Atomically dispersed zeolite-supported rhodium complex: Selective and stable catalyst for acetylene semi-hydrogenation

Zhao, Yuxin; Bozkurt, Özge D.; Kurtoğlu-Öztulum, Samira F.; Yordanli, Melisa Su; Hoffman, Adam S.; Hong, Jiyun; Perez-Aguilar, Jorge E.; Saltuk, Aylin; Akgül, Deniz; Demircan, Oktay; Ateşin, Tülay A.; Aviyente, Viktorya; Gates, Bruce C.; Bare, Simon R.; Uzun, Alper

doi:10.1016/j.jcat.2023.115196

Title: Atomically dispersed zeolite-supported rhodium complex: Selective and stable catalyst for acetylene semi-hydrogenation

Journal Article · 04 November 2023 · Journal of Catalysis

DOI: https://doi.org/10.1016/j.jcat.2023.115196 · OSTI ID:2328668

Zhao, Yuxin ^[1];

^[1]; Kurtoğlu-Öztulum, Samira F. ^[1]; Yordanli, Melisa Su ^[2];

^[3];

^[3]; Perez-Aguilar, Jorge E. ^[3]; Saltuk, Aylin ^[2];

^[2];

^[4];

^[2];

^[5];

^[3];

^[1]

Koç Univ., Istanbul (Turkey)
Bogazici Univ., Istanbul (Turkey)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
University of Texas Rio Grande Valley, Edinburg, TX (United States)
Univ. of California, Davis, CA (United States)

In this study, supported rhodium catalysts are known to be unselective for semi-hydrogenation reactions. Here, by tuning the electronic structure of supported mononuclear rhodium sites determined by the metal nuclearity and the electron-donor properties of the support, we report that atomically dispersed HY zeolite-supported rhodium with reactive acetylene ligands affords a stable ethylene selectivity > 90 % for acetylene semi-hydrogenation at 373 K and atmospheric pressure, even when ethylene is present in a large excess over acetylene. Infrared and X-ray absorption spectra and measurements of rates of the catalytic reaction complemented with calculations at the level of density functional theory show how the catalyst performance depends on the electronic structure of the rhodium, influenced by the support as a ligand that is a weak electron donor.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Univ. of California, Davis, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Center for High Performance Computing of Turkey (UHEM); USDOE

Grant/Contract Number:: AC02-76SF00515; FG02-04ER15513; 1006502019

OSTI ID:: 2328668

Alternate ID(s):: OSTI ID: 2222514

Journal Information:: Journal of Catalysis, Vol. 429; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (53)

