调整RhNi/CeO2催化剂的性能以提高氯酸盐还原效率

IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL
Le Yu , Lei Wang , Zhaoyi Xu , Shourong Zheng , Tao Long
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引用次数: 0

摘要

氯酸盐(ClO3-)是水环境中常见的氧阴离子污染物,催化加氢还原氧阴离子已成为一种很有前途的水处理策略。负载Rh催化剂因其对H2具有较高的活化能力而在液相催化加氢中得到了广泛的应用,但探索对不同污染物具有高活性和稳定性的催化剂仍然是一个很大的挑战。通过浸渍法将过渡金属Ni引入到Rh基催化剂Rh/CeO2中,得到双金属催化剂RhNi10/CeO2,用于ClO3-的催化加氢还原。原位漂移鉴定了催化剂中高度分散的Rh纳米颗粒,XPS表征确定了负载的双金属Rh- ni和CeO2载体之间的强金属-载体相互作用。RhNi10/CeO2的初始活性是Rh/CeO2的27倍。此外,理论计算证实了实验观察,当氯酸盐吸附在Rh表面时,释放的能量随着Ni的引入而增加。我们发现通过改变ClO3-浓度,RhNi10/CeO2的反应性增强,从而使其在催化剂表面的吸附更有利。此外,还通过添加氯离子(Cl-)和催化剂回收来测试催化剂的可重复使用性。结果表明,尽管Cl-(浓度为0.4 mM的12倍)对RhNi10/CeO2有轻微的抑制作用,但RhNi10/CeO2的去除率仍保持在100 %。循环5次后,活度损失保持在9 %以下,去除率为100 %。双金属协同作用增加了对氯离子干扰的抵抗力,提供了高的催化稳定性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Tailoring the properties of RhNi/CeO2 catalysts for improved chlorate reduction efficiency
Chlorate (ClO3-) are commonly identified oxyanions pollutant in the water environment, and catalytic hydrogenation reduction of oxyanions has emerged as a promising water treatment strategy. Supported Rh catalysts have been widely applied in the liquid phase catalytic hydrogenation due to their high activation capacity for H2, while exploring highly active and stable catalysts for different pollutants remains a great challenge. The transition metal Ni was introduced into the Rh-based catalyst Rh/CeO2 by the impregnation method to obtain the bimetallic catalyst RhNi10/CeO2, which was used in the catalytic hydrogenation reduction of ClO3-. In-situ DRIFTS identifies the highly dispersed Rh nanoparticles in the catalyst, and the strong metal-support interaction between the supported bimetallic Rh-Ni and CeO2 supports is determined by XPS characterization. RhNi10/CeO2 exhibits an initial activity approximately 27 times higher than that of Rh/CeO2. Furthermore, theoretical calculations corroborate the experimental observation that when chlorate is adsorbed on the Rh surface, the energy released increases with the introduction of Ni. We reveal the enhanced reactivity of the RhNi10/CeO2 through changing ClO3- concentration, which renders adsorption on catalyst surface pathway sequencely more favorable. In addition, the reusability of the catalyst was tested by adding chloride ions (Cl-) and catalyst recycling. Results revealed that RhNi10/CeO2 maintained 100 % removal efficiency despite slight inhibition by Cl- (12 times the ClO3- concentration of 0.4 mM). After 5 cycles, the activity loss remained below 9 % with 100 % removal efficiency. The bimetallic synergy leads to increased resistance to chloride ion interference, providing high catalytic stability.
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来源期刊
Journal of Environmental Chemical Engineering
Journal of Environmental Chemical Engineering Environmental Science-Pollution
CiteScore
11.40
自引率
6.50%
发文量
2017
审稿时长
27 days
期刊介绍: The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.
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