Gold boosts nitrate reduction and deactivation resistance to indium-promoted palladium catalysts

Sujin Guo; Hao Li; Kimberly N. Heck; Xinying Luan; Wenhua Guo; Graeme Henkelman; Michael S. Wong

doi:10.1016/j.apcatb.2021.121048

Gold boosts nitrate reduction and deactivation resistance to indium-promoted palladium catalysts

Sujin Guo, Hao Li, Kimberly N. Heck, Xinying Luan, Wenhua Guo, Graeme Henkelman, Michael S. Wong

Research output: Contribution to journal › Article › peer-review

14 Citations (Scopus)

Abstract

In-decorated PdAu catalysts were synthesized and investigated for the aqueous reduction of nitrate. We first synthesized PdAu nanoparticles (NPs) with varying Pd:Au ratios onto which we deposited In. These In-on-PdAu NPs showed higher activity than In-on-Pd NPs for NO₃^- (k_cat=4.0–7.2 vs 2.7 L/g_{total_(Pd+In)}/min) due to electronic and ensemble effects. Au-rich NPs had lower activity (k_cat=1.3–1.5 L/g_{total_(Pd+In)}/min) due to unfavorable hydrogen and nitrate/nitrite binding energies. In-on-PdAu NPs showed higher N₂ selectivity than In-on-Pd NPs (90 +% vs 60% at 40% conversion), and had higher activity for NO₂^-. Density functional theory calculations suggest that Au weakens metal-N bonding which enables nitrite reduction over Pd. Nitrate reduction is promoted by greater mobility of H-adatoms to regenerate InO_x and faster spillover of nitrite onto PdAu. When challenged with species found in drinking water, the trimetallic NPs were more active than bimetallic NPs (1.0–1.6 vs 0.6 L/g_{total_(Pd+In)}/min). These results expand the prospects of practical catalytic denitrification.

Original language	English
Article number	121048
Journal	Applied Catalysis B: Environmental
Volume	305
DOIs	https://doi.org/10.1016/j.apcatb.2021.121048
Publication status	Published - 2022 May 15
Externally published	Yes

Keywords

Deactivation resistance
Gold, palladium
Nitrate reduction
Trimetallic catalysts

ASJC Scopus subject areas

Catalysis
Environmental Science(all)
Process Chemistry and Technology

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10.1016/j.apcatb.2021.121048

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@article{dedf37db8ba64202a158ed262ee77887,

title = "Gold boosts nitrate reduction and deactivation resistance to indium-promoted palladium catalysts",

abstract = "In-decorated PdAu catalysts were synthesized and investigated for the aqueous reduction of nitrate. We first synthesized PdAu nanoparticles (NPs) with varying Pd:Au ratios onto which we deposited In. These In-on-PdAu NPs showed higher activity than In-on-Pd NPs for NO3- (kcat=4.0–7.2 vs 2.7 L/gtotal_(Pd+In)/min) due to electronic and ensemble effects. Au-rich NPs had lower activity (kcat=1.3–1.5 L/gtotal_(Pd+In)/min) due to unfavorable hydrogen and nitrate/nitrite binding energies. In-on-PdAu NPs showed higher N2 selectivity than In-on-Pd NPs (90 +% vs 60% at 40% conversion), and had higher activity for NO2-. Density functional theory calculations suggest that Au weakens metal-N bonding which enables nitrite reduction over Pd. Nitrate reduction is promoted by greater mobility of H-adatoms to regenerate InOx and faster spillover of nitrite onto PdAu. When challenged with species found in drinking water, the trimetallic NPs were more active than bimetallic NPs (1.0–1.6 vs 0.6 L/gtotal_(Pd+In)/min). These results expand the prospects of practical catalytic denitrification.",

keywords = "Deactivation resistance, Gold, palladium, Nitrate reduction, Trimetallic catalysts",

author = "Sujin Guo and Hao Li and Heck, {Kimberly N.} and Xinying Luan and Wenhua Guo and Graeme Henkelman and Wong, {Michael S.}",

note = "Funding Information: M.S.W. and S.G. acknowledge partial financial support from the NSF Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment ( EEC-1449500 ) and the China Scholarship Council. The calculations by H.L. and G.H. were supported by the Welch Foundation ( F-1841 ) and the Texas Advanced Computing Center. We dedicate this work in memory of our friend, Dr. Maria Flytzani-Stephanopoulos. Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2022",

month = may,

day = "15",

doi = "10.1016/j.apcatb.2021.121048",

language = "English",

volume = "305",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

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TY - JOUR

T1 - Gold boosts nitrate reduction and deactivation resistance to indium-promoted palladium catalysts

