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化学进展 2022, Vol. 34 Issue (8): 1678-1687 DOI: 10.7536/PC210920 前一篇   后一篇

• 综述 •

贵金属催化剂上氢气选择性催化还原NOx

贾斌1,2, 刘晓磊1,2, 刘志明1,2,*()   

  1. 1 北京化工大学化工资源有效利用国家重点实验室 北京 100029
    2 北京化工大学北京市环境污染控制与资源化工程研究中心 北京 100029
  • 收稿日期:2021-09-18 修回日期:2022-01-04 出版日期:2022-04-01 发布日期:2022-04-01
  • 通讯作者: 刘志明
  • 基金资助:
    国家自然科学基金项目(21876009); 中央高校基本科研业务费项目(JD2110)
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Selective Catalytic Reduction of NOx by Hydrogen over Noble Metal Catalysts

Bin Jia1,2, Xiaolei Liu1,2, Zhiming Liu1,2()   

  1. 1 State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology,Beijing 100029, China
    2 Beijing Center for Environmental Pollution Control and Resource Recovery, Beijing University of Chemical Technology,Beijing 100029, China
  • Received:2021-09-18 Revised:2022-01-04 Online:2022-04-01 Published:2022-04-01
  • Contact: Zhiming Liu
  • Supported by:
    National Natural Science Foundation of China(21876009); Fundamental Research Funds for the Central Universities(JD2110)

NOx的控制对于改善大气环境质量具有重要意义,而氢气选择性催化还原(H2-SCR)NOx作为一种高效环保的脱硝技术而备受关注。本文总结概述了近年来贵金属催化剂在H2-SCR脱硝反应中的研究进展,首先介绍了H2-SCR反应机理,在此基础上分别论述了影响贵金属催化剂性能的因素(如活性组分、载体类型、助剂添加及组分存在形式等)及催化剂结构与性能的构效关系。最后,针对目前存在的问题展望了H2-SCR脱硝未来的发展方向。

关键词： 氮氧化物, H2-SCR, 贵金属催化剂, 反应机理

The control of NOx is very important for the air quality improvement. Selective catalytic reduction of NOx by hydrogen (H2-SCR) has attracted much attention as an efficient and environmentally benign deNOx technology. In this review, we summarize the research development in the H2-SCR of NOx over noble metal catalysts. The typical H2-SCR reaction mechanisms are introduced first. Then the factors affecting the H2-SCR performance of noble metal catalysts, such as the active metal, support type, the added promoter and the nature of active metal, and the structure-activity relationship have been discussed. Finally, the challenges and the prospects for future development of H2-SCR catalyst are proposed.

Contents

1 Introduction

2 The reaction mechanisms of H2-SCR

2.1 Redox mechanism

2.2 Adsorption/dissociation of NO

2.3 Bifunction mechanism

3 Noble metal H2-SCR catalyst

3.1 Effect of active metal

3.2 Effect of the support

3.3 Effects of the additives

3.4 Alloy catalyst

3.5 Single atom catalyst

4 Conclusion and perspective

Key words: nitrogen oxides, H2-SCR, noble metal catalyst, reaction mechanism
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图1 Pt/MgO-CeO2催化剂上H物种表面扩散反应机理[7]
Fig. 1 Mechanism of surface diffusion reaction of H species on Pt/MgO-CeO2 catalyst[7]
图2 Pt/La0.5Ce0.5MnO3催化剂上的NO吸附-离解机理[14]
Fig. 2 Schematic diagram of NO adsorption and dissociation over the Pt/La0.5Ce0.5MnO3 catalyst[14]
图3 Pd/V2O5/TiO2-Al2O3催化剂上的H2-SCR反应机理图[15]
Fig. 3 Reaction scheme of H2-SCR of NOx on Pd/V2O5/TiO2-Al2O3 catalyst[15]
图4 Pt/SSZ-13催化剂在不同温度下的反应途径[19]
Fig. 4 Reaction routes of Pt/SSZ-13 catalyst at different temperatures[19]
图5 Pt/h-ZSM-5催化剂在不同温度下的反应路径[18]
Fig. 5 Reaction routes of Pt/h-ZSM-5 catalyst in the different ranges of temperature[18]
图6 Pt-HY催化剂上H2-SCR的反应机理[20]
Fig. 6 Mechanism diagram of H2-SCR reaction on Pt-HY catalyst[20]
图7 NO的转化数(TOF)与Pd粒径的关系[25]
Fig. 7 Relationship between the TOF of NO and the Pd particle size[25]
图8 牺牲碳层策略制备Pt/TiO2催化剂的示意图[27]
Fig. 8 Scheme for the preparation of Pt/TiO2 catalyst using the sacrificial carbon layer strategy[27]
图9 Pt/TiO2和Pt/TiO2(M)催化剂的活性比较[27]
Fig. 9 Comparison of the activities of Pt/TiO2 and Pt/TiO2-M catalysts[27]
图10 MOF材料为模板合成介孔Pt/ZrO2@C纳米八面体流程图[43]
Fig. 10 Schematic illustration of the synthesis of MOF-derived porous Pt/ZrO2@C nano-octahedra[43]
图11 Pt/HZSM-5 和 Pt-W/HZSM-5催化剂H2-SCR活性的比较。反应条件:[NO] = 1000 ppm,[H2] =5000 ppm,[O2] = 10%[48]
Fig. 11 H2-SCR performance of Pt/HZSM-5 and Pt-W/HZSM-5 catalysts. Reaction conditions:[NO] = 1000 ppm, [H2] =5000 ppm, [O2] = 10%[48]
图12 Pt-SAC(a)和Pt-nano(b)催化剂的HAADF-STEM图[62]
Fig. 12 HAADF-STEM images of (a)Pt-SAC and (b)Pt-nano catalysts[62]
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