Engineering Pt-Mn2O3 interface to boost selective oxidation of ethylene glycol to glycolic acid
We successfully realized the directional construction of Pt-Mn2O3 interfacial sites (by the combination of in-situ doping and impregnation methods) to boost selective oxidation of ethylene glycol under mild conditions. It is found that the pre-distribution of Mn2O3 inside support unexpectedly induce...
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| Veröffentlicht in: | Applied catalysis. B, Environmental Environmental, 2021-05, Vol.284, p.119803, Article 119803 |
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| creator | Yan, Hao Yao, Shuang Wang, Jinyao Zhao, Siming Sun, Yinghao Liu, Mengyuan Zhou, Xin Zhang, Guangyu Jin, Xin Feng, Xiang Liu, Yibin Chen, Xiaobo Chen, De Yang, Chaohe |
| description | We successfully realized the directional construction of Pt-Mn2O3 interfacial sites (by the combination of in-situ doping and impregnation methods) to boost selective oxidation of ethylene glycol under mild conditions. It is found that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented glycolic acid oxidation activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %).
[Display omitted]
•Enhanced catalytic performance of ethylene glycol oxidation was achieved.•Strong electron coupling effect was revealed in the Pt-Mn interface.•Quantitative analysis of the intrinsic active sites was performed.•The promotion role of Pt-Mn interfacial on reaction mechanism was correlated.
Rational design of desirable active sites is still a grand challenge for the efficient conversion of polyols to value-added products. Herein, we successfully constructed the Pt-Mn2O3 interfacial sites rather than Pt-MnOx solid solution to boost selective oxidation of ethylene glycol to glycolic acid under mild conditions. X-ray absorption spectroscopy and high-resolution transmission electron microscope revealed that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented catalytic activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %). In addition, quantitative analysis of the intrinsic active sites was performed, and a “volcano-shape” relationship was established between initial reaction rate and Pt/Mn ratio. Moreover, the structure-dependent reaction kinetics and density functional theory calculation revealed that the synergistic effect between the Mn2O3 redox cycle and Pt promotes the adsorption of ethylene glycol and the activation of CH bond, resulting in the lower activation energy of ethylene glycol oxidation. The outcome of this work offers a promising avenue for the direct construction of efficient Pt-based catalysts with desired active sites. |
| doi_str_mv | 10.1016/j.apcatb.2020.119803 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_journals_2622661188</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><els_id>S0926337320312200</els_id><sourcerecordid>2622661188</sourcerecordid><originalsourceid>FETCH-LOGICAL-c334t-94a5ec5f6bf9b091f76f4e3e0d641c8cf1391b63b7cc93ed604e71e7d058f9b83</originalsourceid><addsrcrecordid>eNp9kEtPwzAQhC0EEqXwDzhY4pziR-o4FyRUlYdUVA5wthxnXRwFu9guov-eROHMaVermVnNh9A1JQtKqLjtFnpvdG4WjLDhRGtJ-AmaUVnxgkvJT9GM1EwUnFf8HF2k1BFCGGdyhtTa75wHiM7v8GsuXjzbcux8hmi1AZwDbkJIGSfowWT3DTj8uFZnFzwOFkP-OPbgAe_6own9qJ82Z7A2rr1EZ1b3Ca7-5hy9P6zfVk_FZvv4vLrfFIbzMhd1qZdgllY0tm5ITW0lbAkcSCtKaqSxlNe0EbypjKk5tIKUUFGoWrKUg0PyObqZcvcxfB0gZdWFQ_TDS8UEY0JQKkdVOalMDClFsGof3aeOR0WJGlGqTk0o1YhSTSgH291kg6HBt4OoknHgDbQuDlBUG9z_Ab9KHH7T</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2622661188</pqid></control><display><type>article</type><title>Engineering Pt-Mn2O3 interface to boost selective oxidation of ethylene glycol to glycolic acid</title><source>Elsevier ScienceDirect Journals</source><creator>Yan, Hao ; Yao, Shuang ; Wang, Jinyao ; Zhao, Siming ; Sun, Yinghao ; Liu, Mengyuan ; Zhou, Xin ; Zhang, Guangyu ; Jin, Xin ; Feng, Xiang ; Liu, Yibin ; Chen, Xiaobo ; Chen, De ; Yang, Chaohe</creator><creatorcontrib>Yan, Hao ; Yao, Shuang ; Wang, Jinyao ; Zhao, Siming ; Sun, Yinghao ; Liu, Mengyuan ; Zhou, Xin ; Zhang, Guangyu ; Jin, Xin ; Feng, Xiang ; Liu, Yibin ; Chen, Xiaobo ; Chen, De ; Yang, Chaohe</creatorcontrib><description>We successfully realized the directional construction of Pt-Mn2O3 interfacial sites (by the combination of in-situ doping and impregnation methods) to boost selective oxidation of ethylene glycol under mild conditions. It is found that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented glycolic acid oxidation activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %).
