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磷掺杂氮化碳/磷硫共掺杂氮化碳同质异质结的构建及其增强的光活性。

Construction of phosphorus-doped carbon nitride/phosphorus and sulfur co-doped carbon nitride isotype heterojunction and their enhanced photoactivity.

作者信息

Li Jiaqi, Qi Yi, Mei Yuqing, Ma Shouchun, Li Qi, Xin Baifu, Yao Tongjie, Wu Jie

机构信息

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin, China.

School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, China.

出版信息

J Colloid Interface Sci. 2020 Apr 15;566:495-504. doi: 10.1016/j.jcis.2020.01.102. Epub 2020 Jan 28.

DOI:10.1016/j.jcis.2020.01.102
PMID:32058102
Abstract

Photocatalysis was one of the most promising techniques for environmental remediation. Exploring photocatalysts with high efficiency, low cost and easy preparation was still an ongoing issue. In this work, phosphorus-doped carbon nitride/phosphorus and sulfur co-doped carbon nitride (P-CN/PS-CN) isotype heterojunction was prepared by a two-step calcination method. The composite displayed a sheet-like structure with a surface area of 23 m/g. Compared with pure CN, band gaps of P-CN and PS-CN were only slightly modified during the heteroatom-doping process. Therefore, a well-matched band alignment was constructed, which not only improved the separation efficiency of photogenerated electron-hole pairs, but also well preserved the high oxidizability of holes on valance band and good reducibility of electrons on conduction band. Because of the similarity in physicochemical properties, the interface resistance between P-CN and PS-CN was low, which accelerated the electron transfer and prolonged the lifetime of charge carriers. Although the visible-light utilization was somewhat low in comparison with P-CN and PS-CN, by taking advantage of above merits, P-CN/PS-CN displayed the high photocatalytic activity in rhodamine B degradation, and the reaction rate constant was 0.183 min, about 8.7 and 4.0 times higher than those of P-CN and PS-CN. Besides high catalytic activity, isotype heterojunction displayed good recyclability, since 95.3% of catalytic activity was maintained after the 5 cycle. The method presented here was facile, economic and environmentally benign, thus it was highly attractive for the application in environmental remediation.

摘要

光催化是环境修复领域最具前景的技术之一。探索高效、低成本且易于制备的光催化剂仍是一个持续研究的课题。在本工作中,采用两步煅烧法制备了磷掺杂氮化碳/磷硫共掺杂氮化碳(P-CN/PS-CN)同型异质结。该复合材料呈现出片状结构,比表面积为23 m²/g。与纯氮化碳相比,在杂原子掺杂过程中,P-CN和PS-CN的带隙仅略有改变。因此,构建了匹配良好的能带排列,这不仅提高了光生电子-空穴对的分离效率,还很好地保留了价带上空穴的高氧化性和导带上电子的良好还原性。由于物理化学性质相似,P-CN和PS-CN之间的界面电阻较低,这加速了电子转移并延长了载流子的寿命。尽管与P-CN和PS-CN相比,其可见光利用率有所降低,但利用上述优点,P-CN/PS-CN在罗丹明B降解中表现出高光催化活性,反应速率常数为0.183 min⁻¹,分别约为P-CN和PS-CN的8.7倍和4.0倍。除了高催化活性外,同型异质结还表现出良好的可回收性,因为在5次循环后仍保持95.3%的催化活性。本文提出的方法简便、经济且环境友好,因此在环境修复应用中极具吸引力。

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