C<sub>3</sub>H<sub>6</sub>-SCR denitration characteristics of CuCoCe-LDH catalysts

CHEN Jiayin; NING Shuying; FU Wei; CAI Chen; ZHOU Hao; SU Yaxin

doi:10.19906/j.cnki.JFCT.2023073

Volume 52 Issue 3

Mar. 2024

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2024 > 52(3): 373-383

CHEN Jiayin, NING Shuying, FU Wei, CAI Chen, ZHOU Hao, SU Yaxin. C3H6-SCR denitration characteristics of CuCoCe-LDH catalysts[J]. Journal of Fuel Chemistry and Technology, 2024, 52(3): 373-383. doi: 10.19906/j.cnki.JFCT.2023073

Citation:

CHEN Jiayin, NING Shuying, FU Wei, CAI Chen, ZHOU Hao, SU Yaxin. C₃H₆-SCR denitration characteristics of CuCoCe-LDH catalysts[J]. Journal of Fuel Chemistry and Technology, 2024, 52(3): 373-383. doi: 10.19906/j.cnki.JFCT.2023073

Citation:

PDF( 5356 KB)

C₃H₆-SCR denitration characteristics of CuCoCe-LDH catalysts

doi: 10.19906/j.cnki.JFCT.2023073

CHEN Jiayin^1
,,
NING Shuying^1
,,
FU Wei^1
,,
CAI Chen^1
,,
ZHOU Hao^2
,,
SU Yaxin^{1
,
,}

1.
School of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
2.
Changzhou Vocational Institute of Engineering, Changzhou 213164, China

Funds: The project was supported by the National Natural Science Foundation of China (52276103).

Received Date: 2023-07-20
Accepted Date: 2023-09-19
Rev Recd Date: 2023-09-18

Available Online: 2023-09-28

Publish Date: 2024-03-10

Abstract

Abstract

A series of Cu_(x)Co_(y)Ce_(z)-LDH precursors were synthesized by one-step hydrothermal method, and Cu_(x)Co_(y)Ce_(z)O mixed metal oxide catalysts were prepared after calcination and used to study the selective catalytic reduction of NO by C₃H₆ (C₃H₆-SCR) with a fixed bed micro-reactor. Due to the strong synergy between Cu, Co and Ce, Cu_(0.21)Co_(0.48)Ce_(0.31)O achieves 95% NO conversion and 90% N₂ selectivity at 225 ℃. In addition, ICP, XRD, TEM, XPS, H₂-TPR were used to characterize the basic physical-chemical properties of the catalysts to investigate the relationship between physicochemical properties and catalytic reduction abilities. XRD results show that solid solutions are formed between Cu, Co and Ce, which promotes the dispersion of active metals. XPS and H₂-TPR further demonstrate that redox reactions occur between Cu and Co, promoting the formation of oxygen vacancies, thereby improving their catalytic reduction capacity.
- nitrogen oxides,
- selective catalytic reduction,
- C₃H₆,
- CuCoCe-LDH,
- hydrothermal method

FullText(HTML)

References(59)