[Display omitted]
•Enhanced catalytic performance of ethylene glycol oxidation was achieved.•Strong electron coupling effect was revealed in the Pt-Mn interface.•Quantitative analysis of the intrinsic active sites was performed.•The promotion role of Pt-Mn interfacial on reaction mechanism was correlated.
Rational design of desirable active sites is still a grand challenge for the efficient conversion of polyols to value-added products. Herein, we successfully constructed the Pt-Mn2O3 interfacial sites rather than Pt-MnOx solid solution to boost selective oxidation of ethylene glycol to glycolic acid under mild conditions. X-ray absorption spectroscopy and high-resolution transmission electron microscope revealed that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented catalytic activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %). In addition, quantitative analysis of the intrinsic active sites was performed, and a “volcano-shape” relationship was established between initial reaction rate and Pt/Mn ratio. Moreover, the structure-dependent reaction kinetics and density functional theory calculation revealed that the synergistic effect between the Mn2O3 redox cycle and Pt promotes the adsorption of ethylene glycol and the activation of CH bond, resulting in the lower activation energy of ethylene glycol oxidation. The outcome of this work offers a promising avenue for the direct construction of efficient Pt-based catalysts with desired active sites.</description><identifier>ISSN: 0926-3373</identifier><identifier>EISSN: 1873-3883</identifier><identifier>DOI: 10.1016/j.apcatb.2020.119803</identifier><language>eng</language><publisher>Amsterdam: Elsevier B.V</publisher><subject>Absorption spectroscopy ; Catalysts ; Catalytic activity ; Density functional theory ; DFT calculations ; Ethylene ; Ethylene glycol ; Glycolic acid ; Hydrogen bonds ; Interfacial active site ; Manganese oxides ; Oxidation ; Oxidation of ethylene glycol ; Polyols ; Reaction kinetics ; Solid solutions ; Synergistic effect ; Volcanoes ; X ray absorption ; X-ray absorption spectroscopy</subject><ispartof>Applied catalysis. B, Environmental, 2021-05, Vol.284, p.119803, Article 119803</ispartof><rights>2020 Elsevier B.V.</rights><rights>Copyright Elsevier BV May 5, 2021</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c334t-94a5ec5f6bf9b091f76f4e3e0d641c8cf1391b63b7cc93ed604e71e7d058f9b83</citedby><cites>FETCH-LOGICAL-c334t-94a5ec5f6bf9b091f76f4e3e0d641c8cf1391b63b7cc93ed604e71e7d058f9b83</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0926337320312200$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3537,27901,27902,65306</link.rule.ids></links><search><creatorcontrib>Yan, Hao</creatorcontrib><creatorcontrib>Yao, Shuang</creatorcontrib><creatorcontrib>Wang, Jinyao</creatorcontrib><creatorcontrib>Zhao, Siming</creatorcontrib><creatorcontrib>Sun, Yinghao</creatorcontrib><creatorcontrib>Liu, Mengyuan</creatorcontrib><creatorcontrib>Zhou, Xin</creatorcontrib><creatorcontrib>Zhang, Guangyu</creatorcontrib><creatorcontrib>Jin, Xin</creatorcontrib><creatorcontrib>Feng, Xiang</creatorcontrib><creatorcontrib>Liu, Yibin</creatorcontrib><creatorcontrib>Chen, Xiaobo</creatorcontrib><creatorcontrib>Chen, De</creatorcontrib><creatorcontrib>Yang, Chaohe</creatorcontrib><title>Engineering Pt-Mn2O3 interface to boost selective oxidation of ethylene glycol to glycolic acid</title><title>Applied catalysis. B, Environmental</title><description>We successfully realized the directional construction of Pt-Mn2O3 interfacial sites (by the combination of in-situ doping and impregnation methods) to boost selective oxidation of ethylene glycol under mild conditions. It is found that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented glycolic acid oxidation activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %).
