In Situ Immobilizing Atomically Dispersed Ru on Oxygen-Defective Co3O4 for Efficient Oxygen Evolution
The synergistic regulation of the electronic structures of transition-metal oxide-based catalysts via oxygen vacancy defects and single-atom doping is efficient to boost their oxygen evolution reaction (OER) performance, which remains challenging due to complex synthetic procedures. Herein, a facile...
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creator | Yuan, Cheng-Zong Wang, Shuo San Hui, Kwan Wang, Kaixi Li, Junfeng Gao, Haixing Zha, Chenyang Zhang, Xiaomeng Dinh, Duc Anh Wu, Xi-Lin Tang, Zikang Wan, Jiawei Shao, Zongping Hui, Kwun Nam |
description | The synergistic regulation of the electronic structures of transition-metal oxide-based catalysts via oxygen vacancy defects and single-atom doping is efficient to boost their oxygen evolution reaction (OER) performance, which remains challenging due to complex synthetic procedures. Herein, a facile defect-induced in situ single-atom deposition strategy is developed to anchor atomically dispersed Ru single-atom onto oxygen vacancy-rich cobalt oxides (Ru/Co3O4–x ) based on the spontaneous redox reaction between Ru3+ ions and nonstoichiometric Co3O4–x . Accordingly, the as-prepared Ru/Co3O4–x electrocatalyst with the coexistence of oxygen vacancies and Ru atoms exhibits excellent performances toward OER with a low overpotential of 280 mV at 10 mA cm–2, a small Tafel slope value of 86.9 mV dec–1, and good long-term stability in alkaline media. Furthermore, density functional theory calculations uncover that oxygen vacancy and atomically dispersed Ru could synergistically tailor electron decentralization and d-band center of Co atoms, further optimizing the adsorption of oxygen-based intermediates (*OH, *O, and *OOH) and reducing the reaction barriers of OER. This work proposes an available strategy for constructing electrocatalysts with abundant oxygen vacancies and atomically dispersed noble metal and presents a deep understanding of synergistic electronic engineering of transition-metal-based catalysts to boost oxygen evolution. |
doi_str_mv | 10.1021/acscatal.2c04946 |
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Herein, a facile defect-induced in situ single-atom deposition strategy is developed to anchor atomically dispersed Ru single-atom onto oxygen vacancy-rich cobalt oxides (Ru/Co3O4–x ) based on the spontaneous redox reaction between Ru3+ ions and nonstoichiometric Co3O4–x . Accordingly, the as-prepared Ru/Co3O4–x electrocatalyst with the coexistence of oxygen vacancies and Ru atoms exhibits excellent performances toward OER with a low overpotential of 280 mV at 10 mA cm–2, a small Tafel slope value of 86.9 mV dec–1, and good long-term stability in alkaline media. Furthermore, density functional theory calculations uncover that oxygen vacancy and atomically dispersed Ru could synergistically tailor electron decentralization and d-band center of Co atoms, further optimizing the adsorption of oxygen-based intermediates (*OH, *O, and *OOH) and reducing the reaction barriers of OER. This work proposes an available strategy for constructing electrocatalysts with abundant oxygen vacancies and atomically dispersed noble metal and presents a deep understanding of synergistic electronic engineering of transition-metal-based catalysts to boost oxygen evolution.