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定制碳微球中铁纳米颗粒的组装以实现高性能电催化反硝化

Tailoring the Assembly of Iron Nanoparticles in Carbon Microspheres toward High-Performance Electrocatalytic Denitrification.

作者信息

Su Li, Han Dandan, Zhu Guanjia, Xu Hui, Luo Wei, Wang Lianjun, Jiang Wan, Dong Angang, Yang Jianping

机构信息

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering , Donghua University , Shanghai 201620 , China.

Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and Department of Chemistry , Fudan University , Shanghai 200433 , China.

出版信息

Nano Lett. 2019 Aug 14;19(8):5423-5430. doi: 10.1021/acs.nanolett.9b01925. Epub 2019 Aug 1.

Abstract

Electrocatalytic denitrification is considered as the most promising technology to transform nitrates to nitrogen gas in sewage so far. Although noble metal-based catalysts as a cathode material have reached decent removal capacity of nitrate, the high cost is the main hamper of electrocatalytic reduction. Therefore, the development of alternative catalysis toward highly effective denitrification is imperative yet still remains a significant challenge. Herein, a corchorifolius-like structure, where Fe nanoparticles are sealed in carbon microspheres (CL-Fe@C) with a rough surface, has been elaborately designed by self-assemble strategy. Impressively, the architectured CL-Fe@C microspheres are surrounded with a lot of small iron nanoparticles and contain the high iron content of ∼74%. As a result, an excellent removal capacity of 1816 mg N/g Fe and a high nitrogen selectivity of 98% under a very low nitrate concentration of 100 mg/L are achieved when using the CL-Fe@C microspheres as electrocatalytic denitrification. The present work not only explores high performance electrocatalysis for the denitrification but also promote new inspiration for the preparation of other iron-based functional materials for diverse applications.

摘要

电催化反硝化被认为是目前将污水中的硝酸盐转化为氮气最具前景的技术。尽管基于贵金属的催化剂作为阴极材料已达到相当不错的硝酸盐去除能力,但高成本是电催化还原的主要阻碍。因此,开发用于高效反硝化的替代催化剂势在必行,但仍然是一项重大挑战。在此,通过自组装策略精心设计了一种类似苘麻叶的结构,其中铁纳米颗粒被封装在具有粗糙表面的碳微球(CL-Fe@C)中。令人印象深刻的是,这种结构化的CL-Fe@C微球被许多小铁纳米颗粒包围,并且含有约74%的高铁含量。结果,当使用CL-Fe@C微球进行电催化反硝化时,在极低的100 mg/L硝酸盐浓度下实现了1816 mg N/g Fe的优异去除能力和98%的高氮选择性。本工作不仅探索了用于反硝化的高性能电催化,还为制备用于各种应用的其他铁基功能材料提供了新的灵感。

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