Khadija Talbi , Francesc Penas-Hidalgo , Amanda L. Robinson , Philipp Gotico , Winfried Leibl , Pierre Mialane , Maria Gomez-Mingot , Marc Fontecave , Albert Solé-Daura , Caroline Mellot-Draznieks , Anne Dolbecq
{"title":"镍取代的多氧金属卤化物光催化二氧化碳还原：结构-活性关系和机理启示","authors":"Khadija Talbi , Francesc Penas-Hidalgo , Amanda L. Robinson , Philipp Gotico , Winfried Leibl , Pierre Mialane , Maria Gomez-Mingot , Marc Fontecave , Albert Solé-Daura , Caroline Mellot-Draznieks , Anne Dolbecq","doi":"10.1016/j.apcatb.2023.123681","DOIUrl":null,"url":null,"abstract":"<div><p>The photocatalytic activity for CO<sub>2</sub> reduction of a series of Ni-substituted polyoxometalates (POMs) differing in nuclearity, shape and size, has been investigated under visible light irradiation, with [Ru(bpy)<sub>3</sub>]<sup>2+</sup><span> (bpy = 2,2′-bipyridine) as photosensitizer and triethanolamine as sacrificial donor. The tetrabutylammonium salt of the </span><strong>Ni</strong><sub><strong>4</strong></sub> tetranuclear species was found to exhibit the highest CO production and its stability under photocatalytic conditions was demonstrated. The catalytic performance was significantly lower for the alkaline salt due to the separation of the POM from its counter-ions occurring only for the tetrabutylammonium salt. Photophysical experiments evidenced a bimolecular electron transfer from the reduced photosensitizer [Ru(bpy)<sub>3</sub>]<sup>+</sup> to the <strong>Ni</strong><sub><strong>4</strong></sub> POM, the former arising from the reductive quenching of the [Ru(bpy)<sub>3</sub>]<sup>2+</sup> excited state by triethanolamine. This was further supported by DFT calculations, which also showed that the <strong>Ni</strong><sub><strong>4</strong></sub> POM accumulates at least two electrons and four protons to carry out the CO<sub>2</sub> reduction catalytic process.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"345 ","pages":"Article 123681"},"PeriodicalIF":20.2000,"publicationDate":"2024-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Photocatalytic CO2 reduction by Ni-substituted polyoxometalates: Structure-activity relationships and mechanistic insights\",\"authors\":\"Khadija Talbi , Francesc Penas-Hidalgo , Amanda L. Robinson , Philipp Gotico , Winfried Leibl , Pierre Mialane , Maria Gomez-Mingot , Marc Fontecave , Albert Solé-Daura , Caroline Mellot-Draznieks , Anne Dolbecq\",\"doi\":\"10.1016/j.apcatb.2023.123681\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The photocatalytic activity for CO<sub>2</sub> reduction of a series of Ni-substituted polyoxometalates (POMs) differing in nuclearity, shape and size, has been investigated under visible light irradiation, with [Ru(bpy)<sub>3</sub>]<sup>2+</sup><span> (bpy = 2,2′-bipyridine) as photosensitizer and triethanolamine as sacrificial donor. The tetrabutylammonium salt of the </span><strong>Ni</strong><sub><strong>4</strong></sub> tetranuclear species was found to exhibit the highest CO production and its stability under photocatalytic conditions was demonstrated. The catalytic performance was significantly lower for the alkaline salt due to the separation of the POM from its counter-ions occurring only for the tetrabutylammonium salt. Photophysical experiments evidenced a bimolecular electron transfer from the reduced photosensitizer [Ru(bpy)<sub>3</sub>]<sup>+</sup> to the <strong>Ni</strong><sub><strong>4</strong></sub> POM, the former arising from the reductive quenching of the [Ru(bpy)<sub>3</sub>]<sup>2+</sup> excited state by triethanolamine. This was further supported by DFT calculations, which also showed that the <strong>Ni</strong><sub><strong>4</strong></sub> POM accumulates at least two electrons and four protons to carry out the CO<sub>2</sub> reduction catalytic process.</p></div>\",\"PeriodicalId\":244,\"journal\":{\"name\":\"Applied Catalysis B: Environmental\",\"volume\":\"345 \",\"pages\":\"Article 123681\"},\"PeriodicalIF\":20.2000,\"publicationDate\":\"2024-01-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis B: Environmental\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926337323013243\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis B: Environmental","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926337323013243","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Photocatalytic CO2 reduction by Ni-substituted polyoxometalates: Structure-activity relationships and mechanistic insights
The photocatalytic activity for CO2 reduction of a series of Ni-substituted polyoxometalates (POMs) differing in nuclearity, shape and size, has been investigated under visible light irradiation, with [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) as photosensitizer and triethanolamine as sacrificial donor. The tetrabutylammonium salt of the Ni4 tetranuclear species was found to exhibit the highest CO production and its stability under photocatalytic conditions was demonstrated. The catalytic performance was significantly lower for the alkaline salt due to the separation of the POM from its counter-ions occurring only for the tetrabutylammonium salt. Photophysical experiments evidenced a bimolecular electron transfer from the reduced photosensitizer [Ru(bpy)3]+ to the Ni4 POM, the former arising from the reductive quenching of the [Ru(bpy)3]2+ excited state by triethanolamine. This was further supported by DFT calculations, which also showed that the Ni4 POM accumulates at least two electrons and four protons to carry out the CO2 reduction catalytic process.
期刊介绍：
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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