Theoretical study on effect of additive Ni on catalytic reduction of NO by NH<sub>3</sub> on Cu(111) surface

WANG Xuhui; GUO Yang; WU Jiao; GUO Congxiu; NIU Yu

doi:10.12434/j.issn.2097-2547.20230415

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Theoretical study on effect of additive Ni on catalytic reduction of NO by NH₃ on Cu(111) surface

- Theoretical study on effect of additive Ni on catalytic reduction of NO by NH₃ on Cu(111) surface
- Vol. 49, Issue 10, Pages: 66-71(2024)
- 作者机构：
  
  1.山西大学电力与建筑学院，山西太原 030006
  2.中国能源建设集团广东火电工程有限公司，广东广州 510735
- 作者简介：
- 基金信息：
- DOI：10.12434/j.issn.2097-2547.20230415
  CLC： TQ426;O643.32
- Published：25 October 2024，
  
  Received：18 December 2023，
  
  Revised：24 January 2024，
- 稿件说明：
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王旭慧,郭洋,吴娇等.助剂Ni对Cu(111)表面催化NH₃还原NO反应影响的理论研究[J].低碳化学与化工,2024,49(10):66-71.

WANG Xuhui,GUO Yang,WU Jiao,et al.Theoretical study on effect of additive Ni on catalytic reduction of NO by NH₃ on Cu(111) surface[J].Low-carbon Chemistry and Chemical Engineering,2024,49(10):66-71.
王旭慧,郭洋,吴娇等.助剂Ni对Cu(111)表面催化NH₃还原NO反应影响的理论研究[J].低碳化学与化工,2024,49(10):66-71. DOI： 10.12434/j.issn.2097-2547.20230415.

WANG Xuhui,GUO Yang,WU Jiao,et al.Theoretical study on effect of additive Ni on catalytic reduction of NO by NH₃ on Cu(111) surface[J].Low-carbon Chemistry and Chemical Engineering,2024,49(10):66-71. DOI： 10.12434/j.issn.2097-2547.20230415.

摘要

针对商用钒钛脱硝催化剂存在的环境污染和易中毒问题，采用无毒环保的单金属铜催化剂并使用助剂Ni掺杂提高其脱硝性能。基于密度泛函理论（DFT），探究了助剂Ni对Cu(111)表面催化NH

还原NO反应的影响。通过分析催化剂表面反应物种的吸附、反应机理和电子结构，对比了助剂Ni掺杂前后Cu(111)表面的催化活性。结果表明，所有反应物种在CuNi(111)表面上的吸附效果均优于在Cu(111)表面的吸附效果。CuNi(111)表面发生的三步基元反应需克服的能垒均低于Cu(111)表面，其中，速控步骤（NH

NO → N

+ H

O）的能垒降低了63.6 kJ/mol，可见CuNi(111)表面催化活性明显较高。相比Cu(111)表面，CuNi(111)表面的

带中心更靠近费米能级，说明助剂Ni的掺杂增强了Cu(111)表面电子的活跃性，从而提高了其催化活性。

Abstract

In view of the environmental pollution and easy poisoning problems of commercial vanadium-titanium denitrification catalys

a non-toxic and environmentally friendly single-metal copper catalyst was used and the addition of additive Ni was used to improve its denitrification performance. Based on density functional theory (DFT)

the effect of additive Ni on the catalytic reduction of NO by NH

on Cu(111) surface was investigated. By analyzing the adsorption of reactive species

reaction mechanism and electronic structure on the catalysts surface

the catalytic activities of Cu(111) surface before and after additive Ni doping were compared. The results show that the adsorption effect of all reactive species on the CuNi(111) surface is better than that on the Cu(111) surface. The energy barriers for the three elementary reactions occurring on the CuNi(111) surface are lower than those on the Cu(111) surface

among which the energy barrier for the rate-determining step (NH

NO → N

+ H

O) decreases by 63.6 kJ/mol

indicating that the catalytic activity of CuNi(111) surface is significantly higher. Compared with the Cu(111) surface

the

-band center of the CuNi(111) surface is closer to the Fermi level

indicating that the doping of additive Ni enhances the electronic activity of the Cu(111) surface

thereby improving its catalytic activity.

