Application and performance enhancement challenges of H2-SCR modified platinum-based catalysts for low-temperature denitrification

doi:10.16085/j.issn.1000-6613.2022-1453

Chemical Industry and Engineering Progress ›› 2023, Vol. 42 ›› Issue (6): 2954-2962.DOI: 10.16085/j.issn.1000-6613.2022-1453

• Industrial catalysis • Previous Articles Next Articles

Application and performance enhancement challenges of H₂-SCR modified platinum-based catalysts for low-temperature denitrification

ZHANG Wei¹^,²(), QIN Chuan¹^,², XIE Kang¹^,², ZHOU Yunhe¹^,², DONG Mengyao¹^,², LI Jie¹^,², TANG Yunhao¹^,², MA Ying³, SONG Jian⁴

^1.School of Energy and Power Engineering, Changsha University of Science and Technology, Changsha 410114, Hunan, China
^2.Key Laboratory of Renewable Energy and Electric Power Technology of Hunan Province, Changsha 410114, Hunan, China
^3.Yonker Environmental Protection Company Limited, Changsha 410330, Hunan, China
^4.Hunan Datang Energy-saving Technology Company Limited, Changsha 410007, Hunan, China

Received:2022-08-03 Revised:2022-12-25 Online:2023-06-29 Published:2023-06-25
Contact: ZHANG Wei

H₂-SCR改性铂系催化剂低温脱硝的应用及性能强化挑战

张巍¹^,²(), 秦川¹^,², 谢康¹^,², 周运河¹^,², 董梦瑶¹^,², 李婕¹^,², 汤云灏¹^,², 马英³, 宋健⁴

^1.长沙理工大学能源与动力工程学院，湖南长沙 410114
^2.可再生能源电力技术湖南省重点实验室，湖南长沙 410114
^3.永清环保股份有限公司，湖南长沙 410330
^4.湖南大唐节能科技有限公司，湖南长沙 410007

通讯作者: 张巍
作者简介:张巍（1974—），男，博士，副教授，硕士生导师，研究方向为高效清洁燃烧与污染物控制。E-mail：weizhang@csust.edu.cn。
基金资助:
国家留学基金(201808430112);湖南省自然科学基金(2020JJ4098);湖南省教育厅科学研究项目重点项目(21A0216);长沙理工大学青年教师成长计划(2019QJCZ044);“可再生能源电力技术”湖南省重点实验室开放基金(2018ZNDL004)

Abstract

Abstract:

The emission of nitrogen oxides (NO _x ) has seriously harmed the ecological environment and human health, and they are mainly from fixed source of flue gas emissions and mobile source of exhaust emissions. In recent years, hydrogen selective catalytic reduction (H₂-SCR) to modify platinum based catalysts to control mobile source NO _x has attracted extensive attention. Because different modification methods can promote the electron migration between platinum and the support to form bifunctional reaction mechanism acid sites, Therefore, it is of far-reaching significance to develop efficient mobile source denitration catalysts by deeply understanding the NO _x catalytic reaction mechanism of platinum based H₂-SCR catalysts. In this paper, the types of platinum based H₂-SCR denitration catalysts are reviewed, and the mechanisms of H₂/NO adsorption, NO oxidation reduction, and dual function reaction on their surfaces are described. The strengthening methods to improve the stability, sulfur resistance and selectivity of platinum based H₂-SCR catalysts are summarized. Further investigations of the multivalence and electron mobility of highly efficient metal oxide and molecular sieve-loaded Pt-based H₂-SCR catalysts and the mechanism of NO, H₂, and O₂ on the catalyst surface, as well as the reduction of Pt loading for cost reduction, are also foreseen.

