Ni2P active site ensembles tune electrocatalytic nitrate reduction selectivity

Emily Nishiwaki; Peter S. Rice; Ding-Yuan Kuo; Florence Y. Dou; Anthony Pyka; Bryce Reid; Hao A. Nguyen; Eric M. Stuve; Simone Raugei; Brandi M. Cossairt

doi:10.1039/D4CC01834F

Ni₂P active site ensembles tune electrocatalytic nitrate reduction selectivity†

Emily Nishiwaki,

^a Peter S. Rice,

^b Ding-Yuan Kuo,

^a Florence Y. Dou,

^a Anthony Pyka,^c Bryce Reid,^c Hao A. Nguyen,^a Eric M. Stuve,^c Simone Raugei

^b and Brandi M. Cossairt

*^a

Author affiliations

* Corresponding authors

^a Department of Chemistry, University of Washington, Seattle, WA 98195, USA
E-mail: cossairt@uw.edu

^b Pacific Northwest National Laboratory, Richland, Washington, WA 99352, USA

^c Department of Chemical Engineering, University of Washington, Seattle, WA 98195, USA

Abstract

We demonstrate that active site ensembles on transition metal phosphides tune the selectivity of the nitrate reduction reaction. Using Ni₂P nanocrystals as a case study, we report a mechanism involving competitive co-adsorption of H* and NO_x* intermediates. A near 100% faradaic efficiency for nitrate reduction over hydrogen evolution is observed at −0.4 V, while NH₃ selectivity is maximized at −0.2 V vs. RHE.

This article is part of the themed collections: Small Molecule Transformations of Energy Relevance and ChemComm 60th Anniversary Collection

Chemical Communications

Ni₂P active site ensembles tune electrocatalytic nitrate reduction selectivity†

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Ni₂P active site ensembles tune electrocatalytic nitrate reduction selectivity

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