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新型类纳米花状磷、钾共掺杂石墨相氮化碳用于高效光生羟基自由基的合成

Synthesis of novel nanoflowers-like P, K co-doped graphitic carbon nitride for efficient HO photoproduction.

作者信息

Liang Huagen, Zhao Jingbo, Wang Anhu, Kannan Palanisamy, Jing Shengyu, Chen Fu, Tsiakaras Panagiotis

机构信息

Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization, Carbon Neutrality Institute, China University of Mining and Technology, Xuzhou 221008, China; Laboratory of Alternative Energy Conversion Systems, Department of Mechanical Engineering, School of Engineering, University of Thessaly, Pedion Areos 38834, Greece.

School of Information and Control Engineering, China University of Mining and Technology, Xuzhou 221116, China.

出版信息

J Colloid Interface Sci. 2025 Jan;677(Pt B):729-739. doi: 10.1016/j.jcis.2024.08.058. Epub 2024 Aug 9.

Abstract

Photocatalytic oxygen reduction is considered an economical and green way to produce HO. Graphitic carbon nitride is a common photocatalyst, but its activity is limited by the low specific surface area and the high recombination rate of photogenerated electron-hole pairs. Herein, nanoflowers-like phosphorus (P) and potassium (K) co-doped graphitic carbon nitride (PKCN) is synthesized by co-polymerization of ammonium dihydrogen phosphate and melamine in the mixed molten salt (KCl/LiCl) medium. Within 90 min, the synthesized PKCN-0.05 can produce 4.97 mmol L of HO, which is 7.8 times higher than that of pure bulk g-CN. The enhanced photocatalytic performance of PKCN-0.05 is mainly attributed to the following: 1) KCl/LiCl molten salt induces melamine to form a three-dimensional flower-like morphology, which expands the specific surface area, exposes more active sites, and improves the light utilization efficiency; 2) high crystallinity of PKCN-0.05 and the K ions inserted between the interlayers are beneficial for accelerating electron transfer; 3) the formation of PN bonds and the existence of N vacancies promotes the separation of photoproduced carriers; 4) the negatively shifted conduction band of PKCN-0.05 favors oxygen reduction.

摘要

光催化氧还原被认为是一种经济且绿色的产生过氧化氢的方式。石墨相氮化碳是一种常见的光催化剂,但其活性受到低比表面积和光生电子 - 空穴对高复合率的限制。在此,通过在混合熔盐(KCl/LiCl)介质中使磷酸二氢铵和三聚氰胺共聚合成了纳米花状的磷(P)和钾(K)共掺杂石墨相氮化碳(PKCN)。在90分钟内,合成的PKCN - 0.05可产生4.97 mmol/L的过氧化氢,这比纯块状g - CN高出7.8倍。PKCN - 0.05增强的光催化性能主要归因于以下几点:1)KCl/LiCl熔盐诱导三聚氰胺形成三维花状形态,扩大了比表面积,暴露出更多活性位点,并提高了光利用效率;2)PKCN - 0.05的高结晶度以及插入层间的K离子有利于加速电子转移;3)PN键的形成和N空位的存在促进了光生载流子的分离;4)PKCN - 0.05的导带负移有利于氧还原。

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