References

[1]	BONINGARI T, SMIRNIOTIS P G. Impact of nitrogen oxides on the environment and human health: Mn-based materials for the NO_x abatement[J]. Curr Opin Chem Eng,2016,13:133−141. doi: 10.1016/j.coche.2016.09.004
[2]	SHAN W, GENG Y, CHEN X, et al. A highly efficient CeWO_x catalyst for the selective catalytic reduction of NO_x with NH₃[J]. Catal Sci Technol,2016,6(4):1195−200. doi: 10.1039/C5CY01282A
[3]	ZHANG X, SU Y, CHENG J, et al. Effect of Ag on deNO_x performance of SCR-C₃H₆ over Fe/Al-PILC catalysts[J]. J Fuel Chem Technol,2019,47(11):1368−1378. doi: 10.1016/S1872-5813(19)30055-6
[4]	XU J, WANG H, GUO F, et al. Recent advances in supported molecular sieve catalysts with wide temperature range for selective catalytic reduction of NO_x with C₃H₆[J]. RSC Adv,2019,9(2):824−838. doi: 10.1039/C8RA08635D
[5]	周皞, 苏亚欣, 邓文义等. 金属氧化物类催化剂上HC-SCR研究进展[J]. 环境科学与技术,2016,39(1):93−100. ZHOU Hao, SU Yaxin, DENG Wenyi, et al. A review of HC-SCR over metal oxides-based catalysts[J]. Environ Sci Technol,2016,39(1):93−100.
[6]	宁淑英, 苏亚欣, 杨洪海等. 用于HC-SCR还原NO_x的Cu基分子筛催化剂研究进展[J]. 化工进展,2023,42(3):1308−1320. NING Shuying, SU Yaxin, YANG Honghai, et al. Research progress on supported Cu-based zeolite catalysts for the selective catalytic reduction of NO_x with hydrocarbons[J]. Chem Ind Eng Prog,2023,42(3):1308−1320.
[7]	KASHIF M, YUAN M, SU Y, et al. A review on pillared clay-based catalysts for low-temperature selective catalytic reduction of NO with hydrocarbons[J]. Appl Clay Sci,2023,233:106847. doi: 10.1016/j.clay.2023.106847
[8]	HUANG F, HU W, CHEN J, et al. Insight into enhancement of NO reduction with methane by multifunctional catalysis over a mixture of Ce/HZSM-5 and CoO_x in excess of oxygen[J]. Ind Eng Chem Res,2018,57(40):13312−13317. doi: 10.1021/acs.iecr.8b00773
[9]	SERHAN N, TSOLAKIS A, WAHBI A, et al. Modifying catalytically the soot morphology and nanostructure in diesel exhaust: Influence of silver De-NO_x catalyst (Ag/Al₂O₃)[J]. Appl Catal B: Environ,2019,241:471−482. doi: 10.1016/j.apcatb.2018.09.068
[10]	YUAN D, LI X, ZHAO Q, et al. A novel CuTi-containing catalyst derived from hydrotalcite-like compounds for selective catalytic reduction of NO with C₃H₆ under lean-burn conditions[J]. J Catal,2014,309:268−279. doi: 10.1016/j.jcat.2013.09.010
[11]	YAN Q, HOU X, LIU G, et al. Recent advances in layered double hydroxides (LDHs) derived catalysts for selective catalytic reduction of NO_x with NH₃[J]. J Hazard Mater,2020,400:123260. doi: 10.1016/j.jhazmat.2020.123260
[12]	LIU X, FAN X, HUANG H, et al. Electronic modulation of oxygen evolution on metal doped NiFe layered double hydroxides[J]. J Colloid Interface Sci,2021,587:385−392. doi: 10.1016/j.jcis.2020.12.023
[13]	WU X, LIU J, LIU X, et al. Fabrication of carbon doped Cu-based oxides as superior NH₃-SCR catalysts via employing sodium dodecyl sulfonate intercalating CuMgAl-LDH[J]. J Catal,2022,407:265−280. doi: 10.1016/j.jcat.2022.02.004
[14]	DU Y, LIU L, FENG Y, et al. Enhancement of NH₃-SCR performance of LDH-based MMnAl (M=Cu, Ni, Co) oxide catalyst: influence of dopant M[J]. RSC Adv,2019,9(68):39699−39708. doi: 10.1039/C9RA08391J
