TY - JOUR
T1 - Atom-by-Atom Synthesis of Multiatom-Supported Catalytic Clusters by Liquid-Phase Atomic Layer Deposition
AU - Le Monnier, Benjamin P.
AU - Savereide, Louisa
AU - Klllç, Murat
AU - Schnyder, Raphael
AU - Mensi, Mounir D.
AU - Avalos, Claudia E.
AU - Rothlisberger, Ursula
AU - Luterbacher, Jeremy S.
N1 - Funding Information:
This work was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Starting Grant: CATACOAT, No. 758653) and by EPFL. This work was also accomplished within the framework of the Swiss Competence Center for Bioenergy Research (SCCER-BIOSWEET). The authors wish to acknowledge Dr. Adam Clark and Prof. Maarten Nachtegaal for the access to and acquisition of X-ray absorption spectra at the Swiss Light Source of the Paul Scherrer institute. We also thank Nathalia Gasilova and Sylvain Coudret for the ICP measurements. Murat Kılıç and Ursula Rothlisberger acknowledge HPC resources of CSCS (Swiss National Supercomputer Centre).
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/3/21
Y1 - 2022/3/21
N2 - Here, we introduce a method for the synthesis of atomically precise, supported, multiatom catalysts by liquid-phase atomic layer deposition. This technique is based on consecutive grafting reactions in mild conditions that build supported active sites atom by atom. The atomically controlled synthesis procedure led to the growth of well-defined multinuclear (Al, Mg, Si, Zn, and O) clusters. The composition of the clusters was verified by titrations ICP-OES, STEM-EDX, and XPS, while their structure was resolved from the synthesis sequence, elemental composition, and extensive characterization (X-ray absorption, solid-state NMR, STEM, XPS, and DFT calculations). Propane dehydrogenation was used as a probe reaction to demonstrate the potential to control and tailor the activity and stability of these catalytic clusters. Notably, we were able to alternatively multiply the initial activity of a known single-atom catalyst by 6 fold or improve its stability against thermal deactivation by simply using different elements and modifying the deposition sequence.
AB - Here, we introduce a method for the synthesis of atomically precise, supported, multiatom catalysts by liquid-phase atomic layer deposition. This technique is based on consecutive grafting reactions in mild conditions that build supported active sites atom by atom. The atomically controlled synthesis procedure led to the growth of well-defined multinuclear (Al, Mg, Si, Zn, and O) clusters. The composition of the clusters was verified by titrations ICP-OES, STEM-EDX, and XPS, while their structure was resolved from the synthesis sequence, elemental composition, and extensive characterization (X-ray absorption, solid-state NMR, STEM, XPS, and DFT calculations). Propane dehydrogenation was used as a probe reaction to demonstrate the potential to control and tailor the activity and stability of these catalytic clusters. Notably, we were able to alternatively multiply the initial activity of a known single-atom catalyst by 6 fold or improve its stability against thermal deactivation by simply using different elements and modifying the deposition sequence.
KW - Atomic layer deposition
KW - Rational catalyst design
KW - Single-site catalyst
KW - Supported clusters
KW - Surface organometallic chemistry
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U2 - 10.1021/acssuschemeng.1c07056
DO - 10.1021/acssuschemeng.1c07056
M3 - Article
AN - SCOPUS:85126616283
VL - 10
SP - 3455
EP - 3465
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
SN - 2168-0485
IS - 11
ER -