Yang You, Aijie Xu, Yao Lv, Lide Yang, Xuan Tang, Jie Tang, Yanglong Guo, Yao Cui, Wangcheng Zhan, Li Wang, Yun Guo, Sheng Dai
{"title":"构建三配位 Al (AlIII) 位点,促进 Pt/Al2O3 催化剂的丙烷完全氧化作用","authors":"Yang You, Aijie Xu, Yao Lv, Lide Yang, Xuan Tang, Jie Tang, Yanglong Guo, Yao Cui, Wangcheng Zhan, Li Wang, Yun Guo, Sheng Dai","doi":"10.1039/d4cy00582a","DOIUrl":null,"url":null,"abstract":"Complete oxidation of propane has drawn great attention in the fields of automotive emission control and volatile organic compound elimination. However, it is challenging to achieve high activity of this reaction due to the stability of propane. We here utilize a facile solvothermal method to construct tri-coordinated Al (Al<small><sub>III</sub></small>) sites on the as-synthesized ST-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> support to alter the properties of supported Pt species. It is demonstrated that Al<small><sub>III</sub></small> sites facilitate the dispersion and electron enrichment of supported Pt sites. Thus, Pt/ST-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> exhibits a superior activity toward complete propane oxidation, showing a 6.7-fold improvement in the turnover frequency over commercial Pt/Al<small><sub>2</sub></small>O<small><sub>3</sub></small> catalysts. Meanwhile, Pt/ST-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> possesses a distinct reaction route originating from its stronger C–H and C–C cleavage capability, while having excellent activity not only in complete propane oxidation but also in the complete oxidation of other alkanes (CH<small><sub>4</sub></small>, C<small><sub>2</sub></small>H<small><sub>6</sub></small>, and <em>n</em>-C<small><sub>4</sub></small>H<small><sub>10</sub></small>). In addition, the Al<small><sub>III</sub></small> construction strategy is successfully extended to more cases, <em>e.g.</em>, Pd/ST-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> with higher Pd dispersion and electron density. This work provides a promising strategy for the control of the oxide support for advanced design and synthesis of alkane oxidation catalysts.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":4.4000,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Constructing tri-coordinated Al (AlIII) sites to boost complete propane oxidation of the Pt/Al2O3 catalyst\",\"authors\":\"Yang You, Aijie Xu, Yao Lv, Lide Yang, Xuan Tang, Jie Tang, Yanglong Guo, Yao Cui, Wangcheng Zhan, Li Wang, Yun Guo, Sheng Dai\",\"doi\":\"10.1039/d4cy00582a\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Complete oxidation of propane has drawn great attention in the fields of automotive emission control and volatile organic compound elimination. However, it is challenging to achieve high activity of this reaction due to the stability of propane. We here utilize a facile solvothermal method to construct tri-coordinated Al (Al<small><sub>III</sub></small>) sites on the as-synthesized ST-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> support to alter the properties of supported Pt species. It is demonstrated that Al<small><sub>III</sub></small> sites facilitate the dispersion and electron enrichment of supported Pt sites. Thus, Pt/ST-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> exhibits a superior activity toward complete propane oxidation, showing a 6.7-fold improvement in the turnover frequency over commercial Pt/Al<small><sub>2</sub></small>O<small><sub>3</sub></small> catalysts. Meanwhile, Pt/ST-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> possesses a distinct reaction route originating from its stronger C–H and C–C cleavage capability, while having excellent activity not only in complete propane oxidation but also in the complete oxidation of other alkanes (CH<small><sub>4</sub></small>, C<small><sub>2</sub></small>H<small><sub>6</sub></small>, and <em>n</em>-C<small><sub>4</sub></small>H<small><sub>10</sub></small>). In addition, the Al<small><sub>III</sub></small> construction strategy is successfully extended to more cases, <em>e.g.</em>, Pd/ST-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> with higher Pd dispersion and electron density. 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Constructing tri-coordinated Al (AlIII) sites to boost complete propane oxidation of the Pt/Al2O3 catalyst
Complete oxidation of propane has drawn great attention in the fields of automotive emission control and volatile organic compound elimination. However, it is challenging to achieve high activity of this reaction due to the stability of propane. We here utilize a facile solvothermal method to construct tri-coordinated Al (AlIII) sites on the as-synthesized ST-Al2O3 support to alter the properties of supported Pt species. It is demonstrated that AlIII sites facilitate the dispersion and electron enrichment of supported Pt sites. Thus, Pt/ST-Al2O3 exhibits a superior activity toward complete propane oxidation, showing a 6.7-fold improvement in the turnover frequency over commercial Pt/Al2O3 catalysts. Meanwhile, Pt/ST-Al2O3 possesses a distinct reaction route originating from its stronger C–H and C–C cleavage capability, while having excellent activity not only in complete propane oxidation but also in the complete oxidation of other alkanes (CH4, C2H6, and n-C4H10). In addition, the AlIII construction strategy is successfully extended to more cases, e.g., Pd/ST-Al2O3 with higher Pd dispersion and electron density. This work provides a promising strategy for the control of the oxide support for advanced design and synthesis of alkane oxidation catalysts.
期刊介绍:
A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis.
Editor-in-chief: Bert Weckhuysen
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