[15]	CHEN S, YAN Q, ZHANG C, et al. A novel highly active and sulfur resistant catalyst from Mn-Fe-Al layered double hydroxide for low temperature NH₃-SCR[J]. Catal Today,2019,327:81−89. doi: 10.1016/j.cattod.2018.06.006
[16]	YUAN D, LI X, ZHAO Q. Preparation and characterization of Ni-Ti-O mixed oxide for selective catalytic reduction of NO under lean-burn conditions[J]. Chin J Catal,2013,34(7):1449−1455. doi: 10.1016/S1872-2067(12)60614-7
[17]	TRET’YAKOV V F, ZAKIROVA A G, SPOZHAKINA A A, et al. Selective reduction of nitrogen oxides by hydrocarbons on hydrotalcite Co and Ni catalysts[J]. Catal Ind,2010,2(1):62−66. doi: 10.1134/S2070050410010101
[18]	WEN N, SU Y, DENG W, et al. Synergy of CuNiFe-LDH based catalysts for enhancing low-temperature SCR-C₃H₆ performance: Surface properties and reaction mechanism[J]. Chem Eng J,2022,438:135570. doi: 10.1016/j.cej.2022.135570
[19]	ADAMOWSKA M, KRZTOŃ A, NAJBAR M, et al. DRIFT study of the interaction of NO and O₂ with the surface of Ce_0.62Zr_0.38O₂ as deNO_x catalyst[J]. Catal Today,2008,137(2/4):288−291. doi: 10.1016/j.cattod.2008.01.013
[20]	ZHAO L, ZHANG Y, BI S, et al. Metal-organic framework-derived CeO₂-ZnO catalysts for C₃H₆-SCR of NO: An in situ DRIFTS study[J]. RSC Adv,2019,9(33):19236−19242. doi: 10.1039/C9RA03103K
[21]	LI X, LU G, QU Z, et al. The role of titania pillar in copper-ion exchanged titania pillared clays for the selective catalytic reduction of NO by propylene[J]. Appl Catal A: Gen,2011,398(1/2):82−87. doi: 10.1016/j.apcata.2011.03.020
[22]	AMIN N A S, TAN E F, MANAN Z A. Selective reduction of NO_x with C₃H₆ over Cu and Cr promoted CeO₂ catalysts[J]. Appl Catal B: Environ,2003,43(1):57−69. doi: 10.1016/S0926-3373(02)00275-8
[23]	WEN N, SU Y, DENG W, et al. Selective catalytic reduction of NO with C₃H₆ over CuFe-containing catalysts derived from layered double hydroxides[J]. Fuel,2021,283:119296. doi: 10.1016/j.fuel.2020.119296
[24]	WANG X, WEN W, MI J, et al. The ordered mesoporous transition metal oxides for selective catalytic reduction of NO_x at low temperature[J]. Appl Catal B: Environ,2015,176:454−463.
[25]	PAN K, YU F, LIU Z, et al. Enhanced low-temperature CO-SCR denitration performance and mechanism of two-dimensional CuCoAl layered double oxide[J]. J Environ Chem Eng,2022,10(3):108030. doi: 10.1016/j.jece.2022.108030
[26]	ZHANG X P, CUI Y Z, TAN B J, et al. The adsorption and catalytic oxidation of the element mercury over cobalt modified Ce–ZrO₂ catalyst[J]. RSC Adv,2016,6(91):88332−88339. doi: 10.1039/C6RA19450H
[27]	WANG Z, LAN J, HANEDA M, et al. Selective catalytic reduction of NO_x with NH₃ over a novel Co-Ce-Ti catalyst[J]. Catal Today,2021,376:222−228. doi: 10.1016/j.cattod.2020.05.040
[28]	LI Z, CHEN J, JIANG M, Et al. Study on SO₂ poisoning mechanism of CO catalytic oxidation reaction on copper-cerium catalyst[J]. Catal Lett,2021,152:2729−2737.
[29]	SHI M, YE S, QU H, et al. Synergistic effect of Cu²⁺ doping and sulfation in Cu-Ce-S, tolerance to H₂O and SO₂ and decomposition behaviors of ammonia salts[J]. Mol Catal,2018,459:135−140. doi: 10.1016/j.mcat.2018.08.023
[30]	YAN Q, CHEN S, QIU L, et al. The synthesis of Cu_yMn_zAl_1-zO_x mixed oxide as a low-temperature NH₃-SCR catalyst with enhanced catalytic performance[J]. Dalton Trans,2018,47(9):2992−3004. doi: 10.1039/C7DT02000G
