{"title":"在 Pd/C-TiO2/g-C3N4 光催化剂上将 CH4 高效光催化转化为 C1 烯酸盐","authors":"Jiale Shi, Ruixue Zhang, Ya-Ge Liu, Yibing Jia, Zhenyu Han, Hongna Zhang* and Hai-Ying Jiang*, ","doi":"10.1021/acs.energyfuels.4c0256010.1021/acs.energyfuels.4c02560","DOIUrl":null,"url":null,"abstract":"<p >In this work, a Pd<i><sub>x</sub></i>/C-TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub>-<i>y</i> photocatalyst was synthesized by combining g-C<sub>3</sub>N<sub>4</sub> with Ti<sub>3</sub>C<sub>2</sub> through heat treatment, followed by loading with noble metal Pd. Morphological characterization and XPS before and after reaction revealed the formation of a C-TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub> Z-scheme heterojunction system with Pd deposited on top. The optimal catalyst, Pd<sub>0.8</sub>/C-TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub>-5, exhibited significantly enhanced total C1 yields under mild conditions, achieving 6.1 and 2.6 times the yields of g-C<sub>3</sub>N<sub>4</sub> and C-TiO<sub>2</sub>, respectively. Notably, the HCHO yield was improved to 3854.79 μmol·g<sup>–1</sup>·h<sup>–1</sup>. Mechanistic studies indicated that the C-TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub> heterojunction significantly enhanced the CH<sub>4</sub> conversion performance by effectively suppressing photogenerated charge recombination. Additionally, the loaded Pd promoted CH<sub>4</sub> adsorption and activity, further improving the CH<sub>4</sub> conversion efficiency. Furthermore, Pd contributed to the high C1 yield by accelerating the generation of both and •OH radicals.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"38 17","pages":"16949–16956 16949–16956"},"PeriodicalIF":5.3000,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient Photocatalytic CH4 Conversion to C1 Oxygenates on Pd/C-TiO2/g-C3N4 Photocatalyst\",\"authors\":\"Jiale Shi, Ruixue Zhang, Ya-Ge Liu, Yibing Jia, Zhenyu Han, Hongna Zhang* and Hai-Ying Jiang*, \",\"doi\":\"10.1021/acs.energyfuels.4c0256010.1021/acs.energyfuels.4c02560\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >In this work, a Pd<i><sub>x</sub></i>/C-TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub>-<i>y</i> photocatalyst was synthesized by combining g-C<sub>3</sub>N<sub>4</sub> with Ti<sub>3</sub>C<sub>2</sub> through heat treatment, followed by loading with noble metal Pd. Morphological characterization and XPS before and after reaction revealed the formation of a C-TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub> Z-scheme heterojunction system with Pd deposited on top. The optimal catalyst, Pd<sub>0.8</sub>/C-TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub>-5, exhibited significantly enhanced total C1 yields under mild conditions, achieving 6.1 and 2.6 times the yields of g-C<sub>3</sub>N<sub>4</sub> and C-TiO<sub>2</sub>, respectively. Notably, the HCHO yield was improved to 3854.79 μmol·g<sup>–1</sup>·h<sup>–1</sup>. Mechanistic studies indicated that the C-TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub> heterojunction significantly enhanced the CH<sub>4</sub> conversion performance by effectively suppressing photogenerated charge recombination. Additionally, the loaded Pd promoted CH<sub>4</sub> adsorption and activity, further improving the CH<sub>4</sub> conversion efficiency. Furthermore, Pd contributed to the high C1 yield by accelerating the generation of both and •OH radicals.</p>\",\"PeriodicalId\":35,\"journal\":{\"name\":\"Energy & Fuels\",\"volume\":\"38 17\",\"pages\":\"16949–16956 16949–16956\"},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2024-08-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Energy & Fuels\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.energyfuels.4c02560\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Fuels","FirstCategoryId":"5","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.energyfuels.4c02560","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Efficient Photocatalytic CH4 Conversion to C1 Oxygenates on Pd/C-TiO2/g-C3N4 Photocatalyst
In this work, a Pdx/C-TiO2/g-C3N4-y photocatalyst was synthesized by combining g-C3N4 with Ti3C2 through heat treatment, followed by loading with noble metal Pd. Morphological characterization and XPS before and after reaction revealed the formation of a C-TiO2/g-C3N4 Z-scheme heterojunction system with Pd deposited on top. The optimal catalyst, Pd0.8/C-TiO2/g-C3N4-5, exhibited significantly enhanced total C1 yields under mild conditions, achieving 6.1 and 2.6 times the yields of g-C3N4 and C-TiO2, respectively. Notably, the HCHO yield was improved to 3854.79 μmol·g–1·h–1. Mechanistic studies indicated that the C-TiO2/g-C3N4 heterojunction significantly enhanced the CH4 conversion performance by effectively suppressing photogenerated charge recombination. Additionally, the loaded Pd promoted CH4 adsorption and activity, further improving the CH4 conversion efficiency. Furthermore, Pd contributed to the high C1 yield by accelerating the generation of both and •OH radicals.
期刊介绍:
Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.