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缺陷在制备具有增强光催化析氢性能的聚合氮化碳同质结中的关键作用。

The pivotal role of defects in fabrication of polymeric carbon nitride homojunctions with enhanced photocatalytic hydrogen evolution.

作者信息

Deng Quanhua, Li Haiping, Ba Guiming, Huo Tingting, Hou Wanguo

机构信息

School of Chemistry and Chemical Engineering, Shandong University, Jinan, Shandong 250100, China.

National Engineering Research Center for Colloidal Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan, Shandong 250100, China.

出版信息

J Colloid Interface Sci. 2021 Mar 15;586:748-757. doi: 10.1016/j.jcis.2020.10.144. Epub 2020 Nov 13.

Abstract

Fabrication of homojunctions is a cost-effective efficient way to enhance the photocatalytic performance of polymeric carbon nitride (CN), but the generation of defects upon synthesizing CN homojunctions and their roles in the homojunction fabrication were hardly reported. Herein, nitrogen-deficient CN homojunctions were simply synthesized by calcining dicyandiamide-loaded CN (prepared from urea and denoted as UCN) with dicyandiamide polymerizing into CN (denoted as DCN) and simultaneous formation of nitrogen vacancies in the surface of UCN. Fabrication of the nitrogen-deficient UCN (dUCN)/DCN homojunction depends on the nitrogen vacancy content in dUCN which can tune the energy band structure of dUCN from not matching to matching with that of DCN. The dUCN/DCN homojunction exhibits extended optical absorption and remarkably enhanced charge separation and photocatalytic H evolution, compared with UCN and DCN. This work illustrates the pivotal role of defects in fabricating CN homojunctions and supplies a new facile way to synthesize nitrogen-deficient CN.

摘要

制备同质结是提高聚合氮化碳(CN)光催化性能的一种经济高效的方法,但在合成CN同质结时缺陷的产生及其在同质结制备中的作用鲜有报道。在此,通过煅烧负载双氰胺的CN(由尿素制备,记为UCN),使双氰胺聚合成CN(记为DCN),同时在UCN表面形成氮空位,简单地合成了缺氮的CN同质结。缺氮的UCN(dUCN)/DCN同质结的制备取决于dUCN中的氮空位含量,其可以将dUCN的能带结构从不匹配调整为与DCN匹配。与UCN和DCN相比,dUCN/DCN同质结表现出扩展的光吸收以及显著增强的电荷分离和光催化析氢性能。这项工作阐明了缺陷在制备CN同质结中的关键作用,并提供了一种合成缺氮CN的新的简便方法。

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