Ionic Liquid Sheath Stabilizes Atomically Dispersed Reduced Graphene Aerogel‐Supported Iridium Complexes during Ethylene Hydrogenation Catalysis

Kurtoğlu‐Öztulum, Samira F.; Yalçın, Kaan; Hoffman, Adam S.; Jalal, Ahsan; Zhao, Yuxin; Gates, Bruce C.; Bare, Simon R.; Unal, Ugur; Uzun, Alper

doi:10.1002/cctc.202200553

Title: Ionic Liquid Sheath Stabilizes Atomically Dispersed Reduced Graphene Aerogel‐Supported Iridium Complexes during Ethylene Hydrogenation Catalysis

Journal Article · Tue Aug 30 00:00:00 EDT 2022 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.202200553· OSTI ID:1891681

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Department of Chemical and Biological Engineering Koç University Rumelifeneri Yolu 34450 Sariyer Istanbul Turkey, Koç University TÜPRAŞ Energy Center (KUTEM) Koç University Rumelifeneri Yolu 34450 Sariyer Istanbul Turkey
SSRL SLAC National Accelerator Laboratory 94025 Menlo Park CA USA
Department of Chemical Engineering University of California 95616 Davis CA USA
Koç University TÜPRAŞ Energy Center (KUTEM) Koç University Rumelifeneri Yolu 34450 Sariyer Istanbul Turkey, Department of Chemistry Koç University Rumelifeneri Yolu 34450 Sariyer Istanbul Turkey, Koç University Surface Science and Technology Center (KUYTAM) Koç University Rumelifeneri Yolu 34450 Sariyer Istanbul Turkey
Department of Chemical and Biological Engineering Koç University Rumelifeneri Yolu 34450 Sariyer Istanbul Turkey, Koç University TÜPRAŞ Energy Center (KUTEM) Koç University Rumelifeneri Yolu 34450 Sariyer Istanbul Turkey, Koç University Surface Science and Technology Center (KUYTAM) Koç University Rumelifeneri Yolu 34450 Sariyer Istanbul Turkey

Abstract An atomically dispersed reduced graphene aerogel (rGA)‐supported iridium catalyst having reactive ethylene ligands was synthesized at an iridium loading of 9.9 wt % and coated with an ionic liquid, 1‐ethyl‐3‐methylimidazolium acetate ([EMIM][OAc]). Continuous‐scan X‐ray absorption spectra demonstrated that the iridium remained site‐isolated in flowing equimolar C ₂ H ₄ and H ₂ during a temperature ramp to 100 °C. The data further showed the lack of detectable iridium aggregation when the feed was H ₂ ‐rich or even pure H ₂ at 100 °C. An Arrhenius plot determined for ethylene hydrogenation catalysis with the sample in flowing equimolar ethylene and hydrogen showed no variation in the apparent activation energy at temperatures up to 100 °C, confirming that the active sites remained intact at the higher temperatures. The results point to opportunities for overcoming the stability limitations of atomically dispersed supported noble metal catalysts by choice of electron‐donor supports and ionic liquid sheaths.

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Sponsoring Organization:: USDOE

OSTI ID:: 1891681

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Vol. 14 Journal Issue: 19; ISSN 1867-3880

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

Country of Publication:: Germany

Language:: English

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