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Developing Pt-M/C catalyst (M=Pb, Cu) for efficient catalytic wet air oxidation of phenol wastewater under mild conditions

催化作用 苯酚 化学 湿式氧化 废水 核化学 合金 无机化学 化学工程 环境工程 有机化学 环境科学 工程类
作者
Huici Shan,Rena Oh,Jintu Fan,Xiang Zhang,Nuowei Zhang,Xiaoyang Huang,Gyeong-Su Park,Qunhao Zheng,Hong‐Liang Lu,Bing Hui Chen
标识
DOI:10.1016/j.jece.2023.109854
摘要

Catalytic wet air oxidation (CWAO) is a promising process for degrading phenol in wastewater to CO2 and H2O. To achieve an active and stable Pt catalyst working at lower temperature, efficient catalysts are here developed by building a Pt-M (M=Pb, Cu) alloy structure where Pt is mainly in the form of Pt0 while M is mainly in the form of M2+. Firstly, carbon supported Pt-Pb/XC-72R and Pt-Pb/EC-300 catalysts are prepared for CWAO of phenol wastewater. It is found that Pt-Pb/XC-72R is highly active and stable for CWAO of phenol even at 100 °C. The initial TOC conversion is 91.1% and can be maintained higher than 75% in five consecutive cycles. Contrarily, Pt-Pb/EC-300 rapidly deactivates and TOC conversion decreased from 91.2% to 47.1% after five cycles. The characterization results indicate that two Pt-Pb alloy catalysts contained comparably high Pt0 concentration, which is responsible for the high activity. However, the Pb2+ concentration of Pt-Pb/XC-72R is much higher than that of Pt-Pb/EC-300, and higher Pb2+ concentration favors surface oxidation and keeps Pt0 from being oxidized during CWAO process, thus enhancing stability. For Pt-Pb/EC-300, both Pt0 and Pb0 are oxidized during the reaction, resulting in deactivation. To avoid using Pb in environmental considerations, the Pt-Pb is then replaced by Pt-Cu nanoparticles, where high catalytic activity and stability are maintained. More importantly, increasing Cu2+ can further enhance the catalytic performance. Tuning the second metal chemical state of Pt-based bimetallic alloy can be an effective approach to develop new catalysts for CWAO technology.
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