EFFECT OF SYNTHESIS METHOD ON PERFORMANCE OF Ce-MnO<sub><i>x</i></sub> FOR SELECTIVE CATALYTIC OXIDATION OF AMMONIA

SHENG Yujia; CHEN Dong; LIU Haibo; CHEN Tianhu; SHU Daobing; ZHANG Bin

doi:10.13205/j.hjgc.202201010

Volume 40 Issue 1

Mar. 2022

Turn off MathJax

Article Contents

Article Navigation > ENVIRONMENTAL ENGINEERING > 2022 > 40(1): 60-68

SHENG Yujia, CHEN Dong, LIU Haibo, CHEN Tianhu, SHU Daobing, ZHANG Bin. EFFECT OF SYNTHESIS METHOD ON PERFORMANCE OF Ce-MnOx FOR SELECTIVE CATALYTIC OXIDATION OF AMMONIA[J]. ENVIRONMENTAL ENGINEERING , 2022, 40(1): 60-68. doi: 10.13205/j.hjgc.202201010

Citation:

SHENG Yujia, CHEN Dong, LIU Haibo, CHEN Tianhu, SHU Daobing, ZHANG Bin. EFFECT OF SYNTHESIS METHOD ON PERFORMANCE OF Ce-MnO_x FOR SELECTIVE CATALYTIC OXIDATION OF AMMONIA[J]. ENVIRONMENTAL ENGINEERING , 2022, 40(1): 60-68. doi: 10.13205/j.hjgc.202201010

Citation:

PDF( 4249 KB)

EFFECT OF SYNTHESIS METHOD ON PERFORMANCE OF Ce-MnO_x FOR SELECTIVE CATALYTIC OXIDATION OF AMMONIA

doi: 10.13205/j.hjgc.202201010

Key Laboratory of Nano-minerals and Pollution Control of Anhui Higher Education Institutes, School of Resources & Environmental Engineering, Hefei University of Technology, Hefei 230009, China

Received Date: 2021-01-12
Available Online: 2022-03-30
Publish Date: 2022-03-30

Abstract

Abstract

In this paper, Ce-MnO_x was prepared for selective catalytic oxidation(SCO) of ammonia by hydrothermal and impregnation method respectively. The results demonstrated that Ce-MnO_x catalysts exhibited the best NH₃ oxidation activity which composited by hydrothermal method. Among them, Ce(5)-MnO_x(HY) reached 98% of NH₃ conversion rate and 91% of N₂ selectivity, at reaction temperature of 200 ℃. The properties of the Ce-MnO_x catalysts were analyzed by XRD, BET, Raman, XPS, SEM, and H₂-TPR. Hydrothermally prepared Ce-MnO_x possessed larger surface area(94.37 m²/g). At the same time, the distinguished catalytic activity of Ce-MnO_x was attributed to abundant Mn⁴⁺ and Ce³⁺, high adsorbed oxygen concentration on the surface, a large number of active sites, and interaction between Mn and Ce. The results of in-situ DRIFTS showed that the —NH₂ and —NH intermediates could be generated by adsorbed NH₃ dehydrogenation. Consequently, —NH and atomic oxygen combined to form —HNO, which could be quickly oxidized to NO by O₂. Finally, N₂ and H₂O were formed during the following reaction of NO with —NH₂. This dissertation has significant reference value for the study of manganese-based catalysts in low-temperature ammonia oxidation and selectivity.
- ammonia,
- selective catalytic oxidation,
- hydrothermal,
- impregnation,
- Ce-MnO_x

FullText(HTML)

References(49)