</description><identifier>ISSN: 2155-5435</identifier><identifier>EISSN: 2155-5435</identifier><identifier>DOI: 10.1021/acscatal.2c04946</identifier><language>eng</language><publisher>American Chemical Society</publisher><ispartof>ACS catalysis, 2023-02, Vol.13 (4), p.2462-2471</ispartof><rights>2023 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0002-9008-2323 ; 0000-0002-3008-8571 ; 0000-0001-7089-7587 ; 0000-0002-4767-8957 ; 0000-0002-0056-7782</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acscatal.2c04946$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acscatal.2c04946$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,27076,27924,27925,56738,56788</link.rule.ids></links><search><creatorcontrib>Yuan, Cheng-Zong</creatorcontrib><creatorcontrib>Wang, Shuo</creatorcontrib><creatorcontrib>San Hui, Kwan</creatorcontrib><creatorcontrib>Wang, Kaixi</creatorcontrib><creatorcontrib>Li, Junfeng</creatorcontrib><creatorcontrib>Gao, Haixing</creatorcontrib><creatorcontrib>Zha, Chenyang</creatorcontrib><creatorcontrib>Zhang, Xiaomeng</creatorcontrib><creatorcontrib>Dinh, Duc Anh</creatorcontrib><creatorcontrib>Wu, Xi-Lin</creatorcontrib><creatorcontrib>Tang, Zikang</creatorcontrib><creatorcontrib>Wan, Jiawei</creatorcontrib><creatorcontrib>Shao, Zongping</creatorcontrib><creatorcontrib>Hui, Kwun Nam</creatorcontrib><title>In Situ Immobilizing Atomically Dispersed Ru on Oxygen-Defective Co3O4 for Efficient Oxygen Evolution</title><title>ACS catalysis</title><addtitle>ACS Catal</addtitle><description>The synergistic regulation of the electronic structures of transition-metal oxide-based catalysts via oxygen vacancy defects and single-atom doping is efficient to boost their oxygen evolution reaction (OER) performance, which remains challenging due to complex synthetic procedures. Herein, a facile defect-induced in situ single-atom deposition strategy is developed to anchor atomically dispersed Ru single-atom onto oxygen vacancy-rich cobalt oxides (Ru/Co3O4–x ) based on the spontaneous redox reaction between Ru3+ ions and nonstoichiometric Co3O4–x . Accordingly, the as-prepared Ru/Co3O4–x electrocatalyst with the coexistence of oxygen vacancies and Ru atoms exhibits excellent performances toward OER with a low overpotential of 280 mV at 10 mA cm–2, a small Tafel slope value of 86.9 mV dec–1, and good long-term stability in alkaline media. Furthermore, density functional theory calculations uncover that oxygen vacancy and atomically dispersed Ru could synergistically tailor electron decentralization and d-band center of Co atoms, further optimizing the adsorption of oxygen-based intermediates (*OH, *O, and *OOH) and reducing the reaction barriers of OER. This work proposes an available strategy for constructing electrocatalysts with abundant oxygen vacancies and atomically dispersed noble metal and presents a deep understanding of synergistic electronic engineering of transition-metal-based catalysts to boost oxygen evolution.</description><issn>2155-5435</issn><issn>2155-5435</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><sourceid/><recordid>eNpNkF1LwzAYhYMoOObuvcwPsDOfbXM5tukGg4If1yVN34yMLJE1Hc5fb8UKnptz4BzeFx6E7imZU8Loozad0Un7OTNEKJFfoQmjUmZScHn9L9-iWdcdyCAh87IgEwTbgF9d6vH2eIyN8-7LhT1epHh0Rnt_wSvXfcCpgxa_9DgGXH1e9hCyFVgwyZ0BLyOvBLbxhNfWOuMgpHGE1-fo--RiuEM3VvsOZqNP0fvT-m25yXbV83a52GWaKpayRtGGl7qVBdBWUdboHJgllgtSkJYURimilBEqpyWDhoKkXJpSFg3RQyH4FD383h2A1IfYn8Lwraak_qFU_1GqR0r8G8U5XFw</recordid><startdate>20230217</startdate><enddate>20230217</enddate><creator>Yuan, Cheng-Zong</creator><creator>Wang, Shuo</creator><creator>San Hui, Kwan</creator><creator>Wang, Kaixi</creator><creator>Li, Junfeng</creator><creator>Gao, Haixing</creator><creator>Zha, Chenyang</creator><creator>Zhang, Xiaomeng</creator><creator>Dinh, Duc Anh</creator><creator>Wu, Xi-Lin</creator><creator>Tang, Zikang</creator><creator>Wan, Jiawei</creator><creator>Shao, Zongping</creator><creator>Hui, Kwun Nam</creator><general>American Chemical Society</general><scope/><orcidid>https://orcid.org/0000-0002-9008-2323</orcidid><orcidid>https://orcid.org/0000-0002-3008-8571</orcidid><orcidid>https://orcid.org/0000-0001-7089-7587</orcidid><orcidid>https://orcid.org/0000-0002-4767-8957</orcidid><orcidid>https://orcid.org/0000-0002-0056-7782</orcidid></search><sort><creationdate>20230217</creationdate><title>In Situ Immobilizing Atomically Dispersed Ru on Oxygen-Defective Co3O4 for