Research progress of passive NOx adsorbent in diesel vehicle for cold start emission control

doi:10.16085/j.issn.1000-6613.2021-0295

Abstract

Abstract:

Vehicle exhaust is one of the most important sources of NO_x emission. However, the common NO_x reduction techniques of diesel vehicle exhaust have poor performance during the cold start, so passive NO_x adsorbent (PNA) has been proposed. PNA can adsorb NO_x at low temperature and desorb NO_x at high temperature, then the released NO_x is thoroughly purified by downstream NO_x treatment unit, such as selective catalytic reduction (SCR) or storage reduction (NSR). This review summarizes the recent progress of PNA materials for NO_x purification during cold start at low temperature, and compares the structure and properties of different types of PNA materials. Among them, Pd/zeolites show good NO_x adsorption-desorption performance at low temperature, high sulfur resistance and hydrothermal stability. Further, Pd/zeolites are discussed in depth, including the NO_x storage mechanism and the influence factors. Finally, the problems of PNA in the low-temperature adsorption-desorption of NO_x are analyzed and the prospects are also outlooked. It is pointed out that increasing the number of NO_x adsorption sites with excellent water resistance and the Pd species dispersion are the important prerequisites for the development of high-performance PNA.

Key words: passive NO_x adsorbent, cold start (PNA), adsorption, desorption, influence factors

摘要：

机动车尾气是氮氧化物（NO_x）重要来源之一，常见柴油车尾气NO_x处理技术对冷启动阶段NO_x减排效果较差，被动NO_x吸附剂（PNA）应运而生。PNA可低温吸附存储NO_x、高温脱附释放NO_x，释放的NO_x经过下游NO_x处理单元[选择性催化还原（SCR）或NO_x储存还原（NSR）]被彻底净化。本文综述了近年来PNA材料在低温冷启动过程中净化NO_x的研究进展，对不同类型PNA材料进行结构及性能比对，其中Pd/分子筛表现出良好的低温NO_x吸附-脱附性能、抗硫性以及水热稳定性，成为PNA优选。深入讨论了Pd/分子筛存储NO_x机制以及影响因素。此外，分析了PNA在低温吸附-脱附NO_x中面临的问题并展望其前景，指出提高具有优异抗水性能的NO_x吸附位点数量及Pd物种分散程度是开发高性能PNA的重要前提。

关键词: 被动NO_x吸附剂, 冷启动, 吸附, 脱附, 影响因素

CLC Number:

X511

PAN Rouxing, YU Qingjun, TANG Xiaolong, YI Honghong, GAO Fengyu, ZHAO Shunzheng, ZHOU Yuansong, LIU Yuanyuan. Research progress of passive NO_x adsorbent in diesel vehicle for cold start emission control[J]. Chemical Industry and Engineering Progress, 2022, 41(1): 400-417.

潘柔杏, 于庆君, 唐晓龙, 易红宏, 高凤雨, 赵顺征, 周远松, 刘媛媛. 被动NO_x吸附剂在柴油车冷启动排放控制中的研究进展[J]. 化工进展, 2022, 41(1): 400-417.