Key words: platinum catalyst, H₂-selective catalytic reduction (SCR), low temperature denitrification, catalyst support

摘要：

氮氧化物（NO _x ）的排放严重危害了生态环境和人类健康，其主要来源有固定源烟气排放和移动源尾气排放。近年来，利用氢气选择性催化还原（H₂-SCR）改性铂系催化剂控制移动源NO _x 的相关研究引起了广泛的关注，由于不同的改性方法可以促进铂与载体之间的电子迁移，从而形成双功能反应机制酸位点，因而通过深入认识铂系H₂-SCR催化剂的NO _x 催化反应机制并获得良好的改性方法对于开发高效移动源脱硝催化剂具有深远的意义。本文综述了铂系H₂-SCR脱硝催化剂的种类，阐述了其表面的H₂/NO吸附机制、NO氧化还原机制和双功能反应机制，总结了提高铂系H₂-SCR催化剂的稳定性、抗硫性和选择性的强化方法。进一步阐述了金属氧化物和分子筛负载型铂系H₂-SCR催化剂可变的多价态，电子迁移能力，NO、H₂和O₂在催化剂表面的反应机理，并对铂负载减量化降低成本的相关研究进行了展望。

关键词: 铂系催化剂, H₂-选择性催化还原, 低温脱硝, 催化剂载体

CLC Number:

X511

ZHANG Wei, QIN Chuan, XIE Kang, ZHOU Yunhe, DONG Mengyao, LI Jie, TANG Yunhao, MA Ying, SONG Jian. Application and performance enhancement challenges of H₂-SCR modified platinum-based catalysts for low-temperature denitrification[J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2954-2962.

张巍, 秦川, 谢康, 周运河, 董梦瑶, 李婕, 汤云灏, 马英, 宋健. H₂-SCR改性铂系催化剂低温脱硝的应用及性能强化挑战[J]. 化工进展, 2023, 42(6): 2954-2962.

Figures/Tables 6

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催化剂	制备方法	最佳反应温度/最佳脱硝效率/最佳N₂选择性	反应条件	参考文献
Pt/MnO _x	共沉淀法	100℃/64%/30%	0.048mL/min NO，5%（体积分数）O₂，He平衡，空速（GHSV）为78000h^-1	[24]
Pt/ZrO₂	浸渍法	150℃/71%/75%	0.2mL/min NO _x，1mL/min H₂，10%（体积分数）O₂，N₂为平衡气，温度60~280℃，总流量200mL/min	[18]
Pt/MgO	浸渍法	150℃/71.4%/62%	0.2mL/min NO _x，1mL/min H₂，10%（体积分数）O₂，N₂为平衡气，温度60~280℃，总流量200mL/min	[18]
Pt/Al₂O₃	浸渍法	91℃/88%/90%	4.8mL/min NO，1vol% H₂, 5vol% O₂，N₂为平衡气，温度20~350℃，总流量2400mL/min，GHSV为12000h^-1	[25]
Pt/Mg₃Al₁O _x	共沉淀法	200~220℃/92%/60%	0.125mL/min NO _x，0.5%~2%（体积分数）H₂，0~10%（体积分数）O₂，Ar为平衡气，总流量200~300mL/min，GHSV为12000h^-1	[26]
Pt/Ce_0.5Zr_0.5O₂	溶胶-凝胶法	120~220℃/92%/78%	0.03mL/min NO，2.5%（体积分数）O₂，0.8%（体积分数）H₂，10%（体积分数）CO₂，15%（体积分数）H₂O，0.5%（体积分数）C₃H₆，总流量200mL/min，GHSV为33000h^-1	[19]
Pt/MgO-CeO₂	湿浸渍法	150℃/94%/80%	0.25%（摩尔分数）NO，1.0%（摩尔分数）H₂，5%（摩尔分数）O₂，He为平衡气体，总流量100mL/min，GHSV为80000h^-1	[27]

