Mechanism of heterogeneous reduction of NO over graphite-supported single-atom Fe catalyst: DFT study

ZHAO Yan; LI Xiang; HUANG Jinkai; LI Xianchun; ZHU Yaming; WANG Huanran

doi:10.1016/S1872-5813(23)60407-4

Volume 52 Issue 5

May 2024

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2024 > 52(5): 717-724

ZHAO Yan, LI Xiang, HUANG Jinkai, LI Xianchun, ZHU Yaming, WANG Huanran. Mechanism of heterogeneous reduction of NO over graphite-supported single-atom Fe catalyst: DFT study[J]. Journal of Fuel Chemistry and Technology, 2024, 52(5): 717-724. doi: 10.1016/S1872-5813(23)60407-4

Citation:

ZHAO Yan, LI Xiang, HUANG Jinkai, LI Xianchun, ZHU Yaming, WANG Huanran. Mechanism of heterogeneous reduction of NO over graphite-supported single-atom Fe catalyst: DFT study[J]. Journal of Fuel Chemistry and Technology, 2024, 52(5): 717-724. doi: 10.1016/S1872-5813(23)60407-4

Citation:

ZHAO Yan, LI Xiang, HUANG Jinkai, LI Xianchun, ZHU Yaming, WANG Huanran. Mechanism of heterogeneous reduction of NO over graphite-supported single-atom Fe catalyst: DFT study[J]. Journal of Fuel Chemistry and Technology, 2024, 52(5): 717-724. doi: 10.1016/S1872-5813(23)60407-4

PDF( 5096 KB)

Mechanism of heterogeneous reduction of NO over graphite-supported single-atom Fe catalyst: DFT study

doi: 10.1016/S1872-5813(23)60407-4

ZHAO Yan^1
,,
LI Xiang^1
,,
HUANG Jinkai^1
,,
LI Xianchun^2
,,
ZHU Yaming^2
,,
WANG Huanran^{1
,
,}

1.
University of Science and Technology Liaoning School of Civil Engineering, Anshan 114051, China
2.
University of Science and Technology Liaoning School of Chemical Engineering, Anshan 114051, China

Funds: The project was supported by Youth Project of Liaoning Department of Education (JYTQN2023237).

Received Date: 2023-11-30
Accepted Date: 2023-12-27
Rev Recd Date: 2023-12-27

Available Online: 2024-01-18

Publish Date: 2024-05-01

Abstract

Abstract

The mechanism of nitrogen oxide (NO) reduction over graphite carbon-supported single-atom iron (Fe) catalyst (Fe/G) was investigated by density functional theory (DFT) and transition state theory (TST). The catalyst deactivation was also analyzed. The results revealed that the NO reduction, based on the Eley-Rideal (E-R) mechanism, underwent four stages including N₂O formation and release as well as N₂ formation and release. However, the NO reduction only involved two stages according to Langmuir-Hinshelwood (L-H) mechanism: N₂ formation and release. Furthermore, for the E-R mechanism, the rate-controlling step was NO reduction, where a NO molecule was adsorbed on an Fe atom with an N, O-down structure with energy barrier of 15.5 kJ/mol, lower than that of other paths. Energy barrier analysis indicated that the energy barrier for the reduction of reactive oxygen species was higher than that for the formation of N₂. Reactive oxygen species remaining on the surface of Fe atoms after NO decomposition inhibited the adsorption and reduction of NO, leading to catalyst deactivation due to the absence of active sites. The single-atom Fe species promoted the NO reduction. Kinetic analysis results suggested that, upon increasing the reaction temperature, the NO reduction rate increased more significantly than the reactive oxygen transfer rate.
- singe-atom Fe catalyst,
- nitrogen oxides,
- density functional theory,
- mechanism,
- deactivation

FullText(HTML)

References(31)

