Jiaojiao Fang, Chengyang Zhu, Lincan Fang, Yukai Chen, Huiling Hu, Yan Wu, Qingqing Chen, Junjie Mao
{"title":"耦合异质结的钯纳米粒子中的高效电荷转移转向可促进 CO2 光还原为 C2H6","authors":"Jiaojiao Fang, Chengyang Zhu, Lincan Fang, Yukai Chen, Huiling Hu, Yan Wu, Qingqing Chen, Junjie Mao","doi":"10.1007/s40843-024-2995-0","DOIUrl":null,"url":null,"abstract":"<p>Solar-driven CO<sub>2</sub> conversion to prepare value-added products is highly desirable but challenging. Central to the achievement of multi-carbon products <i>via</i> CO<sub>2</sub> photoconversion is to break the bottlenecks of C–C coupling and multi-electron transfer. Herein, a charge relay system consisting of Pd-decorated BiOCl-wrapped CuBi<sub>2</sub>O<sub>4</sub> is reported by taking advantage of the synergy of Pd nanoparticles (PdNPs) and heterojunction for efficient CO<sub>2</sub>-to-C<sub>2</sub>H<sub>6</sub> photoconversion. The C<sub>2</sub>H<sub>6</sub> production rate reached 167.1 µmol g<sup>−1</sup> h<sup>−1</sup> with the electron selectivity of 81.1% in the absence of any sacrificial agents. The spectroscopic characterizations indicated that BiOCl nanosheets, acting as the charge relay, directionally transferred the photogenerated electrons from itself and CuBi<sub>2</sub>O<sub>4</sub> nanorods to PdNPs for C–C coupling. The coordinated ensemble of PdNPs and heterojunction significantly elevated the charge separation and transfer efficiency. Moreover, the <i>in-situ</i> spectroscopic analysis supported by theoretical simulations demonstrated that the electron-rich PdNPs generated by the charge relay of PdNPs and heterojunction optimized the CO<sub>2</sub>-to-C<sub>2</sub>H<sub>6</sub> reaction pathway and reduced the energy barrier of the key *CHOCO intermediates. This work develops an innovative strategy to design the multifunctional catalysts for the photoconversion of CO<sub>2</sub> to value-added carbon products.\n</p>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":null,"pages":null},"PeriodicalIF":6.8000,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient charge relay steering in Pd nanoparticles coupled with the heterojunction for boosting CO2 photoreduction to C2H6\",\"authors\":\"Jiaojiao Fang, Chengyang Zhu, Lincan Fang, Yukai Chen, Huiling Hu, Yan Wu, Qingqing Chen, Junjie Mao\",\"doi\":\"10.1007/s40843-024-2995-0\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Solar-driven CO<sub>2</sub> conversion to prepare value-added products is highly desirable but challenging. Central to the achievement of multi-carbon products <i>via</i> CO<sub>2</sub> photoconversion is to break the bottlenecks of C–C coupling and multi-electron transfer. Herein, a charge relay system consisting of Pd-decorated BiOCl-wrapped CuBi<sub>2</sub>O<sub>4</sub> is reported by taking advantage of the synergy of Pd nanoparticles (PdNPs) and heterojunction for efficient CO<sub>2</sub>-to-C<sub>2</sub>H<sub>6</sub> photoconversion. The C<sub>2</sub>H<sub>6</sub> production rate reached 167.1 µmol g<sup>−1</sup> h<sup>−1</sup> with the electron selectivity of 81.1% in the absence of any sacrificial agents. The spectroscopic characterizations indicated that BiOCl nanosheets, acting as the charge relay, directionally transferred the photogenerated electrons from itself and CuBi<sub>2</sub>O<sub>4</sub> nanorods to PdNPs for C–C coupling. The coordinated ensemble of PdNPs and heterojunction significantly elevated the charge separation and transfer efficiency. Moreover, the <i>in-situ</i> spectroscopic analysis supported by theoretical simulations demonstrated that the electron-rich PdNPs generated by the charge relay of PdNPs and heterojunction optimized the CO<sub>2</sub>-to-C<sub>2</sub>H<sub>6</sub> reaction pathway and reduced the energy barrier of the key *CHOCO intermediates. This work develops an innovative strategy to design the multifunctional catalysts for the photoconversion of CO<sub>2</sub> to value-added carbon products.\\n</p>\",\"PeriodicalId\":773,\"journal\":{\"name\":\"Science China Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.8000,\"publicationDate\":\"2024-07-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science China Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1007/s40843-024-2995-0\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science China Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1007/s40843-024-2995-0","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Efficient charge relay steering in Pd nanoparticles coupled with the heterojunction for boosting CO2 photoreduction to C2H6
Solar-driven CO2 conversion to prepare value-added products is highly desirable but challenging. Central to the achievement of multi-carbon products via CO2 photoconversion is to break the bottlenecks of C–C coupling and multi-electron transfer. Herein, a charge relay system consisting of Pd-decorated BiOCl-wrapped CuBi2O4 is reported by taking advantage of the synergy of Pd nanoparticles (PdNPs) and heterojunction for efficient CO2-to-C2H6 photoconversion. The C2H6 production rate reached 167.1 µmol g−1 h−1 with the electron selectivity of 81.1% in the absence of any sacrificial agents. The spectroscopic characterizations indicated that BiOCl nanosheets, acting as the charge relay, directionally transferred the photogenerated electrons from itself and CuBi2O4 nanorods to PdNPs for C–C coupling. The coordinated ensemble of PdNPs and heterojunction significantly elevated the charge separation and transfer efficiency. Moreover, the in-situ spectroscopic analysis supported by theoretical simulations demonstrated that the electron-rich PdNPs generated by the charge relay of PdNPs and heterojunction optimized the CO2-to-C2H6 reaction pathway and reduced the energy barrier of the key *CHOCO intermediates. This work develops an innovative strategy to design the multifunctional catalysts for the photoconversion of CO2 to value-added carbon products.
期刊介绍:
Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.