Research progress of zeolite for VOCs removal

doi:10.16085/j.issn.1000-6613.2022-1947

Abstract

Abstract:

Adsorption coupled with catalytic oxidation is the most efficient, economical and environmentally friendly method to remove volatile organic compounds (VOCs) at present. Zeolite possesses large specific surface area, regular microporous channel and stable structure. Therefore, zeolite has important application value in the removal of industrial VOCs as adsorbent and catalyst. This paper summarizes the rules of VOCs adsorption by zeolites and the effects of microstructure and surface properties of zeolites on the catalytic oxidation of VOCs in recent years. The key factors affecting the adsorption of VOCs include the zeolite topology and its cation type, pore multipolarization, and hydrophobicity. Zeolite catalysts loaded with noble/non-noble metals are mainly discussed. The key points to obtain efficient catalysts are: effective controlling the particle size of metal species on the zeolite carrier of suitable structure and morphology, regulating the chemical state of active species and their interactions with zeolite carriers and understanding deeply the influence of zeolite microstructure, active species status and other factors on the catalytic performance.

Key words: volatile organic compounds (VOCs), zeolites, catalyst, adsorption, catalytic oxidation

摘要：

目前，吸附及催化氧化技术是去除挥发性有机化合物（VOCs）最为高效、经济、环境友好的方法。分子筛具有较大的比表面积、规整的微孔孔道和稳定的结构，因此其作为吸附剂及催化剂在工业VOCs的去除过程中有重要的应用价值。本文总结了近年来分子筛吸附VOCs的规律性研究以及分子筛微结构和表面性质对催化氧化的影响。其中影响吸附VOCs的关键因素包括分子筛拓扑结构、阳离子类型、孔道多极化、亲疏水性等；针对催化氧化技术，主要讨论了负载贵金属/非贵金属的分子筛催化剂，其中获得高效催化氧化VOCs催化剂的关键在于以下几个方面：以结构形貌适宜的分子筛载体为基础，构建有效调控金属物种粒子尺寸的制备方法；调控活性物种的化学状态及其与分子筛载体的相互作用；深入理解分子筛微结构、活性物种的状态等因素对催化性能的影响。

关键词: 挥发性有机化合物, 分子筛, 催化剂, 吸附, 催化氧化

CLC Number:

O643.3

GE Yafen, SUN Yu, XIAO Peng, LIU Qi, LIU Bo, SUN Chengying, GONG Yanjun. Research progress of zeolite for VOCs removal[J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4716-4730.

葛亚粉, 孙宇, 肖鹏, 刘琦, 刘波, 孙成蓥, 巩雁军. 分子筛去除VOCs的研究进展[J]. 化工进展, 2023, 42(9): 4716-4730.

Figures/Tables 11

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拓扑结构	分子筛	Si/Al	比表面积/m²·g^-1	VOCs	吸附容量/mmol·g^-1	相对湿度/%	吸附温度/℃	文献
MFI	Silicate-1	∞	377	正己烷	1.30	0	25	[20]
MFI	Silicate-1	∞	377	丙酮	1.82	0	25	[20]
MFI	Silicate-1	∞	377	对二甲苯	1.28	0	25	[20]
*BEA	Beta	—	493	正己烷	1.23	0	25	[20]
*BEA	Beta	—	493	丙酮	2.15	0	25	[20]
*BEA	Beta	—	493	对二甲苯	1.17	0	25	[20]
STT	SSZ-23	—	536	正己烷	1.13	0	25	[20]
STT	SSZ-23	—	536	丙酮	2.43	0	25	[20]
STT	SSZ-23	—	536	对二甲苯	0.97	0	25	[20]
CHA	Chabazite	—	803	正己烷	0.18	0	25	[20]
CHA	Chabazite	—	803	丙酮	0.10	0	25	[20]
CHA	Chabazite	—	803	对二甲苯	0.04	0	25	[20]
FAU	NaX	1.1	938	甲苯	2.75	0	30	[24]
FAU	USY	23.7	893	甲苯	1.99	0	30	[24]
MFI	Silicate-1	∞	365	甲苯	1.49	0	30	[24]
FAU	NaY	2.5	758	正己烷	1.25	0	30	[25]
*BEA	Beta	412.0	781	甲苯	4.13	30	35	[26]
FAU	NaY	5.42	888	甲苯	3.2	0	25	[27]
FAU	USY	100	646	甲苯	0.93	0	—	[28]
FAU	USY	100	646	甲苯	0.36	40	—	[28]
MFI	ZSM-5	400	364	甲苯	0.69	0	—	[28]
MFI	ZSM-5	400	364	甲苯	0.48	40	—	[28]