关键词

Cu表面Ni助剂脱硝密度泛函理论

Keywords

Cu surfaceadditive Nidenitrificationdensity functional theory

references

CHEN C, FENG C, WANG Y X, et al. Design of robust Co-doped Mn3O4 spinel catalysts for selective catalytic reduction of NO with NH3 at low temperatures [J]. Applied Surface Science, 2022, 602: 154384.

JONES C B, KHURANA I, KRISHNA S H, et al. Effects of dioxygen pressure on rates of NOx selective catalytic reduction with NH3 on Cu-CHA zeolites [J]. Journal of Catalysis, 2020, 389: 140-149.

LUO W, RONG J, ZHAO W X, et al. Morphology and crystal-plane dependence of CeO2-TiO2 catalysts: Activity and mechanism for the selective catalytic reduction of NOx with NH3 [J]. Chemical Engineering Journal, 2022, 444 (2): 136488.

HU W S, ZOU R Z, DONG Y, et al. Synergy of vanadia and ceria in the reaction mechanism of low-temperature selective catalytic reduction of NOx by NH3 [J]. Journal of Catalysis, 2020, 391: 145-154.

LIU Y Z, GUO R T, DUAN C P, et al. A highly effective urchin-like MnCrOx catalyst for the selective catalytic reduction of NOx with NH3 [J]. Fuel, 2020, 271(3): 117667.

ZHU N, SHAN W P, SHAN Y L, et al. Effects of alkali and alkaline earth metals on Cu-SSZ-39 catalyst for the selective catalytic reduction of NOx with NH3 [J]. Chemical Engineering Journal, 2020, 388(10): 124250.

GAO E H, PAN H, ZHANG W, et al. Insights on the mechanism of enhanced selective catalytic reduction of NO with NH3 over Zr-doped MnCr2O4: A combination of in situ DRIFTS and DFT [J]. Chemical Engineering Journal, 2020, 386: 123956.

LV W, MENG P, QIN Z, et al. A comparison of Al-rich Cu-SSZ-13 zeolites synthesized by different methods in their Al distribution, hydrothermal stability and catalytic performance in the selective catalytic reduction of NOx with NH3 [J]. Microporous Mesoporous Mater, 2021, 313(9): 110851.

LI Y, LI Y P, WANG P F, et al. Low-temperature selective catalytic reduction of NOx with NH3 over MnFeOx nanorods [J]. Chemical Engineering Journal, 2017, 330: 213-222.

XUE L, ZHANG C B, HE H, et al. Catalytic decomposition of N2O over CeO2 promoted Co3O4 spinel catalyst [J]. Applied Catalysis B: Environmental, 2007, 75(3/4): 167-174.

PU Y J, XIE X Y, JIANG W J, et al. Low-temperature selective catalytic reduction of NOx with NH3 over zeolite catalysts: A review [J]. Chinese Chemical Letter, 2020, 31(10): 2549-2555.

SI W Z, LIU H Y, YAN T, et al. Sn-doped rutile TiO2 for vanadyl catalysts: Improvements on activity and stability in SCR reaction [J]. Applied Catalysis B: Environmental, 2020, 269(2): 118797.

ZHAO X Y, MA S B, LI Z B, et al. Synthesis of CenTiOx flakes with hierarchical structure and its enhanced activity for selective catalytic reduction of NOx with NH3 [J]. Chemical Engineering Journal, 2020, 392(9): 123801.

SI W Z, LIU H Y, YAN T, et al. Sn-doped rutile TiO2 for vanadyl catalysts: Improvements on activity and stability in SCR reaction [J]. Applied Catalysis B: Environmental, 2020, 269(11): 118797.

孟繁伟, 高琦, 叶青, 等. Cu-SAPO-18催化剂氨选择性催化还原NOx钾中毒机理的研究 [J]. 高等化学学报, 2021, 41(9): 2832-2841.

MENG F W, GAO Q, YE Q, et al. Potassium poisoning mechanism of Cu-SAPO-18 catalyst for selective catalytic reduction of NOx by ammonia [J]. Chemical Journal of Chinese Universities, 2021, 41(9): 2832-2841.

CHEN R Y, FANG X Y, LI J H, et al. Mechanistic investigation of the enhanced SO2 resistance of Co-modified MnOx catalyst for the selective catalytic reduction of NOx by NH3 [J]. Chemical Engineering Journal, 2023, 452: 139207.

