Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology, College of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing 102617, China.
J Environ Sci (China). 2022 Oct;120:105-114. doi: 10.1016/j.jes.2021.06.027. Epub 2022 Feb 2.
Catalytic wet air oxidation (CWAO) coupled desalination technology provides a possibility for the effective and economic degradation of high salinity and high organic wastewater. Chloride widely occurs in natural and wastewaters, and its high content jeopardizes the efficacy of Advanced oxidation process (AOPs). Thus, a novel chlorine ion resistant catalyst B-site Ru doped LaFeRuO in CWAO treatment of chlorine ion wastewater was examined. Especially, LaFeRuO was 45.5% better than that of the 6%RuO@TiO (commercial carrier) on total organic carbon (TOC) removal. Also, doped catalysts LaFeRuO showed better activity than supported catalysts RuO@LaFeO and RuO@TiO with the same Ru content. Moreover, LaFeRuO has novel chlorine ion resistance no matter the concentration of Cl and no Ru dissolves after the reaction. X-ray diffraction (XRD) refinement, X-ray photoelectron spectroscopy (XPS), transmission electron microscope (TEM), and X-ray absorption fine structure (XAFS) measurements verified the structure of LaFeRuO. Kinetic data and density functional theory (DFT) proved that Fe is the site of acetic acid oxidation and adsorption of chloride ions. The existence of Fe in LaFeRuO could adsorb chlorine ion (catalytic activity inhibitor), which can protect the Ru site and other active oxygen species to exert catalytic activity. This work is essential for the development of chloride-resistant catalyst in CWAO.
催化湿式氧化 (CWAO) 耦合脱盐技术为有效且经济地降解高盐和高有机废水提供了可能性。氯离子广泛存在于天然水和废水中,其高含量危及高级氧化工艺 (AOPs) 的效果。因此,研究了一种新型的耐氯离子催化剂 B 位 Ru 掺杂 LaFeRuO 在 CWAO 处理含氯离子废水中的应用。特别是,LaFeRuO 在总有机碳 (TOC) 去除方面比商业载体 6%RuO@TiO 好 45.5%。此外,掺杂催化剂 LaFeRuO 比具有相同 Ru 含量的负载型催化剂 RuO@LaFeO 和 RuO@TiO 具有更好的活性。此外,无论 Cl 的浓度如何,LaFeRuO 都具有新型的耐氯离子性,并且反应后没有 Ru 溶解。X 射线衍射 (XRD) 精修、X 射线光电子能谱 (XPS)、透射电子显微镜 (TEM) 和 X 射线吸收精细结构 (XAFS) 测量证实了 LaFeRuO 的结构。动力学数据和密度泛函理论 (DFT) 证明了 Fe 是醋酸氧化和氯离子吸附的位置。LaFeRuO 中 Fe 的存在可以吸附氯离子(催化活性抑制剂),从而保护 Ru 位和其他活性氧物种发挥催化活性。这项工作对于开发 CWAO 中的耐氯离子催化剂至关重要。