Applied Surface Science ( IF 6.3 ) Pub Date : 2021-06-11 , DOI: 10.1016/j.apsusc.2021.150042 Xin Li , Jingru Guan , Haopeng Jiang , Xianghai Song , Pengwei Huo , Huiqin Wang
Construction of multi-interface contact step-scheme (S-scheme) photocatalyst is a promising pathway to achieve high-electron transfer efficiency for photocatalytic CO2 reduction. In this paper, g-C3N4 nanosheets were selected as the main photocatalyst, rod-like CeO2 (R-CeO2) with unique Ce4+→Ce3+ conversion property and rGO were loaded on the g-C3N4 surface to construct 2D-1D-2D sandwich photocatalyst. The yields of CO and CH4 were about 63.18 and 32.67 μmol/g after 4 h when the rGO/R-CeO2/g-C3N4 was used as catalyst, which were about 4 and 6 times higher than that of pure CN, respectively. Cyclic experiments proved that the composite had excellent photocatalytic and material stability. Photoelectrochemical tests showed that the construction of S-scheme electron transfer model and the introduction of rGO can great enhance the electron transmission and separation of photogenerated electron-hole pairs. CO2 adsorption test identified that the loading of R-CeO2 and rGO obviously enhanced the CO2 adsorption ability of pure g-C3N4. Density functional theory (DFT) calculations used to analyze the electron transfer path and the formation of the build-in electric field at the semiconductor interface. In-situ FTIR and 13CO2 element-tracer detection carried out to research the process of CO2 photoreduction. A possible multi-interface contact S-scheme electron transfer mechanism for enhanced CO2 photoreduction activity has been discussed.
中文翻译:
rGO 修饰的 R-CeO 2 /gC 3 N 4多界面接触 S 型光催化剂用于高效 CO 2光还原
多界面接触阶梯式(S-scheme)光催化剂的构建是实现光催化CO 2还原高电子转移效率的有希望的途径。在本文中,选择gC 3 N 4纳米片作为主要的光催化剂,将具有独特Ce 4+ →Ce 3+转化性能的棒状CeO 2 (R-CeO 2 )和rGO负载在gC 3 N 4表面上以构建2D-1D-2D夹心光催化剂。当rGO/R-CeO 2 /gC 3 N 4 4 h后CO和CH 4的产率分别为63.18和32.67 μmol/g用作催化剂,分别比纯 CN 高约 4 倍和 6 倍。循环实验证明该复合材料具有优异的光催化和材料稳定性。光电化学测试表明,S-scheme电子转移模型的构建和rGO的引入可以极大地增强光生电子-空穴对的电子传输和分离。CO 2吸附试验表明,R-CeO 2和rGO的负载明显增强了纯gC 3 N 4对CO 2 的吸附能力。密度泛函理论 (DFT) 计算用于分析电子转移路径和半导体界面内建电场的形成。进行原位FTIR 和13 CO 2元素示踪剂检测以研究 CO 2 光还原过程。已经讨论了用于增强 CO 2 光还原活性的可能的多界面接触 S 型电子转移机制。