Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-05-22 , DOI: 10.1016/j.apcatb.2020.119156 Shasha Guo , Jun Di , Chao Chen , Chao Zhu , Meilin Duan , Cheng Lian , Mengxia Ji , Weiqiang Zhou , Manzhang Xu , Pin Song , Ran Long , Xun Cao , Kaizhi Gu , Jiexiang Xia , Honglai Liu , Yanli Zhao , Li Song , Yujie Xiong , Shuzhou Li , Zheng Liu
Photocatalytic CO2 reduction suffers from the weakness of high energy barrier, low efficiency and poor selectivity. Exploring effective strategy to enhance the adsorption and activation behavior of CO2 molecules is an alternative approach to boost CO2 photoreduction performance. In this work, abundant oxygen vacancies (VO) are introduced onto Bi2Sn2O7 nanoparticles (NPs) by decreasing their size down to about 4 nm. The VO mediated NPs exhibit a tremendous 8.1 times enhanced performance than the bulk counterpart towards CO2-to−CO conversion in pure water. This is attributed to fast charge diffusion and abundant Vo for effective CO2 adsorption and activation in the ultra-small nanoparticles. The VO mediated Bi2Sn2O7 NPs have electron back donation nature and optimized electronic structure for effectively activating CO2, which were demonstrated by density functional theory calculations. During the reduction process, the Vo can effeciently stabilize the COOH* intermediates, and also lower the energy barrier of CO desorption determining step.
中文翻译:
氧空位介导的锡酸铋超小纳米粒子对光催化CO 2 -CO转化
光催化还原CO 2的缺点在于高能垒,低效率和选择性差。探索增强CO 2分子吸附和活化行为的有效策略是提高CO 2光还原性能的另一种方法。在这项工作中,通过将Bi 2 Sn 2 O 7纳米颗粒的尺寸减小到大约4 nm ,将大量的氧空位(V O)引入到Bi 2 Sn 2 O 7纳米颗粒(NPs)上。V O介导的NPs表现出比大量CO 2强大的8.1倍。在纯水中的二氧化碳转化为二氧化碳。这归因于电荷的快速扩散和丰富的Vo,可有效吸收超小纳米颗粒中的CO 2并活化。由V O介导的Bi 2 Sn 2 O 7 NPs具有电子返给性质和有效激活CO 2的优化电子结构,这通过密度泛函理论计算得到证明。在还原过程中,Vo可以有效稳定COOH *中间体,并降低CO解吸确定步骤的能垒。