Figures/Tables 14

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载体	金属	负载量（质量分数）/%	存储温度/℃	存储性能（NSE值或NO_x/Pd）	释放性能（NDE值或温度范围）	参考文献
CeO₂	Pt	1~2	80~120	NSE约40%	<350℃，NDE约20% 350~500℃	［25-26］
	Pd	1~2	80~120	NSE 25%~50%	<350℃，NDE约40% 180~500℃	［8，25-28］
	Pd-Pt	1-1	80	—	280~500℃	［26］
Al₂O₃	Pt	0.43g/L 2	80~200	NSE约37%	380~500℃	［26，37］
	Pd	0.43g/L 2	80~200	NSE约14%	150~350℃	［26，37］
	Pt-La	1-1	80~160	NSE 60%~90%	250~500℃，NDE约60%	［31］
	Pd-Pt	1-1	80	—	150~500℃	［26］
	Ag	1.3	120	NSE约50%	250~470℃	［34］
ZrO₂	Pd	1	120	NSE约33%	<350℃，NDE约70%	［43］
ZrO₂	—	—	—	NSE约10.5%	<350℃，释放量与吸附量相当	［43］
CeO₂-Pr₂O₃	Pt	1	120	NSE约68%	<350℃，NDE约40%	［35］
CeO₂-Pr₂O₃	Pd	1	120	NSE约50%	<350℃，NDE约41%	［35］
CeO₂-ZrO₂	Pt	1	120	NSE约70%	<350℃，NDE约60%	［39］
	Pd	1~2	80~120	NSE约20%	<350℃，NDE约80% 250~500℃	［27，39］
	Pt-Pd	0.5-0.5	120	NSE约50%	<350℃，NDE约70%	［39］
CeO₂-Al₂O₃	Pt	2.3	80	NSE约10%	300~400℃	［36］
CeO₂-Al₂O₃	Pd	2.3	80	NSE约5%	100~200℃	［36］
WO₃-ZrO₂	Pd	1	120	NSE约80%	<350℃，NDE约100%	［43］
WO₃-ZrO₂	—	—	—	NSE约0	<350℃，释放量与吸附量相当	［43］
SSZ-13	Pd	1~2	80~120	NSE约90% NO_x/Pd 0.41	250~450℃	［8，28，48，56］
SSZ-13	Co	—	100	NSE约96%	250~400℃	［50］
Beta	Pd	1	100	NSE约90%	200~450℃	［8］
Beta	CaO	10	40	NO_x穿透时间102min	500~550℃	［49］
ZSM-5	Pd	0~2	50~150	NSE约90% NO_x/Pd 0.3~0.83	200~450℃	［8，55，60］
LTA	Pd	1.4	80	NO_x/Pd 0.52	300~400℃	［48］
SSZ-39	Pd	0.7	100	NSE约90%	230~350℃	［47］
FER	Pd	1.8	100	NO_x/Pd 0.9	200~300℃	［59］
MCM-22	Pd	1.22	100	NO_x/Pd 0.55	180~300℃	［55］

载体	金属	负载量（质量分数）/%	存储温度/℃	存储性能（NSE值或NO_x/Pd）	释放性能（NDE值或温度范围）	参考文献
CeO₂	Pt	1~2	80~120	NSE约40%	<350℃，NDE约20% 350~500℃	［25-26］
	Pd	1~2	80~120	NSE 25%~50%	<350℃，NDE约40% 180~500℃	［8，25-28］
	Pd-Pt	1-1	80	—	280~500℃	［26］
Al₂O₃	Pt	0.43g/L 2	80~200	NSE约37%	380~500℃	［26，37］
	Pd	0.43g/L 2	80~200	NSE约14%	150~350℃	［26，37］
	Pt-La	1-1	80~160	NSE 60%~90%	250~500℃，NDE约60%	［31］
	Pd-Pt	1-1	80	—	150~500℃	［26］
	Ag	1.3	120	NSE约50%	250~470℃	［34］
ZrO₂	Pd	1	120	NSE约33%	<350℃，NDE约70%	［43］
ZrO₂	—	—	—	NSE约10.5%	<350℃，释放量与吸附量相当	［43］
CeO₂-Pr₂O₃	Pt	1	120	NSE约68%	<350℃，NDE约40%	［35］
CeO₂-Pr₂O₃	Pd	1	120	NSE约50%	<350℃，NDE约41%	［35］
CeO₂-ZrO₂	Pt	1	120	NSE约70%	<350℃，NDE约60%	［39］
	Pd	1~2	80~120	NSE约20%	<350℃，NDE约80% 250~500℃	［27，39］
	Pt-Pd	0.5-0.5	120	NSE约50%	<350℃，NDE约70%	［39］
CeO₂-Al₂O₃	Pt	2.3	80	NSE约10%	300~400℃	［36］
CeO₂-Al₂O₃	Pd	2.3	80	NSE约5%	100~200℃	［36］
WO₃-ZrO₂	Pd	1	120	NSE约80%	<350℃，NDE约100%	［43］
WO₃-ZrO₂	—	—	—	NSE约0	<350℃，释放量与吸附量相当	［43］
SSZ-13	Pd	1~2	80~120	NSE约90% NO_x/Pd 0.41	250~450℃	［8，28，48，56］
SSZ-13	Co	—	100	NSE约96%	250~400℃	［50］
Beta	Pd	1	100	NSE约90%	200~450℃	［8］
Beta	CaO	10	40	NO_x穿透时间102min	500~550℃	［49］
ZSM-5	Pd	0~2	50~150	NSE约90% NO_x/Pd 0.3~0.83	200~450℃	［8，55，60］
LTA	Pd	1.4	80	NO_x/Pd 0.52	300~400℃	［48］
SSZ-39	Pd	0.7	100	NSE约90%	230~350℃	［47］
FER	Pd	1.8	100	NO_x/Pd 0.9	200~300℃	［59］
MCM-22	Pd	1.22	100	NO_x/Pd 0.55	180~300℃	［55］

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