Separation and Purification Technology ( IF 8.1 ) Pub Date : 2022-09-17 , DOI: 10.1016/j.seppur.2022.122145 Mingya Yao , Meng Xie , Shiyong Zhang , Jinpeng Yuan , Lingxi Zhao , Ru-Song Zhao
In this work, new covalent organic framework (COF) materials with high crystallinity and large specific surface areas were used as cobalt-loaded supports. Cobalt nanoparticle-embedded nitrogen-doped carbon porous catalysts (Co@COF) were obtained by high-temperature pyrolysis of the COF materials and cobalt salts. With multiple active sites (Co0, pyridine N, and graphitic N), Co@COF exhibited superior catalytic properties for peroxymonosulfate (PMS) activation toward the degradation of sulfamerazine (SMZ). The efficiency of SMZ degradation reached 92.4 % within 10 min and the total organic carbon (TOC) removal rate reached 70.3 % within 30 min. Using radical quenching experiments and electron paramagnetic resonance (EPR) analysis, sulfate radicals (SO4•−), hydroxyl radicals (•OH), and singlet oxygen (1O2) were identified in this system, while 1O2 was the dominant active species for SMZ removal. The degradation intermediates of SMZ in Co@COF/PMS were monitored by high performance liquid chromatography–time of flight mass spectrometry (HPLC–TOFMS).
中文翻译:
钴纳米粒子包裹在氮掺杂纳米碳中,衍生自钴改性的共价有机骨架作为过氧单硫酸盐活化剂用于磺胺嘧啶降解
在这项工作中,具有高结晶度和大比表面积的新型共价有机骨架(COF)材料被用作载钴载体。通过COF材料和钴盐的高温热解获得钴纳米颗粒嵌入的氮掺杂碳多孔催化剂(Co@COF)。Co@COF具有多个活性位点(Co 0、吡啶 N 和石墨 N),在过氧单硫酸盐(PMS)活化对磺胺嘧啶(SMZ)降解方面表现出优异的催化性能。SMZ降解效率在10分钟内达到92.4%,总有机碳(TOC)去除率在30分钟内达到70.3%。使用自由基猝灭实验和电子顺磁共振 (EPR) 分析,硫酸根 (SO 4 •−)、羟基自由基( • OH) 和单线态氧( 1 O 2 ) 在该系统中被识别出来,而1 O 2是去除SMZ 的主要活性物质。通过高效液相色谱-飞行时间质谱 (HPLC-TOFMS) 监测 SMZ 在 Co@COF/PMS 中的降解中间体。