[Display omitted]
•Enhanced catalytic performance of ethylene glycol oxidation was achieved.•Strong electron coupling effect was revealed in the Pt-Mn interface.•Quantitative analysis of the intrinsic active sites was performed.•The promotion role of Pt-Mn interfacial on reaction mechanism was correlated.
Rational design of desirable active sites is still a grand challenge for the efficient conversion of polyols to value-added products. Herein, we successfully constructed the Pt-Mn2O3 interfacial sites rather than Pt-MnOx solid solution to boost selective oxidation of ethylene glycol to glycolic acid under mild conditions. X-ray absorption spectroscopy and high-resolution transmission electron microscope revealed that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented catalytic activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %). In addition, quantitative analysis of the intrinsic active sites was performed, and a “volcano-shape” relationship was established between initial reaction rate and Pt/Mn ratio. Moreover, the structure-dependent reaction kinetics and density functional theory calculation revealed that the synergistic effect between the Mn2O3 redox cycle and Pt promotes the adsorption of ethylene glycol and the activation of CH bond, resulting in the lower activation energy of ethylene glycol oxidation. The outcome of this work offers a promising avenue for the direct construction of efficient Pt-based catalysts with desired active sites.</description><subject>Absorption spectroscopy</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Density functional theory</subject><subject>DFT calculations</subject><subject>Ethylene</subject><subject>Ethylene glycol</subject><subject>Glycolic acid</subject><subject>Hydrogen bonds</subject><subject>Interfacial active site</subject><subject>Manganese oxides</subject><subject>Oxidation</subject><subject>Oxidation of ethylene glycol</subject><subject>Polyols</subject><subject>Reaction kinetics</subject><subject>Solid solutions</subject><subject>Synergistic effect</subject><subject>Volcanoes</subject><subject>X ray absorption</subject><subject>X-ray absorption spectroscopy</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp9kEtPwzAQhC0EEqXwDzhY4pziR-o4FyRUlYdUVA5wthxnXRwFu9guov-eROHMaVermVnNh9A1JQtKqLjtFnpvdG4WjLDhRGtJ-AmaUVnxgkvJT9GM1EwUnFf8HF2k1BFCGGdyhtTa75wHiM7v8GsuXjzbcux8hmi1AZwDbkJIGSfowWT3DTj8uFZnFzwOFkP-OPbgAe_6own9qJ82Z7A2rr1EZ1b3Ca7-5hy9P6zfVk_FZvv4vLrfFIbzMhd1qZdgllY0tm5ITW0lbAkcSCtKaqSxlNe0EbypjKk5tIKUUFGoWrKUg0PyObqZcvcxfB0gZdWFQ_TDS8UEY0JQKkdVOalMDClFsGof3aeOR0WJGlGqTk0o1YhSTSgH291kg6HBt4OoknHgDbQuDlBUG9z_Ab9KHH7T</recordid><startdate>20210505</startdate><enddate>20210505</enddate><creator>Yan, Hao</creator><creator>Yao, Shuang</creator><creator>Wang, Jinyao</creator><creator>Zhao, Siming</creator><creator>Sun, Yinghao</creator><creator>Liu, Mengyuan</creator><creator>Zhou, Xin</creator><creator>Zhang, Guangyu</creator><creator>Jin, Xin</creator><creator>Feng, Xiang</creator><creator>Liu, Yibin</creator><creator>Chen, Xiaobo</creator><creator>Chen, De</creator><creator>Yang, Chaohe</creator><general>Elsevier B.V</general><general>Elsevier BV</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7ST</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>JG9</scope><scope>KR7</scope><scope>L7M</scope><scope>SOI</scope></search><sort><creationdate>20210505</creationdate><title>Engineering Pt-Mn2O3 interface to boost selective oxidation of ethylene glycol to glycolic acid</title><author>Yan, Hao ; Yao, Shuang ; Wang, Jinyao ; Zhao, Siming ; Sun, Yinghao ; Liu, Mengyuan ; Zhou, Xin ; Zhang, Guangyu ; Jin, Xin ; Feng, Xiang ; Liu, Yibin ; Chen, Xiaobo ; Chen, De ; Yang, Chaohe</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c334t-94a5ec5f6bf9b091f76f4e3e0d641c8cf1391b63b7cc93ed604e71e7d058f9b83</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Absorption spectroscopy</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Density functional theory</topic><topic>DFT calculations</topic><topic>Ethylene</topic><topic>Ethylene glycol</topic><topic>Glycolic acid</topic><topic>Hydrogen bonds</topic><topic>Interfacial active site</topic><topic>Manganese oxides</topic><topic>Oxidation</topic><topic>Oxidation of ethylene glycol</topic><topic>Polyols</topic><topic>Reaction kinetics</topic><topic>Solid