Acetylene ligands stabilize atomically dispersed supported rhodium complexes under harsh conditions

Zhao, Yuxin; Kurtoğlu-Öztulum, Samira F.; Hoffman, Adam S.; Hong, Jiyun; Perez-Aguilar, Jorge E.; Bare, Simon R.; Uzun, Alper

doi:10.1016/j.cej.2024.149738

Acetylene ligands stabilize atomically dispersed supported rhodium complexes under harsh conditions

Journal Article · Fri Feb 16 00:00:00 EST 2024 · Chemical Engineering Journal

DOI:https://doi.org/10.1016/j.cej.2024.149738· OSTI ID:2407120

Zhao, Yuxin ^[1]; Kurtoğlu-Öztulum, Samira F. ^[2]; Hoffman, Adam S. ^[3]; Hong, Jiyun ^[3]; Perez-Aguilar, Jorge E. ^[3]; Bare, Simon R. ^[3]; ^[2]

Koc Univ., Istanbul (Turkey); SLAC
Koc Univ., Istanbul (Turkey)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Facile sintering of atomically dispersed supported noble metal catalysts at catalytically relevant temperatures, particularly under reducing conditions, poses a challenge for their practical applications. Some ligands, such as carbonyls, aid in improving the stability at the expense of severely suppressing the catalytic activity. In this work, we demonstrate that substitution of the carbonyl ligands with reactive acetylene ligands can maintain the atomic dispersion of the supported mononuclear rhodium complex under harsh reducing conditions (>573 K), as confirmed by in-situ X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectroscopies. In contrast, the supported rhodium carbonyl complex aggregates into nanoclusters under identical conditions. Furthermore, our results indicate that the acetylene ligands provide this anti-sintering ability while retaining the hydrogenation activity.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2407120

Alternate ID(s):: OSTI ID: 2369994

Journal Information:: Chemical Engineering Journal, Journal Name: Chemical Engineering Journal Vol. 485; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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