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Grain-boundary surface terminations incorporating oxygen vacancies for selectively boosting CO2 photoreduction activity
Nano Energy ( IF 16.8 ) Pub Date : 2021-02-16 , DOI: 10.1016/j.nanoen.2021.105869
Xiaojie She , Xingwang Zhu , Jinman Yang , Yanhua Song , Yuanbin She , Daobin Liu , Jingjie Wu , Qing Yu , Huaming Li , Zheng Liu , Pulickel M. Ajayan , Hui Xu

Developing highly active and stable photocatalysts is a crucial endeavor to harvest valuable carbon-based fuels and feedstocks for photocatalytic CO2 conversion. The excellent photocatalysts must satisfy the thermodynamic condition for the redox reaction and possess the accelerated reaction kinetics. Here, we report a strategy using grain-boundary surface terminations and oxygen vacancies to synergistically and selectively boost photocatalytic CO2 reduction activity. Thereinto, grain boundaries as bulk defects create high-energy surfaces by stabilizing dislocations that are kinetically trapped for catalysis owing to the lattice strain of the photocatalyst. Oxygen vacancies are used to tailor the band structure and enhance the adsorption ability of reactants or intermediates. High-energy surface structures arisen from these bulk defects may be more resistant to the relaxation effect, resulting in excellent stability for photocatalytic CO2 reduction. In light of the anticipated increase for photocatalytic CO2 reduction activity, this work provides a strategy for broader exploitation of bulk defects in heterogeneous catalysis.



中文翻译:

结合氧空位的晶界表面终端,可选择性地提高CO 2的光还原活性

开发高活性和稳定的光催化剂是收获宝贵的碳基燃料和原料以进行光催化CO 2转化的关键性工作。优良的光催化剂必须满足氧化还原反应的热力学条件,并具有加速的反应动力学。在这里,我们报告了一种使用晶界表面终止和氧空位来协同和选择性增强光催化CO 2的策略减少活动。其中,作为晶界缺陷的晶界通过稳定由于光催化剂的晶格应变而被动力学俘获的位错来稳定高能表面。氧空位用于调整能带结构并增强反应物或中间体的吸附能力。由这些体积缺陷产生的高能表面结构可能对松弛效应更具抵抗力,从而为光催化还原CO 2带来出色的稳定性。鉴于光催化CO 2还原活性的预期增加,这项工作提供了一种在非均相催化中更广泛地利用本体缺陷的策略。

更新日期:2021-03-04
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