基于 Co-MOF/g-CN 复合材料的绿色高效合成催化剂用于激活过一硫酸盐降解抗抑郁药文拉法辛。
Green and efficient synthesis of Co-MOF-based/g-CN composite catalysts to activate peroxymonosulfate for degradation of the antidepressant venlafaxine.
机构信息
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, Jiangsu 210023, PR China.
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, Jiangsu 210023, PR China; Department of Chemistry, Tsinghua University, Beijing 100084, PR China.
出版信息
J Colloid Interface Sci. 2022 Mar 15;610:280-294. doi: 10.1016/j.jcis.2021.11.162. Epub 2021 Dec 1.
Based on single metal-organic framework (MOF) composite catalyst ZIF-67/g-CN (ZG), the composite catalysts ZIF-67/MOF-74(Ni)/g-CN (ZNG) and ZIF-67/MIL-100(Fe)/g-CN (ZMG) with double MOFs were synthesized, used to effectively activate peroxymonosulfate (PMS) for degrade venlafaxine (VEN). Various characterization methods (XRD, FT-IR, Raman, SEM, EDS, TEM and TG) showed that ZIF-67 and g-CN; ZIF-67, MOF-74(Ni) and g-CN; as well as ZIF-67, MIL-100(Fe) and g-CN successfully formed heterostructures. The series of catalytic degradation results showed that within 120 min, the degradation rate of VEN by ZMG achieved 100% and the mineralization rate reached 51.32%. The removal rate of VEN by ZNG was 91.38%, while that by ZG was only 27.75%. Free radical quenching tests and EPR further confirmed the production of OH and SO, which could be conducive to the degradation of VEN. The mechanism analysis of PMS activation confirmed that the interaction of Fe/Co was stronger than that of Ni/Co, and it was an important driving force to significantly enhance the synergistic effect. Finally, Gauss theory calculation and HPLC-MS/MS were used to analyze the intermediate products of VEN. It was verified that the main chemical reactions in the degradation process of VEN were hydroxylation, dehydration, demethylation and tertiary amine substitution.
基于单一金属有机骨架（MOF）复合催化剂 ZIF-67/g-CN（ZG），合成了具有双 MOF 的复合催化剂 ZIF-67/MOF-74（Ni）/g-CN（ZNG）和 ZIF-67/MIL-100（Fe）/g-CN（ZMG），用于有效激活过一硫酸盐（PMS）降解文拉法辛（VEN）。各种表征方法（XRD、FT-IR、Raman、SEM、EDS、TEM 和 TG）表明，ZIF-67 和 g-CN；ZIF-67、MOF-74（Ni）和 g-CN；以及 ZIF-67、MIL-100（Fe）和 g-CN 成功形成了异质结构。一系列催化降解结果表明，在 120 分钟内，ZMG 对 VEN 的降解率达到 100%，矿化率达到 51.32%。ZNG 对 VEN 的去除率为 91.38%，而 ZG 仅为 27.75%。自由基猝灭试验和 EPR 进一步证实了 OH 和 SO 的产生，这有利于 VEN 的降解。PMS 活化的机理分析证实，Fe/Co 的相互作用强于 Ni/Co，这是显著增强协同效应的重要动力。最后，使用高斯理论计算和 HPLC-MS/MS 分析了 VEN 的中间产物。验证了 VEN 降解过程中的主要化学反应是羟化、脱水、脱甲基和叔胺取代。
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