediates via the atomic sulfur doping. The results in this work feature a facile and effective approach for engineering a high performance C₃N₄-based electrocatalyst, which may also enlighten the designing and fabrication of other metal-free materials as next-generation electrocatalysts. |
| Author | Zhu, Minshen Zhi, Chunyi Huang, Yang Zhao, Jingxiang Huang, Yan Pei, Zengxia Wang, Zifeng Chen, Zhongfang |
| Author_xml | – sequence: 1 givenname: Zengxia surname: Pei fullname: Pei, Zengxia organization: Department of Physics and Materials Science, City University of Hong Kong, Kowloon, China – sequence: 2 givenname: Jingxiang surname: Zhao fullname: Zhao, Jingxiang organization: Department of Chemistry, The Institute for Functional Nanomaterials, University of Puerto Rico, Rio Piedras Campus, San Juan – sequence: 3 givenname: Yan surname: Huang fullname: Huang, Yan organization: Department of Physics and Materials Science, City University of Hong Kong, Kowloon, China – sequence: 4 givenname: Yang surname: Huang fullname: Huang, Yang organization: Department of Physics and Materials Science, City University of Hong Kong, Kowloon, China – sequence: 5 givenname: Minshen surname: Zhu fullname: Zhu, Minshen organization: Department of Physics and Materials Science, City University of Hong Kong, Kowloon, China – sequence: 6 givenname: Zifeng surname: Wang fullname: Wang, Zifeng organization: Department of Physics and Materials Science, City University of Hong Kong, Kowloon, China – sequence: 7 givenname: Zhongfang surname: Chen fullname: Chen, Zhongfang organization: Department of Chemistry, The Institute for Functional Nanomaterials, University of Puerto Rico, Rio Piedras Campus, San Juan – sequence: 8 givenname: Chunyi surname: Zhi fullname: Zhi, Chunyi organization: Department of Physics and Materials Science, City University of Hong Kong, Kowloon, China, Shenzhen Research Institute |
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| Snippet | Atomic doping has always been demonstrated as a feasible way to effectively alter the catalytic properties of metal-free electrocatalysts. Herein, we report... |
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| SubjectTerms | adsorption carbon nitride Catalysts Doping durability Electrocatalysts electrochemistry engineering graphene Hydrogen evolution hydrogen production Oxygen porous media Reduction Stems Sulfur |
| Title | Toward enhanced activity of a graphitic carbon nitride-based electrocatalyst in oxygen reduction and hydrogen evolution reactions via atomic sulfur doping |
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