References

[1]	LI P X,ZHANG R D,LIU N,et al.Efficiency of Cu and Pd substitution in Fe-based perovskites to promote N₂ formation during NH₃ selective catalytic oxidation (NH₃-SCO)[J].Applied Catalysis B:Environmental,2017,203:174-188.
[2]	PAN Y,TIAN S,LIU D,et al.Fossil fuel combustion-related emissions dominate atmospheric ammonia sources during severe haze episodes:evidence from (15)N-Stable isotope in size-resolved aerosol ammonium[J].Environmental Science & Technology,2016,50 (15):8049-8056.
[3]	WANG F,HE G Z,ZHANG B,et al.Insights into the activation effect of H₂ pretreatment on Ag/Al₂O₃ catalyst for the selective oxidation of ammonia[J].ACS Catalysis,2019,9 (2):1437-1445.
[4]	郭晶晶,李俊华,彭悦,等.铜前驱体对Cu/SSZ-13催化剂选择性催化氧化NH₃性能的影响[J].环境科学学报,2019,39(11):3724-3731.
[5]	唐晓龙,李东,王文勤,等.预处理对CNTs低温催化氧化NH₃性能的影响[J].环境工程学报,2016,10(4):1939-1944.
[6]	WANG F,MA J Z,HE G Z,et al.Nanosize effect of Al₂O₃ in Ag/Al₂O₃ catalyst for the selective catalytic oxidation of ammonia[J].ACS Catalysis,2018,8(4):2670-2682.
[7]	王慧敏,宁平,张秋林,等.不同RuO₂含量对RuO₂-Fe₂O₃催化剂氨选择性催化氧化性能的影响[J].燃料化学学报,2019,47(2):215-223.
[8]	SUN M M,LIU J Y,SONG C,et al.Different reaction mechanisms of ammonia oxidation reaction on Pt/Al₂O₃ and Pt/CeZrO₂ with various Pt states[J].ACS Applied Materials Interfaces,2019,11(26):23102-23111.
[9]	ZHOU M D,WANG Z,SUN Q,et al.High-performance Ag-Cu nanoalloy catalyst for the selective catalytic oxidation of ammonia[J].ACS Applied Materials Interfaces,2019,11(50):46875-46885.
[10]	KADDOURI A,DUPONT N,GELIN P,et al.Selective oxidation of gas phase ammonia over copper chromites catalysts prepared by the sol-gel process[J].Catalysis Communications,2011,15(1):32-36.
[11]	GENG Y,SHAN W P,LIU F D,et al.Adjustment of operation temperature window of Mn-Ce oxide catalyst for the selective catalytic reduction of NO_x with NH₃[J].Journal of Hazardous Materials,2021,405:124223.
[12]	周鹏飞,尤晓晨,李舒健,等.改性MnO_x-CeO₂/石墨烯催化剂低温SCR脱硝性能[J].环境工程,2018,36(11):94-99.
[13]	QU Z P,FAN R,WANG Z,et al.Selective catalytic oxidation of ammonia to nitrogen over MnO₂ prepared by urea-assisted hydrothermal method[J].Applied Surface Science,2015,351:573-579.
[14]	王文勤,唐晓龙.低温NH₃选择性氧催化氧化研究[D].昆明:昆明理工大学,2013.
[15]	从其良,马赫遥,杨鸣刚,等.新型花状CeO₂的NH₃-SCR性能及机制研究[J].高校化学工程学报,2020,3(34):810-815.
[16]	ZHANG X Y,WANG H,JIANG X,et al.Study of synergistic effect between CuO and CeO₂ over CuO@CeO core-shell nanocomposites for NH₃-SCO[J].Catalysis Science & Technology 2019,9:2968-2981.
[17]	BONINGARI T,ETTIREDDY P R,SOMOGYVARI A,et al.Influence of elevated surface texture hydrated titania on Ce-doped Mn/TiO₂ catalysts for the low-temperature SCR of NO_x under oxygen-rich conditions[J].Journal of Catalysis,2015,325 (5):145-155.
[18]	LIU Z M,YI Y,ZHANG S Y,et al.Selective catalytic reduction of NO_x with NH₃ over Mn-Ce mixed oxide catalyst at low temperatures[J].Catalysis Today,2013,216:76-81.
