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用于处理哌嗪废水的FeMnCe活化半焦催化剂的湿式催化氧化

Wet Catalytic Oxidation of a FeMnCe-Activated Semi-Coke Catalyst for Treating Piperazine Wastewater.

作者信息

Ren Kaiwen, Liu Shuo, Dong Zhiyu, Wang Junfeng

机构信息

College of Mining and Technology, Taiyuan University of Technology, Taiyuan 030024, China.

School of Safety and Emergency Management Engineering, Taiyuan University of Technology, Taiyuan 030024, China.

出版信息

ACS Omega. 2023 Feb 22;8(9):8683-8694. doi: 10.1021/acsomega.2c08074. eCollection 2023 Mar 7.

Abstract

A FeMnCe-activated semi-coke catalyst (FeMnCe/ASC) was prepared by the co-precipitation method using semi-coke as the raw material. The structure and morphology were characterized by X-ray diffraction, Brunauer-Emmett-Teller, scanning electron microscopy, and transmission electron microscopy analyses. The catalytic activity and stability of the FeMnCe/ASC catalyst were investigated with piperazine as the target degradation pollutant and ammonia nitrogen and chemical oxygen demand (COD) as the evaluation indexes. The results showed that the average pore size of FeMnCe/ASC mesopores was 6.68 nm, and the active components were uniformly dispersed on the carrier surface. Under the optimum conditions of piperazine solution including a mass concentration of 100 mg/L, a catalyst mass concentration of 4.0 g/L, a reaction temperature of 240 °C, an oxygen partial pressure of 1.2 MPa, a stirring speed of 500 rpm, and a reaction time of 120 min, the degradation rates of both ammonia nitrogen and COD reached 100%. After the catalyst was recycled five times, the degradation rates of ammonia nitrogen and COD still reached more than 90%. The elemental valence changes before and after the reaction were analyzed by X-ray photoelectron spectroscopy, and the intermediate products generated from piperazine degradation were analyzed by gas chromatography-mass spectroscopy to evaluate the mechanism of piperazine degradation and speculate about the degradation pathway of piperazine.

摘要

以半焦为原料,采用共沉淀法制备了FeMnCe活化半焦催化剂(FeMnCe/ASC)。通过X射线衍射、布鲁诺尔-埃米特-泰勒法、扫描电子显微镜和透射电子显微镜分析对其结构和形貌进行了表征。以哌嗪为目标降解污染物,以氨氮和化学需氧量(COD)为评价指标,研究了FeMnCe/ASC催化剂的催化活性和稳定性。结果表明,FeMnCe/ASC介孔的平均孔径为6.68nm,活性组分均匀分散在载体表面。在哌嗪溶液质量浓度为100mg/L、催化剂质量浓度为4.0g/L、反应温度为240℃、氧分压为1.2MPa、搅拌速度为500rpm、反应时间为120min的最佳条件下,氨氮和COD的降解率均达到100%。催化剂循环使用5次后,氨氮和COD的降解率仍达到90%以上。通过X射线光电子能谱分析反应前后元素价态变化,采用气相色谱-质谱联用仪分析哌嗪降解产生的中间产物,以评价哌嗪的降解机理并推测哌嗪的降解途径。

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