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Synergistic effect of Lewis acid-base sites in Zr4+-doped layered double hydroxides promotes rapid decontamination of nerve and blister agents under ambient conditions
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2024-11-19 , DOI: 10.1016/j.jhazmat.2024.136565 Chengcheng Huang, Ying Yang, Xin Hu, Qian Wang, Hongchen Fu, Pingjing Wang, Yunshan Zhou, Lijuan Zhang, Yuxu Zhong
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2024-11-19 , DOI: 10.1016/j.jhazmat.2024.136565 Chengcheng Huang, Ying Yang, Xin Hu, Qian Wang, Hongchen Fu, Pingjing Wang, Yunshan Zhou, Lijuan Zhang, Yuxu Zhong
Nerve and blister agents are among the deadliest chemicals posing a major threat to the society, and the development of materials that can rapidly decontaminate them under solvent-free ambient conditions is a major societal challenge. In this paper, layered double hydroxides (ZnAlxZr1-x-LDH) with varying Zr4+ doping content were synthesized and the decontamination properties of nerve and blister agents were investigated under ambient conditions. The results show that, compared to ZnAl-LDH, the ZnAl0.4Zr0.6-LDH with the highest amount of Zr4+ dopant reduced the decontamination reaction half-life of sarin (GB) and soman (GD) by 10 and 9 times, respectively. Mechanism studies revealed that ZnAl0.4Zr0.6-LDH employs the synergistic effect of Lewis acid-base sites to catalyze the decomposition of GB and GD into hydrolysis products and surface-bound hydrolysis products. The study also showed that under ambient conditions, ZnAl0.4Zr0.6-LDH demonstrated superior decontamination performance for the sulfur mustard (HD) simulant 2-chloroethyl ethyl sulfide (CEES) compared to ZnAl-LDH, effectively catalyzing the detoxification of CEES into dehydrohalogenation (EVS) and 1,2-bis-(ethylthio) ethane (BETE). ZnAl0.4Zr0.6-LDH also had satisfactory decontamination performance against HD. This work provides not only a green and efficient catalyst with potential for practical applications but also new insights for constructing broad-spectrum, highly efficient self-detoxifying materials.
中文翻译:
Zr4+ 掺杂层状双氢氧化物中 Lewis 酸碱位点的协同作用促进了环境条件下神经和泡罩剂的快速去污
神经和泡罩剂是对社会构成重大威胁的最致命的化学品之一,开发能够在无溶剂环境条件下快速净化它们的材料是一项重大的社会挑战。本文合成了具有不同 Zr4+ 掺杂含量的层状双氢氧化物 (ZnAlxZr1-x-LDH),并研究了神经和水泡剂在环境条件下的去污性能。结果表明,与 ZnAl-LDH 相比,Zr4+ 掺杂剂含量最高的 ZnAl0.4Zr0.6-LDH 将沙林 (GB) 和索曼 (GD) 的去污反应半衰期分别降低了 10 倍和 9 倍。机理研究表明,ZnAl0.4Zr0.6-LDH 利用路易斯酸碱位点的协同作用催化 GB 和 GD 分解成水解产物和表面结合水解产物。研究还表明,在环境条件下,与 ZnAl-LDH 相比,ZnAl0.4Zr0.6-LDH 对硫芥子气 (HD) 模拟物 2-氯乙基硫化物 (CEES) 表现出卓越的净化性能,有效地催化 CEES 解毒为脱卤化氢 (EVS) 和 1,2-双-(乙基硫代)乙烷 (BETE)。ZnAl0.4Zr0.6-LDH 对 HD 也有令人满意的去污性能。这项工作不仅提供了一种具有实际应用潜力的绿色高效催化剂,而且为构建广谱、高效的自解毒材料提供了新的见解。
更新日期:2024-11-19
中文翻译:
Zr4+ 掺杂层状双氢氧化物中 Lewis 酸碱位点的协同作用促进了环境条件下神经和泡罩剂的快速去污
神经和泡罩剂是对社会构成重大威胁的最致命的化学品之一,开发能够在无溶剂环境条件下快速净化它们的材料是一项重大的社会挑战。本文合成了具有不同 Zr4+ 掺杂含量的层状双氢氧化物 (ZnAlxZr1-x-LDH),并研究了神经和水泡剂在环境条件下的去污性能。结果表明,与 ZnAl-LDH 相比,Zr4+ 掺杂剂含量最高的 ZnAl0.4Zr0.6-LDH 将沙林 (GB) 和索曼 (GD) 的去污反应半衰期分别降低了 10 倍和 9 倍。机理研究表明,ZnAl0.4Zr0.6-LDH 利用路易斯酸碱位点的协同作用催化 GB 和 GD 分解成水解产物和表面结合水解产物。研究还表明,在环境条件下,与 ZnAl-LDH 相比,ZnAl0.4Zr0.6-LDH 对硫芥子气 (HD) 模拟物 2-氯乙基硫化物 (CEES) 表现出卓越的净化性能,有效地催化 CEES 解毒为脱卤化氢 (EVS) 和 1,2-双-(乙基硫代)乙烷 (BETE)。ZnAl0.4Zr0.6-LDH 对 HD 也有令人满意的去污性能。这项工作不仅提供了一种具有实际应用潜力的绿色高效催化剂,而且为构建广谱、高效的自解毒材料提供了新的见解。