title: Electrocatalytic Hydrogenation of Oxygenates using Earth-Abundant Transition-Metal Nanoparticles under Mild Conditions.
abstract: Electrocatalytic hydrogenation (ECH) is a sustainable pathway for the synthesis of value-added organic compounds, provided affordable catalysts with high activity, selectivity and durability are developed. Here, we synthesize Cu/C, Ni/C, and CuNi/C nanoparticles and compare their performance to Pt/C, Ru/C, PtRu/C for the ECH of hydroxyacetone, a bio-derived feedstock surrogate containing a carbonyl and a hydroxyl functional group. The non-precious metal electrocatalysts show promising conversion-time behavior, product selectivities, and Faradaic efficiencies. Ni/C forms propylene glycol with a selectivity of 89 % (at 80 % conversion), while Cu/C catalyzes ECH (52 % selectivity) and hydrodeoxygenation (HDO, 48 % selectivity, accounting for evaporation). CuNi/C shows increased turnover frequencies but reduced ECH selectivity (80 % at 80 % conversion) as compared to the Ni/C catalyst. Importantly, stability studies show that the non-precious metal catalysts do not leach at operating conditions.
authors.affiliation: Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave, Cambridge, MA, 02139, USA.
authors.forename: Kyler J
authors.initials: KJ
authors.lastname: Carroll
authors.affiliation: Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave, Cambridge, MA, 02139, USA.|Department of Chemistry, Technical University of Munich, Lichtenbergstraße 4, 85748, Garching, Germany.
authors.forename: Thomas
authors.initials: T
authors.lastname: Burger
authors.affiliation: Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave, Cambridge, MA, 02139, USA.|Institute for Chemical and Bioengineering, ETH Zürich, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.
authors.forename: Lukas
authors.initials: L
authors.lastname: Langenegger
authors.affiliation: Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave, Cambridge, MA, 02139, USA.
authors.forename: Steven
authors.initials: S
authors.lastname: Chavez
authors.affiliation: Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave, Cambridge, MA, 02139, USA.
authors.forename: Sean T
authors.initials: ST
authors.lastname: Hunt
authors.affiliation: Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave, Cambridge, MA, 02139, USA.
authors.forename: Yuriy
authors.initials: Y
authors.lastname: Román-Leshkov
authors.affiliation: Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave, Cambridge, MA, 02139, USA. brushett@mit.edu.
authors.forename: Fikile R
authors.identifier: 0000-0002-7361-6637
authors.initials: FR
authors.lastname: Brushett
mesh_terms: D002244:Carbon / Q000737:chemistry; D002384:Catalysis; D004563:Electrochemistry; D006865:Hydrogenation; D053768:Metal Nanoparticles / Q000737:chemistry*; D008958:Models, Molecular; D008968:Molecular Conformation; D010100:Oxygen / Q000737:chemistry*; D028561:Transition Elements / Q000737:chemistry*
chemical_list: D028561:Transition Elements; D002244:Carbon; D010100:Oxygen
keywords: electrocatalysis; heterogeneous catalysis; hydrogenation; nickel; renewable resources