金属有机框架衍生物CuFe_(2)O_(4)@C的制备及其催化苯酚湿式空气氧化性能  

Preparation of Metal-Organic Framework Derived CuFe_(2)O_(4)@C and Its Catalytic Performance for Wet Air Oxidation of Phenol

作　　者：吕岩锋 郑泉辉 杭瑞强 王欣 LYU Yanfeng;ZHENG Quanhui;HANG Ruiqiang;WANG Xin(College of Materials Science and Engineering,Taiyuan University of Technology,Taiyuan 030024,China)

机构地区：[1]太原理工大学材料科学与工程学院,山西太原030024

出　　处：《热加工工艺》2025年第5期127-133,共7页Hot Working Technology

基　　金：山西省应用基础研究项目(201901D111110)。

摘　　要：本研究在常温下一步合成铜铁双金属有机框架(Cu/Fe-MOFs)前驱体,再经退火处理得到CuFe_(2)O_(4)@C催化剂。利用TG-DTG、XRD、XPS、SEM等技术系统表征了材料的组织结构。通过单因素变量法系统研究了退火温度、苯酚底物浓度、催化剂用量和反应温度对苯酚和COD去除效果的影响。结果表明:Cu/Fe-MOFs高温退火后生成CuFe_(2)O_(4)@C并较好地保持了原有结构,XPS进一步证明Fe(Ⅱ)、Fe(Ⅲ)、Cu(Ⅰ)和Cu(Ⅱ)共存,有利于催化反应的发生。退火温度700℃、底物浓度100 mg/L、催化剂用量20 mg、反应温度220℃下反应180 min,苯酚去除率达到97.6%,且COD去除率超过96%。推测反应机理为体系中的金属离子在与氧气和苯酚反应的过程中发生完整的氧化还原过程,在氧气充足的条件下不断生成·O_(2)^(-)、·OH^(-)等活性物质,从而将苯酚分解为CO_(2)和H_(2)O。Bimetallic copper-iron organic frameworks(Cu/Fe-MOFs)were synthesized by one-step method at room temperature.Then the precursors were annealed to obtain CuFe_(2)O_(4)@C catalysts.The structure and composition of as-prepared samples were characterized by using TG-DTG,XRD,XPS and SEM.The effects of annealing temperature,phenol substrate concentration,catalyst dosage and reaction temperature on the removal effect of phenol and COD were systematically studied by univariate variable method.The results show that CuFe_(2)O_(4)@C is formed by high temperature annealing of Cu/Fe-MOFs,which almost maintains the strucutre of the MOF precursor.XPS further demonstrates the coexistence of Fe(Ⅱ),Fe(Ⅲ),Cu(Ⅰ)and Cu(Ⅱ),which is beneficial to the catalytic reaction.The phenol removal rate is 97.6%and the COD removal rate is over 96%at annealing temperature of 700℃,substrate concentration of 100 mg/L,catalyst dosage of 20 mg and reaction temperature of 220℃ for 180 min.The reaction mechanism is presumed to be that the metal ions in the system form a complete redox process during the reaction with oxygen and phenol,and the phenol is continuously decomposed into CO_(2) and H_(2)O by the production of·O_(2)^(-),·OH^(-)and other reactive substances under the condition of sufficient oxygen.

关 键 词：退火 金属有机框架(MOF) CuFe_(2)O_(4)@C 苯酚 

分 类 号：TB383[一般工业技术—材料科学与工程]