Polymorphic cobalt diselenide as extremely stable electrocatalyst in acidic media via a phase-mixing strategy
Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use often suffers from undesirable structural degradation and hence poor stability, especially in acidic media. We report here an alkali-heating...
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| Published in | Nature communications Vol. 10; no. 1; pp. 5338 - 9 |
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| Main Authors | , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
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London
Nature Publishing Group UK
25.11.2019
Nature Publishing Group Nature Portfolio |
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| Abstract | Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use often suffers from undesirable structural degradation and hence poor stability, especially in acidic media. We report here an alkali-heating synthesis to achieve phase-mixed cobalt diselenide material with nearly homogeneous distribution of cubic and orthorhombic phases. Using water electroreduction as a model reaction, we observe that the phase-mixed cobalt diselenide reaches the current density of 10 milliamperes per square centimeter at overpotential of mere 124 millivolts in acidic electrolyte. The catalyst shows no sign of deactivation after more than 400 h of continuous operation and the polarization curve is well retained after 50,000 potential cycles. Experimental and computational investigations uncover a boosted covalency between Co and Se atoms resulting from the phase mixture, which substantially enhances the lattice robustness and thereby the material stability. The findings provide promising design strategy for long-lived catalysts in acid through crystal phase engineering.
Noble-metal-free catalysts often show stability issues in acidic media due to structural degradation. Here authors show that phase-mixed engineering of cobalt diselenide electrocatalysts can enable greater covalency of Co-Se bonds and improve robustness for catalyzing hydrogen evolution in acid. |
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| AbstractList | Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use often suffers from undesirable structural degradation and hence poor stability, especially in acidic media. We report here an alkali-heating synthesis to achieve phase-mixed cobalt diselenide material with nearly homogeneous distribution of cubic and orthorhombic phases. Using water electroreduction as a model reaction, we observe that the phase-mixed cobalt diselenide reaches the current density of 10 milliamperes per square centimeter at overpotential of mere 124 millivolts in acidic electrolyte. The catalyst shows no sign of deactivation after more than 400 h of continuous operation and the polarization curve is well retained after 50,000 potential cycles. Experimental and computational investigations uncover a boosted covalency between Co and Se atoms resulting from the phase mixture, which substantially enhances the lattice robustness and thereby the material stability. The findings provide promising design strategy for long-lived catalysts in acid through crystal phase engineering. Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use often suffers from undesirable structural degradation and hence poor stability, especially in acidic media. We report here an alkali-heating synthesis to achieve phase-mixed cobalt diselenide material with nearly homogeneous distribution of cubic and orthorhombic phases. Using water electroreduction as a model reaction, we observe that the phase-mixed cobalt diselenide reaches the current density of 10 milliamperes per square centimeter at overpotential of mere 124 millivolts in acidic electrolyte. The catalyst shows no sign of deactivation after more than 400 h of continuous operation and the polarization curve is well retained after 50,000 potential cycles. Experimental and computational investigations uncover a boosted covalency between Co and Se atoms resulting from the phase mixture, which substantially enhances the lattice robustness and thereby the material stability. The findings provide promising design strategy for long-lived catalysts in acid through crystal phase engineering. Noble-metal-free catalysts often show stability issues in acidic media due to structural degradation. Here authors show that phase-mixed engineering of cobalt diselenide electrocatalysts can enable greater covalency of Co-Se bonds and improve robustness for catalyzing hydrogen evolution in acid. Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use often suffers from undesirable structural degradation and hence poor stability, especially in acidic media. We report here an alkali-heating synthesis to achieve phase-mixed cobalt diselenide material with nearly homogeneous distribution of cubic and orthorhombic phases. Using water electroreduction as a model reaction, we observe that the phase-mixed cobalt diselenide reaches the current density of 10 milliamperes per square centimeter at overpotential of mere 124 millivolts in acidic electrolyte. The catalyst shows no sign of deactivation after more than 400 h of continuous operation and the polarization curve is well retained after 50,000 potential cycles. Experimental and computational investigations uncover a boosted covalency between Co and Se atoms resulting from the phase mixture, which substantially enhances the lattice robustness and thereby the material stability. The findings provide promising design strategy for long-lived catalysts in acid through crystal phase engineering.Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use often suffers from undesirable structural degradation and hence poor stability, especially in acidic media. We report here an alkali-heating synthesis to achieve phase-mixed cobalt diselenide material with nearly homogeneous distribution of cubic and orthorhombic phases. Using water electroreduction as a model reaction, we observe that the phase-mixed cobalt diselenide reaches the current density of 10 milliamperes per square centimeter at overpotential of mere 124 millivolts in acidic electrolyte. The catalyst shows no sign of deactivation after more than 400 h of continuous operation and the polarization curve is well retained after 50,000 potential cycles. Experimental and computational investigations uncover a boosted covalency between Co and Se atoms resulting from the phase mixture, which substantially enhances the lattice robustness and thereby the material stability. The findings provide promising design strategy for long-lived catalysts in acid through crystal phase engineering. Noble-metal-free catalysts often show stability issues in acidic media due to structural degradation. Here authors show that phase-mixed engineering of cobalt diselenide electrocatalysts can enable greater covalency of Co-Se bonds and improve robustness for catalyzing hydrogen evolution in acid. |
| ArticleNumber | 5338 |
| Author | Zheng, Ya-Rong Zheng, Xiao Ma, Cheng Gao, Fei-Yue Yang, Peng-Peng Yu, Xingxing Zhu, Jun-Fa Hu, Shao-Jin Gu, Chao Zhang, Xiao-Long Wu, Rui Niu, Zhuang-Zhuang Zheng, Xu-Sheng Gao, Min-Rui Yu, Shu-Hong |
| Author_xml | – sequence: 1 givenname: Xiao-Long surname: Zhang fullname: Zhang, Xiao-Long organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 2 givenname: Shao-Jin surname: Hu fullname: Hu, Shao-Jin organization: Division of Theoretical and Computational Sciences, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China – sequence: 3 givenname: Ya-Rong orcidid: 0000-0003-2129-7774 surname: Zheng fullname: Zheng, Ya-Rong organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 4 givenname: Rui surname: Wu fullname: Wu, Rui organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 5 givenname: Fei-Yue surname: Gao fullname: Gao, Fei-Yue organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 6 givenname: Peng-Peng surname: Yang fullname: Yang, Peng-Peng organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 7 givenname: Zhuang-Zhuang surname: Niu fullname: Niu, Zhuang-Zhuang organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 8 givenname: Chao surname: Gu fullname: Gu, Chao organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 9 givenname: Xingxing surname: Yu fullname: Yu, Xingxing organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 10 givenname: Xu-Sheng surname: Zheng fullname: Zheng, Xu-Sheng organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 11 givenname: Cheng surname: Ma fullname: Ma, Cheng organization: Department of Materials Science and Engineering, University of Science and Technology of China – sequence: 12 givenname: Xiao orcidid: 0000-0002-9804-1833 surname: Zheng fullname: Zheng, Xiao organization: Division of Theoretical and Computational Sciences, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China – sequence: 13 givenname: Jun-Fa orcidid: 0000-0003-0888-4261 surname: Zhu fullname: Zhu, Jun-Fa organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 14 givenname: Min-Rui orcidid: 0000-0002-7805-803X surname: Gao fullname: Gao, Min-Rui email: mgao@ustc.edu.cn organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China – sequence: 15 givenname: Shu-Hong orcidid: 0000-0003-3732-1011 surname: Yu fullname: Yu, Shu-Hong email: shyu@ustc.edu.cn organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Dalian National Laboratory for Clean Energy |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31767845$$D View this record in MEDLINE/PubMed |
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| Snippet | Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use... Noble-metal-free catalysts often show stability issues in acidic media due to structural degradation. Here authors show that phase-mixed engineering of cobalt... |
| SourceID | doaj pubmedcentral proquest pubmed crossref springer |
| SourceType | Open Website Open Access Repository Aggregation Database Index Database Enrichment Source Publisher |
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| SubjectTerms | 119/118 639/301/299/886 639/638/161/886 639/925/357/537 Catalysts Cobalt Computer applications Deactivation Electrolytes Energy Humanities and Social Sciences Laboratories multidisciplinary Phase transitions Physical sciences Platinum Science Science (multidisciplinary) Transmission electron microscopy |
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| Title | Polymorphic cobalt diselenide as extremely stable electrocatalyst in acidic media via a phase-mixing strategy |
| URI | https://link.springer.com/article/10.1038/s41467-019-12992-y https://www.ncbi.nlm.nih.gov/pubmed/31767845 https://www.proquest.com/docview/2317922195 https://www.proquest.com/docview/2318725294 https://pubmed.ncbi.nlm.nih.gov/PMC6877578 https://doaj.org/article/a430b5998fb6455fb01a8f6db0d529ad |
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