Sulfate promotion of selective catalytic reduction of nitric oxide by ammonia on ceria

Chen, Linxiao; Agrawal, Vaibhav; Tait, Steven L.

doi:10.1039/c8cy02590h

Title: Sulfate promotion of selective catalytic reduction of nitric oxide by ammonia on ceria

Journal Article · Sat Mar 02 00:00:00 EST 2019 · Catalysis Science and Technology

DOI:https://doi.org/10.1039/c8cy02590h· OSTI ID:1612500

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Indiana Univ., Bloomington, IN (United States)

Selective catalytic reduction of nitric oxide by ammonia (NH₃-SCR) is a promising technology for NO_x emission control. In this work, the recently discovered sulfate promotion effect in this reaction was thoroughly investigated on ceria. Sulfates derived from different organic S precursors all exhibit a promotion effect. Mechanistic studies generate a reaction network including both Langmuir–Hinshelwood and Eley–Rideal mechanisms. Sulfates were shown to be versatile promoters with multiple functions: they tune the adsorption of reactants towards a more balanced intermediate coverage by creating strong Lewis acid sites, facilitate *NH₂ formation, and suppress ammonia oxidation through surface oxygen deactivation. The comparison between sulfates and the classic inorganic promoter FeO_x revealed that sulfates are more effective, especially at high temperature. This is mainly attributed to the high coverages of Eley–Rideal intermediates and low ammonia oxidation activity on sulfated ceria. Overall, this work provides fundamental understanding of the role of surface sulfates in NH₃-SCR, which are essential under actual operation conditions. This understanding presents an exciting opportunity for future catalyst design with high durability and low cost.

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Research Organization:: Indiana Univ., Bloomington, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0016367

OSTI ID:: 1612500

Alternate ID(s):: OSTI ID: 1499819

Journal Information:: Catalysis Science and Technology, Vol. 9, Issue 8; ISSN 2044-4753

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 24 works

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In situ DRIFTS-MS studies on the oxidation of adsorbed NH3 by NOx over a Cu-SSZ-13 zeolite Zhu, Haiyang; Kwak, Ja Hun; Peden, Charles H. F. Catalysis Today, Vol. 205 https://doi.org/10.1016/j.cattod.2012.08.043	journal	April 2013
The Origin of an Unexpected Increase in NH ₃ –SCR Activity of Aged Cu-LTA Catalysts Ahn, Nak Ho; Ryu, Taekyung; Kang, Yonjoo ACS Catalysis, Vol. 7, Issue 10 https://doi.org/10.1021/acscatal.7b02852	journal	September 2017
Titania Supported Bimetallic Transition Metal Oxides for Low-Temperature SCR of NO with NH ₃ Sreekanth, Pavani M.; Peña, Donovan A.; Smirniotis, Panagiotis G. Industrial & Engineering Chemistry Research, Vol. 45, Issue 19 https://doi.org/10.1021/ie060485l	journal	September 2006
FTIR in situ mechanistic study of the NH3NO/NO2 “Fast SCR” reaction over a commercial Fe-ZSM-5 catalyst Ruggeri, Maria Pia; Grossale, Antonio; Nova, Isabella Catalysis Today, Vol. 184, Issue 1 https://doi.org/10.1016/j.cattod.2011.10.036	journal	April 2012
Superior ion-exchanged ZSM-5 catalysts for selective catalytic oxidation of ammonia to nitrogen Long, Richard Q.; Yang, Ralph T. Chemical Communications, Issue 17 https://doi.org/10.1039/b004957n	journal	January 2000
SO2 poisoning impact on the NH3-SCR reaction over a commercial Cu-SAPO-34 SCR catalyst Zhang, Li; Wang, Di; Liu, Yong Applied Catalysis B: Environmental, Vol. 156-157 https://doi.org/10.1016/j.apcatb.2014.03.030	journal	September 2014
Deactivation of PdO–Al2O3 oxidation catalyst in lean-burn natural gas engine exhaust: aged catalyst characterization and studies of poisoning by H2O and SO2 Mowery, Deborah L.; Graboski, Michael S.; Ohno, Tim R. Applied Catalysis B: Environmental, Vol. 21, Issue 3 https://doi.org/10.1016/S0926-3373(99)00017-X	journal	July 1999
MnO _x −CeO ₂ Binary Oxides for Catalytic NO _x Sorption at Low Temperatures. Sorptive Removal of NO _x Machida, Masato; Uto, Masatoshi; Kurogi, Daisuke Chemistry of Materials, Vol. 12, Issue 10 https://doi.org/10.1021/cm000207r	journal	October 2000
Impact of nitrogen oxides on the environment and human health: Mn-based materials for the NO x abatement Boningari, Thirupathi; Smirniotis, Panagiotis G. Current Opinion in Chemical Engineering, Vol. 13 https://doi.org/10.1016/j.coche.2016.09.004	journal	August 2016
Fourier transform-infrared study of the adsorption and coadsorption of nitric oxide, nitrogen dioxide and ammonia on vanadia-titania and mechanism of selective catalytic reduction Ramis, Gianguido; Busca, G.; Bregani, F. Applied Catalysis, Vol. 64 https://doi.org/10.1016/S0166-9834(00)81565-1	journal	September 1990
Transmission FT-IR and Knudsen Cell Study of the Heterogeneous Reactivity of Gaseous Nitrogen Dioxide on Mineral Oxide Particles Underwood, G. M.; Miller, T. M.; Grassian, V. H. The Journal of Physical Chemistry A, Vol. 103, Issue 31 https://doi.org/10.1021/jp991586i	journal	August 1999

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Improvement in alkali metal resistance of commercial V2O5–WO3/TiO2 SCR catalysts modified by Ce and Cu Li, Huirong; Miao, Jifa; Su, Qingfa Journal of Materials Science, Vol. 54, Issue 24 https://doi.org/10.1007/s10853-019-03919-5	journal	August 2019

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