[19]	TANGX F,LI Y G,HUANG X M,et al.MnO_x-CeO₂ mixed oxide catalysts for complete oxidation of formaldehyde:effect of preparation method and calcination temperature[J].Applied Catalysis B:Environmental,2006,62(3/4):265-273.
[20]	HAN Z Y,WANG C,ZOU X H,et al.Diatomite-supported birnessite-type MnO₂ catalytic oxidation of formaldehyde:preparation,performance and mechanism[J].Applied Surface Science,2019,502:144201.
[21]	REDDY B M,BHARILI P,THRIMURTHULU G,et al.Catalytic efficiency of ceria-zirconia and ceria-hafnia nanocomposite oxides for soot oxidation[J].Catalysis Letters,2008,123(3/4):327-333.
[22]	MCBRIDE J R,HASS K C,POINDEXTER B D,et al.Raman and x-ray studies of Ce_1-_xRE_xO_2-_y,where RE=La,Pr,Nd,Eu,Gd,and Tb[J].Journal of Applied Physics,1998,76(4):2435-2441.
[23]	QU Z P,KANG G,QIANG F,et al.Low-temperature catalytic oxidation of toluene over nanocrystal-like Mn-Co oxides prepared by two-step hydrothermal method[J].Catalysis Communications,2014,52(1):31-35.
[24]	LEE S M,PARK K H,HONG S C.MnO_x/CeO₂-TiO₂ mixed oxide catalysts for the selective catalytic reduction of NO with NH₃ at low temperature[J].Chemical Engineering Journal,2012,195/196:323-331.
[25]	FEI Z Y,YANG Y R,WANG M H,et al.Precisely fabricating Ce-O-Ti structure to enhance performance of Ce-Ti based catalysts for selective catalytic reduction of NO with NH₃[J].Chemical Engineering Journal,2018,353:930-939.
[26]	彭莎,刘志明.Ce基氧化物的形貌调控及其对NH₃选择性催化还原NO_x的研究[D].北京:北京工业大学,2017.
[27]	PAPPAS D K,BONOGARI T,BOOLCHAND P,et al.Novel manganese oxide confined interweaved titania nanotubes for the low-temperature selective catalytic reduction (SCR) of NO_x by NH₃[J].Journal of Catalysis,2016,334:1-13.
[28]	SERRANO L A,IGLESIAS J A,MONTE M,et al.MnO₂-supported catalytic bodies for selective reduction of NO with NH₃:influence of NO₂ and H₂O[J].Molecular Catalysis,2020,491:111004.
[29]	LI C C,LIU X H,LU G Z,et al.Redox properties and CO₂ capture ability of CeO₂ prepared by a glycol solvothermal method[J].Chinese Journal of Catalysis,2014,8(35):1346-1375.
[30]	CHEN X,XU X H,FEI Z Y,et al.CeO₂ nanodots embedded in a porous silica matrix as an active yet durable catalyst for HCl oxidation[J].Catalysis Science & Technology,2016,6(13):5116-5123.
[31]	LI H L,WU C Y,LI Y,et al.Superior activity of MnO_x-CeO₂/TiO₂ catalyst for catalytic oxidation of elemental mercury at low flue gas temperatures[J].Applied Catalysis B:Environmental,2012,111:381-388.
[32]	SEIFVAND N,KOWSARI E.TiO₂/in-situ reduced GO/functionalized with an IL-Cr complex as a ternary photocatalyst composite for efficient carbon monoxide deterioration from air[J].Applied Catalysis B:Environmental,2017,206:184-193.
[33]	XIA Y S,DAI H X,ZHANG L,et al.Ultrasound-assisted nanocasting fabrication and excellent catalytic performance of three-dimensionally ordered mesoporous chromia for the combustion of formaldehyde,acetone,and methanol[J].Applied Catalysis B:Environmental,2010,100(1/2):229-237.