solutions</topic><topic>Synergistic effect</topic><topic>Volcanoes</topic><topic>X ray absorption</topic><topic>X-ray absorption spectroscopy</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Yan, Hao</creatorcontrib><creatorcontrib>Yao, Shuang</creatorcontrib><creatorcontrib>Wang, Jinyao</creatorcontrib><creatorcontrib>Zhao, Siming</creatorcontrib><creatorcontrib>Sun, Yinghao</creatorcontrib><creatorcontrib>Liu, Mengyuan</creatorcontrib><creatorcontrib>Zhou, Xin</creatorcontrib><creatorcontrib>Zhang, Guangyu</creatorcontrib><creatorcontrib>Jin, Xin</creatorcontrib><creatorcontrib>Feng, Xiang</creatorcontrib><creatorcontrib>Liu, Yibin</creatorcontrib><creatorcontrib>Chen, Xiaobo</creatorcontrib><creatorcontrib>Chen, De</creatorcontrib><creatorcontrib>Yang, Chaohe</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Environment Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Materials Research Database</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Environment Abstracts</collection><jtitle>Applied catalysis. B, Environmental</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Yan, Hao</au><au>Yao, Shuang</au><au>Wang, Jinyao</au><au>Zhao, Siming</au><au>Sun, Yinghao</au><au>Liu, Mengyuan</au><au>Zhou, Xin</au><au>Zhang, Guangyu</au><au>Jin, Xin</au><au>Feng, Xiang</au><au>Liu, Yibin</au><au>Chen, Xiaobo</au><au>Chen, De</au><au>Yang, Chaohe</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Engineering Pt-Mn2O3 interface to boost selective oxidation of ethylene glycol to glycolic acid</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2021-05-05</date><risdate>2021</risdate><volume>284</volume><spage>119803</spage><pages>119803-</pages><artnum>119803</artnum><issn>0926-3373</issn><eissn>1873-3883</eissn><abstract>We successfully realized the directional construction of Pt-Mn2O3 interfacial sites (by the combination of in-situ doping and impregnation methods) to boost selective oxidation of ethylene glycol under mild conditions. It is found that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented glycolic acid oxidation activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %).
[Display omitted]
•Enhanced catalytic performance of ethylene glycol oxidation was achieved.•Strong electron coupling effect was revealed in the Pt-Mn interface.•Quantitative analysis of the intrinsic active sites was performed.•The promotion role of Pt-Mn interfacial on reaction mechanism was correlated.
Rational design of desirable active sites is still a grand challenge for the efficient conversion of polyols to value-added products. Herein, we successfully constructed the Pt-Mn2O3 interfacial sites rather than Pt-MnOx solid solution to boost selective oxidation of ethylene glycol to glycolic acid under mild conditions. X-ray absorption spectroscopy and high-resolution transmission electron microscope revealed that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented catalytic activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %). In addition, quantitative analysis of the intrinsic active sites was performed, and a “volcano-shape” relationship was established between initial reaction rate and Pt/Mn ratio. Moreover, the structure-dependent reaction kinetics and density functional theory calculation revealed that the synergistic effect between the Mn2O3 redox cycle and Pt promotes the adsorption of ethylene glycol and the activation of CH bond, resulting in the lower activation energy of ethylene glycol oxidation. The outcome of this work offers a promising avenue for the direct construction of efficient Pt-based catalysts with desired active sites.</abstract><cop>Amsterdam</cop><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2020.119803</doi></addata></record> |
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| subjects | Absorption spectroscopy Catalysts Catalytic activity Density functional theory DFT calculations Ethylene Ethylene glycol Glycolic acid Hydrogen bonds Interfacial active site Manganese oxides Oxidation Oxidation of ethylene glycol Polyols Reaction kinetics Solid solutions Synergistic effect Volcanoes X ray absorption X-ray absorption spectroscopy |
| title | Engineering Pt-Mn2O3 interface to boost selective oxidation of ethylene glycol to glycolic acid |
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