Tang Jun-Ying, Liu Xiao-Jing, Guo Rui-Tang, Wang Juan, Wang Qing-Shan, Pan Wei-Guo
School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai, China.
College of Energy and Mechanical Engineering, Shanghai University of Electric Power, Shanghai, China.
Dalton Trans. 2024 Feb 27;53(9):4088-4097. doi: 10.1039/d3dt04191c.
Effectively harnessing solar energy for the conversion of CO into valuable chemical energy presents a viable solution to address energy scarcity and climate change concerns. Nonetheless, the limited light absorption and sluggish charge kinetics significantly hinder the photoreduction of CO. In this study, we employed a facile sol-gel method combined with wetness impregnation to synthesize Cu-doped TiO coated with NiO nanoparticles. Various characterizations verified the successful incorporation of Cu ions into the TiO crystal lattice and the formation of NiO co-catalysts within the composites. The optimal performance attained with CTN-0.5 demonstrates an output of 11.85 μmol h g for CO and 9.51 μmol h g for CH, which represent a 4.4-fold and 15.6-fold increase, respectively, compared to those achieved with pure TiO. The induced Cu defect band broadens the light absorption by decreasing the conduction band edge of TiO, while NiO upshifts the valence band of TiO because of the interaction of valence orbitals. Light irradiation EPR and FTIR tests suggest that the collaboration of CuO and NiO promotes the formation of oxygen vacancies/defects and a rapid charge transfer pathway, thereby provides numerous active sites and electrons to enhance CO photoreduction performance.
有效地利用太阳能将一氧化碳转化为有价值的化学能,为解决能源短缺和气候变化问题提供了一个可行的解决方案。然而,有限的光吸收和缓慢的电荷动力学严重阻碍了一氧化碳的光还原。在本研究中,我们采用简便的溶胶-凝胶法结合湿浸渍法合成了包覆有氧化镍纳米颗粒的铜掺杂二氧化钛。各种表征证实了铜离子成功掺入二氧化钛晶格以及复合材料中氧化镍助催化剂的形成。CTN-0.5所达到的最佳性能表明,一氧化碳的产量为11.85 μmol h g,甲烷的产量为9.51 μmol h g,与纯二氧化钛相比,分别提高了4.4倍和15.6倍。诱导产生的铜缺陷带通过降低二氧化钛的导带边缘来拓宽光吸收,而氧化镍由于价轨道的相互作用使二氧化钛的价带向上移动。光照射电子顺磁共振和傅里叶变换红外光谱测试表明,氧化铜和氧化镍的协同作用促进了氧空位/缺陷的形成和快速电荷转移途径,从而提供了大量活性位点和电子,以提高一氧化碳的光还原性能。