拓扑结构	分子筛	Si/Al	比表面积/m²·g^-1	VOCs	吸附容量/mmol·g^-1	相对湿度/%	吸附温度/℃	文献
MFI	Silicate-1	∞	377	正己烷	1.30	0	25	[20]
MFI	Silicate-1	∞	377	丙酮	1.82	0	25	[20]
MFI	Silicate-1	∞	377	对二甲苯	1.28	0	25	[20]
*BEA	Beta	—	493	正己烷	1.23	0	25	[20]
*BEA	Beta	—	493	丙酮	2.15	0	25	[20]
*BEA	Beta	—	493	对二甲苯	1.17	0	25	[20]
STT	SSZ-23	—	536	正己烷	1.13	0	25	[20]
STT	SSZ-23	—	536	丙酮	2.43	0	25	[20]
STT	SSZ-23	—	536	对二甲苯	0.97	0	25	[20]
CHA	Chabazite	—	803	正己烷	0.18	0	25	[20]
CHA	Chabazite	—	803	丙酮	0.10	0	25	[20]
CHA	Chabazite	—	803	对二甲苯	0.04	0	25	[20]
FAU	NaX	1.1	938	甲苯	2.75	0	30	[24]
FAU	USY	23.7	893	甲苯	1.99	0	30	[24]
MFI	Silicate-1	∞	365	甲苯	1.49	0	30	[24]
FAU	NaY	2.5	758	正己烷	1.25	0	30	[25]
*BEA	Beta	412.0	781	甲苯	4.13	30	35	[26]
FAU	NaY	5.42	888	甲苯	3.2	0	25	[27]
FAU	USY	100	646	甲苯	0.93	0	—	[28]
FAU	USY	100	646	甲苯	0.36	40	—	[28]
MFI	ZSM-5	400	364	甲苯	0.69	0	—	[28]
MFI	ZSM-5	400	364	甲苯	0.48	40	—	[28]

催化剂	VOCs	T₅₀/℃	T₉₀/℃	VOCs浓度/μL·L^-1	反应流速/mL·min^-1	空速/mL·g^-1·h^-1	参考文献
10%Co/MCM-22	甲苯	293	307	1000	100	60000	[15]
PdCu/ZSM-5	甲苯	—	152	50	30	36000	[16]
Cu-ZSM-5	正丁胺	—	279	375	100	12000	[57]
Cu-Hβ	正丁胺	163	340	375	100	12000	[57]
Cu-SAPO-34	正丁胺	275	330	375	100	12000	[57]
Cu-MCM-22	正丁胺	177	280	375	100	12000	[57]
Co₃O₄/HZSM-5/β-CD	甲苯	281	288	—	100	15000	[58]
Co₃O₄/ZSM-5	二氯甲烷	—	370	1000	100	30000	[58]
MnO _x /HZSM-5	甲苯	245	255	—	100	15000	[61]
Pt/CsZSM-5-60	甲苯	167	170	1000	100	60000	[67]
Pt/ZSM-5	甲苯	147	155	1000	100	60000	[68]
Pd₃@Beta	甲苯	169	—	1000	100	60000	[69]
PtMn_0.2@ZSM5	甲苯	160	175	800	50	30000	[72]
Pt@ZSM-5	甲苯	201	—	1000	100	60000	[79]

催化剂	VOCs	T₅₀/℃	T₉₀/℃	VOCs浓度/μL·L^-1	反应流速/mL·min^-1	空速/mL·g^-1·h^-1	参考文献
10%Co/MCM-22	甲苯	293	307	1000	100	60000	[15]
PdCu/ZSM-5	甲苯	—	152	50	30	36000	[16]
Cu-ZSM-5	正丁胺	—	279	375	100	12000	[57]
Cu-Hβ	正丁胺	163	340	375	100	12000	[57]
Cu-SAPO-34	正丁胺	275	330	375	100	12000	[57]
Cu-MCM-22	正丁胺	177	280	375	100	12000	[57]
Co₃O₄/HZSM-5/β-CD	甲苯	281	288	—	100	15000	[58]
Co₃O₄/ZSM-5	二氯甲烷	—	370	1000	100	30000	[58]
MnO _x /HZSM-5	甲苯	245	255	—	100	15000	[61]
Pt/CsZSM-5-60	甲苯	167	170	1000	100	60000	[67]
Pt/ZSM-5	甲苯	147	155	1000	100	60000	[68]
Pd₃@Beta	甲苯	169	—	1000	100	60000	[69]
PtMn_0.2@ZSM5	甲苯	160	175	800	50	30000	[72]
Pt@ZSM-5	甲苯	201	—	1000	100	60000	[79]

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