Polycondensation as a Universal Method for Preparing High‐Density Single‐Atom Catalyst Libraries
Abstract
AbstractSingle‐atom catalysts (SACs) present a promising subclass of classic heterogeneous catalysts by maximizing metal dispersion and enhancing efficiency. Although high‐density SACs (HD‐SACs) are reported, their synthesis is typically constrained to specific metal‐support combinations and high‐temperature annealing, limiting their translation to wider applications. Herein, a universal bottom‐up approach for the preparation of mono‐ and bimetallic HD‐SACs based on the polycondensation of 1,2,4,5‐benzenetetramine with a wide range of metal monomers containing 1,10‐phenanthroline‐5,6‐dione ligands is introduced. The synthesized materials are atomically dispersed and exhibit metal loadings up to 27.5 wt% with high structural stability. Their versatility as catalysts is explored in electrocatalytic and photocatalytic applications. The materials exhibit remarkable stability under operational conditions. Furthermore, this synthetic strategy is scaled up and automated, demonstrating the robustness and reproducibility and laying the groundwork for self‐optimizing data‐driven materials discovery.
Article Details
Authors (22)
Jaques‐Christopher Schmidt
Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
Jan Romano‐deGea
Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
Dragos C. Stoian
The Swiss‐Norwegian Beamlines (SNBL) European Synchrotron Radiation Facility (ESRF) Grenoble 38000 France
Mounir Mensi
Institute of Chemical Sciences and Engineering (ISIC), X-Ray Diffraction and Surface Analytics Platform (XRDSAP)
Miyeon Chang
Laboratory of Inorganic Synthesis and Catalysis (LSCI), Institute of Chemical Sciences and Engineering
Ariana Serban
Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
Satyadeep Waiba
Department of Chemistry, University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
Xinbang Wu
Lindsey E. K. Frederiksen
Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
Rosie J. Somerville
Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
Roland C. Turnell‐Ritson
Department of Chemistry Chemistry Research Laboratory University of Oxford 12 Mansfield Road Oxford OX1 3TA UK
Xunhui Wang
Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne Switzerland
Laura Piveteau
Institut des Sciences et Ingénierie Chimiques (ISIC)
Daniel Ortiz
Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
Niccolò Martinolli
Nanoelectronic Devices Laboratory (Nanolab) Institute of Electrical and Micro Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
David Reyes
Interdisciplinary Center for Electron Microscopy
Jordi Espín
Timo M. O. Felder
Laboratory for Functional Inorganic Materials (LFIM), Institute of Chemical Sciences and Engineering (ISIC)
Stefano Di Leone
Swiss Cat+ West Hub École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
Pascal Miéville
Swiss Cat+ West Hub École Polytechnique Fédérale de Lausanne (EPFL) Lausanne 1015 Switzerland
Shoubhik Das
Department of Chemistry, University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
Paul J. Dyson