CeO2-CuO composites prepared via supercritical antisolvent precipitation for photocatalytic hydrogen production from lactic acid aqueous solution

IF 7.2 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of CO2 Utilization Pub Date : 2024-07-01 DOI:10.1016/j.jcou.2024.102878
Maria Chiara Iannaco, Stefania Mottola, Vincenzo Vaiano, Giuseppina Iervolino, Iolanda De Marco
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Abstract

The global increase in energy demand requires a continuous search for renewable and clean alternative resources to fossil fuels. Hydrogen is emerging as a promising energy carrier for the future; its production via photocatalysis, driven by sunlight, can directly convert solar energy into a usable or storable energy resource. However, water splitting requires sacrificial agents or electron donors/hole scavengers, such as short-chain organic acids. This research explores the use of lactic acid as a source for photocatalytic hydrogen production, offering valuable alternatives for wastewater management and renewable energy production. This study employed the innovative supercritical antisolvent (SAS) technique to micronize the precursors of both the active phase (CeO2) and co-catalyst (CuO), ensuring rapid and complete solvent removal and size reduction of photocatalyst precursors. The prepared samples were characterized by field emission scanning electron microscopy (FESEM), Fourier transform infrared (FT-IR) spectroscopy, dynamic light scattering (DLS) analysis, Brunauer-Emmett-Teller (BET) analysis and thermogravimetric analysis (TGA). This study has shown that the micronization process resulted in a notable improvement in CeO2 photocatalytic activity, attributed to the reduction of the dimensions of the powders. Hydrogen production was equal to 3989 μmol L−1 for the SAS-produced photocatalyst while using a commercial CeO2 sample resulted in H2 production of 2519 μmol L−1. The enhanced photoactivity of CeO2-CuO composites was found to be related to the presence of CuO. The optimal CuO amount was equal to 0.5 wt%, determining a hydrogen production of 9313 μmol L−1 after 4 h of UV irradiation time. A photocatalytic test carried out with deuterated water (D2O) instead of distilled H2O demonstrated that hydrogen was preferentially produced from water splitting reaction, whereas lactic acid acted as a sacrificial agent being oxidized from positive holes photogenerated in the valence band of CuO.

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通过超临界反溶剂沉淀制备 CeO2-CuO 复合材料,用于光催化乳酸水溶液制氢
全球能源需求的增长要求我们不断寻找可再生的清洁资源来替代化石燃料。氢正在成为一种前景广阔的未来能源载体;在阳光的驱动下,通过光催化技术生产氢,可以直接将太阳能转化为可用或可储存的能源资源。然而,水分裂需要牺牲剂或电子供体/空穴清除剂,如短链有机酸。本研究探讨了使用乳酸作为光催化制氢的来源,为废水管理和可再生能源生产提供了有价值的替代品。本研究采用了创新的超临界反溶剂(SAS)技术,将活性相(CeO2)和助催化剂(CuO)的前体微粉化,确保快速、完全地去除溶剂并减小光催化剂前体的尺寸。制备的样品通过场发射扫描电子显微镜(FESEM)、傅立叶变换红外光谱(FT-IR)、动态光散射(DLS)分析、Brunauer-Emmett-Teller(BET)分析和热重分析(TGA)进行了表征。研究表明,微粉化过程显著提高了 CeO2 的光催化活性,这归功于粉末尺寸的减小。SAS 生产的光催化剂的产氢量为 3989 μmol L-1,而使用商用 CeO2 样品的产氢量为 2519 μmol L-1。研究发现,CeO2-CuO 复合材料光活性的增强与 CuO 的存在有关。最佳的 CuO 含量为 0.5 wt%,在紫外线照射 4 小时后,氢气产量为 9313 μmol L-1。用氘化水(D2O)代替蒸馏水进行的光催化测试表明,氢气优先从水分裂反应中产生,而乳酸则作为牺牲品,被 CuO 价带中光生成的正空穴氧化。
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来源期刊
Journal of CO2 Utilization
Journal of CO2 Utilization CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.90
自引率
10.40%
发文量
406
审稿时长
2.8 months
期刊介绍: The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials. The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications. The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.
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