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Progress in Chemistry 2022, Vol. 34 Issue (12): 2638-2650 DOI: 10.7536/PC220422 Previous Articles   Next Articles

• CONTENTS •

Application of Transition Metal Based MOF Materials in Selective Catalytic Reduction of Nitrogen Oxides

Wei Zhang1,2(), Kang Xie1,2, Yunhao Tang1,2, Chuan Qin1,2, Shan Cheng1,2, Ying Ma3   

  1. 1 College of Energy and Power Engineering, Changsha University of Science and Technology,Changsha 410114, China
    2 Key Laboratory of Renewable Energy and Electric Power Technology of Hunan Province,Changsha 410114, China
    3 Yonker Environmental Protection Company Limited,Changsha 410330, China.
  • Received: Revised: Online: Published:
  • Contact: Wei Zhang
  • Supported by:
    national natural science foundation of China(52006016); state scholarship fund awarded by China scholarship(201808430112); natural science foundation of Hunan province(2020JJ4098); natural science foundation of Hunan province(2021JJ40573); Key projects of scientific research project of Hunan Provincial Department of Education(21A0216); Changsha Municipal Natural Science Foundation(kq2014104); young teachers growth plan project of CSUST(2019QJCZ044); key laboratory of renewable energy electric technology of Hunan province(2018ZNDL004); key laboratory of renewable energy electric technology of Hunan province(2020ZNDL001); 2022 Graduate research and innovation project at Changsha University of Science and Technology(CXCLY2022092)
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Selective catalytic reduction (SCR) technology is the most widely used industrial denitration technology at present, the development of catalyst system with excellent activity and anti-poisoning performance is the focus of researchers. Transition metal oxides and metal organic framework (MOF) materials have been widely studied and applied in the field of denitration catalysts because of their excellent redox performance, and researchers found that the combination of transition metal oxides and MOF materials can further improve the denitration activity of the catalyst. This paper summarizes the research progress of a series of single transition metal based MOF denitration catalysts and composite transition metal based MOF denitration catalysts mainly used in NH3-SCR reaction in recent years, and expounds the strengthening methods of water resistance, sulfur poisoning resistance and thermal stability of transition metal based MOF denitration catalysts, The main research directions of transition metal based MOF denitration catalysts in the future are prospected: new transition metal based MOF denitration catalysts with excellent denitration activity, water and sulfur resistance and thermal stability can be prepared by comprehensively utilizing the characteristics of different transition metal oxides and combined with the strong interaction between metal oxides. Further, transition metal based MOF denitration catalyst can be prepared by combining experiment and simulation to selectively catalyze the reduction of nitrogen oxides to meet the needs of industrialization.

Contents

1 Introduction

2 Transition metal based MOF denitration catalyst

2.1 Mono-transition metal based MOF denitration catalysts

2.2 Double-transition metal based MOF denitration catalysts

3 Enhancement of antitoxicity of transition metal based MOF denitration catalysts

3.1 Enhancing the water resistance of transition metal based MOF denitration catalysts

3.2 Enhancing the sulfur resistance of transition metal based MOF denitration catalysts

4 Method for enhancing thermal stability of transition metal based MOF denitration catalysts

4.1 Adding metal clusters

4.2 Optimizing the molar ratio of metal ions to organic ligands

5 Conclusion and Prospect

Key words: selective catalytic reduction, metal organic framework, transition metal oxide, poison resistance, thermal stability
Table 1 Mono-transition metal based MOF denitration catalysts reported in the literature in recent years
Catalyst Optimal denitration efficiency Anti-poisoning property Thermal stability
(thermal decomposition
temperature)		 Reaction condition ref
Mn-MOF-74 > 95% (200~250 ℃) Good water resistance, poor sulfur resistance 275 ℃ NO=1000 ppm,O2=2%,NH3=1000 ppm,Ar as balance gas,total flow=100 mL/min,GHSV=50,000 h-1 20
MIL-100(Fe) > 98% (250~300 ℃) Good water resistance, good sulfur resistance 300 ℃ NO=500 ppm,O2=5%,NH3=500 ppm,N2 as balance gas,GHSV=30,000 h-1 27
Cu-BTC 100% (220~280 ℃) Poor water resistance, poor sulfur resistance 330 ℃ NO=500 ppm,O2=5%,NH3=500 ppm,N2 as balance gas,total flow=100 mL/min,GHSV=30,000 h-1 32
Cu-MOF-74 97.8% (230 ℃) Good water resistance, poor sulfur resistance 310 ℃ NO=1000 ppm,O2=2%,NH3=1000 ppm,Ar as balance gas,total flow=100 mL/min,GHSV=50,000 h-1 39
Co-MOF-74 70% (210 ℃) Good water resistance, good sulfur resistance 275 ℃ NO=1000 ppm,O2=2%,NH3=1000 ppm,Ar as balance gas,total flow=100 mL/min,GHSV=50,000 h-1 35
Ni-MOF > 90% (275~440 ℃) Good water resistance, poor sulfur resistance 440 ℃ NO=500 ppm,O2=5%,NH3=500 ppm,N2 as balance gas,total flow=100 mL/min,GHSV=15,000 h-1 12
MIL-88B(V) > 80% (275~300 ℃) Poor water resistance, poor sulfur resistance 320 ℃ NO/NH3=1.05,N2 as balance gas,total flow=100 mL/min,GHSV=10,000 h-1 40
Fig. 1 Bimetallic modified MOF denitration catalysts[44]
Fig. 2 Elements with practical application and development potential for the preparation of MOF denitration catalyst (Blue: elements that have been used to prepare MOF denitration catalyst; Yellow: elements that have been applied to prepare MOF catalyst; Red: elements that have been used to prepare denitration catalyst; Orange: elements that have been used to prepare MOF catalyst and denitration catalyst, but not used to prepare MOF denitration catalyst)
Fig.3 TEM images of (a) Mn-MOF-74, (b) P123-Mn-MOF-74, (c) PVP-Mn-MOF-74 and (d) Mn-MOF-74- CH3[11]
Fig.4 Mn/Ce-400-Air (a)Mechanism of SO2 removal by NH3-SCR (b) Sedimentation and decomposition of Ce2(SO4)3[127]
Fig.5 Comparison of thermal stability of NJU-Bai62 with some representative MOFs with permanent porosity[133]
Fig.6Summ ary and prospect of transition metal based MOF denitration catalysts concept map
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