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界面电荷主导主要活性物种和降解途径:以碳基光催化剂为例。

Interfacial charge dominating major active species and degradation pathways: An example of carbon based photocatalyst.

机构信息

School of Materials Science and Engineering, Key Laboratory of Advanced Ceramics and Machining Technology, Ministry of Education, Tianjin University, Tianjin 300350, PR China.

School of Materials Science and Engineering, Key Laboratory of Advanced Ceramics and Machining Technology, Ministry of Education, Tianjin University, Tianjin 300350, PR China.

出版信息

J Colloid Interface Sci. 2019 Oct 15;554:743-751. doi: 10.1016/j.jcis.2019.07.077. Epub 2019 Jul 27.

Abstract

In this work, the chlorine-doped and undoped hydrothermal carbonation carbon (Cl-HTCC, HTCC) photocatalysts were used to study the correlation of their interfacial charge and photocatalytic performance. For degradation of aromatic dye, rhodamine B (RhB), Cl-HTCC manifests much better photocatalytic performance compared with that of undoped HTCC. Besides the slightly enhanced charge transfer brought, the Cl-HTCC showed more negatively interfacial charge and thus a stronger adsorption of positively charged RhB. This made the photogenerated holes (h) directly react with the adsorbed RhB, which does not require the h to produce hydroxyl radical (OH) and reduce its lost during the transformation, thus enhanced the performance of Cl-HTCC. While for undoped HTCC, it showed a weaker adsorption of RhB, and the photogenerated h firstly reacted with HO molecules to produce OH. Then, the OH can attack the RhB. Besides, the intermediates and the degradation pathways are also evaluated here via UPLC-MS. Results show that the interfacial charge also dominated the degradation pathways. This work provides a novel metal-free photocatalyst for environmental remediation and will inspire further efforts to enhance the photocatalytic performance by concerning interfacial conditions.

摘要

在这项工作中,使用了氯掺杂和未掺杂水热碳化碳(Cl-HTCC,HTCC)光催化剂来研究它们的界面电荷和光催化性能之间的相关性。对于芳香族染料罗丹明 B(RhB)的降解,Cl-HTCC 的光催化性能明显优于未掺杂的 HTCC。除了略微增强的电荷转移外,Cl-HTCC 还表现出更负的界面电荷,因此对带正电荷的 RhB 具有更强的吸附能力。这使得光生空穴(h)可以直接与吸附的 RhB 反应,而不需要 h 产生羟基自由基(OH)并减少其在转化过程中的损失,从而提高了 Cl-HTCC 的性能。而对于未掺杂的 HTCC,它对 RhB 的吸附能力较弱,光生 h 首先与 HO 分子反应生成 OH。然后,OH 可以攻击 RhB。此外,还通过 UPLC-MS 评估了中间体和降解途径。结果表明,界面电荷也主导了降解途径。这项工作为环境修复提供了一种新型的无金属光催化剂,并将激发进一步的努力,通过关注界面条件来提高光催化性能。

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