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通过调节 Bi/BiOBr 的电子结构增强可见光驱动的双酚 A 的光催化降解。

Enhanced visible-light driven photocatalytic degradation of bisphenol A by tuning electronic structure of Bi/BiOBr.

机构信息

School of Civil and Transportation Engineering, Guangdong University of Technology, Guangzhou 510006, China.

School of Environmental and Civil Engineering, Jiangnan University, Wuxi, 214122, China.

出版信息

Chemosphere. 2022 Dec;308(Pt 2):136276. doi: 10.1016/j.chemosphere.2022.136276. Epub 2022 Sep 1.

Abstract

Visible-light (VL) photocatalysis has been regarded as an intriguing technology for the control of persistent environmental pollutants. In this study, the novel homogeneous Co doped-Bi/BiOBr nanocomposites (CB-X) were prepared via a facile one-step hydrothermal method, featured with a uniform 0D Bi nanodots distribution on 2D Co-doped BiOBr nanosheets, and the photocatalytic performance was evaluated by decomposing the BPA as a prototype contaminant. The degradation experiment indicated that the optimal CB-2 nanocomposite exhibited the best photocatalytic activity with a 94% removal efficiency of BPA under the VL irradiation of 30 min; And the corresponding apparent rate constant (k) was as high as 0.107 min, which was 10.7 times greater than that of Bi/BiOBr (0.010 min). Benefiting from the modulation effect of Co-doping on the intrinsic electron configuration of Bi/BiOBr, the elevated VL adsorption capacity and accelerated h/e pairs separation rate were achieved, which were evidenced by photoluminescence (PL) spectroscopy, photo-electrochemical measurements and density functional theory (DFT) calculation. Moreover, the major reactive species in CB-X/VL system were uncovered to be O and O, whereas OH and h presented a secondary contribution in the BPA elimination. Finally, the possible photocatalytic mechanism involved in CB-X nanocomposites and BPA degradation pathways were proposed on the basis of the various intermediates and products detected by LC-MS/MS.

摘要

可见光(VL)光催化被认为是控制持久性环境污染物的一种有趣技术。在这项研究中,通过简便的一步水热法制备了新型均相 Co 掺杂-Bi/BiOBr 纳米复合材料(CB-X),其特征是在 2D Co 掺杂 BiOBr 纳米片上均匀分布 0D Bi 纳米点,并用分解 BPA 作为原型污染物来评估光催化性能。降解实验表明,最佳的 CB-2 纳米复合材料在 VL 照射 30 分钟下表现出最好的光催化活性,BPA 的去除效率达到 94%;相应的表观速率常数(k)高达 0.107 min,是 Bi/BiOBr 的 10.7 倍(0.010 min)。受益于 Co 掺杂对 Bi/BiOBr 本征电子结构的调制作用,实现了 VL 吸附能力的提高和 h/e 对分离速率的加速,这一点通过光致发光(PL)光谱、光电化学测量和密度泛函理论(DFT)计算得到了证明。此外,在 CB-X/VL 体系中发现主要的活性物质是 O 和 O,而 OH 和 h 在 BPA 消除中起次要作用。最后,根据 LC-MS/MS 检测到的各种中间产物和产物,提出了 CB-X 纳米复合材料和 BPA 降解途径的可能光催化机制。

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