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Identification of Non-Precious Metal Alloy Catalysts for Selective Hydrogenation of Acetylene Studt, F.; Abild-Pedersen, F.; Bligaard, T. Science, Vol. 320, Issue 5881 https://doi.org/10.1126/science.1156660	journal	June 2008
Ethene Dimerization and Hydrogenation over a Zeolite-Supported Rh(I)-Carbonyl Complex: Mechanistic Insights from DFT Modeling Vummaleti, Sai V. C.; Genest, Alexander; Kuriakose, Nishamol ACS Catalysis, Vol. 8, Issue 10 https://doi.org/10.1021/acscatal.8b02573	journal	September 2018
Gold Catalysis Hashmi, A. Stephen K.; Hutchings, Graham J. Angewandte Chemie International Edition, Vol. 45, Issue 47 https://doi.org/10.1002/anie.200602454	journal	December 2006
The hydrogenation of acetyleneII. The reaction of acetylene with hydrogen catalyzed by alumina-supported palladium Bond, G.; Wells, P. Journal of Catalysis, Vol. 5, Issue 1 https://doi.org/10.1016/S0021-9517(66)80126-4	journal	February 1966
567. The metal-catalysed reaction between acetylene and hydrogen. Part VI. The reaction over rhodium and iridium Sheridan, J.; Reid, W. D. Journal of the Chemical Society (Resumed) https://doi.org/10.1039/jr9520002962	journal	January 1952
Oxide- and Zeolite-Supported Isostructural Ir(C ₂ H ₄ ) ₂ Complexes: Molecular-Level Observations of Electronic Effects of Supports as Ligands Lu, Jing; Aydin, Ceren; Browning, Nigel D. Langmuir, Vol. 28, Issue 35 https://doi.org/10.1021/la302522a	journal	August 2012
Catalysis by Supported Single Metal Atoms Liu, Jingyue ACS Catalysis, Vol. 7, Issue 1 https://doi.org/10.1021/acscatal.6b01534	journal	November 2016
Atomic Charges Wiberg, Kenneth B.; Rablen, Paul R. The Journal of Organic Chemistry, Vol. 83, Issue 24 https://doi.org/10.1021/acs.joc.8b02740	journal	November 2018
Limits of Detection for EXAFS Characterization of Heterogeneous Single-Atom Catalysts Finzel, Jordan; Sanroman Gutierrez, Kenzie M.; Hoffman, Adam S. ACS Catalysis, Vol. 13, Issue 9 https://doi.org/10.1021/acscatal.3c01116	journal	April 2023
Highly Selective Hydrogenation of CO ₂ to Ethanol via Designed Bifunctional Ir ₁ –In ₂ O ₃ Single-Atom Catalyst Ye, Xue; Yang, Chongya; Pan, Xiaoli Journal of the American Chemical Society, Vol. 142, Issue 45 https://doi.org/10.1021/jacs.0c08607	journal	October 2020
Ab initio effective core potentials for molecular calculations. Potentials for K to Au including the outermost core orbitals Hay, P. Jeffrey; Wadt, Willard R. The Journal of Chemical Physics, Vol. 82, Issue 1, p. 299-310 https://doi.org/10.1063/1.448975	journal	January 1985
Ethene Hydroformylation Catalyzed by Rhodium Dispersed with Zinc or Cobalt in Silanol Nests of Dealuminated Zeolite Beta Qi, Liang; Das, Sonali; Zhang, Yanfei Journal of the American Chemical Society, Vol. 145, Issue 5 https://doi.org/10.1021/jacs.2c11075	journal	January 2023
Selective Methane Oxidation by Heterogenized Iridium Catalysts Li, Haoyi; Fei, Muchun; Troiano, Jennifer L. Journal of the American Chemical Society, Vol. 145, Issue 2 https://doi.org/10.1021/jacs.2c09434	journal	January 2023
Structural Regulation and Support Coupling Effect of Single‐Atom Catalysts for Heterogeneous Catalysis Liu, Daobin; He, Qun; Ding, Shiqing Advanced Energy Materials, Vol. 10, Issue 32 https://doi.org/10.1002/aenm.202001482	journal	July 2020
Tracking Rh Atoms in Zeolite HY: First Steps of Metal Cluster Formation and Influence of Metal Nuclearity on Catalysis of Ethylene Hydrogenation and Ethylene Dimerization Yang, Dong; Xu, Pinghong; Browning, Nigel D. The Journal of Physical Chemistry Letters, Vol. 7, Issue 13 https://doi.org/10.1021/acs.jpclett.6b01153	journal	June 2016
Gold Atoms Stabilized on Various Supports Catalyze the Water–Gas Shift Reaction Flytzani-Stephanopoulos, Maria Accounts of Chemical Research, Vol. 47, Issue 3 https://doi.org/10.1021/ar4001845	journal	November 2013
Solid state packing of [Rh(β-diketonato)(CO)2] complexes. Crystal structure of [Rh(PhCOCHCOC4H3S)(CO)2] Conradie, Marrigje Marianne; Conradie, Jeanet Journal of Molecular Structure, Vol. 1051 https://doi.org/10.1016/j.molstruc.2013.07.046	journal	November 2013