AU - Guo, Sujin

AU - Li, Hao

AU - Heck, Kimberly N.

AU - Luan, Xinying

AU - Guo, Wenhua

AU - Henkelman, Graeme

AU - Wong, Michael S.

N1 - Funding Information: M.S.W. and S.G. acknowledge partial financial support from the NSF Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment ( EEC-1449500 ) and the China Scholarship Council. The calculations by H.L. and G.H. were supported by the Welch Foundation ( F-1841 ) and the Texas Advanced Computing Center. We dedicate this work in memory of our friend, Dr. Maria Flytzani-Stephanopoulos. Publisher Copyright: © 2022 Elsevier B.V.

PY - 2022/5/15

Y1 - 2022/5/15

N2 - In-decorated PdAu catalysts were synthesized and investigated for the aqueous reduction of nitrate. We first synthesized PdAu nanoparticles (NPs) with varying Pd:Au ratios onto which we deposited In. These In-on-PdAu NPs showed higher activity than In-on-Pd NPs for NO3- (kcat=4.0–7.2 vs 2.7 L/gtotal_(Pd+In)/min) due to electronic and ensemble effects. Au-rich NPs had lower activity (kcat=1.3–1.5 L/gtotal_(Pd+In)/min) due to unfavorable hydrogen and nitrate/nitrite binding energies. In-on-PdAu NPs showed higher N2 selectivity than In-on-Pd NPs (90 +% vs 60% at 40% conversion), and had higher activity for NO2-. Density functional theory calculations suggest that Au weakens metal-N bonding which enables nitrite reduction over Pd. Nitrate reduction is promoted by greater mobility of H-adatoms to regenerate InOx and faster spillover of nitrite onto PdAu. When challenged with species found in drinking water, the trimetallic NPs were more active than bimetallic NPs (1.0–1.6 vs 0.6 L/gtotal_(Pd+In)/min). These results expand the prospects of practical catalytic denitrification.

AB - In-decorated PdAu catalysts were synthesized and investigated for the aqueous reduction of nitrate. We first synthesized PdAu nanoparticles (NPs) with varying Pd:Au ratios onto which we deposited In. These In-on-PdAu NPs showed higher activity than In-on-Pd NPs for NO3- (kcat=4.0–7.2 vs 2.7 L/gtotal_(Pd+In)/min) due to electronic and ensemble effects. Au-rich NPs had lower activity (kcat=1.3–1.5 L/gtotal_(Pd+In)/min) due to unfavorable hydrogen and nitrate/nitrite binding energies. In-on-PdAu NPs showed higher N2 selectivity than In-on-Pd NPs (90 +% vs 60% at 40% conversion), and had higher activity for NO2-. Density functional theory calculations suggest that Au weakens metal-N bonding which enables nitrite reduction over Pd. Nitrate reduction is promoted by greater mobility of H-adatoms to regenerate InOx and faster spillover of nitrite onto PdAu. When challenged with species found in drinking water, the trimetallic NPs were more active than bimetallic NPs (1.0–1.6 vs 0.6 L/gtotal_(Pd+In)/min). These results expand the prospects of practical catalytic denitrification.

KW - Deactivation resistance

KW - Gold, palladium

KW - Nitrate reduction

KW - Trimetallic catalysts

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DO - 10.1016/j.apcatb.2021.121048

M3 - Article

AN - SCOPUS:85122624714

SN - 0926-3373

VL - 305

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 121048

ER -

Gold boosts nitrate reduction and deactivation resistance to indium-promoted palladium catalysts

Abstract

Keywords

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