JEON S W, SONG I, LEE H, et al. Enhanced SO2 resistance of V2O5/WO3-TiO2 catalyst physically mixed with alumina for the selective catalytic reduction of NOx with NH3 [J]. Chemical Engineering Journal, 2022, 433: 133836.

YOON W, KIM Y, JONG K G, et al. Boosting low temperature De-NOx performance and SO2 resistance over Ce-doped two dimensional Mn-Cr layered double oxide catalyst [J]. Chemical Engineering Journal, 2022, 434: 134676.

QIN B, GUO R T, ZHOU J, et al. Promotional role of Nb modification on CuCeOx catalyst for low temperature selective catalytic reduction of NO with NH3: A mechanism investigatio [J]. Fuel, 2022, 329(7): 125390.

QI K, XIE J L, FANG D, et al. Phase segregation studies on role plays and synergies in supported CuSO4/TiO2 catalysts for NO abatement based on experimental and theoretical investigations [J]. Journal of Clean Production, 2020, 256: 120411.

ZENG Y Q, WANG T X, ZHANG S L, et al. Sol-gel synthesis of CuO-TiO2 catalyst with high dispersion CuO species for selective catalytic oxidation of NO [J]. Applied Surface Science, 2017, 411: 227-234.

WAN J P, YANG H P, SHI Y J, et al. Effect of Cu loading content on the catalytic performance of Cu-USY catalysts for selective catalytic reduction of NO with NH3 [J]. Journal of Environmental Science (China), 2023, 126: 445-458.

SI Z C, WENG D, WU X D, et al. Structure, acidity and activity of CuOx/WOx-ZrO2 catalyst for selective catalytic reduction of NO by NH3 [J]. Journal of Catalysis, 2010, 271(1): 43-51.

下转第80页)

SHWAN S, SKOGLUNDH M, LUNDEGAARD L F, et al. Solid-state ion-exchange of copper into zeolites facilitated by ammonia at low temperature [J]. ACS Catalysis, 2015, 5(1): 16-19.

LIU X S, WU X D, WENG D, et al. Evolution of copper species on Cu/SAPO-34 SCR catalysts upon hydrothermal aging [J]. Catalysis Today, 2017, 281: 596-604.

YE D, WANG X X, LIU H, et al. Insights into the effects of sulfate species on CuO/TiO2 catalysts for NH3-SCR reactions [J]. Molecular Catalysis, 2020, 496: 111191.

GRYBO J, FEDYNA M, MOZGAWA B, et al. Mechanistic stages of the SCR reaction-Insights into the trade-off between NO reduction and NH3 oxidation over CuSSZ-13 catalysts via isotopic 15NH3 and 18O2 TPSR and steady state studies supported by IR 2D COS and and DFT modeling [J]. Applied Catalysis B: Environmental, 2023, 325(2): 122309.

朱晓. 活性炭低温NH3选择性催化还原NOx及强化机制 [D]. 济南: 山东大学, 2022.

ZHU X. Selective catalytic reduction of NOx and enhancement mechanism by NH3 at low temperture on activated carbon catalysts [D]. Jinan: Shandong university, 2022.

HAN B Y, LING L X, FAN M, et al. A DFT study and microkinetic analysis of CO oxidation to dimethyl oxalate over Pd stripe and Pd single atom-doped Cu(111) surfaces [J]. Applied Surface Science, 2019, 479(79): 1057-1067.

AN J W, WANG X H, ZHAO J X, et al. Density-functional theory study on hydrogenation of dimethyl oxalate to methyl glycolate over copper catalyst: Effect of copper valence state [J]. Molecular Catalysis, 2019, 482(6): 110667.

王智瑶, 方志刚, 曾鑫渔, 等. 基于密度泛函理论的团簇Co3MoS催化性质研究[J]. 天然气化工—C1化学与化工, 2021, 46(5): 55-61.

WANG Z Y, FANG Z G, ZENG X Y, et al. Study on catalytic properties of cluster Co3MoS based on density functional theory [J]. Natural Gas Chemical Industry, 2021, 46(5): 55-61.

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Theoretical study on effect of additive Ni on catalytic reduction of NO by NH3 on Cu(111) surface

DOI：10.12434/j.issn.2097-2547.20230415

摘要

Abstract

关键词

Keywords

references

Theoretical study on effect of additive Ni on catalytic reduction of NO by NH₃ on Cu(111) surface