Highly Active Gas Phase Organometallic Catalysis Supported Within Metal–Organic Framework Pores Peralta, Ricardo A.; Huxley, Michael T.; Evans, Jack D. Journal of the American Chemical Society, Vol. 142, Issue 31 https://doi.org/10.1021/jacs.0c05286	journal	July 2020
Tuning Catalytic Selectivity: Zeolite- and Magnesium Oxide-Supported Molecular Rhodium Catalysts for Hydrogenation of 1,3-Butadiene Yardimci, Dicle; Serna, Pedro; Gates, Bruce C. ACS Catalysis, Vol. 2, Issue 10 https://doi.org/10.1021/cs300475c	journal	September 2012
Room-temperature electrochemical acetylene reduction to ethylene with high conversion and selectivity Shi, Run; Wang, Zeping; Zhao, Yunxuan Nature Catalysis, Vol. 4, Issue 7 https://doi.org/10.1038/s41929-021-00640-y	journal	July 2021
CO Oxidation Catalyzed by Single Gold Atoms Supported on Aluminum Oxide Clusters Li, Zi-Yu; Yuan, Zhen; Li, Xiao-Na Journal of the American Chemical Society, Vol. 136, Issue 40 https://doi.org/10.1021/ja508547z	journal	August 2014
Ligand effects in the rhodium-catalyzed carbonylation of methanol Thomas, C. Coordination Chemistry Reviews, Vol. 243, Issue 1-2 https://doi.org/10.1016/S0010-8545(03)00051-1	journal	August 2003
Rhodium Single‐Atom Catalyst Design through Oxide Support Modulation for Selective Gas‐Phase Ethylene Hydroformylation Farpón, Marcos G.; Henao, Wilson; Plessow, Philipp N. Angewandte Chemie, Vol. 135, Issue 1 https://doi.org/10.1002/ange.202214048	journal	November 2022
Isostructural Zeolite-Supported Rhodium and Iridium Complexes: Tuning Catalytic Activity and Selectivity by Ligand Modification Martinez-Macias, Claudia; Serna, Pedro; Gates, Bruce C. ACS Catalysis, Vol. 5, Issue 10 https://doi.org/10.1021/acscatal.5b00995	journal	August 2015
Prospects of Heterogeneous Hydroformylation with Supported Single Atom Catalysts Amsler, Jonas; Sarma, Bidyut B.; Agostini, Giovanni Journal of the American Chemical Society, Vol. 142, Issue 11 https://doi.org/10.1021/jacs.9b12171	journal	March 2020
Metal Sites in Zeolites: Synthesis, Characterization, and Catalysis Zhang, Qiang; Gao, Shiqin; Yu, Jihong Chemical Reviews, Vol. 123, Issue 9 https://doi.org/10.1021/acs.chemrev.2c00315	journal	September 2022
The preparation and properties of tris(triphenylphosphine)halogenorhodium(I) and some reactions thereof including catalytic homogeneous hydrogenation of olefins and acetylenes and their derivatives Osborn, J. A.; Jardine, F. H.; Young, J. F. Journal of the Chemical Society A: Inorganic, Physical, Theoretical https://doi.org/10.1039/j19660001711	journal	January 1966
A highly CO-tolerant atomically dispersed Pt catalyst for chemoselective hydrogenation Lin, Lili; Yao, Siyu; Gao, Rui Nature Nanotechnology, Vol. 14, Issue 4 https://doi.org/10.1038/s41565-019-0366-5	journal	February 2019
Isolated Metal Atom Geometries as a Strategy for Selective Heterogeneous Hydrogenations Kyriakou, Georgios; Boucher, Matthew B.; Jewell, April D. Science, Vol. 335, Issue 6073 https://doi.org/10.1126/science.1215864	journal	March 2012
Structure and Bonding of a Site-Isolated Transition Metal Complex: Rhodium Dicarbonyl in Highly Dealuminated Zeolite Y Goellner, Jesse F.; Gates, Bruce C.; Vayssilov, Georgi N. Journal of the American Chemical Society, Vol. 122, Issue 33 https://doi.org/10.1021/ja001209f	journal	August 2000
Identification of single-site gold catalysis in acetylene hydrochlorination Malta, Grazia; Kondrat, Simon A.; Freakley, Simon J. Science, Vol. 355, Issue 6332 https://doi.org/10.1126/science.aal3439	journal	March 2017
Selective Hydrogenation of Ethyne in Ethene‐Rich Streams on Palladium Catalysts. Part 1. Effect of Changes to the Catalyst During Reaction Borodziński, Andrzej; Bond, Geoffrey C. Catalysis Reviews, Vol. 48, Issue 2 https://doi.org/10.1080/01614940500364909	journal	July 2006
Competition of C‐C bond formation and C‐H bond formation For acetylene hydrogenation on transition metals: A density functional theory study Zhao, Zhi‐Jian; Zhao, Jiubing; Chang, Xin AIChE Journal, Vol. 65, Issue 3 https://doi.org/10.1002/aic.16492	journal	December 2018
