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基于金属有机骨架的三元金属碳基催化剂用于电芬顿去除水中农药。

Trimetallic carbon-based catalysts derived from metal-organic frameworks for electro-Fenton removal of aqueous pesticides.

机构信息

Key Laboratory of Novel Materials for Sensor of Zhejiang Province, Institute of Advanced Magnetic Materials, Hangzhou Dianzi University, Hangzhou 310018, China; College of Environmental and Resource Science, Zhejiang University, Hangzhou 310058, China.

Linde+Robinson Laboratories California Institute of Technology, Pasadena, CA 91125, United States.

出版信息

Sci Total Environ. 2022 Apr 20;818:151747. doi: 10.1016/j.scitotenv.2021.151747. Epub 2021 Nov 23.

Abstract

Pesticide overuse has posed a threat to agricultural community as well as aquatic animals. Heterogeneous electro-Fenton (HEF) processes have received considerable attention for aqueous contaminants removal, and metal-organic frameworks (MOFs) serve as promising templates for fabrication of carbon-based HEF catalysts with low Fe leaching and enhanced stability. Herein, multimetallic MOF-derived HEF catalysts CMOFs@PCM have been demonstrated as efficient and stable HEF catalysts for aqueous pesticide degradation and mineralization. The porous carbon monolith (PCM) substrate effectively catalyzed 2-electron oxygen reduction reaction (ORR) over the pH range of 4-10 to in situ generate HO, which was then activated by the anchored FeO, FeC and NiO into OH for pesticide degradation. FeAlNi-CMOF@PCM achieved over 90% napropamide degradation within 60 min in the pH range of 4-10, and 96% degradation at neutral condition, 39% higher than monometallic CMIL-88(Fe)@PCM. Meanwhile, the embedded NiO and γ-AlO showed synergistic effect in promoting the catalytic activity of Fe sites, resulting in substantially enhanced performance of trimetallic FeAlNi-CMOF@PCM compared to the monometallic counterparts. On the other hand, the unique core-shell structure and FeC interlayer formed by co-pyrolyzing Fe-containing MOFs-NH with PCM greatly minimized the metal leaching and enhanced the stability of the electrocatalysts.

摘要

农药过度使用不仅对农业社区,而且对水生动物也构成了威胁。多相电芬顿(HEF)工艺因其对水污染物的去除而受到广泛关注,金属有机骨架(MOFs)作为制备基于碳的 HEF 催化剂的有前途的模板,具有低铁浸出和增强的稳定性。本文展示了多金属 MOF 衍生的 HEF 催化剂 CMOFs@PCM 作为高效且稳定的 HEF 催化剂,用于水中农药的降解和矿化。多孔碳整体式(PCM)基底有效地催化了 2 电子氧还原反应(ORR),在 pH 值为 4-10 的范围内原位生成 HO,然后被锚定的 FeO、FeC 和 NiO 激活为 OH 以降解农药。FeAlNi-CMOF@PCM 在 pH 值为 4-10 的范围内,在 60 分钟内实现了超过 90%的napropamide 降解,在中性条件下降解了 96%,比单金属 CMIL-88(Fe)@PCM 高 39%。同时,嵌入的 NiO 和 γ-AlO 协同促进了 Fe 位的催化活性,使得三金属 FeAlNi-CMOF@PCM 的性能相对于单金属催化剂有了显著提高。另一方面,通过共热解含 Fe 的 MOFs-NH 与 PCM 形成的独特核壳结构和 FeC 夹层大大减少了金属浸出并增强了电催化剂的稳定性。

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