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基于氧空位的WO/SnO通过双电子水氧化反应促进电化学HO积累并降解有毒的均二甲基肼。

Oxygen vacancy based WO/SnO promote electrochemical HO accumulation by two-electron water oxidation reaction and toxic uniform dimethylhydrazine degradation.

作者信息

Zhang Mengqiong, Wang Dong, Ma Hongchao, Wei Huangzhao, Wang Guowen

机构信息

School of Light Industry and Chemical Engineering, Dalian Polytechnic University, No. 1 Qinggongyuan, Ganjinzi District, Dalian 116034, PR China.

College of Marine Science-Technology and Environment, Dalian Ocean University, No. 52 Heishijiao, Shahekou District, Dalian 116023, PR China.

出版信息

Sci Total Environ. 2024 May 10;924:171383. doi: 10.1016/j.scitotenv.2024.171383. Epub 2024 Mar 10.

DOI:10.1016/j.scitotenv.2024.171383
PMID:38462003
Abstract

The key to constructing an anodic electro-Fenton system hinges on two pivotal criteria: enhancing the catalyst activity and selectivity in water oxidation reaction (WOR), while simultaneously inhibiting the decomposition of hydrogen peroxide (HO) which is on-site electrosynthesized at the anode. To address the issues, we synthesized novel WO/SnO electrocatalysts, enriched with oxygen vacancies, capitalize on the combined activity and selectivity advantages of both WO and SnO for the two-electron pathway electrocatalytic production of HO. Moreover, the introduction of oxygen vacancies plays a critical role in impeding the decomposition of HO. This innovative design ensures that the Faraday efficiency and yield of HO are maintained at over 80 %, with a noteworthy production rate of 0.2 mmol h cm. We constructed a novel electro-Fenton system that operates using only HO as its feedstock and applied it to treat highly toxic uniform dimethylhydrazine (UDMH) from rocket launch effluent. Our experiments revealed a substantial total organic carbon (TOC) removal, achieving approximately 90 % after 120 mins of treatment. Additionally, the toxicity of N-nitrosodimethylamine (NDMA), a byproduct of great concern, was shown to be effectively mitigated, as evidenced by acute toxicity evaluations using zebrafish embryos. The degradation mechanism of UDMH is predominantly characterized by the advanced oxidative action of HO and hydroxyl radicals, as well as by complex electron transfer processes that warrant further investigation.

摘要

构建阳极电芬顿系统的关键取决于两个关键标准

提高水氧化反应(WOR)中的催化剂活性和选择性,同时抑制在阳极现场电合成的过氧化氢(HO)的分解。为了解决这些问题,我们合成了富含氧空位的新型WO/SnO电催化剂,利用WO和SnO在两电子途径电催化生产HO方面的综合活性和选择性优势。此外,氧空位的引入在阻碍HO的分解方面起着关键作用。这种创新设计确保了HO的法拉第效率和产率保持在80%以上,值得注意的生产率为0.2 mmol h cm。我们构建了一种仅使用HO作为原料运行的新型电芬顿系统,并将其应用于处理火箭发射废水中剧毒的偏二甲肼(UDMH)。我们的实验表明总有机碳(TOC)去除率很高,处理120分钟后达到约90%。此外,通过使用斑马鱼胚胎的急性毒性评估证明,备受关注的副产物N-亚硝基二甲胺(NDMA)的毒性得到有效缓解。UDMH的降解机制主要以HO和羟基自由基的高级氧化作用以及需要进一步研究的复杂电子转移过程为特征。

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