Rongjun Sun, Zijian Zhu, Na Tian, Yihe Zhang, Hongwei Huang
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Notably, during photocatalytic reaction, Bi<sup>0</sup> and Ni<sup>0</sup> are in situ performed in heterojunction, which separately act as electron transport mediator and electron trap to further accelerate charge transfer efficiency up to 71.2 %. Theoretical calculations further demonstrate that the existence of Bi<sup>0</sup> strengthens the IEF. Therefore, high-speed spatial charge separation is realized in Bi<sup>0</sup>/BiOBr@Ni<sup>0</sup>/NiFe-LDH, leading to a prominent photocatalytic activity with a tetracycline removal ratio of 88.3 % within 7 min under visible-light irradiation and the presence of persulfate, far exceeding majority of photocatalysts reported previously. 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引用次数: 0
摘要
对于异质结体系,由于缺乏稳定的界面驱动力和明确的电荷转移通道,电荷分离和转移效率并不理想。发生在界面上的光反应机制也较少受到关注。本文合成了具有丰富界面氢键和强界面电场(IEF)的大面积接触的二维/二维 Z 型结 BiOBr@NiFe-LDH,并证明了原位光诱导金属物种辅助电荷转移机制。BiOBr 的 O 原子和 NiFe-LDH 的 H 原子之间的氢键诱导了显著的界面电荷再分布,从而建立了强大的 IEF。值得注意的是,在光催化反应过程中,Bi0 和 Ni0 从异质结中的 BiOBr 和 NiFe-LDH 中原位分离出来,分别作为电子传输介质和电子捕获器,进一步提高了电荷转移效率,最高可达 71.2%。理论计算进一步证明,Bi0 的存在增强了 IEF。因此,Bi0/BiOBr@Ni0/NiFe-LDH 实现了高速的空间电荷分离,从而具有突出的光催化活性,在可见光照射和过硫酸盐存在的条件下,7 分钟内四环素的去除率达到 88.3%,远远超过了之前报道的大多数光催化剂。这项研究为设计氢键异质结系统提供了有效的启示,并推进了对界面原位光反应机理的理解。
Hydrogen Bonds and In situ Photoinduced Metallic Bi0/Ni0 Accelerating Z-Scheme Charge Transfer of BiOBr@NiFe-LDH for Highly Efficient Photocatalysis.
For heterojunction system, the lack of stable interfacial driving force and definite charge transfer channel makes the charge separation and transfer efficiency unsatisfactory. The photoreaction mechanism occurring at the interface also receives less attention. Herein, a 2D/2D Z-scheme junction BiOBr@NiFe-LDH with large-area contact featured by short interface hydrogen bonds and strong interfacial electric field (IEF) is synthesized, and in situ photoinduced metallic species assisting charge transfer mechanism is demonstrated. The hydrogen bonds between O atoms from BiOBr and H atoms from NiFe-LDH induce a significant interfacial charge redistribution, establishing a robust IEF. Notably, during photocatalytic reaction, Bi0 and Ni0 are in situ performed in heterojunction, which separately act as electron transport mediator and electron trap to further accelerate charge transfer efficiency up to 71.2 %. Theoretical calculations further demonstrate that the existence of Bi0 strengthens the IEF. Therefore, high-speed spatial charge separation is realized in Bi0/BiOBr@Ni0/NiFe-LDH, leading to a prominent photocatalytic activity with a tetracycline removal ratio of 88.3 % within 7 min under visible-light irradiation and the presence of persulfate, far exceeding majority of photocatalysts reported previously. This study provides valid insights for designing hydrogen bonding heterojunction systems, and advances mechanistic understanding on in situ photoreaction at interfaces.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.