[31]	ZHANG Y, ZHAO L, KANG M, et al. Insights into high CO-SCR performance of CuCoAlO catalysts derived from LDH/MOFs composites and study of H₂O/SO₂ and alkali metal resistance[J]. Chem Eng J,2021,426:131873. doi: 10.1016/j.cej.2021.131873
[32]	WANG L, YANG Z, LIAO Y, et al. Synthesis of reusable and anti-fouling Co-Al-Ce LDHs coated stainless steel mesh for ultrafast oil/water separation and photocatalytic degradation[J]. Appl Clay Sci,2023,232:106769. doi: 10.1016/j.clay.2022.106769
[33]	DING J, HAN Y, HONG G. Tailoring the activity of NiFe layered double hydroxide with CeCO₃OH as highly efficient water oxidation electrocatalyst[J]. Int J Hydrogen Energy,2021,46(2):2018−2025. doi: 10.1016/j.ijhydene.2020.10.075
[34]	JING F, LIU S, WANG R, et al. Hydrogen production through glycerol steam reforming over the NiCe_xAl catalysts[J]. Renewable Energy,2020,158:192−201. doi: 10.1016/j.renene.2020.05.044
[35]	ZHANG Q, XU R, LIU N, et al. In situ Ce-doped catalyst derived from NiCeAl-LDHs with enhanced low-temperature performance for CO₂ methanation[J]. Appl Surf Sci,2022,579:152204. doi: 10.1016/j.apsusc.2021.152204
[36]	HE C, YU Y, YUE L, et al. Low-temperature removal of toluene and propanal over highly active mesoporous CuCeO_x catalysts synthesized via a simple self-precipitation protocol[J]. Appl Catal B: Environ,2014,147:156−166. doi: 10.1016/j.apcatb.2013.08.039
[37]	YAN Q, GAO Y, LI Y, et al. Promotional effect of Ce doping in Cu₄Al₁O_x – LDO catalyst for low-T practical NH₃-SCR: Steady-state and transient kinetics studies[J]. Appl Catal B: Environ,2019,255:117749. doi: 10.1016/j.apcatb.2019.117749
[38]	YAO X, KANG K, CAO J, et al. Enhancing the denitration performance and anti-K poisoning ability of CeO₂-TiO₂/P25 catalyst by H₂SO₄ pretreatment: Structure-activity relationship and mechanism study[J]. Appl Catal B: Environ,2020,269:118808. doi: 10.1016/j.apcatb.2020.118808
[39]	LI D, LIU X, ZHANG Q, et al. Cobalt and copper composite oxides as efficient catalysts for preferential oxidation of CO in H₂-rich stream[J]. Catal Lett,2008,127(3/4):377−385.
[40]	VARGHESE S, CUTRUFELLO M G, ROMBI E, et al. CO oxidation and preferential oxidation of CO in the presence of hydrogen over SBA-15-templated CuO-Co₃O₄ catalysts[J]. Appl Catal A: Gen,2012,443:161−170.
[41]	IVANOVA S, PETIT C, PITCHON V. A new preparation method for the formation of gold nanoparticles on an oxide support[J]. Appl Catal A: Gen,2004,267(1/2):191−201. doi: 10.1016/j.apcata.2004.03.004
[42]	NIVANGUNE N T, RANADE V V, KELKAR A A. MgFeCe ternary layered double hydroxide as highly efficient and recyclable heterogeneous base catalyst for synthesis of dimethyl carbonate by transesterification[J]. Catal Lett,2017,147(10):2558−2569. doi: 10.1007/s10562-017-2146-x
[43]	YANG H, LIU X, QIN K, et al. Enhancement strategy of photoelectrocatalytic activity of cobalt-copper layer double hydroxide toward methanol oxidation: Cerium doping and modification with porphyrin[J]. Inorg Chem,2022,61(19):7414−7425. doi: 10.1021/acs.inorgchem.2c00438
[44]	DU Y, LIU X, LIU J, et al. DeNO_x performance enhancement of Cu-based oxides via employing a TiO₂ phase to modify LDH precursors[J]. RSC Adv,2022,12(16):10142−10153. doi: 10.1039/D2RA00316C
