煤气化细渣负载CoO活化PMS高效降解双酚A

doi:10.16085/j.issn.1000-6613.2022-2276

化工进展 ›› 2023, Vol. 42 ›› Issue (11): 5993-6004.DOI: 10.16085/j.issn.1000-6613.2022-2276

• 资源与环境化工 • 上一篇

煤气化细渣负载CoO活化PMS高效降解双酚A

焦路畅¹(), 卫月星¹, 张禹洵¹, 秦育红¹(), 崔丽萍¹, 燕可洲², 郭舒岗³, 申浩楠¹, 贺冲¹

^1.太原理工大学环境科学与工程学院，山西太原 030024
^2.山西大学国家环境保护煤炭废弃物资源化高效利用重点实验室，山西太原 030006
^3.山西省疾病预防控制中心，山西太原 030012

收稿日期:2022-12-07 修回日期:2023-02-08 出版日期:2023-11-20 发布日期:2023-12-15
通讯作者: 秦育红
作者简介:焦路畅（1999—），女，硕士研究生，研究方向为工业固废的资源化应用。E-mail：jiaoluchang1087@link.tyut.edu.cn。
基金资助:
国家自然科学基金(22206149);山西省应用基础研究项目(20210302124220)

Coal gasification fine slag supported CoO catalyst for the efficient degradation of bisphenol A by activating peroxymonosulfate process

JIAO Luchang¹(), WEI Yuexing¹, ZHANG Yuxun¹, QIN Yuhong¹(), CUI Liping¹, YAN Kezhou², GUO Shugang³, SHEN Haonan¹, HE Chong¹

^1.College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^2.National Key Laboratory of Environmental Protection and Efficient Utilization of Coal Waste Resources, Shanxi University, Taiyuan 030006, Shanxi, China
^3.Shanxi Provincial Center for Disease Control and Prevention, Taiyuan 030012, Shanxi, China

Received:2022-12-07 Revised:2023-02-08 Online:2023-11-20 Published:2023-12-15
Contact: QIN Yuhong

摘要/Abstract

摘要：

以航天炉煤气化细渣（FS）为载体，对其经简单水洗后，通过超声浸渍法在其表面负载CoO制备了分散性良好的煤气化细渣负载型复合催化剂CoO@FSC，并将其用于活化过氧化单硫酸盐（PMS）高效降解含双酚A（BPA）废水。结果表明，CoO颗粒均匀分布在细渣表面，避免了金属氧化物在实际催化降解过程中的聚集，为活化PMS提供了更多的活性位点。所制备催化剂CoO@FSC可在30℃、催化剂投加量0.2g/L、PMS投加量6mmol/L、BPA浓度50mg/L的条件下，25min内实现BPA的完全降解，且降解过程可以适应从弱酸到碱性基质的广泛pH范围。通过自由基淬灭实验发现，BPA的催化降解路径中的主要活性物质为¹O₂和·O $2 -$ 。CoO@FSC在活化PMS降解BPA方面表现出的良好性能，证明了煤气化细渣在有机污染物去除中的应用潜力，为后续进一步实现煤气化细渣的资源化应用提供了理论依据。

关键词: 煤气化细渣, 活化, 过氧化单硫酸盐, 催化, 降解

Abstract:

The resource application of coal gasification fine slag is an important way to achieve the “carbon peaking and carbon neutrality” in China. In this study, the coal gasification fine slag (FS) obtained from Space Furnace was used as the catalyst carrier after simple water washing and ultrasonic impregnation to prepare CoO@FSC with well dispersion. The as-prepared catalyst was used to activate peroxide single sulfate (PMS) for the efficient degradation of wastewater containing bisphenol A (BPA). The results showed that the CoO particles were uniformly distributed on the surface of the fine slag, which avoided the accumulation of metal oxides in the actual catalytic degradation process and thus provided more active sites for activating PMS. BPA could be completely degraded within 25 minutes by CoO@FSC under the conditions of 30℃, 0.2g/L catalyst dosage, 6mmol/L PMS dosage and 50mg/L BPA concentration and the degradation could be effective a wide pH range from weak acid to alkaline substrate. The free radical quenching experiment confirmed that the main active substances in the BPA catalytic degradation process were ¹O₂ and ·O $2 -$ . The good catalytic performance of CoO@FSC demonstrated the potential application of coal gasification fine slag in the degradation of organic pollutants, and provided a theoretical basis for its further utilization.

Key words: coal gasification fine slag, activation, peroxide monosulfate, catalysis, degradation

中图分类号:

X752

焦路畅, 卫月星, 张禹洵, 秦育红, 崔丽萍, 燕可洲, 郭舒岗, 申浩楠, 贺冲. 煤气化细渣负载CoO活化PMS高效降解双酚A[J]. 化工进展, 2023, 42(11): 5993-6004.

JIAO Luchang, WEI Yuexing, ZHANG Yuxun, QIN Yuhong, CUI Liping, YAN Kezhou, GUO Shugang, SHEN Haonan, HE Chong. Coal gasification fine slag supported CoO catalyst for the efficient degradation of bisphenol A by activating peroxymonosulfate process[J]. Chemical Industry and Engineering Progress, 2023, 42(11): 5993-6004.

图/表 11

表1 FS的化学组成及含量

组分	质量分数/%
SiO₂	31.28
Fe₂O₃	28.15
Al₂O₃	15.84
SO₃	4.04
CaO	13.65
TiO₂	1.73
K₂O	1.73
P₂O₅	1.06
Na₂O	0.87
Cl	0.58
MgO	0.59
ZrO₂	0.18
SrO	0.14
MnO	0.09
ZnO	0.07

表2 FS及FSC的比表面积、孔结构和孔径

样品	S_BET/m²·g^-1	孔体积/cm³·g^-1	平均孔径/nm
FS	1.688	0.001	2.736
FSC	32.726	0.026	3.178

图1 FSC的SEM图像和EDS图谱

表3 FSC的有机元素分析

元素	质量分数/%
N	0.21
C	21.02
H	0.24
S	3.44

图2 CoO@FSC的SEM图像和EDS图谱

图3 FSC和CoO@FSC的XRD谱图、Raman谱图和FTIR谱图

图4 不同催化剂/PMS体系降解BPA效果对比实验条件：[BPA]0=20mg/L，[PMS]0=4mmol/L，[FS]0=0.1g/L，T=30℃，初始pH=6.0[FSC]0=0.1g/L，[CoO]0=0.1g/L，[ACF]0=0.1g/L，[CoO@FSC]0=0.1g/L，

图5 不同影响因素对CoO@FSC /PMS体系降解BPA的影响实验条件：[BPA]0=50mg/L，[PMS]0=6mmol/L，[CoO@FSC]0=0.2/0.5g/L，T=30℃，初始pH=6.0

图6 反应后CoO@FSC的SEM图像和EDS图谱

图7 CoO@FSC反应前后的XPS总谱图和分谱图

图8 BPA降解过程中主要自由基的作用实验条件：[BPA]0=50mg/L，[PMS]0=6mmol/L，[CoO@FSC]0=0.2g/L，T=30℃，初始pH=6.0，[EtOH]0=0.4mol/L，[TBA]0=0.4mol/L，[p-BQ]0=0.1mol/L，[FFA]0=0.2mol/L

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煤气化细渣负载CoO活化PMS高效降解双酚A

Coal gasification fine slag supported CoO catalyst for the efficient degradation of bisphenol A by activating peroxymonosulfate process

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