电催化末端产生H_(2)O_(2)诱导含铀酰(Ⅵ)废水生成纳米过氧化铀  

Post electro-catalytically produced H_(2)O_(2) induced the formation of nano-uranyl peroxide from uranyl(Ⅵ)-containing wastewater

作　　者：张馨月 雷新颖 孙洪飞 张生凯 许敬轩 文涛 Xinyue Zhang;Xinying Lei;Hongfei Sun;Shengkai Zhang;Jingxuan Xu;Tao Wen(MOE Key Laboratory of Resources and Environmental System Optimization,College of Environmental Science and Engineering,North China Electric Power University,Beijing 102206,China)

机构地区：[1]华北电力大学环境科学与工程学院,资源环境系统优化教育部重点实验室,北京102206

出　　处：《中国科学:化学》2025年第2期495-504,共10页SCIENTIA SINICA Chimica

基　　金：国家自然科学基金(编号:22476046)资助项目。

摘　　要：核能作为清洁、低碳、高效的基荷能源,可以有效地解决传统化石能源所带来的环境污染问题.但在铀矿选冶、乏燃料后处理等过程中产生的含铀废水对人类健康和生态环境造成了潜在的威胁.过氧化氢(H_(2)O_(2))作为一种环保、高效的氧化剂,在许多领域中具有广泛应用.工业上通常采用蒽醌法产生H_(2)O_(2),但传统的工业蒽醌工艺需要复杂的基础设施,不适合小规模操作.因此,可通过光/电催化工艺小规模高效生产H_(2)O_(2),进而与六价铀(U(Ⅵ))发生反应生成过氧化铀,实现含铀废水的高效处理.本文主要针对于电催化产生H_(2)O_(2)的后端应用,系统地探究了不同环境介质对H_(2)O_(2)与U(Ⅵ)的反应影响因素.通过静态批示法,系统性地探究H_(2)O_(2)浓度、U(Ⅵ)的浓度、pH、温度、干扰离子等因素对H_(2)O_(2)与U(Ⅵ)的反应的影响.结果表明,在pH=3.0和pH=6.0条件下,6.72 mM的H_(2)O_(2)对高浓度U(Ⅵ)的去除率接近100%,除Cu^(2+)、Fe^(3+)、VO_(3)^(-)外,其它干扰离子存在下,均能得到过氧化铀沉淀.本文提出了一种可行性的电催化产生H_(2)O_(2)诱导含铀废水生成纳米过氧化铀的策略.Nuclear energy is widely regarded as one of the most clean,low-carbon and highly efficient baseload energies,which can effectively solve for environmental pollution issues from traditional fossil energy sources.However,uranium-containing wastewater associated with the development of nuclear energy,such as mining,refining and spent fuel reprocessing,poses a potential threat to the health of human beings and environmental ecosystems.Hydrogen peroxide(H_(2)O_(2))is an environment-friendly and efficient oxidant with a wide range of applications in many fields.The traditional industrial anthraquinone process for H_(2)O_(2) requires complex infrastructure and is not feasible for small-scale operations.Therefore,developing high-performance catalysts for the small-scale and efficient production of H_(2)O_(2) by photo/electro-catalytic processes can be straightforwardly consumed with hexavalent uranyl ions(U(Ⅵ))for uraniumcontaining wastewater treatment.In this paper,aiming to the post electro-catalytically produced H_(2)O_(2),we utilized the electrochemical H_(2)O_(2) products to systematically investigate the influences of different environmental media on between the reaction of H_(2)O_(2) and U(Ⅵ),including H_(2)O_(2) concentration,initial U(Ⅵ)concentration,temperature,pH and interfering ions through the batch experiments.The results show that the removal efficiencies of high U(Ⅵ)concentration by 6.72 mM H_(2)O_(2) were up to 100%at pH=3.0 and pH=6.0,and nano-uranyl peroxide were formed in the majority of interfering ions except(Cu^(2+),Fe^(3+),VO_(3)^(-))ions.This study demonstrates the great potential of electrocatalytic production of H_(2)O_(2) to induce the formation of nano-uranyl peroxide from uranium-containing wastewater.

关 键 词：电催化 过氧化氢 U(Ⅵ) 过氧化铀 核废水 

分 类 号：X771[环境科学与工程—环境工程]