Synthesis and application of Cu-CaTiO3-GO ternary composite: A new visible-light active multifunctional photocatalyst efficient towards antibiotic cefixime degradation and H2 evolution reaction

Q1 Environmental Science
Manjusha Passi, Bonamali Pal
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引用次数: 0

Abstract

To combat the issues of energy scarcity and environmental pollution, a visible-light responsive, ternary photocatalyst (Cu-CaTiO3-GO) was fabricated, by photo-depositing Cu nanoparticles over a CaTiO3-GO binary composite. The physicochemical characteristics of Cu-CaTiO3-GO were investigated using XRD, HR-TEM, FE-SEM, EDS-mapping XPS, Raman, FT-IR, BET, EIS, UV–vis DRS, and PL techniques. In comparison with pristine CaTiO3, and binary composites (Cu-CaTiO3, CaTiO3-GO), the ternary hybrid exhibited superior photocatalytic activity for H2 generation as well as antibiotic cefixime (CFX) degradation. Under LED light, the rate of H2 generation over Cu-CaTiO3-GO accumulated to 57.69 mmolh−1, while the photodegradation efficiency for CFX reached 94.1 % in 100 min with 53.4 % of TOC removal. The upgraded performance is credited to synergistic effects of Cu NPs (SPR effect), CaTiO3 (specialized cuboid-like morphology), and GO (high conductivity), co-existing in the trio-hybrid, which resulted in a greatly increased surface area, an expanded spectral response range, a stronger adsorption property, efficient charge migration and separation extent. Ternary catalyst performed well even in the 4 recycling tests (retaining 79.4 % CFX removal and 52.51 mmolh−1 H2 evolution efficiency). In Cu-CaTiO3-GO system, the electron transport channel (Cu → CaTiO3 → GO) with adequate band potentials effectively supports both photocatalytic oxidation and reduction. Photoelectrons are enriched and transferred by plasmonic Cu, and then captured by GO, an e- sink. This maximizes composite photo redox capability, rapidly generating active radicals (OH), and (O2-), degrading CFX to simpler molecules and reducing proton to H2. The effectiveness of Cu-CaTiO3-GO was even tested in the real water matrices. Besides, degradation intermediates of CFX were elucidated using LC-MS, and the decomposition pathway was suggested. Finally, the probable photocatalytic reaction mechanism was deduced for both the degradation and H2 generation processes. The current study proposes a non-noble transition metal-based perovskite-type photocatalytic material for both clean energy generation and wastewater treatment.

Abstract Image

Cu-CaTiO3-GO 三元复合材料的合成与应用:一种新型可见光活性多功能光催化剂,可高效降解抗生素头孢克肟并进行 H2 进化反应
为解决能源短缺和环境污染问题,通过在 CaTiO3-GO 二元复合材料上光沉积铜纳米粒子,制备了一种可见光响应型三元光催化剂(Cu-CaTiO3-GO)。利用 XRD、HR-TEM、FE-SEM、EDS-mapping XPS、拉曼、傅立叶变换红外光谱、BET、EIS、紫外-可见 DRS 和 PL 技术研究了 Cu-CaTiO3-GO 的物理化学特性。与原始 CaTiO3 和二元复合材料(Cu-CaTiO3、CaTiO3-GO)相比,三元杂化物在生成 H2 和降解抗生素头孢克肟(CFX)方面表现出更高的光催化活性。在 LED 光下,Cu-CaTiO3-GO 产生 H2 的速率积累到 57.69 mmolh-1,而 CFX 的光降解效率在 100 分钟内达到 94.1%,TOC 去除率为 53.4%。性能的提升归功于三元杂化物中共存的 Cu NPs(SPR 效应)、CaTiO3(特殊的立方体状形态)和 GO(高导电性)的协同效应,从而大大增加了比表面积,扩大了光谱响应范围,增强了吸附性能,提高了电荷迁移和分离效率。三元催化剂即使在 4 次循环测试中也表现良好(保留了 79.4 % 的 CFX 去除率和 52.51 mmolh-1 的 H2 进化效率)。在 Cu-CaTiO3-GO 系统中,电子传输通道(Cu → CaTiO3 → GO)具有足够的带电位,可有效支持光催化氧化和还原。光电子由等离子体铜富集和转移,然后被作为电子汇的 GO 捕获。这最大限度地提高了复合光氧化还原能力,迅速产生活性自由基(OH)和(O2-),将 CFX 降解为更简单的分子,并将质子还原为 H2。Cu-CaTiO3-GO 的有效性甚至在真实的水基质中进行了测试。此外,还利用 LC-MS 分析了 CFX 的降解中间产物,并提出了其分解途径。最后,还推导出了降解和产生 H2 过程的可能光催化反应机制。本研究提出了一种基于非贵金属的包晶型光催化材料,可用于清洁能源生产和废水处理。
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来源期刊
Environmental Nanotechnology, Monitoring and Management
Environmental Nanotechnology, Monitoring and Management Environmental Science-Water Science and Technology
CiteScore
13.00
自引率
0.00%
发文量
132
审稿时长
48 days
期刊介绍: Environmental Nanotechnology, Monitoring and Management is a journal devoted to the publication of peer reviewed original research on environmental nanotechnologies, monitoring studies and management for water, soil , waste and human health samples. Critical review articles, short communications and scientific policy briefs are also welcome. The journal will include all environmental matrices except air. Nanomaterials were suggested as efficient cost-effective and environmental friendly alternative to existing treatment materials, from the standpoints of both resource conservation and environmental remediation. The journal aims to receive papers in the field of nanotechnology covering; Developments of new nanosorbents for: •Groundwater, drinking water and wastewater treatment •Remediation of contaminated sites •Assessment of novel nanotechnologies including sustainability and life cycle implications Monitoring and Management papers should cover the fields of: •Novel analytical methods applied to environmental and health samples •Fate and transport of pollutants in the environment •Case studies covering environmental monitoring and public health •Water and soil prevention and legislation •Industrial and hazardous waste- legislation, characterisation, management practices, minimization, treatment and disposal •Environmental management and remediation
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