Upcycling contaminated biomass into metal-supported heterogeneous catalyst for electro-Fenton degradation of thiamethoxam: Preparation, mechanisms, and implications

Upcycling contaminated biomass into metal-supported heterogeneous catalyst for electro-Fenton degradation of thiamethoxam: Preparation, mechanisms, and implications
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将受污染的生物质升级改造为金属负载的多相催化剂,用于电芬顿降解噻虫嗪:制备、机制和影响

DOI:
10.1016/j.cej.2022.139814
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发表时间:
2022-10
影响因子:
15.1
通讯作者:
Cheng Peng
Cheng Peng
中科院分区:
工程技术1区
文献类型:
--
作者:
Youzheng Chai;Ma Bai;Anwei Chen;Xiyan Xu;Zhaohui Tong;Jiayi Yuan;Liang Peng;Jihai Shao;Jiahao Xiong;Cheng Peng

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•提出了一种从污染生物质中提取的多相Fenton催化剂。•使用最佳的BHFC-600在短时间内实现了THX的深度去除。•生物质中金属含量的上升促进了衍生催化剂的性能。•h +、·OH和·o2 -是THX降解的主要反应物质。•从受污染的生物质中制备功能性催化剂是有前途的。重金属污染生物质的安全处理和资源化利用一直是一个巨大的挑战。将重金属污染秸秆通过热解直接制备生物质源多金属负载非均相Fenton催化剂(BHFC)降解噻虫胺(THX)是解决这一问题的双赢策略。在该方法中,从矿区收集的污染生物质中的Fe、Mn、Cu和Zn以活性金属的形式释放,并以金属氧化物的形式加载在具有介孔结构的生物质热解生物炭上。多种金属的存在加速了相互氧化还原,增加了氧的流动性,协同促进了羟基自由基的产生,使用最优的BHFC-600在20 min内达到100%的THX降解率和90%的总有机碳去除率。不同重金属污染的生物质制备的BHFC在催化性能上存在差异。高金属含量生物质制备的BHFC的THX降解率比低金属含量生物质提高了1.2倍。采用密度泛函理论计算等方法研究了THX降解的可能途径和机制。THX的降解主要是由于h +、·OH和·o2 -攻击了福井指数较高的区域。本研究为制备可持续的环境功能材料提供了一种有前景的策略,并为污染生物质的安全处理提供了新的可行思路。
• A heterogeneous Fenton catalyst derived from contaminated biomass was proposed. • The deep removal of THX was achieved in a short time using optimal BHFC-600. • Rising metal contents in biomass promote the performance of derived catalysts. • h + , · OH, and · O 2 - served as the main reactive species for THX degradation. • The preparation of functional catalysts from contaminated biomass is promising. The safe disposal and resource utilization of heavy metal contaminated biomass has long posed a huge challenge. The direct preparation of heavy metal-contaminated straw into a biomass-derived multi-metal loading heterogeneous Fenton catalyst (BHFC) through pyrolysis for thiamethoxam (THX) degradation is a win-win strategy to address this problem. In this method, Fe, Mn, Cu, and Zn in contaminated biomass collected from mineral areas are released as active metals and loaded in the form of metal oxides on biomass pyrolysis biochar with a mesoporous structure. The presence of multiple metals accelerated the mutual redox, increased oxygen mobility, synergistically promoted the generation of hydroxyl radicals, and reached 100% THX degradation rate and 90% total organic carbon removal within 20 min using the optimum BHFC-600. The BHFC derived from biomass contaminated with different heavy metal contents showed differences in catalytic performance. The THX degradation rate of BHFC prepared from higher metal level biomass increased by 1.2-fold compared to the low level. Possible pathways and mechanisms of THX degradation was investigated using different methods, including density functional theory calculations. The degradation of THX can be mainly attributed to h + , · OH, and · O 2 - attacking the region with a high Fukui index. This study presents a promising strategy for preparing sustainable environmentally functional materials and provides new feasible ideas for the safe treatment of contaminated biomass.
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