Precise preparation of CoO @KSB catalysts by atomic layer deposition for peroxymonosulfate activation and landfill leachate treatment

Wenjie Gao, Guanyun Wu, Xu He, Zhanjun Cheng, Beibei Yan, Guanyi Chen, Ning Li
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Abstract

The construction of desired active sites is critical for enhanced activity in heterogeneous peroxymonosulfate (PMS) systems. In view of the shortcomings of the current construction methods, such as low precision and harsh conditions, CoOx@KSB catalysts were precisely prepared at the atomic level using atomic layer deposition in this study. Using alkali-modified sludge biochar (KSB) as a feedstock, two different deposition processes were proposed to investigate the preparation pattern on the treatment efficiency of landfill leachate. Results showed that the small-cycle layer-by-layer deposition (B process) not only preserved the original N sites of the catalyst after 150 depositions, but also obtained satisfactory Co2+. Under the optimal experimental conditions, KSB-B150 degraded more than 90% of SMX within 120 min. After 8 h of continuous operation in the packed column reactor, the COD concentration of the effluent landfill leachate was still below 100 mg/L, and the biotoxicity of the effluent was reduced to 0.41 times of the original. The Co2+, OV and graphite N sites could generate SO4•− and •OH, which played dominant roles in SMX degradation. This study provides a new strategy for constructing active sites in heterogeneous PMS system. It is beneficial to promote the application of heterogeneous advanced oxidation technology in landfill leachate treatment.
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原子层沉积法制备CoO @KSB催化剂,用于过氧单硫酸盐活化及垃圾渗滤液处理
在非均相过氧单硫酸盐(PMS)体系中,理想活性位点的构建是提高活性的关键。针对目前构建方法精度低、条件苛刻等缺点,本研究采用原子层沉积技术在原子水平上精确制备CoOx@KSB催化剂。以碱改性污泥生物炭(KSB)为原料,研究了两种不同沉积工艺对垃圾渗滤液处理效率的影响规律。结果表明,小循环层积法(B法)在沉积150次后,不仅保留了催化剂原有的N位,而且获得了满意的Co2+。在最佳实验条件下,KSB-B150在120 min内对SMX的降解率达到90%以上,在填料塔反应器中连续运行8 h后,出水垃圾渗滤液的COD浓度仍低于100 mg/L,出水生物毒性降至原来的0.41倍。Co2+、OV和石墨N位点可生成SO4•−和•OH,在SMX降解中起主导作用。本研究为异构PMS系统中活性位点的构建提供了新的策略。有利于推广非均相深度氧化技术在垃圾渗滤液处理中的应用。
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