催化剂	制备方法	最佳反应温度/最佳脱硝效率/最佳N₂选择性	反应条件	参考文献
Pt/MnO _x	共沉淀法	100℃/64%/30%	0.048mL/min NO，5%（体积分数）O₂，He平衡，空速（GHSV）为78000h^-1	[24]
Pt/ZrO₂	浸渍法	150℃/71%/75%	0.2mL/min NO _x，1mL/min H₂，10%（体积分数）O₂，N₂为平衡气，温度60~280℃，总流量200mL/min	[18]
Pt/MgO	浸渍法	150℃/71.4%/62%	0.2mL/min NO _x，1mL/min H₂，10%（体积分数）O₂，N₂为平衡气，温度60~280℃，总流量200mL/min	[18]
Pt/Al₂O₃	浸渍法	91℃/88%/90%	4.8mL/min NO，1vol% H₂, 5vol% O₂，N₂为平衡气，温度20~350℃，总流量2400mL/min，GHSV为12000h^-1	[25]
Pt/Mg₃Al₁O _x	共沉淀法	200~220℃/92%/60%	0.125mL/min NO _x，0.5%~2%（体积分数）H₂，0~10%（体积分数）O₂，Ar为平衡气，总流量200~300mL/min，GHSV为12000h^-1	[26]
Pt/Ce_0.5Zr_0.5O₂	溶胶-凝胶法	120~220℃/92%/78%	0.03mL/min NO，2.5%（体积分数）O₂，0.8%（体积分数）H₂，10%（体积分数）CO₂，15%（体积分数）H₂O，0.5%（体积分数）C₃H₆，总流量200mL/min，GHSV为33000h^-1	[19]
Pt/MgO-CeO₂	湿浸渍法	150℃/94%/80%	0.25%（摩尔分数）NO，1.0%（摩尔分数）H₂，5%（摩尔分数）O₂，He为平衡气体，总流量100mL/min，GHSV为80000h^-1	[27]

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[8]	ZENG Junjian, ZHAO Jigang. Research progress of gold based mercury-free catalysts for acetylene hydrochlorination [J]. Chemical Industry and Engineering Progress, 2022, 41(7): 3589-3596.
[9]	TANG Jinqiong, KONG Yong, SHEN Xiaodong. Advances in the synthesis and application of the carbide-derived carbons [J]. Chemical Industry and Engineering Progress, 2022, 41(2): 791-802.
[10]	ZHANG Yongxiang, WANG Delong, GUO Xiaoyan, SHAO Huaiqi. Structure and performance of CrO _x /Ti-Al₂O₃ catalysts for propane dehydrogenation [J]. Chemical Industry and Engineering Progress, 2022, 41(11): 5879-5886.
[11]	CHEN Zhiqiang, CHE Chunxia, WU Dengfeng, WEN He, HAN Wei, ZHANG Feng, XU Haoxiang, CHENG Daojian. Advances in catalysts for selective hydrogenation of acetylene [J]. Chemical Industry and Engineering Progress, 2022, 41(10): 5390-5405.
[12]	DAI Xiaojun, CHENG Yan, WANG Xiaohan, HUANG Wenbin, WEI Qiang, ZHOU Yasong. Research progress in the synthesis of small particle-size SAPO-11 molecular sieves [J]. Chemical Industry and Engineering Progress, 2021, 40(S1): 191-203.
[13]	ZHANG Wenhui, HUA Rui, QI Suitao. Research progress of low temperature Fischer-Tropsch synthetic wax oil hydrocracking refining technology [J]. Chemical Industry and Engineering Progress, 2021, 40(S1): 81-87.
[14]	DING Xin, ZHANG Dongming, JIAO Weizhou, LIU Youzhi. Research progress of anode catalysts for direct methanol fuel cells [J]. Chemical Industry and Engineering Progress, 2021, 40(9): 4918-4930.
[15]	ZENG Maozhu, SHE Yuqi, HU Yubin, WU Linjun, YUAN Manjing, QI Yi, WANG Huan, LIN Xuliang, QIN Yanlin. Progress in preparation and application of lignin porous carbon [J]. Chemical Industry and Engineering Progress, 2021, 40(8): 4573-4586.