Tailoring activation sites of metastable distorted 1T′-phase MoS2 by Ni doping for enhanced hydrogen evolution
Heteroatom doping is a promising approach to enhance catalytic activity by modulating physical properties, electronic structure, and reaction pathway. Herein, we demonstrate that appropriate Ni-doping could trigger a preferential transition of the basal plane from 2H (trigonal prismatic) to 1T′ (clu...
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| Published in | Nano research Vol. 15; no. 7; pp. 5946 - 5952 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Beijing
Tsinghua University Press
01.07.2022
|
| Subjects | |
| Online Access | Get full text |
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| Abstract | Heteroatom doping is a promising approach to enhance catalytic activity by modulating physical properties, electronic structure, and reaction pathway. Herein, we demonstrate that appropriate Ni-doping could trigger a preferential transition of the basal plane from 2H (trigonal prismatic) to 1T′ (clustered Mo) by inducing lattice distortion and S vacancy (SV) and thus dramatically facilitate its catalytic hydrogen evolution activity. It is noteworthy that the unique catalysts did possess superior catalytic performance of hydrogen evolution reaction (HER). The rate of photocatalytic hydrogen evolution could reach 20.45 mmol·g
−1
·h
−1
and reduced only slightly in the long period of the photocatalytic process. First-principles calculations reveal that the distorted Ni-1T′-MoS
2
with SV could generate favorable water adsorption energy (
E
ad
(H
2
O)) and Gibbs free energy of hydrogen adsorption (Δ
G
H
). This work exhibits a facile and promising pathway for synergistically regulating physical properties, electronic structure, or wettability based on the doping strategy for designing HER electrocatalysts. |
|---|---|
| AbstractList | Heteroatom doping is a promising approach to enhance catalytic activity by modulating physical properties, electronic structure, and reaction pathway. Herein, we demonstrate that appropriate Ni-doping could trigger a preferential transition of the basal plane from 2H (trigonal prismatic) to 1T′ (clustered Mo) by inducing lattice distortion and S vacancy (SV) and thus dramatically facilitate its catalytic hydrogen evolution activity. It is noteworthy that the unique catalysts did possess superior catalytic performance of hydrogen evolution reaction (HER). The rate of photocatalytic hydrogen evolution could reach 20.45 mmol·g−1·h−1 and reduced only slightly in the long period of the photocatalytic process. First-principles calculations reveal that the distorted Ni-1T′-MoS2 with SV could generate favorable water adsorption energy (Ead(H2O)) and Gibbs free energy of hydrogen adsorption (ΔGH). This work exhibits a facile and promising pathway for synergistically regulating physical properties, electronic structure, or wettability based on the doping strategy for designing HER electrocatalysts. Heteroatom doping is a promising approach to enhance catalytic activity by modulating physical properties, electronic structure, and reaction pathway. Herein, we demonstrate that appropriate Ni-doping could trigger a preferential transition of the basal plane from 2H (trigonal prismatic) to 1T′ (clustered Mo) by inducing lattice distortion and S vacancy (SV) and thus dramatically facilitate its catalytic hydrogen evolution activity. It is noteworthy that the unique catalysts did possess superior catalytic performance of hydrogen evolution reaction (HER). The rate of photocatalytic hydrogen evolution could reach 20.45 mmol·g −1 ·h −1 and reduced only slightly in the long period of the photocatalytic process. First-principles calculations reveal that the distorted Ni-1T′-MoS 2 with SV could generate favorable water adsorption energy ( E ad (H 2 O)) and Gibbs free energy of hydrogen adsorption (Δ G H ). This work exhibits a facile and promising pathway for synergistically regulating physical properties, electronic structure, or wettability based on the doping strategy for designing HER electrocatalysts. |
| Author | Sun, Chun Zhao, Qiang Liu, Mingming Wang, Longlu Zhuang, Zechao Wang, Jin Xie, Lingbin Tang, Meng Liu, Shijie Li, Hengxu Sun, Shujiang Liu, Shujuan |
| Author_xml | – sequence: 1 givenname: Mingming surname: Liu fullname: Liu, Mingming organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 2 givenname: Hengxu surname: Li fullname: Li, Hengxu organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 3 givenname: Shijie surname: Liu fullname: Liu, Shijie organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 4 givenname: Longlu surname: Wang fullname: Wang, Longlu email: wanglonglu@njupt.edu.cn organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 5 givenname: Lingbin surname: Xie fullname: Xie, Lingbin organization: State Key Laboratory of Organic Electronics and Information Displays & Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM) & Institute of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 6 givenname: Zechao surname: Zhuang fullname: Zhuang, Zechao organization: Department of Chemistry, Tsinghua University – sequence: 7 givenname: Chun surname: Sun fullname: Sun, Chun organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 8 givenname: Jin surname: Wang fullname: Wang, Jin email: jin@njupt.edu.cn organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 9 givenname: Meng surname: Tang fullname: Tang, Meng organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 10 givenname: Shujiang surname: Sun fullname: Sun, Shujiang organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 11 givenname: Shujuan surname: Liu fullname: Liu, Shujuan organization: State Key Laboratory of Organic Electronics and Information Displays & Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM) & Institute of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications – sequence: 12 givenname: Qiang surname: Zhao fullname: Zhao, Qiang email: iamqzhao@njupt.edu.cn organization: College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications, State Key Laboratory of Organic Electronics and Information Displays & Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM) & Institute of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications |
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| Keywords | hydrogen evolution Ni doping S vacancy phase transformation electronic structure |
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| Snippet | Heteroatom doping is a promising approach to enhance catalytic activity by modulating physical properties, electronic structure, and reaction pathway. Herein,... |
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| SubjectTerms | Adsorbed water Adsorption Atomic/Molecular Structure and Spectra Basal plane Biomedicine Biotechnology Carbon Catalysis Catalysts Catalytic activity Chemistry and Materials Science Condensed Matter Physics Doping Electrocatalysts Electronic structure Energy Engineering Evolution First principles Free energy Gibbs free energy Graphene Hydrogen Hydrogen evolution reactions Hydrogen-based energy Lattice vacancies Materials Science Molybdenum disulfide Nanotechnology Nickel Phase transitions Photocatalysis Physical properties Research Article Wettability |
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| Title | Tailoring activation sites of metastable distorted 1T′-phase MoS2 by Ni doping for enhanced hydrogen evolution |
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