TY - JOUR

T1 - Low-temperature non-equilibrium synthesis of anisotropic multimetallic nanosurface alloys for electrochemical CO2 reduction

AU - Koolen, Cedric David

AU - Oveisi, Emad

AU - Zhang, Jie

AU - Li, Mo

AU - Safonova, Olga V.

AU - Pedersen, Jack K.

AU - Rossmeisl, Jan

AU - Luo, Wen

AU - Züttel, Andreas

N1 - Funding Information: This research was supported by Swiss National Science Foundation (Ambizione Project PZ00P2_179989). M.L. acknowledges the financial support from China Scholarship Council (grant no. 201506060156). J.K.P. and J.R. acknowledge support from the Danish National Research Foundation Center for High Entropy Alloy Catalysis (CHEAC) DNRF-149. L. Menin and N. Gasilova of the Mass Spectrometry and Elemental Analysis Platform (MSEAP), Institute of Chemical Sciences and Engineering (ISIC), Basic Science Faculty (SB), École Polytechnique Fédérale de Lausanne (EPFL) Valais/Wallis, Energypolis, Sion, Switzerland, are acknowledged for their facilitation of the ICP–MS/OES measurements. S. Phadke is acknowledged for his assistance in the preparation of the capillaries. Publisher Copyright: © 2023, The Author(s), under exclusive licence to Springer Nature Limited.

PY - 2024

Y1 - 2024

N2 - Multimetallic nanoparticles are of interest as functional materials due to their highly tunable properties. However, synthesizing congruent mixtures of immiscible components is limited by the need for high-temperature procedures followed by rapid quenching that lack size and shape control. Here we report a low-temperature (≤80 °C) non-equilibrium synthesis of nanosurface alloys (NSAs) with tunable size, shape and composition regardless of miscibility. We show the generality of our method by producing both bulk miscible and immiscible monodisperse anisotropic Cu-based NSAs of up to three components. We demonstrate our synthesis as a screening platform to investigate the effects of crystal facet and elemental composition by testing tetrahedral, cubic and truncated-octahedral NSAs as catalysts in the electroreduction of CO2. The use of machine learning has enabled the prediction and informed synthesis of both multicarbon-product-selective and phase-stable Cu–Ag–Pd compositions. This combination of non-equilibrium synthesis and theory-guided candidate selection is expected to accelerate test–learn–repeat cycles of structure–performance optimization processes. [Figure not available: see fulltext.].

AB - Multimetallic nanoparticles are of interest as functional materials due to their highly tunable properties. However, synthesizing congruent mixtures of immiscible components is limited by the need for high-temperature procedures followed by rapid quenching that lack size and shape control. Here we report a low-temperature (≤80 °C) non-equilibrium synthesis of nanosurface alloys (NSAs) with tunable size, shape and composition regardless of miscibility. We show the generality of our method by producing both bulk miscible and immiscible monodisperse anisotropic Cu-based NSAs of up to three components. We demonstrate our synthesis as a screening platform to investigate the effects of crystal facet and elemental composition by testing tetrahedral, cubic and truncated-octahedral NSAs as catalysts in the electroreduction of CO2. The use of machine learning has enabled the prediction and informed synthesis of both multicarbon-product-selective and phase-stable Cu–Ag–Pd compositions. This combination of non-equilibrium synthesis and theory-guided candidate selection is expected to accelerate test–learn–repeat cycles of structure–performance optimization processes. [Figure not available: see fulltext.].

U2 - 10.1038/s44160-023-00387-3

DO - 10.1038/s44160-023-00387-3

M3 - Journal article

AN - SCOPUS:85169931233

VL - 3

SP - 47

EP - 57

JO - Nature Synthesis

JF - Nature Synthesis

SN - 2731-0582

ER -