CeMnO3 Nanoparticle-Decorated g-C3N4 Nanosheets as Z-Scheme Heterostructures for Efficient Photocatalytic Degradation of Dyes

光催化 材料科学 异质结 光降解 电子顺磁共振 线性扫描伏安法 甲基橙 光化学 纳米颗粒 可见光谱 半导体 化学工程 纳米技术 光电子学 循环伏安法 化学 催化作用 电化学 物理化学 有机化学 物理 电极 核磁共振 工程类
作者
Bhagyashree Munisha,Lokanath Patra,Jyotirmayee Nanda,Ravindra Pandey,Subhra S. Brahma
出处
期刊:ACS applied nano materials [American Chemical Society]
卷期号:6 (22): 20539-20555 被引量:29
标识
DOI:10.1021/acsanm.3c02156
摘要

The design of efficient photocatalysts for dye degradation is a challenging task for the scientific community. Semiconductor-based photocatalysts such as g-C 3 N 4 and oxides, utilizing solar energy, have been proven to be effective and promising approaches to resolve this issue to some extent. Constructing Z-scheme heterostructures by coupling g-C 3 N 4 with suitable oxide semiconductors has shown substantial enhancement of the photocatalytic performance. In this article, perovskite-type CeMnO 3 (5, 15, 25%) nanoparticle-decorated g-C 3 N 4 nanosheets are fabricated as heterostructures, using a hydrothermal synthesis process, for efficient photocatalysis of organic dyes. The formations of heterostructures are confirmed through structural, microstructural, and elemental state analysis. Brunauer–Emmett–Teller (BET) and Barrett–Joyner–Halenda (BJH) characterization techniques exhibited enhanced surface area and pore sizes, respectively. Ultraviolet–visible (UV–vis) diffuse reflectance spectroscopy (DRS), Mott–Schottky, and linear sweep voltammetry (LSV) analyses along with density functional theory (DFT) calculations predicted a p–n junction heterostructure. Electron paramagnetic resonance (EPR) studies revealed a broad spectrum with sextet hyperfine lines corresponding to Mn 4+ and Mn 2+ ions and enhanced intensity as compared to the parent ones, signifying the creation of oxygen vacancies in the heterostructure. The CeMnO 3 (25 wt %)/g-C 3 N 4 heterostructure showed highly efficient photocatalytic degradation of methylene blue under direct sunlight irradiation, with up to 99% degradation achieved in 120 min and excellent recyclability. The robustness of this photocatalyst was tested by adopting a similar process for methylene orange dye degradation, exhibiting 94% yield in 120 min. A tentative degradation mechanism is proposed based on the enhanced photodegradation efficiency and results obtained from electrochemical impedance (EIS), photoluminescence (PL), LSV, and first principal studies, which provides more insights into the photogenerated charge separation, enhanced photocurrent, and interfacial transfer efficiency through the Z-scheme charge transfer process. This study offers opportunities for designing high-performance Z-scheme hybrid photocatalysts for environmental remediation.
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