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水体中的微污染物，包括真菌毒素、内分泌干扰素、药物分子等，对人类健康和生态环境具有巨大的威胁。生物降解技术，特别是酶降解法，是一种温和、高效的污染物降解技术。为了应对酶降解技术易失活、专一性过强及回收难等问题，本研究结合膜技术和多孔金属-有机骨架材料（MOFs）优势，制备了多种MOFs基膜材料，通过改善膜的吸附性能或利用MOFs的仿酶特性，使制得的生物/仿酶催化膜具有优异的去除效率、稳定性和普适性。主要研究内容如下：（1）开发了一种基于“3D修饰”策略的新型生物催化膜用于微污染物去除。通过荷电聚合物、MOFs和聚多巴胺涂层对聚丙烯腈超滤膜各部分的修饰，增强了膜对漆酶的固定能力。其中，荷电聚合物聚乙烯亚胺分子通过静电吸附固定化酶对膜的生物催化性能具有决定性作用，而MOFs的装载则通过改善酶的分布和减少酶泄露显著增强了膜的pH稳定性和循环使用性能。MOFs基生物催化膜不仅水通量高（渗透性达708 L m?2 h?1 bar?1）、微污染物去除效果好（92%）、稳定性好，同其他漆酶型生物催化膜相比，酶用量最少（0.63 U cm-2）。（2）制备了一种仿过氧化物酶MOFs基催化膜并首次用于黄曲霉毒素B1（AFB1）的去除。仿酶MOFs因其不同的空间结构和元素价态组成，在AFB1去除过程中显示出截然不同的吸附和催化性能。同时，仿酶MOFs还具有优异的抗干扰能力。经仿酶MOFs脱毒后，AFB1主要的毒性基团被破坏，脱毒产物不再对小鼠肝细胞造成损伤。此外，仿酶MOFs能够被装载在超滤膜内，可根据实际需要选择不同的操作模式，具有优异的稳定性。（3）开发了一种全新的“仿酶MOFs-介体体系（PLMMS）”用于微污染物去除。利用仿酶MOFs的结构特性和催化特性将活性介体可控的限域固定在MOFs骨架内并促进其转化再生，实现了对AFB1的超高效去除（10 min，90%）和对双酚A及双氯芬酸的高效去除。通过原位合成法制得新型仿酶MOFs基催化膜，操作简便，循环性能优异。本论文的研究对于提高生物/仿生催化膜在水体微污染物处理领域的效率、稳定性和普适性等方面具有积极的指导作用。;Organic micropollutants in water and food, including mycotoxins, endocrine disrupting chemicals, drug molecules, etc., have great harms to human health and ecological environment. Biodegradation technology, especially enzymatic degradation technology, is mild, efficient and harmless. However, the instability, excessive specificity and difficulty in reusability restrict its applications. To solve these problems, we combined the advantages of membrane technology and porous metal-organic framework materials (MOFs), and prepared a series of MOFs-based membranes to enhance their adsorption or biomimetic catalysis ability, thus resulting in good stability, reusability and high efficiency in the removal of micropollutants.(1) A “3D modification” strategy was developed to prepare a novel biocatalytic membrane for removal of micropollutants. The separation layer, support layer and non-woven layer of polyacrylonitrile membrane were modified by charged polymer, MOFs and polydopamine coating. After laccase immobilization, a high-throughput biocatalytic membrane was prepared for micropollutants removal. It was found that the molecular weight of polyethyleneimine played a decisive role in the biocatalytic performance of membranes due to the difference in electrostatic adsorption, while the loading of MOFs significantly enhanced the pH stability and recycling performance of membranes attributed to the enzyme distribution improvement and enzyme leakage reduction. Compared with other biocatalytic membranes with laccase, this biocatalytic membrane had the highest bisphenol A (BPA) removal efficiency (91%) and the lowest enzyme dosage (0.63 U cm-2), accompanied by high permeability (708 L m?2 h?1 bar?1) and stability.(2) Peroxidase-like MOFs-based catalytic membrane was prepared for removal of aflatoxin B1(AFB1) for the first time. Different MOFs had distinct adsorption and catalytic properties due to their different crystal/pore structure and element valence. Those MOFs could resist interference from nutrients in food during mycotoxin removal. After detoxification by the peroxidase-like MOFs, the main toxic group of AFB1 was destroyed, and the detoxification product no longer caused damage to mouse hepatocytes. The catalytic membranes with biomimetic MOFs could remove AFB1 through "adsorption-regeneration mode" and " synergetic removal mode" respectively, which both had high stability.(3) A novel "peroxidase-like MOFs-mediator (PLMMS)" system was developed for rapid and repeatable removal of micropollutants. Based on the structural and catalytic properties of MOFs, we confined the active mediator into MOFs by a controllable way. The ultra-fast removal of AFB1 (10 min, 90%) as well as the efficient removal of BPA and diclofenac were realized. In addition, PLMMS-base membrane was synthesized by in-situ growth method, which showed a good reusability in AFB1 removal.These works play an active role in improving the efficiency, stability and universality of biocatalytic/biomimetic membrane in the removal of aqueous micropollutant.
|任重远. 金属有机骨架基生物/仿生催化膜及其微污染物去除研究[D]. 中国科学院大学,2020.|
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