Optimization of catalytic oxidation of trichloroethylene over Mn-Ce/HZSM-5 using response surface methodology

doi:10.16085/j.issn.1000-6613.2022-0089

Chemical Industry and Engineering Progress ›› 2022, Vol. 41 ›› Issue (11): 5830-5842.DOI: 10.16085/j.issn.1000-6613.2022-0089

• Industrial catalysis • Previous Articles Next Articles

Optimization of catalytic oxidation of trichloroethylene over Mn-Ce/HZSM-5 using response surface methodology

CHANG Tian¹^,²^,³^,⁴(), WANG Yu¹, ZHAO Zuotong¹, HU Jinchao¹, SHEN Zhenxing²()

^1.School of Environmental Science and Engineering, Shaanxi University of Science & Technology, Xi’an 710021, Shaanxi, China
^2.School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an 710049, Shaanxi, China
^3.State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, Ningxia, China
^4.State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, CAS, Xi’an 710049, Shaanxi, China

Received:2022-01-12 Revised:2022-05-20 Online:2022-11-28 Published:2022-11-25
Contact: SHEN Zhenxing

响应面法优化Mn-Ce/HZSM-5催化氧化三氯乙烯

常甜¹^,²^,³^,⁴(), 王宇¹, 赵作桐¹, 胡锦超¹, 沈振兴²()

^1.陕西科技大学环境科学与工程学院，陕西西安 710021
^2.西安交通大学能源与动力工程学院，陕西西安 710049
^3.省部共建煤炭高效利用与绿色化工国家重点实验室（宁夏大学），宁夏银川 750021
^4.中国科学院地球环境研究所黄土与第四纪地质国家重点实验室，陕西西安 710049

通讯作者: 沈振兴
作者简介:常甜（1988—），女，副教授，硕士生导师，研究方向为大气挥发性有机物监测与控制。E-mail：changtian@sust.edu.cn。
基金资助:
省部共建煤炭高效利用与绿色化工国家重点实验室开放课题(2022-K45);中国科学院地球环境研究所黄土与第四纪地质国家重点实验室开放课题(SKLLQG2129);陕西省自然科学基础研究计划(2022JQ-101)

Abstract

Abstract:

Trichloroethylene (TCE) is a widely used industrial raw material, but its emission seriously threatens the ecological environment and human health. How to efficiently remove TCE is still a crucial issue to be solved urgently. In this study, a series of Mn-Ce/HZSM-5 catalysts with different molar ratios of Ce/Mn were prepared by a deposition-precipitation method, and then used for the catalytic oxidation of TCE. The effects of various process parameters on the catalytic performance of the TCE decomposition were investigated using response surface methodology (RSM). The Mn-Ce/HZSM-5 catalyst demonstrated good catalytic activity for TCE decomposition, and MnCe_0.8/HZSM-5 catalyst exhibited the highest catalytic activity due to its high reducibility and abundant surface oxygen species. In addition, the RSM analysis results showed that temperature was the most significant factor affecting the TCE removal efficiency and CO₂ selectivity, followed by the gas flow rate and relative humidity (RH) in catalytic oxidation of TCE by MnCe_0.8/HZSM-5. The best TCE removal efficiency (77.1%) and CO₂ selectivity (70.0%) were acquired at a gas flow rate of 0.2L/min, temperature of 450℃ and RH of 16%. Moreover, the MnCe_0.8/HZSM-5 catalyst also showed good stability. The results provided an effective method for the removal of chlorinated volatile organic compounds.

Key words: Mn-Ce/HZSM-5 catalyst, trichloroethylene, reactivity, response surface methodology, optimization

摘要：

三氯乙烯（TCE）是用途广泛的工业原料，其排放严重威胁着生态环境和人体健康。如何高效去除TCE成为亟待解决的关键问题。本文采用沉积-沉淀法制备了一系列不同Ce/Mn摩尔比的Mn-Ce/HZSM-5催化剂，用于催化去除TCE，并用响应面分析的方法探究不同因素对TCE催化氧化过程的影响。结果表明：Mn-Ce/HZSM-5催化剂对TCE有较好的催化活性，当Ce/Mn摩尔比为0.8时催化活性最高，主要归因于该催化剂较高的还原性和丰富的表面氧物种。另外，响应面分析结果表明：在MnCe_0.8/HZSM-5催化氧化TCE过程中，温度是影响TCE去除率和CO₂选择性的最关键因素，其次是流量和相对湿度（RH）。当气体流量为0.2L/min、温度为450℃、RH为16%时，最优TCE去除率为77.1%，CO₂选择性为70.0%，且MnCe_0.8/HZSM-5催化剂表现出较好的稳定性。研究结果为含氯挥发性有机物的去除提供了一种有效方法。

关键词: Mn-Ce/HZSM-5催化剂, 三氯乙烯, 活性, 响应面法, 优化

CLC Number:

CHANG Tian, WANG Yu, ZHAO Zuotong, HU Jinchao, SHEN Zhenxing. Optimization of catalytic oxidation of trichloroethylene over Mn-Ce/HZSM-5 using response surface methodology[J]. Chemical Industry and Engineering Progress, 2022, 41(11): 5830-5842.

常甜, 王宇, 赵作桐, 胡锦超, 沈振兴. 响应面法优化Mn-Ce/HZSM-5催化氧化三氯乙烯[J]. 化工进展, 2022, 41(11): 5830-5842.

