Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution Reaction
Abstract Catalytically active metals atomically dispersed on supports presents the ultimate atom utilization efficiency and cost‐effective pathway for electrocatalyst design. Optimizing the coordination nature of metal atoms represents the advanced strategy for enhancing the catalytic activity and t...
| Main Authors: | , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2021-06-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202100347 |
| _version_ | 1818741954323677184 |
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| author | Kai Ling Zhou Chang Bao Han Zelin Wang Xiaoxing Ke Changhao Wang Yuhong Jin Qianqian Zhang Jingbing Liu Hao Wang Hui Yan |
| author_facet | Kai Ling Zhou Chang Bao Han Zelin Wang Xiaoxing Ke Changhao Wang Yuhong Jin Qianqian Zhang Jingbing Liu Hao Wang Hui Yan |
| author_sort | Kai Ling Zhou |
| collection | DOAJ |
| description | Abstract Catalytically active metals atomically dispersed on supports presents the ultimate atom utilization efficiency and cost‐effective pathway for electrocatalyst design. Optimizing the coordination nature of metal atoms represents the advanced strategy for enhancing the catalytic activity and the selectivity of single‐atom catalysts (SACs). Here, we designed a transition‐metal based sulfide‐Ni3S2 with abundant exposed Ni vacancies created by the interaction between chloride ions and the functional groups on the surface of Ni3S2 for the anchoring of atomically dispersed Pt (PtSA‐Ni3S2). The theoretical calculation reveals that unique Pt‐Ni3S2 support interaction increases the d orbital electron occupation at the Fermi level and leads to a shift‐down of the d ‐band center, which energetically enhances H2O adsorption and provides the optimum H binding sites. Introducing Pt into Ni position in Ni3S2 system can efficiently enhance electronic field distribution and construct a metallic‐state feature on the Pt sites by the orbital hybridization between S‐3p and Pt‐5d for improved reaction kinetics. Finally, the fabricated PtSA‐Ni3S2 SAC is supported by Ag nanowires network to construct a seamless conductive three‐dimensional (3D) nanostructure (PtSA‐Ni3S2@Ag NWs), and the developed catalyst shows an extremely great mass activity of 7.6 A mg−1 with 27‐time higher than the commercial Pt/C HER catalyst. |
| first_indexed | 2024-12-18T02:04:49Z |
| format | Article |
| id | doaj.art-8c1051c16db340ac9f9a7dc79609d600 |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-12-18T02:04:49Z |
| publishDate | 2021-06-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-8c1051c16db340ac9f9a7dc79609d6002022-12-21T21:24:38ZengWileyAdvanced Science2198-38442021-06-01812n/an/a10.1002/advs.202100347Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution ReactionKai Ling Zhou0Chang Bao Han1Zelin Wang2Xiaoxing Ke3Changhao Wang4Yuhong Jin5Qianqian Zhang6Jingbing Liu7Hao Wang8Hui Yan9Faculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaFaculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Education Ministry of China Beijing University of Technology Beijing 100124 P. R. ChinaAbstract Catalytically active metals atomically dispersed on supports presents the ultimate atom utilization efficiency and cost‐effective pathway for electrocatalyst design. Optimizing the coordination nature of metal atoms represents the advanced strategy for enhancing the catalytic activity and the selectivity of single‐atom catalysts (SACs). Here, we designed a transition‐metal based sulfide‐Ni3S2 with abundant exposed Ni vacancies created by the interaction between chloride ions and the functional groups on the surface of Ni3S2 for the anchoring of atomically dispersed Pt (PtSA‐Ni3S2). The theoretical calculation reveals that unique Pt‐Ni3S2 support interaction increases the d orbital electron occupation at the Fermi level and leads to a shift‐down of the d ‐band center, which energetically enhances H2O adsorption and provides the optimum H binding sites. Introducing Pt into Ni position in Ni3S2 system can efficiently enhance electronic field distribution and construct a metallic‐state feature on the Pt sites by the orbital hybridization between S‐3p and Pt‐5d for improved reaction kinetics. Finally, the fabricated PtSA‐Ni3S2 SAC is supported by Ag nanowires network to construct a seamless conductive three‐dimensional (3D) nanostructure (PtSA‐Ni3S2@Ag NWs), and the developed catalyst shows an extremely great mass activity of 7.6 A mg−1 with 27‐time higher than the commercial Pt/C HER catalyst.https://doi.org/10.1002/advs.202100347architectural nanostructure engineeringhydrogen evolution reaction (HER)metal‐support interactionsingle‐atom catalysts (SACs)sulfides |
| spellingShingle | Kai Ling Zhou Chang Bao Han Zelin Wang Xiaoxing Ke Changhao Wang Yuhong Jin Qianqian Zhang Jingbing Liu Hao Wang Hui Yan Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution Reaction Advanced Science architectural nanostructure engineering hydrogen evolution reaction (HER) metal‐support interaction single‐atom catalysts (SACs) sulfides |
| title | Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution Reaction |
| title_full | Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution Reaction |
| title_fullStr | Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution Reaction |
| title_full_unstemmed | Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution Reaction |
| title_short | Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution Reaction |
| title_sort | atomically dispersed platinum modulated by sulfide as an efficient electrocatalyst for hydrogen evolution reaction |
| topic | architectural nanostructure engineering hydrogen evolution reaction (HER) metal‐support interaction single‐atom catalysts (SACs) sulfides |
| url | https://doi.org/10.1002/advs.202100347 |
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