Modifikation eines Cu‐Pd‐Schaufelrad‐Metall‐Organischen Gerüsts für die selektive CO 2 ‐Elektroreduktion

Zhang, Ruirui; Liu, Yan; Ding, Pan; Huang, Juanjuan; Dierolf, Martin; Kelly, Shelly D.; Qiu, Xinqi; Chen, Yishuo; Hussain, Mian Zahid; Li, Weijin; Bunzen, Hana; Achterhold, Klaus; Pfeiffer, Franz; Sharp, Ian D.; Warnan, Julien; Fischer, Roland A.

doi:10.1002/ange.202414600

Title: Modifikation eines Cu‐Pd‐Schaufelrad‐Metall‐Organischen Gerüsts für die selektive CO ₂ ‐Elektroreduktion

Journal Article · 15 November 2024 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202414600 · OSTI ID:2480380

Zhang, Ruirui ^[1]; Liu, Yan ^[2]; Ding, Pan ^[3]; Huang, Juanjuan ^[4]; Dierolf, Martin ^[5]; Kelly, Shelly D. ^[4]; Qiu, Xinqi ^[1]; Chen, Yishuo ^[1]; Hussain, Mian Zahid ^[1]; Li, Weijin ^[1]; Bunzen, Hana ^[6]; Achterhold, Klaus ^[5]; Pfeiffer, Franz ^[5]; Sharp, Ian D. ^[3]; Warnan, Julien ^[1];

^[7]

Chair of Inorganic and Metal-Organic Chemistry Department of Chemistry and TUM School of Natural Sciences Technische Universität München Lichtenbergstraße 4 D-85748 Garching Germany
College of Chemistry and Materials Science Anhui Normal University Wuhu Anhui 241000 P. R. China
Walter Schottky Institute and TUM School of Natural Sciences Technische Universität München Am Coulombwall 4 85748 Garching Germany
X-ray Science Division and Advanced Photon Source Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
Chair of Biomedical Physics Department of Physics and TUM School of Natural Sciences Technische Universität München 85748 Garching Germany
Chair of Solid State and Materials Chemistry and Institute of Physics Universität Augsburg 86159 Augsburg Germany
Chair of Inorganic and Metal-Organic Chemistry Department of Chemistry and TUM School of Natural Sciences Technische Universität München Lichtenbergstraße 4 D-85748 Garching Germany, Catalysis Research Center Technische Universität München Ernst-Otto-Fischer-Str.1 85748 Garching Germany

Abstract Die Optimierung der Bindungsenergie zwischen dem Intermediat und dem aktiven Zentrum ist ein entscheidender Faktor, um die katalytische Produktselektivität und Aktivität bei der elektrochemischen Kohlendioxidreduktion (CO ₂ RR) zu steuern. Es ist bekannt, dass Kupferatome als aktive Zentren CO ₂ zu Kohlenwasserstoffen und Sauerstoffverbindungen reduzieren, jedoch unter schlechter Produktselektivität leiden, da mehrere Intermediate nur moderate Bindungsenergien aufweisen. Hier berichten wir über eine Ionenaustauschstrategie zur Konstruktion von Cu−Pd‐Schaufelrad‐Dimeren innerhalb von Cu‐basierten metallorganischen Gerüsten (MOFs), [Cu _3‐x Pdx(BTC) ₂ ] (BTC=1,3,5‐Benzoltricarbonsäure), ohne die strukturellen Eigenschaften des MOFs zu verändern. Im Vergleich zum reinen Cu‐MOF ([Cu ₃ (BTC) ₂ ], HKUST‐1) verlagert der Cu−Pd‐MOF die Produkte der CO ₂ ‐Elektroreduktion von einer Vielzahl chemischer Spezies hin zu einer selektiven CO‐Erzeugung. Eine in situ‐Röntgenabsorptions‐Feinstrukturanalyse der Oxidationsstufe des Katalysators und der lokalen Geometrie, kombiniert mit theoretischen Berechnungen, zeigt, dass die Einfügung von Pd in die Knotenpunkte der Cu‐Schaufelradstruktur des MOFs die Adsorption des Schlüsselintermediats COOH* am Cu‐Zentrum fördert. Dies ermöglicht CO‐selektive katalytische Mechanismen und verbessert somit unser Verständnis über das Zusammenspiel von Struktur und Aktivität bei der elektrochemischen CO ₂ ‐Reduktion unter Verwendung molekularer Katalysatoren.

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Sponsoring Organization:: USDOE

OSTI ID:: 2480380

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 51 Vol. 136; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Title: Modifikation eines Cu‐Pd‐Schaufelrad‐Metall‐Organischen Gerüsts für die selektive CO ₂ ‐Elektroreduktion