Figures/Tables 17

References 44

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自变量	因素	水平
自变量	因素	-2	-1	0	1	2
X₁	温度/℃	350	375	400	425	450
X₂	气体流量/L·min^-1	0.2	0.4	0.6	0.8	1
X₃	RH/%	0	10	20	30	40

自变量	因素	水平
自变量	因素	-2	-1	0	1	2
X₁	温度/℃	350	375	400	425	450
X₂	气体流量/L·min^-1	0.2	0.4	0.6	0.8	1
X₃	RH/%	0	10	20	30	40

催化剂	原子比Ce/Mn^①	BET/m²·g^-1	总孔容/cm³·g^-1	平均孔径/nm
HZSM-5	—	410.40	0.20	2.05
MnO _x /HZSM-5	—	252.50	0.26	4.20
MnCe_0.4O _x /HZSM-5	0.39	237.56	0.25	3.38
MnCe_0.8O _x /HZSM-5	0.81	232.50	0.23	3.34
MnCe_1.2O _x /HZSM-5	1.18	211.66	0.19	3.24
CeO₂/HZSM-5	—	243.72	0.23	3.36

催化剂	原子比Ce/Mn^①	BET/m²·g^-1	总孔容/cm³·g^-1	平均孔径/nm
HZSM-5	—	410.40	0.20	2.05
MnO _x /HZSM-5	—	252.50	0.26	4.20
MnCe_0.4O _x /HZSM-5	0.39	237.56	0.25	3.38
MnCe_0.8O _x /HZSM-5	0.81	232.50	0.23	3.34
MnCe_1.2O _x /HZSM-5	1.18	211.66	0.19	3.24
CeO₂/HZSM-5	—	243.72	0.23	3.36

催化剂	Mn⁴⁺/Mn	Mn³⁺/Mn	Ce³⁺/Ce⁴⁺	O_a/O_l
Mn/HZSM-5	0.24	0.48	—	3.4
MnCe_0.4/HZSM-5	0.18	0.44	0.16	3.43
MnCe_0.8/HZSM-5	0.20	0.51	0.21	3.78
MnCe_1.2/HZSM-5	0.17	0.43	0.12	2.86
Ce/HZSM-5	—	—	0.11	3.37

Optimization of catalytic oxidation of trichloroethylene over Mn-Ce/HZSM-5 using response surface methodology

响应面法优化Mn-Ce/HZSM-5催化氧化三氯乙烯

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Figures/Tables 17

References 44

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试验	自变量（X）			响应值（Y）
试验	温度（X₁）/°C	气体流量（X₂）/L·min^-1	RH（X₃）/%	TCE去除率（Y₁）/%	CO₂选择性（Y₂）/%
1	425	0.8	10	56.76	47.39
2	400	0.6	0	43.13	31.69
3	400	0.2	20	55.27	48.19
4	425	0.4	10	61.84	52.87
5	375	0.4	10	40.37	33.92
6	425	0.4	30	57.61	49.42
7	400	0.6	20	48.68	40.68
8	350	0.6	20	27.61	24.29
9	400	0.6	40	32.83	29.15
10	375	0.8	30	28.4	24.4
11	400	0.6	20	48.77	40.78
12	400	1	20	35.63	29.98
13	450	0.6	20	72.48	65.7
14	400	0.6	20	47.12	39.38
15	425	0.8	30	51.26	44.22
16	375	0.8	10	33.43	26.17
17	375	0.4	30	36.94	31.91
18	400	0.6	20	47.43	39.52
19	400	0.6	20	47.35	39.61
20	400	0.6	20	47.62	40.62

来源	平方和	自由度	均方	F值	p值	显著性
合计	2547.81	19
模型	2534.11	9	281.57	205.50	< 0.0001	显著
X₁	1981.81	1	1981.81	1446.38	< 0.0001	显著
X₂	273.82	1	273.82	199.84	< 0.0001	显著
X₃	94.04	1	94.04	68.63	< 0.0001	显著
X₁X₂	2.05	1	2.05	1.50	0.2493	不显著
X₁X₃	0.20	1	0.20	0.15	0.7093	不显著
X₂X₃	1.03	1	1.03	0.75	0.4063	不显著
X₁²	9.04	1	9.04	6.60	0.0280	显著
X₂²	7.58	1	7.58	5.53	0.0405	显著
X₃²	146.83	1	146.83	107.16	< 0.0001	显著
残差	13.70	10	1.37
失拟项	11.16	5	2.23	4.38	0.0653	不显著
纯误差	2.54	5	0.51

来源	平方和	自由度	均方	F值	p值	显著性
合计	2107.39	19
模型	2094.74	9	232.75	184.00	< 0.0001	显著
X₁	1606.41	1	1606.41	1269.94	< 0.0001	显著
X₂	243.05	1	243.05	192.14	< 0.0001	显著
X₃	14.98	1	14.98	11.84	0.0063	显著
X₁X₂	2.62	1	2.62	2.07	0.1805	不显著
X₁X₃	1.01	1	1.01	0.80	0.3930	不显著
X₂X₃	0.03	1	0.03	0.03	0.8734	不显著
X₁²	38.45	1	38.45	30.40	0.0003	显著
X₂²	1.46	1	1.46	1.15	0.3082	不显著
X₃²	145.67	1	145.67	115.16	< 0.0001	显著
残差	12.65	10	1.26
失拟项	10.49	5	2.10	4.85	0.0541	不显著
纯误差	2.16	5	0.43

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