Oxygen vacancy mediated bismuth stannate ultra-small nanoparticle towards photocatalytic CO2-to-CO conversion

Oxygen vacancy mediated bismuth stannate ultra-small nanoparticle towards photocatalytic CO2-to-CO conversion
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氧空位介导的锡酸铋超小纳米粒子用于光催化CO2-CO转化

DOI:
10.1016/j.apcatb.2020.119156
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发表时间:
2020-11
期刊:
Applied Catalysis B: Environmental
影响因子:
--
通讯作者:
Liu Zheng
Liu Zheng
中科院分区:
其他
文献类型:
--
作者:
Guo Shasha;Di Jun;Chen Chao;Zhu Chao;Duan Meilin;Lian Cheng;Ji Mengxia;Zhou Weiqiang;Xu Manzhang;Song Pin;Long Ran;Cao Xun;Gu Kaizhi;Xia Jiexiang;Liu Honglai;Zhao Yanli;Song Li;Xiong Yujie;Li Shuzhou;Liu Zheng

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光催化co2还原存在能量势垒高、效率低、选择性差的缺点。探索增强co2分子吸附和活化行为的有效策略是提高co2光还原性能的另一种途径。在这项工作中,通过将bi2sn2o7纳米粒子(NPs)的尺寸减小到约4 nm,引入了丰富的氧空位(VO)。在纯水中,vmediated NPs在CO2-to - CO转换方面的性能比散装NPs提高了8.1倍。这是由于超小纳米颗粒中的快速电荷扩散和丰富的Vo对co2的有效吸附和活化。通过密度泛函理论计算证实了vmediated Bi2Sn2O7NPs具有电子回给性质和优化的电子结构,能够有效活化CO2。在还原过程中,Vo可以有效地稳定COOH*中间体,同时降低CO脱附决定步骤的能垒。
Photocatalytic CO2reduction suffers from the weakness of high energy barrier, low efficiency and poor selectivity. Exploring effective strategy to enhance the adsorption and activation behavior of CO2molecules is an alternative approach to boost CO2photoreduction performance. In this work, abundant oxygen vacancies (VO) are introduced onto Bi2Sn2O7nanoparticles (NPs) by decreasing their size down to about 4 nm. The VOmediated 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 CO2adsorption and activation in the ultra-small nanoparticles. The VOmediated Bi2Sn2O7NPs 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.
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