Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites
Molecular Co2+ ions were grafted onto doped graphene in a coordination environment, resulting in the formation of molecularly well-defined, highly active electrocatalytic sites at a heterogeneous interface for the oxygen evolution reaction (OER). The S dopants of graphene are suggested to be one of...
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sg-ntu-dr.10356-834122023-12-29T06:47:26Z Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites Wang, Jiong Ge, Xiaoming Liu, Zhaolin Thia, Larissa Yan, Ya Xiao, Wei Wang, Xin School of Chemical and Biomedical Engineering Centre for Programmable Materials Electrocatalysts Oxygen evolution reaction Molecular Co2+ ions were grafted onto doped graphene in a coordination environment, resulting in the formation of molecularly well-defined, highly active electrocatalytic sites at a heterogeneous interface for the oxygen evolution reaction (OER). The S dopants of graphene are suggested to be one of the binding sites and to be responsible for improving the intrinsic activity of the Co sites. The turnover frequency of such Co sites is greater than that of many Co-based nanostructures and IrO2 catalysts. Through a series of carefully designed experiments, the pathway for the evolution of the Co cation-based molecular catalyst for the OER was further demonstrated on such a single Co-ion site for the first time. The Co2+ ions were successively oxidized to Co3+ and Co4+ states prior to the OER. The sequential oxidation was coupled with the transfer of different numbers of protons/hydroxides and generated an active Co4+═O fragment. A side-on hydroperoxo ligand of the Co4+ site is proposed as a key intermediate for the formation of dioxygen. NRF (Natl Research Foundation, S’pore) MOE (Min. of Education, S’pore) Accepted version 2017-08-03T08:08:41Z 2019-12-06T15:21:56Z 2017-08-03T08:08:41Z 2019-12-06T15:21:56Z 2017 Journal Article Wang, J., Ge, X., Liu, Z., Thia, L., Yan, Y., Xiao, W., et al. (2017). Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites. Journal of the American Chemical Society, 139(5), 1878-1884. 0002-7863 https://hdl.handle.net/10356/83412 http://hdl.handle.net/10220/43539 10.1021/jacs.6b10307 en Journal of the American Chemical Society © 2017 American Chemical Society. This is the author created version of a work that has been peer reviewed and accepted for publication by Journal of the American Chemical Society, American Chemical Society. It incorporates referee’s comments but changes resulting from the publishing process, such as copyediting, structural formatting, may not be reflected in this document. The published version is available at: [http://dx.doi.org/10.1021/jacs.6b10307]. 15 p. application/pdf |
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Electrocatalysts Oxygen evolution reaction |
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Electrocatalysts Oxygen evolution reaction Wang, Jiong Ge, Xiaoming Liu, Zhaolin Thia, Larissa Yan, Ya Xiao, Wei Wang, Xin Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites |
| description |
Molecular Co2+ ions were grafted onto doped graphene in a coordination environment, resulting in the formation of molecularly well-defined, highly active electrocatalytic sites at a heterogeneous interface for the oxygen evolution reaction (OER). The S dopants of graphene are suggested to be one of the binding sites and to be responsible for improving the intrinsic activity of the Co sites. The turnover frequency of such Co sites is greater than that of many Co-based nanostructures and IrO2 catalysts. Through a series of carefully designed experiments, the pathway for the evolution of the Co cation-based molecular catalyst for the OER was further demonstrated on such a single Co-ion site for the first time. The Co2+ ions were successively oxidized to Co3+ and Co4+ states prior to the OER. The sequential oxidation was coupled with the transfer of different numbers of protons/hydroxides and generated an active Co4+═O fragment. A side-on hydroperoxo ligand of the Co4+ site is proposed as a key intermediate for the formation of dioxygen. |
| author2 |
School of Chemical and Biomedical Engineering |
| author_facet |
School of Chemical and Biomedical Engineering Wang, Jiong Ge, Xiaoming Liu, Zhaolin Thia, Larissa Yan, Ya Xiao, Wei Wang, Xin |
| format |
Article |
| author |
Wang, Jiong Ge, Xiaoming Liu, Zhaolin Thia, Larissa Yan, Ya Xiao, Wei Wang, Xin |
| author_sort |
Wang, Jiong |
| title |
Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites |
| title_short |
Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites |
| title_full |
Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites |
| title_fullStr |
Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites |
| title_full_unstemmed |
Heterogeneous Electrocatalyst with Molecular Cobalt Ions Serving as the Center of Active Sites |
| title_sort |
heterogeneous electrocatalyst with molecular cobalt ions serving as the center of active sites |
| publishDate |
2017 |
| url |
https://hdl.handle.net/10356/83412 http://hdl.handle.net/10220/43539 |
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1787136540756934656 |