Department of Environmental Engineering & Innovation and Development Center of Sustainable Agriculture & Research Center of Sustainable Energy and Nanotechnology, National Chung Hsing University, 250 Kuo-Kuang Road, Taichung, Taiwan.
Department of Environment and Energy, Sejong University, 209 Neungdong-ro, Gunja-dong, Gwangjin-gu, Seoul, Republic of Korea.
J Colloid Interface Sci. 2021 Feb 15;584:749-759. doi: 10.1016/j.jcis.2020.09.104. Epub 2020 Oct 6.
As sulfosalicylic acid (SUA) is extensively used as a pharmaceutical product, discharge of SUA into the environment becomes an emerging environmental issue because of its low bio-degradability. Thus, SO-based advanced oxidation processes have been proposed for degrading SUA because of many advantages of SO. As Oxone represents a dominant reagent for producing SO, and Co is the most capable metal for activating Oxone to generate SO, it is critical to develop an effective but easy-to-use Co-based catalysts for Oxone activation to degrade SUA. Herein, a 3D hierarchical catalyst is specially created by decorating CoO nanocubes (NCs) on macroscale nitrogen-doped carbon form (NCF). This CoO-decorated NCF (CONCF) is free-standing, macroscale and even squeezable to exhibit interesting and versatile features. More importantly, CONCF consists of CoO NCs evenly distributed on NCF without aggregation. The NCF not only serves as a support for CoO NCs but also offers additional active sites to synergistically enhance catalytic activities towards Oxone activation. Therefore, CONCF exhibits a higher catalytic activity than the conventional CoO nanoparticles for activating Oxone to fully eliminate SUA in 30 min with a rate constant of 0.142 min. CONCF exhibits a much lower Ea value of SUA degradation (35.2 kJ/mol) than reported values, and stable catalytic activities over multi-cyclic degradation of SUA. The mechanism of SUA degradation is also explored, and degradation intermediates of SUA degradation are identified to provide a possible pathway of SUA degradation. These features validate that CONCF is certainly a promising 3D hierarchical catalyst for enhanced Oxone activation to degrade SUA. The findings obtained here are also insightful to develop efficient heterogeneous Oxone-activating catalysts for eliminating emerging contaminants.
由于磺胺水杨酸(SUA)的生物降解性低,作为一种广泛应用于医药产品的物质,其排放已成为一个新出现的环境问题。因此,由于 SO 的诸多优点,基于 SO 的高级氧化工艺已被提议用于降解 SUA。由于过氧单硫酸盐(Oxone)代表产生 SO 的主要试剂,而 Co 是最有能力激活 Oxone 生成 SO 的金属,因此开发一种有效且易于使用的 Co 基催化剂来激活 Oxone 以降解 SUA 至关重要。在此,通过在大尺寸氮掺杂碳形式(NCF)上装饰 CoO 纳米立方体(NCs)专门创建了一种 3D 分层催化剂。这种 CoO 修饰的 NCF(CONCF)是自立的、大尺寸的,甚至可以挤压,具有有趣和多样的特点。更重要的是,CONCF 由均匀分布在 NCF 上的 CoO NCs 组成,没有聚集。NCF 不仅作为 CoO NCs 的载体,还提供额外的活性位点,协同增强对 Oxone 激活的催化活性。因此,CONCF 表现出比传统的 CoO 纳米颗粒更高的催化活性,可在 30 分钟内完全消除 SUA,速率常数为 0.142 min。CONCF 表现出比报道值更低的 SUA 降解 Ea 值(35.2 kJ/mol),并且在 SUA 的多循环降解过程中表现出稳定的催化活性。还探索了 SUA 降解的机制,并鉴定了 SUA 降解的中间产物,为 SUA 降解的可能途径提供了依据。这些特征验证了 CONCF 确实是一种有前途的 3D 分层催化剂,可增强 Oxone 激活以降解 SUA。这里获得的研究结果也为开发用于消除新兴污染物的高效异相 Oxone 激活催化剂提供了启示。