In Situ Formation of Interfacial Defects between Co-Based Spinel/Carbon Nitride Hybrids for Efficient CO2 Photoreduction
In Situ Formation of Interfacial Defects between Co-Based Spinel/Carbon Nitride Hybrids for Efficient CO2 Photoreduction
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DOI：
10.1021/acsaem.0c00881
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发表时间：
2020-05
期刊：
影响因子：
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通讯作者：
Hangfan Ma;Xinyong Li;Shiying Fan;Zhifan Yin;G. Gan;Meichun Qin;Penglei Wang;Yaxuan Li;
中科院分区：
文献类型：
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作者：
Hangfan Ma;Xinyong Li;Shiying Fan;Zhifan Yin;G. Gan;Meichun Qin;Penglei Wang;Yaxuan Li;
构建高效的光催化剂用于CO转化和合成有价值的化学燃料已成为能源危机和温室气体控制的最有前途的策略和挑战之一。在这项研究中，一个界面缺陷的钴基尖晶石/氮化碳直接Z-计划异质结（CoO/CNS）的电荷转移效率高，成功地构建了g-CN纳米片和空心球CoO之间的原位静电组装。与纯g-CN纳米片相比，所构建的异质结CoO/CNS-10%显示出非常先进的光催化性能，CO生成速率（13.31 μmol·g·h）和CH生成速率（3.17 μmol·g·h）分别为纯g-CN纳米片的11.5倍和6.4倍。此外，实验观察和密度泛函理论计算都表明，界面上可以自发形成氧空位，氧空位不仅作为界面电荷复合中心驱动界面电荷的定向转移，而且在一定程度上促进了CO分子的吸附和活化.这项工作不仅提供了深刻的见解异质结结构的高度光催化性能的提升，但也强调了界面缺陷工程的重要性，有效地控制界面电荷转移。
Constructing efficient photocatalysts for CO conversion and synthesis of valuable chemical fuels has been one of the most promising strategies and challenge for both energy crisis and greenhouse gas control. In this study, an interfacial defect in the Co-based spinel/carbon nitride direct Z-scheme heterojunction (CoO/CNS) with ultrahigh charge transfer efficiency was successfully constructed by in situ electrostatic assembly between g-CN nanosheets and a hollow spherical CoO. Compared to pure g-CN nanosheets, the constructed heterojunction CoO/CNS-10% shows a highly advanced photocatalytic capability with approximately 11.5 and 6.4 times in the CO evolution rate (13.31 μmol·g·h) and CH generation rate (3.17 μmol·g·h), respectively. Additionally, both experimental observations and density functional theory calculations reveal that the oxygen vacancies could form spontaneously in the interface, which play a great role in not only driving oriented interface charge transfer through acting as interface charge recombination centers but also improving CO molecule adsorption and activation in a sense. This work would not only provides deep insights into the heterojunction construction for highly photocatalytic performance promotion but also emphasizes the importance of interfacial defect engineering in effectively controllable interface charge transfer.