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铁氮掺杂生物炭催化剂的合成及对有机污染物去除和六价铬还原的性能研究。

Synthesis and characterization of iron-nitrogen-doped biochar catalysts for organic pollutant removal and hexavalent chromium reduction.

机构信息

Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Tunxi Road 193, Hefei 230009, China.

Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Tunxi Road 193, Hefei 230009, China.

出版信息

J Colloid Interface Sci. 2022 Mar 15;610:334-346. doi: 10.1016/j.jcis.2021.11.187. Epub 2021 Dec 1.

Abstract

Fe, N atoms deposited on porous biochar (Fe-N@BC) composites were synthesized and employed as an efficient catalyst for organic pollutant removal and Cr reduction. Naturally abundant, renewable and N-rich pomelo peel as a carbon and nitrogen source and unsubstituted phthalocyanine/iron phthalocyanine complexes as a Fe and nitrogen resource were used to develop the Fe-N@BC via a carbonization process. It is found that Fe-N@BC hybrids have homogeneous dispersion of Fe and N atoms on 3D hierarchically porous biochar, which significantly improves the performance toward the detoxification of organic pollutants using peroxymonosulfate as an oxidant, as well as the reduction of hexavalent chromium by formic acid as a reductant. Furthermore, the effects of Fe loading and pyrolytic temperature on catalysis were comprehensively analyzed and optimized. The excellent activity of Fe-N@BC in acid media can be attributed to the high dispersion of Fe species, high content of doped nitrogen as well as hierarchical micro-mesopores, which induce to expose more active sites for catalysis. Owing to the structure-enabled acidic stability, Fe-N@BC efficiently retains its activity as well as its structural stability after several cycles of reactions. This work provides a new approach to construct Fe, N-doped biochar as an effective catalyst for the detoxification of organic and inorganic pollutants.

摘要

Fe、N 原子负载在多孔生物炭(Fe-N@BC)复合材料上被合成,并作为一种高效的催化剂用于去除有机污染物和还原 Cr。柚子皮作为一种碳和氮源,天然丰富、可再生且富含氮,取代的酞菁/铁酞菁配合物作为 Fe 和氮的来源,通过碳化过程来开发 Fe-N@BC。研究发现,Fe-N@BC 杂化物在 3D 分级多孔生物炭上均匀分散了 Fe 和 N 原子,这显著提高了使用过一硫酸盐作为氧化剂解毒有机污染物的性能,以及使用甲酸作为还原剂还原六价铬的性能。此外,还综合分析和优化了 Fe 负载量和热解温度对催化的影响。Fe-N@BC 在酸性介质中具有优异的活性,可归因于 Fe 物种的高分散性、掺杂氮的高含量以及分级的微孔-介孔,这诱导了更多的催化活性位点的暴露。由于结构赋予的酸性稳定性,Fe-N@BC 在多次反应循环后仍能有效地保持其活性和结构稳定性。这项工作为构建 Fe、N 掺杂生物炭作为去除有机和无机污染物的有效催化剂提供了一种新方法。

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