[45]	WU X, FENG Y, LIU X, et al. Redox & acidity optimizing of LDHs-based CoMnAl mixed oxides for enhancing NH₃-SCR performance[J]. Appl Surf Sci,2019,495:1443513.
[46]	ZANG P, LIU J, HE Y, et al. LDH-derived preparation of CuMgFe layered double oxides for NH₃-SCR and CO oxidation reactions: Performance study and synergistic mechanism[J]. Chem Eng J,2022,446:137414. doi: 10.1016/j.cej.2022.137414
[47]	LI J, ZHU P, ZHOU R. Effect of the preparation method on the performance of CuO-MnO_x-CeO₂ catalysts for selective oxidation of CO in H₂-rich streams[J]. J Power Sources,2011,196(22):9590−9598. doi: 10.1016/j.jpowsour.2011.07.052
[48]	KONSOLAKIS M, CARABINEIRO S A, TAVARES P B, et al. Redox properties and VOC oxidation activity of Cu catalysts supported on Ce_1-xSm_xO delta mixed oxides[J]. J Hazard Mater,2013,261:512−521. doi: 10.1016/j.jhazmat.2013.08.016
[49]	GUO X, WU H, WANG H, et al. Sulfadiazine advanced oxidizing-degradation: Defects generation by boosting electron transfer at interfaces of Co-Cu LDH catalysts[J]. J Environ Chem Eng,2022,10(6):108411. doi: 10.1016/j.jece.2022.108411
[50]	WANG Z, DENG J, LIU Y, et al. Three-dimensionally ordered macroporous CoCr₂O₄-supported Au-Pd alloy nanoparticles: Highly active catalysts for methane combustion[J]. Catal Today,2017,281:467−476. doi: 10.1016/j.cattod.2016.05.035
[51]	HE C, YU Y, CHEN C, et al. Facile preparation of 3D ordered mesoporous CuO_x-CeO₂ with notably enhanced efficiency for the low temperature oxidation of heteroatom-containing volatile organic compounds[J]. RSC Adv,2013,3(42):19639−19656. doi: 10.1039/c3ra42566e
[52]	ZHANG Y, ZHAO L, DUAN J, et al. Insights into deNO_x processing over Ce-modified Cu-BTC catalysts for the CO-SCR reaction at low temperature by in situ DRIFTS[J]. Sep Purif Technol,2020,234:116081. doi: 10.1016/j.seppur.2019.116081
[53]	SUN R, YU F, WAN Y, et al. Reducing N₂O formation over CO-SCR systems with CuCe mixed metal oxides[J]. ChemCatChem,2021,13(11):2709−2718. doi: 10.1002/cctc.202100057
[54]	CAI S, ZHANG D, SHI L, et al. Porous Ni-Mn oxide nanosheets in situ formed on nickel foam as 3D hierarchical monolith de-NO_x catalysts[J]. Nanoscale,2014,6(13):7346−7353. doi: 10.1039/C4NR00475B
[55]	LI L, HAN W, ZHANG J, et al. Controlled pore size of 3D mesoporous Cu-Ce based catalysts and influence of surface textures on the CO catalytic oxidation[J]. Microporous Mesoporpous Mater,2016,231:9−20. doi: 10.1016/j.micromeso.2016.05.018
[56]	LIU Z, LI J, BUETTNER M, et al. Metal-support interactions in CeO₂-and SiO₂-supported cobalt catalysts: Effect of support morphology, reducibility, and interfacial configuration[J]. ACS Appl Mater Interfaces,2019,11(18):17035−17049. doi: 10.1021/acsami.9b02455
[57]	WANG X, ZHANG C, ZHANG Z, et al. Insights into the interfacial effects in Cu-Co/CeO_x catalysts on hydrogenolysis of 5-hydroxymethylfurfural to biofuel 2, 5-dimethylfuran[J]. J Colloid Interf Sci,2022,615:19−29. doi: 10.1016/j.jcis.2022.01.168
[58]	SHEN H, LI H, YANG Z, et al. Magic of hydrogen spillover: Understanding and application[J]. Green Energy Environ,2022,7(6):1161−1198. doi: 10.1016/j.gee.2022.01.013
[59]	XIONG M, GAO Z, QIN Y. Spillover in heterogeneous catalysis: New insights and opportunities[J]. ACS Catal,2021,11(5):3159−3172. doi: 10.1021/acscatal.0c05567