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作 者:王宏杰[1,2] 高亚光 赵子龙 陈冠翰 董文艺 WANG Hongjie1,2, GAO Yaguang1, ZHAO Zilong1, CHEN Guanhan1, DONG Wenyi1,2(1.School of Civil and Environmental Engineering, Harbin Institute of Technology Shenzhen Graduate School, Shenzhen 518055, Guangdong, China; 2.Shenzhen Key Laboratory of Water Resource Application and Environmental Pollution Control, Shenzhen 518055, Guangdong, Chin)
机构地区:[1]哈尔滨工业大学深圳研究生院,广东深圳518055 [2]深圳市水资源利用与环境污染控制重点实验室,广东深圳518055
出 处:《化工学报》2018年第6期2782-2789,共8页CIESC Journal
基 金:国家水体污染控制与治理科技重大专项(2012ZX07206-002);深圳市科技计划项目(JCYJ20160318093930497);广东省自然科学基金项目(2017A030310670)~~
摘 要:以胶原蛋白、木质素和硝酸铜为原料,采用共混热解法制备新型生物炭基铜系催化剂,通过多种表征手段考察制备方法和参数对催化湿式过氧化氢氧化(CWPO)处理Ni-EDTA模拟废液效果的影响,并阐述氧化降解过程中生物炭基铜系催化剂的失活机制。结果表明,相比溶液浸渍法,共混热解法有利于提高催化剂的催化活性,控制活性组分的均质分布和溶出释放,表现为Ni和TOC去除率分别增加13.05%和16.63%,Cu^(2+)溶出量降低93.54%;在焙烧温度为800℃,Cu掺量为10%,胶原蛋白与木质素质量比例为1:3条件下,1000 mg·L^(-1) Ni-EDTA模拟废液经60 min催化氧化后Ni和TOC去除率分别达到65.41%和34.85%,Cu^(2+)溶出量仅为1.7 mg·L^(-1)。氧化降解过程中羧酸类中间降解产物的形成、活性组分反应性溶出和价态转变是致使催化剂失活的主要原因。Novel biochar-based catalysts using the lignin, collagen, and copper nitrate as raw materials were prepared by the co-pyrolysis method. Through the characterization by various techniques, the effects of preparation methods and process parameters on treatment of Ni-EDTA by catalytic wet hydrogen peroxide oxidation(CWPO) were investigated, and the deactivation mechanism of biochar-based catalyst was discussed. The results showed that the co-pyrolysis method was more favorable to the improvement of catalytic performance, homogeneous distribution and dissolution control of active component, exhibiting an increase of 13.05% and 16.63% in Ni and TOC removal efficiencies and a decline of 93.54% Cu leaching, respectively. Removal efficiencies of Ni(65.41%) and TOC(34.85%) were achieved after 60 min treatment at optimum conditions(i.e. calcination temperature of 800℃, Cu dosage of 10%, mass ratio of collagen to lignin of 1:3) and the corresponding leaching content of Cu was merely 1.7 mg·L(-1). Besides, the deactivation mechanism of the biochar-based catalysts herein involved the formation of carboxylic acid intermediates, leaching and valence state transformation of copper.
关 键 词:木质素 胶原蛋白 催化剂 制备 Ni-EDTA 失活
分 类 号:X78[环境科学与工程—环境工程]
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