Fanlin Kong, Xiaoyan Lu, Jing Xie, Zhenjiang Lu, Jindou Hu and Yali Cao
{"title":"通过控制氧空位生成和共建异质结 Pd/CeO2 策略增强光催化二氧化碳还原能力","authors":"Fanlin Kong, Xiaoyan Lu, Jing Xie, Zhenjiang Lu, Jindou Hu and Yali Cao","doi":"10.1039/D4QI00581C","DOIUrl":null,"url":null,"abstract":"<p >Artificial photoreduction of carbon dioxide (CO<small><sub>2</sub></small>) into useful chemicals using solar energy requires stable photocatalysts with efficient charge separation and effective CO<small><sub>2</sub></small> adsorption. Herein, the CeO<small><sub>2</sub></small>-supported Pd catalysts (Pd/CeO<small><sub>2</sub></small>-Vo(r)) with rich oxygen vacancies (Vo) are prepared using the thermal reduction method. The formation of heterojunctions between Pd nanoparticles and CeO<small><sub>2</sub></small> hollow spheres promotes the transfer of photogenerated electrons, and the Vo of CeO<small><sub>2</sub></small> exhibits an electron capture effect, thus this synergistic effect effectively enhances light absorption and facilitates the separation and transfer of photogenerated electrons. Therefore the Pd/CeO<small><sub>2</sub></small>-Vo(r) exhibits excellent photocatalytic CO<small><sub>2</sub></small> reduction to CO with a production rate of 210.9 μmol h<small><sup>−1</sup></small> g<small><sup>−1</sup></small>, which is more competitive than most of the reported photocatalysts. <em>In situ</em> FTIR is used to further reveal the photocatalytic mechanism of CO<small><sub>2</sub></small>, proving that the key intermediates COOH* and CO* are formed during the photoreduction process. This innovation provides a convenient method for designing photocatalysts with significant CO<small><sub>2</sub></small> capture capacity, which could provide novel insights into the photocatalytic reduction of CO<small><sub>2</sub></small>.</p>","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":" 10","pages":" 2932-2944"},"PeriodicalIF":6.4000,"publicationDate":"2024-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced photocatalytic CO2 reduction by controlled oxygen vacancy generation and co-constructed heterojunction strategy for Pd/CeO2†\",\"authors\":\"Fanlin Kong, Xiaoyan Lu, Jing Xie, Zhenjiang Lu, Jindou Hu and Yali Cao\",\"doi\":\"10.1039/D4QI00581C\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Artificial photoreduction of carbon dioxide (CO<small><sub>2</sub></small>) into useful chemicals using solar energy requires stable photocatalysts with efficient charge separation and effective CO<small><sub>2</sub></small> adsorption. Herein, the CeO<small><sub>2</sub></small>-supported Pd catalysts (Pd/CeO<small><sub>2</sub></small>-Vo(r)) with rich oxygen vacancies (Vo) are prepared using the thermal reduction method. The formation of heterojunctions between Pd nanoparticles and CeO<small><sub>2</sub></small> hollow spheres promotes the transfer of photogenerated electrons, and the Vo of CeO<small><sub>2</sub></small> exhibits an electron capture effect, thus this synergistic effect effectively enhances light absorption and facilitates the separation and transfer of photogenerated electrons. Therefore the Pd/CeO<small><sub>2</sub></small>-Vo(r) exhibits excellent photocatalytic CO<small><sub>2</sub></small> reduction to CO with a production rate of 210.9 μmol h<small><sup>−1</sup></small> g<small><sup>−1</sup></small>, which is more competitive than most of the reported photocatalysts. <em>In situ</em> FTIR is used to further reveal the photocatalytic mechanism of CO<small><sub>2</sub></small>, proving that the key intermediates COOH* and CO* are formed during the photoreduction process. 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引用次数: 0
摘要
利用太阳能将二氧化碳(CO2)人工光还原成有用的化学物质需要具有高效电荷分离和有效吸附 CO2 的稳定光催化剂。本文采用热还原法制备了富氧空位(Vo)的 CeO2 支持钯催化剂(Vo-R-Pd/CeO2)。Pd 纳米颗粒与 CeO2 中空球体之间形成的异质结促进了光生电子的转移,而 CeO2 中的 Vo 具有电子捕获效应,因此这种协同效应可有效增强光吸收,促进光生电子的分离和转移。因此,Vo-R-Pd/CeO2 具有优异的光催化 CO2 还原成 CO 的性能,生成率达到 210.9 μmol h-1 g-1,比大多数已报道的光催化剂更具竞争力。利用原位傅立叶变换红外光谱进一步揭示了 CO2 的光催化机理,证明在光还原过程中形成了关键的中间产物 COOH* 和 CO*。这一创新为设计具有显著二氧化碳捕获能力的光催化剂提供了一种便捷的方法,可为二氧化碳的光催化还原提供新的见解。
Enhanced photocatalytic CO2 reduction by controlled oxygen vacancy generation and co-constructed heterojunction strategy for Pd/CeO2†
Artificial photoreduction of carbon dioxide (CO2) into useful chemicals using solar energy requires stable photocatalysts with efficient charge separation and effective CO2 adsorption. Herein, the CeO2-supported Pd catalysts (Pd/CeO2-Vo(r)) with rich oxygen vacancies (Vo) are prepared using the thermal reduction method. The formation of heterojunctions between Pd nanoparticles and CeO2 hollow spheres promotes the transfer of photogenerated electrons, and the Vo of CeO2 exhibits an electron capture effect, thus this synergistic effect effectively enhances light absorption and facilitates the separation and transfer of photogenerated electrons. Therefore the Pd/CeO2-Vo(r) exhibits excellent photocatalytic CO2 reduction to CO with a production rate of 210.9 μmol h−1 g−1, which is more competitive than most of the reported photocatalysts. In situ FTIR is used to further reveal the photocatalytic mechanism of CO2, proving that the key intermediates COOH* and CO* are formed during the photoreduction process. This innovation provides a convenient method for designing photocatalysts with significant CO2 capture capacity, which could provide novel insights into the photocatalytic reduction of CO2.