Efficient Oxygen Evolution</title><author>Yuan, Cheng-Zong ; Wang, Shuo ; San Hui, Kwan ; Wang, Kaixi ; Li, Junfeng ; Gao, Haixing ; Zha, Chenyang ; Zhang, Xiaomeng ; Dinh, Duc Anh ; Wu, Xi-Lin ; Tang, Zikang ; Wan, Jiawei ; Shao, Zongping ; Hui, Kwun Nam</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a192t-b91b38ad57e1d912ba6e2f0f34070d07c99099c496182eb1e5135c857b0a09943</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Yuan, Cheng-Zong</creatorcontrib><creatorcontrib>Wang, Shuo</creatorcontrib><creatorcontrib>San Hui, Kwan</creatorcontrib><creatorcontrib>Wang, Kaixi</creatorcontrib><creatorcontrib>Li, Junfeng</creatorcontrib><creatorcontrib>Gao, Haixing</creatorcontrib><creatorcontrib>Zha, Chenyang</creatorcontrib><creatorcontrib>Zhang, Xiaomeng</creatorcontrib><creatorcontrib>Dinh, Duc Anh</creatorcontrib><creatorcontrib>Wu, Xi-Lin</creatorcontrib><creatorcontrib>Tang, Zikang</creatorcontrib><creatorcontrib>Wan, Jiawei</creatorcontrib><creatorcontrib>Shao, Zongping</creatorcontrib><creatorcontrib>Hui, Kwun Nam</creatorcontrib><jtitle>ACS catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Yuan, Cheng-Zong</au><au>Wang, Shuo</au><au>San Hui, Kwan</au><au>Wang, Kaixi</au><au>Li, Junfeng</au><au>Gao, Haixing</au><au>Zha, Chenyang</au><au>Zhang, Xiaomeng</au><au>Dinh, Duc Anh</au><au>Wu, Xi-Lin</au><au>Tang, Zikang</au><au>Wan, Jiawei</au><au>Shao, Zongping</au><au>Hui, Kwun Nam</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>In Situ Immobilizing Atomically Dispersed Ru on Oxygen-Defective Co3O4 for Efficient Oxygen Evolution</atitle><jtitle>ACS catalysis</jtitle><addtitle>ACS Catal</addtitle><date>2023-02-17</date><risdate>2023</risdate><volume>13</volume><issue>4</issue><spage>2462</spage><epage>2471</epage><pages>2462-2471</pages><issn>2155-5435</issn><eissn>2155-5435</eissn><abstract>The synergistic regulation of the electronic structures of transition-metal oxide-based catalysts via oxygen vacancy defects and single-atom doping is efficient to boost their oxygen evolution reaction (OER) performance, which remains challenging due to complex synthetic procedures. Herein, a facile defect-induced in situ single-atom deposition strategy is developed to anchor atomically dispersed Ru single-atom onto oxygen vacancy-rich cobalt oxides (Ru/Co3O4–x ) based on the spontaneous redox reaction between Ru3+ ions and nonstoichiometric Co3O4–x . Accordingly, the as-prepared Ru/Co3O4–x electrocatalyst with the coexistence of oxygen vacancies and Ru atoms exhibits excellent performances toward OER with a low overpotential of 280 mV at 10 mA cm–2, a small Tafel slope value of 86.9 mV dec–1, and good long-term stability in alkaline media. Furthermore, density functional theory calculations uncover that oxygen vacancy and atomically dispersed Ru could synergistically tailor electron decentralization and d-band center of Co atoms, further optimizing the adsorption of oxygen-based intermediates (*OH, *O, and *OOH) and reducing the reaction barriers of OER. This work proposes an available strategy for constructing electrocatalysts with abundant oxygen vacancies and atomically dispersed noble metal and presents a deep understanding of synergistic electronic engineering of transition-metal-based catalysts to boost oxygen evolution.</abstract><pub>American Chemical Society</pub><doi>10.1021/acscatal.2c04946</doi><tpages>10</tpages><orcidid>https://orcid.org/0000-0002-9008-2323</orcidid><orcidid>https://orcid.org/0000-0002-3008-8571</orcidid><orcidid>https://orcid.org/0000-0001-7089-7587</orcidid><orcidid>https://orcid.org/0000-0002-4767-8957</orcidid><orcidid>https://orcid.org/0000-0002-0056-7782</orcidid></addata></record> |
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title | In Situ Immobilizing Atomically Dispersed Ru on Oxygen-Defective Co3O4 for Efficient Oxygen Evolution |
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