Design of a Pd–Au Nitrite Reduction Catalyst by Identifying and Optimizing Active Ensembles

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dc.citation.firstpage7957en_US
dc.citation.issueNumber9en_US
dc.citation.journalTitleACS Catalysisen_US
dc.citation.lastpage7966en_US
dc.citation.volumeNumber9en_US
dc.contributor.authorLi, Haoen_US
dc.contributor.authorGuo, Sujinen_US
dc.contributor.authorShin, Kihyunen_US
dc.contributor.authorWong, Michael S.en_US
dc.contributor.authorHenkelman, Graemeen_US
dc.date.accessioned2019-10-25T17:53:33Zen_US
dc.date.available2019-10-25T17:53:33Zen_US
dc.date.issued2019en_US
dc.description.abstractNitrate (NO3–) is a ubiquitous contaminant in groundwater that causes serious public health issues around the world. Though various strategies are able to reduce NO3– to nitrite (NO2–), a rational catalyst design strategy for NO2– removal has not been found, in part because of the complicated reaction network of nitrate chemistry. In this study, we show, through catalytic modeling with density functional theory (DFT) calculations, that the performance of mono- and bimetallic surfaces for nitrite reduction can be rapidly screened using N, N2, and NH3 binding energies as reactivity descriptors. With a number of active surface atomic ensembles identified for nitrite reduction, we have designed a series of “metal-on-metal” bimetallics with optimized surface reactivity and a maximum number of active sites. Choosing Pd-on-Au nanoparticles (NPs) as candidate catalysts, both theory and experiment find that a thin monolayer of Pd-on-Au NPs (size: ∼4 nm) leads to high nitrite reduction performance, outperforming pure Pd NPs and the other Pd surface compositions considered. Experiments show that this thin layer of Pd-on-Au has a relatively high selectivity for N2 formation, compared to pure Pd NPs. More importantly, our study shows that a simple model, based upon DFT-calculated thermodynamic energies, can facilitate catalysts design relevant to environmental issues.en_US
dc.identifier.citationLi, Hao, Guo, Sujin, Shin, Kihyun, et al.. "Design of a Pd–Au Nitrite Reduction Catalyst by Identifying and Optimizing Active Ensembles." <i>ACS Catalysis,</i> 9, no. 9 (2019) American Chemical Society: 7957-7966. https://doi.org/10.1021/acscatal.9b02182.en_US
dc.identifier.doihttps://doi.org/10.1021/acscatal.9b02182en_US
dc.identifier.urihttps://hdl.handle.net/1911/107519en_US
dc.language.isoengen_US
dc.publisherAmerican Chemical Societyen_US
dc.rightsThis is an author's peer-reviewed final manuscript, as accepted by the publisher. The published article is copyrighted by the American Chemical Society.en_US
dc.subject.keywordnitrite reductionen_US
dc.subject.keyworddensity functional theoryen_US
dc.subject.keywordcatalyst designen_US
dc.subject.keywordensembleen_US
dc.subject.keywordeffect metal-on-metal structureen_US
dc.titleDesign of a Pd–Au Nitrite Reduction Catalyst by Identifying and Optimizing Active Ensemblesen_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpost-printen_US
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