摘要
由于纺织、印刷等工业规模的迅速扩张,生产过程中产生的染料废水对人类生存环境造成巨大压力。目前,在染料废水修复处理领域,基于SO_(4)^(·-)的高级氧化技术由于其氧化优势备受关注。通常,过一硫酸盐(PMS)可自分解产生SO_(4)^(·-),然而其生成效率很低,因此,探寻有效的PMS催化剂成为研究热点。本研究以5,5′-二苯醚间苯二甲酸(H 4odip)和Ni(NO_(3))_(2)·6H_(2)O为原料,采用溶剂热法制得一种三维结构配合物Ni 4(odip)2-(μ2-OH_(2))2(H_(2)O)8,该材料水稳定性较好且能够在弱酸弱碱环境下稳定存在。采用X射线单晶和粉末衍射、红外光谱、热重及元素分析对配合物的结构和组成进行了表征。利用紫外-可见分光光度计研究其催化降解罗丹明B的活性与机理,系统探讨了配合物和PMS用量、溶液反应温度和pH对罗丹明B降解性能的影响。与不加催化剂相比,配合物的加入可使罗丹明B的降解速率提高两倍。研究表明,在中性环境中,PMS/配合物催化体系具有更强的降解能力,降解率可达92.3%。活性氧物种(ROS)捕获实验和电子顺磁共振波谱结果表明该催化体系降解罗丹明B的ROS有SO_(4)^(·-)、·OH、1O_(2)和O_(2)^(·-),且此四种ROS在降解罗丹明B时的贡献作用相近。综合分析实验结果,该配合物在催化PMS用于染料废水修复处理领域可作为一种有效且能循环使用的新型多相催化剂。
With the rapid expansion of textile and printing industry scale,the dye wastewater generated in the production process has brought huge pressure to living environment.At present,in the field of remediation and treatment of dye wastewater,advanced oxidation technology based on SO_(4)^(·-)has attracted much attention due to its oxidation advantages.In general,peroxymonosulfate(PMS)can self-decompose to produce SO_(4)^(·-),but the efficiency is low,so searching for an effective PMS catalyst has become a focus recently.Here a 3D complex Ni 4(odip)2-(μ2-OH_(2))2(H_(2)O)8 was prepared by solvothermal method using 5,5′-oxydiisophthalic acid(H 4odip)and Ni(NO_(3))2·6H_(2)O,which has good water stability and can exist stably in weak acid and weak alkali environment.To study it’s structure and composition,X-ray single crystal and powder diffraction,infrared spectroscopy,thermogravimetric analysis and elemental analyses are adopted here.The activity and mechanism of catalytic degradation of Rhodamine B were tested by UV-Vis spectrophotometer.At the same time,the effects of the complex and peroxymonosulfate loading,reaction temperature and pH on dye degradation were systematically studied.Compared with no catalyst,the degradation rate of Rhodamine B was increased by two times with the addition of the complex.In the neutral environment,the PMS/complex catalytic system has a stronger degradation ability,and the degradation rate can reach 92.3%.A comprehensive analysis of the active oxygen species(ROS)capture experiment and electron paramagnetic resonance(EPR)test results confirmed that the ROS produced by the PMS/complex system include SO_(4)^(·-),·OH,1O_(2)and O_(2)^(·-),and the contribution of the four ROS in the degradation of rhodamine B was similar.Therefore,the complex can be used as an effective and recyclable new heterogeneous catalyst in the field of catalytic PMS for dye wastewater remediation.
作者
刘洋
马占营
李午戊
郭乃妮
侯磊
樊星宇
王樱嫒
王尧宇
LIU Yang;MA Zhanying;LI Wuwu;GUO Naini;HOU Lei;FAN Xingyu;WANG Ying’ai;WANG Yaoyu(School of Chemistry and Chemical Engineering,Xianyang Normal University,Xianyang 712000,Shaanxi,China;College of Chemistry&Materials Science,Northwest University,Xi’an 710069,China)
出处
《材料导报》
EI
CAS
CSCD
北大核心
2024年第16期252-257,共6页
Materials Reports
基金
陕西省自然科学基金(2023-JC-QN-0173,2023-YBSF-595)
陕西省教育厅科研计划基金(22JK0605)
咸阳市重点研发计划基金(L2023-ZDYF-QYCX-030)
大学生创新创业训练计划基金(xysfxy2024169)
咸阳师范学院研究项目(2023YB23,sjxm202414)。
关键词
配合物
过一硫酸盐
催化降解
罗丹明B
活性与机理
complex
peroxymonosulfate(PMS)
catalytic degradation
rhodamine B(RhB)
activity and mechanism