References

[1]	孙锦昌, 任翠涛, 赵明新, 等. Cu/H_β催化剂NH₃选择性催化还原NO性能研究[J]. 燃料化学学报(中英文),2023,51(6):823−831. SUN Jinchang, REN Cuitao, ZHAO Mingxin, et al. Selective catalytic reduction of NO by Cu/H_β catalyst NH₃[J]. J Fuel Chem Technol,2023,51(6):823−831.
[2]	WU G, FENG X, ZHANG H, et al. The promotional role of Ni in FeVO₄/TiO₂ monolith catalyst for selective catalytic reduction of NO_x with NH₃[J]. Appl Surf Sci,2018,427:24−36. doi: 10.1016/j.apsusc.2017.08.135
[3]	ZHOU Y, REN S, WANG M, et al. Mn and Fe oxides co-effect on nanopolyhedron CeO₂ catalyst for NH₃-SCR of NO[J]. J Energy Inst,2021,99:97−104. doi: 10.1016/j.joei.2021.08.003
[4]	LIU S, XUE W, JI Y, et al. Interfacial oxygen vacancies at Co₃O₄-CeO₂ heterointerfaces boost the catalytic reduction of NO by CO in the presence of O₂[J]. Appl Catal B: Environ,2023,323:122151. doi: 10.1016/j.apcatb.2022.122151
[5]	吕文婷, 焦卫勇, 秦张峰, 等. 制备条件对Cu-SSZ-13分子筛的形貌及其氨选择性催化还原脱硝性能的影响[J]. 燃料化学学报,2022,50(11):1393−1403. LÜ Wenting, JIAO Weiyong, QIN Zhangfeng, et al. Effect of preparation conditions on the morphology of Cu-SSZ-13 molecular sieve and its denitrification performance by selective catalytic reduction of ammonia[J]. J Fuel Chem Technol,2022,50(11):1393−1403.
[6]	OTON L F, OLIXEIRA A C, DE ARAUJO J C S, et al. Selective catalytic reduction of NO_x by CO (CO-SCR) over metal-supported nanoparticles dispersed on porous alumina[J]. Adv Powder Technol,2020,31:464−476. doi: 10.1016/j.apt.2019.11.003
[7]	张恒, 周皞, 温妮妮, 等. Cu-SAPO-44选择性催化丙烯还原NO性能研究[J]. 燃料化学学报,2022,50(18):1064−1074. ZHANG Heng, ZHOU Hao, WEN Nini, et al. Study on the performance of Cu-SAPO-44 selective catalytic reduction of NO by propylene[J]. J Fuel Chem Technol,2022,50(18):1064−1074.
[8]	WANG H, LI X, ZHU M, et al. Preparation and evaluation of catalysts of highly dispersed zerovalent iron (Fe⁰) supported on activated carbon for NO reduction[J]. Fuel,2021,303:121252. doi: 10.1016/j.fuel.2021.121252
[9]	YIN P, YAO T, WU Y, et al. Single cobalt atoms with precise N-coordination as superior oxygen reduction reaction catalysts[J]. Angew Chem Int Ed,2016,55:10800−10805. doi: 10.1002/anie.201604802
[10]	CUI T, LI L, YE C, et al. Heterogeneous single atom environmental catalysis: Fundamentals, applications, and opportunities[J]. Adv Funct Mater,2021,32:2108381.
[11]	张艺严, 陈熙元, 董灵玉, 等. 炭载单原子催化剂在电还原二氧化碳领域的研究进展[J]. 燃料化学学报(中英文),2023,51(11):1617−1632. ZHANG Yiyan, CHEN Xiyuan, DONG Lingyu, et al. Research progress in the field of electroreduction of carbon dioxide by carbon supported single atom catalyst[J]. J Fuel Chem Technol,2023,51(11):1617−1632.
[12]	QIAO B, WANG A, YANG X, et al. Single-atom catalysis of CO oxidation using Pt₁/FeO_x[J]. Nat Chem,2011,3:634−641. doi: 10.1038/nchem.1095
[13]	裴永丽, 郭长江, 张宁, 等. 原子层沉积制备纳米催化剂研究进展[J]. 燃料化学学报,2021,49(9):1281−1293. PEI Yongli, GUO Changjiang, ZHANG Ning, et al. Research progress on preparation of nanocatalysts by atomic layer deposition[J]. J Fuel Chem Technol,2021,49(9):1281−1293.
[14]	JI Y, LIU S, SONG S, et al. Negatively charged single-atom Pt catalyst shows superior SO₂ tolerance in NO_x reduction by CO[J]. ACS Catal,2022,13:224−236.
[15]	YUE S, WANG C, XU Z, et al. A theoretical exploration of the effect and mechanism of CO on NO₂ heterogeneous reduction over carbonaceous surfaces[J]. Fuel,2021,290:120102. doi: 10.1016/j.fuel.2020.120102
