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氮缺陷氧化镝集成的g-CN纳米片上高效光催化产生羟基自由基

Highly efficient photocatalytic HO generation over dysprosium oxide-integrated g-CN nanosheets with nitrogen deficiency.

作者信息

Ahmed Mohamed Tarek, Abdullah Hairus, Kuo Dong-Hau

机构信息

Department of Materials Science and Engineering, National Taiwan University of Science and Technology, No.43, Sec. 4, Keelung Road, Taipei, 10607, Taiwan.

Department of Materials Science and Engineering, National Taiwan University of Science and Technology, No.43, Sec. 4, Keelung Road, Taipei, 10607, Taiwan; Department of Industrial Engineering, Universitas Prima Indonesia, Medan, Indonesia.

出版信息

Chemosphere. 2022 Nov;307(Pt 2):135910. doi: 10.1016/j.chemosphere.2022.135910. Epub 2022 Aug 5.

Abstract

The increasing global crisis considers energy as the fundamental cause to conduct extensive research work to find clean alternative methods with high capabilities such as HO synthesis. Photocatalytic HO production can tackle this growing issue by maintaining environmental remediation. In this work, dysprosium oxide (Dy-oxide)-integrated g-CN has been synthesized and characterized with XRD, SEM, TEM, XPS, EPR, DRS, PL, and electrochemical analyses. Simulated solar light irradiation implemented photocatalytic HO production using the as-prepared catalysts. The facile preparation technique in the Ar atmosphere raises more N deficiency in the g-CN matrix. N-deficient g-CN nanosheets with an exceptionally high photocatalytic performance can be further enhanced by integrating well-dispersed Dysprosium oxide (DyO) particles onto g-CN. This study reports bandgap narrowing and various surface defects on g-CN with trace amounts of DyO. Undoped g-CN (Dy0) yielded 20.27 mM⋅g⋅h, while the optimized photocatalyst Dy15 showed high performance of HO production up to 48.36 mM⋅g⋅h. It is approximately 2.4 times higher than the pristine g-CN. Dy15 proves the positive impact of Dy-oxide on enhancing the N-deficient g-CN performance towards photocatalytic HO production. This work highlights the oxygen reduction reaction (ORR) through a mixed pathway of well-known two-step one-electron and one-step two-electron processes in HO generation.

摘要

日益严重的全球危机将能源视为开展广泛研究工作的根本原因,以寻找具有高能力的清洁替代方法,如羟基自由基(·OH)合成。光催化产生·OH可以通过环境修复来解决这一日益严重的问题。在这项工作中,合成了氧化镝(Dy-氧化物)集成的石墨相氮化碳(g-CN),并通过X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、电子顺磁共振(EPR)、漫反射光谱(DRS)、光致发光(PL)和电化学分析对其进行了表征。使用所制备的催化剂,模拟太阳光照射实现了光催化产生·OH。在氩气气氛中的简便制备技术使g-CN基体中产生更多的氮缺陷。通过将分散良好的氧化镝(DyO)颗粒整合到g-CN上,可以进一步提高具有异常高光催化性能的氮缺陷型g-CN纳米片的性能。本研究报道了g-CN与微量DyO的带隙变窄和各种表面缺陷。未掺杂的g-CN(Dy0)产生20.27 mM·g·h,而优化后的光催化剂Dy15在光催化产生·OH方面表现出高达48.36 mM·g·h的高性能。它比原始g-CN高出约2.4倍。Dy15证明了Dy-氧化物对提高氮缺陷型g-CN光催化产生·OH性能的积极影响。这项工作强调了在·OH生成过程中通过著名的两步单电子和一步双电子过程的混合途径进行氧还原反应(ORR)。

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