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负载于磷掺杂管状氮化碳上的金属有机框架用于增强光催化产氢和胺氧化反应

Metal-organic frameworks loaded on phosphorus-doped tubular carbon nitride for enhanced photocatalytic hydrogen production and amine oxidation.

作者信息

Liu Jianan, Li Qi, Xiao Xudong, Li Fuxiang, Zhao Chen, Sun Qi, Qiao Panzhe, Zhou Jing, Wu Jie, Li Baiyan, Bao Hongliang, Jiang Baojiang

机构信息

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, PR China.

Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, PR China.

出版信息

J Colloid Interface Sci. 2021 May 15;590:1-11. doi: 10.1016/j.jcis.2021.01.031. Epub 2021 Jan 16.

DOI:10.1016/j.jcis.2021.01.031
PMID:33517246
Abstract

It is still a challenge to evolve visible light photocatalysts that possess both efficient oxidation and reduction capabilities. In this paper, phosphorus-doped tubular carbon nitride@UiO-66-NH (p-TCN@U6-X) composites were prepared by in-situ load of UiO-66-NH on the surface of p-TCN based on solvothermal method, which exhibit excellent photocatalytic oxidation and reduction ability. As a result, under visible light irradiation (λ > 420 nm), the photocatalytic H production performance of p-TCN@U6-3 reached 2628 μmol gh, which was 8.19 and 5.36 times higher than that of p-TCN and UiO-66-NH, respectively. Meanwhile, p-TCN@U6-3 also exhibited well selectivity rate (99%) and conversion rate (98%) for oxidative coupling of amine compounds. The high photocatalytic activities can be assigned to the improved visible light adsorption resulted from the tubular structure of p-TCN and enhanced electrical conductivity because of the phosphorus doping in p-TCN. Furthermore, UiO-66-NH plays the role of co-catalyst and active centers in the photocatalytic system to synergistically catalyze the reactions. Transient photocurrent spectra, steady-state photoluminescence (PL) and time-resolved photoluminescence (TRPL) further prove the more effective charge separation and transfer happened in the p-TCN@U6-X system compared with sole p-TCN and UiO-66-NH, respectively. This work provides an effective method for creating novel carbon nitride-based photocatalytic systems with efficient capability for photocatalytic oxidation and reduction.

摘要

开发同时具备高效氧化和还原能力的可见光光催化剂仍然是一项挑战。本文基于溶剂热法,通过在磷掺杂管状氮化碳(p-TCN)表面原位负载UiO-66-NH,制备了磷掺杂管状氮化碳@UiO-66-NH(p-TCN@U6-X)复合材料,该复合材料表现出优异的光催化氧化和还原能力。结果表明,在可见光照射(λ>420 nm)下,p-TCN@U6-3的光催化产氢性能达到2628 μmol g h,分别是p-TCN和UiO-66-NH的8.19倍和5.36倍。同时,p-TCN@U6-3对胺类化合物的氧化偶联也表现出良好的选择性(99%)和转化率(98%)。高光催化活性可归因于p-TCN的管状结构改善了可见光吸附,以及p-TCN中的磷掺杂提高了电导率。此外,UiO-66-NH在光催化体系中起到助催化剂和活性中心的作用,协同催化反应。瞬态光电流光谱、稳态光致发光(PL)和时间分辨光致发光(TRPL)进一步证明,与单独的p-TCN和UiO-66-NH相比,p-TCN@U6-X体系中发生了更有效的电荷分离和转移。这项工作为创建具有高效光催化氧化和还原能力的新型氮化碳基光催化体系提供了一种有效方法。

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