[16]	YAMASHITA H, YAMADA H, TOMITA A. Reaction of nitric oxide with metal-loaded carbon in the presence of oxygen[J]. Appl Catal A: Gen,1991,78:L1−L6. doi: 10.1016/0166-9834(91)80101-2
[17]	DENG C, SU Y, LI F, et al. Understanding activity origin for the oxygen reduction reaction on bi-atom catalysts by DFT studies and machine-learning[J]. J Mater Chem A,2020,8:24563−24571. doi: 10.1039/D0TA08004G
[18]	WANG H, LI X, MENG F, et al. Preparation and evaluation of iron nanoparticles embedded CNTs grown on ZSM-5 as catalysts for NO decomposition[J]. Chem Eng J,2020,392:123798. doi: 10.1016/j.cej.2019.123798
[19]	ZHANG X, WU H, XIE M, et al. A thorough theoretical exploration of the effect mechanism of Fe on HCN heterogeneous formation from nitrogen-containing char[J]. Fuel,2020,280:118662. doi: 10.1016/j.fuel.2020.118662
[20]	WANG H, LI X, WU J, et al. An experimental and density functional theory simulation study of NO reduction mechanisms over Fe(0) supported on graphene with and without CO[J]. Langmuir,2023,39:15369−15379. doi: 10.1021/acs.langmuir.3c02461
[21]	ZHANG H, LIU J, SHEN J, et al. Thermodynamic and kinetic evaluation of the reaction between NO (nitric oxide) and char(N) (char bound nitrogen) in coal combustion[J]. Nat Energy,2015,82:312−321. doi: 10.1016/j.energy.2015.01.040
[22]	SANTOS J C D S D, FERREIRA D F S, DA SILVA C A B, et al. Transitions in electrical behavior of molecular devices based on 1-D and 2-D graphene-phagraphene-graphene hybrid heterojunctions[J]. Mater Chem Phys,2020,253:123420. doi: 10.1016/j.matchemphys.2020.123420
[23]	CHEN N, YANG R T. Ab initio molecular orbital calculation on graphite: Selection of molecular system and model chemistry[J]. Carbon,1998,36:1061−1070. doi: 10.1016/S0008-6223(98)00078-5
[24]	HU L, HU X, WU X, et al. Density functional calculation of transition metal adatom adsorption on graphene[J]. Physica B Condens Matter,2010,405:3337−3341. doi: 10.1016/j.physb.2010.05.001
[25]	MANADE M, VINES F, ILLAS F. Transition metal adatoms on graphene: A systematic density functional study[J]. Carbon,2015,95:525−534. doi: 10.1016/j.carbon.2015.08.072
[26]	BAI Y, BIAN X, WU W. Catalytic properties of CuO/CeO₂-Al₂O₃ catalysts for low concentration NO reduction with CO[J]. Appl Surf Sci,2019,463:435−444. doi: 10.1016/j.apsusc.2018.08.229
[27]	LU T, CHEN Q. Shermo: A general code for calculating molecular thermochemistry properties[J]. Comput Theor Chem,2021,1200:113249. doi: 10.1016/j.comptc.2021.113249
[28]	张秀霞, 谢苗, 伍慧喜, 等. 钙对焦炭非均相还原NO的微观作用机理: DFT研究[J]. 燃料化学学报,2020,48(2):163−171. ZHANG Xiuxia, XIE Miao, WU Huixi, et al. The microscopic mechanism of heterogeneous reduction of NO by calcium in coke: A DFT study[J]. J Fuel Chem Technol,2020,48(2):163−171.
[29]	YANG L, YANG H, LIU Q, et al. Study on the Reaction Performance of Ce- and Co-Modified Mn-Based Catalysts in C₃H₆-SCR[J]. J Phys Chem C,2023,127:15278−15289. doi: 10.1021/acs.jpcc.3c04279
[30]	WANG B, XIONG Y, HAN Y, et al. Preparation of stable and highly active Ni/CeO₂ catalysts by glow discharge plasma technique for glycerol steam reforming[J]. Appl Catal B: Environ,2019,249:257−265. doi: 10.1016/j.apcatb.2019.02.074
[31]	张峰, 孙浩, 张建树, 等. Fe的分散程度对煤焦催化加氢气化的影响[J]. 燃料化学学报,2019,47(4):402−410. ZHANG Feng, SUN Hao, ZHANG Jianshu, et al. Effect of Fe dispersion degree on catalytic hydrogasification of coal coke[J]. J Fuel Chem Technol,2019,47(4):402−410.