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dc.contributor.authorLuo, Hen_US
dc.contributor.authorYukuhiro, VYen_US
dc.contributor.authorFernández, PSen_US
dc.contributor.authorFeng, Jen_US
dc.contributor.authorThompson, Pen_US
dc.contributor.authorRao, RRen_US
dc.contributor.authorCai, Ren_US
dc.contributor.authorFavero, Sen_US
dc.contributor.authorHaigh, SJen_US
dc.contributor.authorDurrant, JRen_US
dc.contributor.authorStephens, IELen_US
dc.contributor.authorTitirici, M-Men_US
dc.description.abstractPt-based bimetallic electrocatalysts are promising candidates to convert surplus glycerol from the biodiesel industry to value-added chemicals and coproduce hydrogen. It is expected that the nature and content of the elements in the bimetallic catalyst can not only affect the reaction kinetics but also influence the product selectivity, providing a way to increase the yield of the desired products. Hence, in this work, we investigate the electrochemical oxidation of glycerol on a series of PtNi nanoparticles with increasing Ni content using a combination of physicochemical structural analysis, electrochemical measurements, operando spectroscopic techniques, and advanced product characterizations. With a moderate Ni content and a homogenously alloyed bimetallic Pt-Ni structure, the PtNi2 catalyst displayed the highest reaction activity among all materials studied in this work. In situ FTIR data show that PtNi2 can activate the glycerol molecule at a more negative potential (0.4 V RHE) than the other PtNi catalysts. In addition, its surface can effectively catalyze the complete C-C bond cleavage, resulting in lower CO poisoning and higher stability. Operando X-ray absorption spectroscopy and UV-vis spectroscopy suggest that glycerol adsorbs strongly onto surface Ni(OH) x sites, preventing their oxidation and activation of oxygen or hydroxyl from water. As such, we propose that the role of Ni in PtNi toward glycerol oxidation is to tailor the electronic structure of the pure Pt sites rather than a bifunctional mechanism. Our experiments provide guidance for the development of bimetallic catalysts toward highly efficient, selective, and stable glycerol oxidation reactions.en_US
dc.format.extent14492 - 14506en_US
dc.relation.ispartofACS Catalen_US
dc.rightsAttribution 3.0 United States*
dc.titleRole of Ni in PtNi Bimetallic Electrocatalysts for Hydrogen and Value-Added Chemicals Coproduction via Glycerol Electrooxidation.en_US
pubs.notesNot knownen_US

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Attribution 3.0 United States
Except where otherwise noted, this item's license is described as Attribution 3.0 United States