[34]	LI P X,ZHANG R D,LIU N,et al.Efficiency of Cu and Pd substitution in Fe-based perovskites to promote N₂ formation during NH₃ selective catalytic oxidation (NH₃-SCO)[J].Applied Catalysis B:Environmental,2017,203:174-188.
[35]	YOU X C,SHENG Z Y,YU D Q,et al.Influence of Mn/Ce ratio on the physicochemical properties and catalytic performance of graphene supported MnO_x-CeO₂ oxides for NH₃-SCR at low temperature[J].Applied Surface Science,2017,423:845-854.
[36]	WANG F,MA J Z,HE G Z,et al.Synergistic effect of TiO₂-SiO₂ in Ag/Si-Ti catalyst for the selective catalytic oxidation of ammonia[J].Industrial & Engineering Chemistry Research,2018,57(35):11903-11910.
[37]	迟斌,曲虹霞.Cu-Ce-La-SSZ-13催化剂的制备及其脱硝性能研究[D].南京:南京理工大学,2018.
[38]	于艳科,孟小然,陈进生,等.SO₂对钾中毒SCR催化剂的活性促进作用研究[C]//中国环境科学学会.2014中国环境科学学会学术年会论文集.成都,2014:1-7.
[39]	QIU L,PANG D D,ZHANG C L,et al.In situ IR studies of Co and Ce doped Mn/TiO₂ catalyst for low-temperature selective catalytic reduction of NO with NH₃[J].Applied Surface Science,2015,357:189-196.
[40]	CHEN W M,MA Y P,QU Z,et al.Mechanism of the selective catalytic oxidation of slip ammonia over Ru-modified Ce-Zr complexes determined by in situ diffuse reflectance infrared fourier transform spectroscopy[J].Environmental Science & Technology,2014,48(20):12199-205.
[41]	LEE S M,LEE H H,HONG S C,Influence of calcination temperature on Ce/TiO₂ catalysis of selective catalytic oxidation of NH₃ to N₂[J].Applied Catalysis A:General,2014,470:189-198.
[42]	ZHANG Q L,WANG H M,NING P,et al.In situ DRIFTS studies on CuO-Fe₂O₃ catalysts for low temperature selective catalytic oxidation of ammonia to nitrogen[J].Applied Surface Science,2017,419:733-743.
[43]	ZHANG L,HE H.Mechanism of selective catalytic oxidation of ammonia to nitrogen over Ag/Al₂O₃[J].Journal of Catalysis,2009,268(1):18-25.
[44]	赵琳琳,黄亚继,宋静,等.V-W/TiO₂/γ-Al₂O₃催化剂催化还原NO的研究[J].环境科学与技术,2012,35(5):85-89.
[45]	YANG S J,WANG C Z,LI J H,et al.Low temperature selective catalytic reduction of NO with NH₃ over Mn-Fe spinel:performance,mechanism and kinetic study[J].Applied Catalysis B:Environmental,2011,110:71-80.
[46]	CHEN L,SI Z C,WU X D,et al.DRIFT study of CuO-CeO₂-TiO₂ mixed oxides for NO_x reduction with NH₃ at low temperatures[J].ACS Applied Materials Interfaces,2014,6(11):8134-45.
[47]	易阳,刘志明.Cu-Ce-Ti催化剂上氨气选择性催化还原NO_x的研究[D].北京:北京化工大学,2013.
[48]	YU X L,WU X M,CHEN Z Y,et al.Oxygen vacancy defect engineering in Mn-doped CeO₂ nanostructures for nitrogen oxides emission abatement[J].Molecular Catalysis,2019,476:110512.
[49]	LIU J,LI X Y,ZHAO Q D,et al.Mechanistic investigation of the enhanced NH₃-SCR on cobalt-decorated Ce-Ti mixed oxide:in situ FTIR analysis for structure-activity correlation[J].Applied Catalysis B:Environmental,2017,200:297-308.