Bifunctional hydroformylation on heterogeneous Rh-WOx pair site catalysts Ro, Insoo; Qi, Ji; Lee, Seungyeon Nature, Vol. 609, Issue 7926 https://doi.org/10.1038/s41586-022-05075-4	journal	September 2022
Report of the international workshop on standards and criteria in X-ray absorption spectroscopy None, None Physica B: Condensed Matter, Vol. 158, Issue 1-3, p. 701-722 https://doi.org/10.1016/0921-4526(89)90447-X	journal	June 1989
Copper Catalysts in Semihydrogenation of Acetylene: From Single Atoms to Nanoparticles Shi, Xianxian; Lin, Yue; Huang, Li ACS Catalysis, Vol. 10, Issue 5 https://doi.org/10.1021/acscatal.9b05321	journal	February 2020
Electronic Structure of Atomically Dispersed Supported Iridium Catalyst Controls Iridium Aggregation Kurtoğlu, Samira F.; Hoffman, Adam S.; Akgül, Deniz ACS Catalysis, Vol. 10, Issue 21 https://doi.org/10.1021/acscatal.0c03909	journal	October 2020
Single-Atom Pd ₁ /Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene Yan, Huan; Cheng, Hao; Yi, Hong Journal of the American Chemical Society, Vol. 137, Issue 33 https://doi.org/10.1021/jacs.5b06485	journal	August 2015
Hydroformylation of Olefins by a Rhodium Single-Atom Catalyst with Activity Comparable to RhCl(PPh ₃ ) ₃ Lang, Rui; Li, Tianbo; Matsumura, Daiju Angewandte Chemie International Edition, Vol. 55, Issue 52 https://doi.org/10.1002/anie.201607885	journal	November 2016
Influence of ionic liquids on the electronic environment of atomically dispersed Ir on (MgO)(100) Akgül, Deniz; Kurtoğlu-Öztulum, Samira F.; Zhao, Yuxin Physical Chemistry Chemical Physics, Vol. 24, Issue 18 https://doi.org/10.1039/D2CP00043A	journal	January 2022
Effect of Si/Al Ratio and Rh Precursor Used on the Synthesis of HY Zeolite-Supported Rhodium Carbonyl Hydride Complexes Khivantsev, Konstantin; Vityuk, Artem; Aleksandrov, Hristiyan A. The Journal of Physical Chemistry C, Vol. 119, Issue 30 https://doi.org/10.1021/acs.jpcc.5b03969	journal	July 2015
Multiple-scattering calculations of x-ray-absorption spectra Zabinsky, S. I.; Rehr, J. J.; Ankudinov, A. Physical Review B, Vol. 52, Issue 4 https://doi.org/10.1103/PhysRevB.52.2995	journal	July 1995
An EXAFS study of the structure of the metal–support interface in highly dispersed Rh/Al ₂ O ₃ catalysts van Zon, J. B. A. D.; Koningsberger, D. C.; van’t Blik, H. F. J. The Journal of Chemical Physics, Vol. 82, Issue 12 https://doi.org/10.1063/1.448563	journal	June 1985
Molecular Heterogeneous Catalysis: A Single-Site Zeolite-Supported Rhodium Complex for Acetylene Cyclotrimerization Kletnieks, Philip W.; Liang, Ann J.; Craciun, Raluca Chemistry - A European Journal, Vol. 13, Issue 26 https://doi.org/10.1002/chem.200700721	journal	September 2007
Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles Liu, Lichen; Corma, Avelino Chemical Reviews, Vol. 118, Issue 10 https://doi.org/10.1021/acs.chemrev.7b00776	journal	April 2018
Stabilizing Isolated Rhodium Cations by MFI Zeolite for Heterogeneous Methanol Carbonylation Shang, Weixiang; Gao, Mingyang; Chai, Yuchao ACS Catalysis, Vol. 11, Issue 12 https://doi.org/10.1021/acscatal.1c00950	journal	June 2021
Mild oxidation of methane to methanol or acetic acid on supported isolated rhodium catalysts Shan, Junjun; Li, Mengwei; Allard, Lawrence F. Nature, Vol. 551, Issue 7682 https://doi.org/10.1038/nature24640	journal	November 2017
Rhodium-Catalyzed Hydroformylation in Supercritical Carbon Dioxide Koch, Daniel; Leitner, Walter Journal of the American Chemical Society, Vol. 120, Issue 51 https://doi.org/10.1021/ja980729w	journal	December 1998
X-ray Structures and DFT Calculations on Rhodium−Olefin Complexes: Comments on the ¹⁰³ Rh NMR Shift−Stability Correlation Bühl, Michael; Håkansson, Mikael; Mahmoudkhani, Amir H. Organometallics, Vol. 19, Issue 26 https://doi.org/10.1021/om000419y	journal	December 2000
Formation of supported rhodium clusters from mononuclear rhodium complexes controlled by the support and ligands on rhodium Serna, Pedro; Yardimci, Dicle; Kistler, Joseph D. Phys. Chem. Chem. Phys., Vol. 16, Issue 3 https://doi.org/10.1039/C3CP53057D	journal	January 2014
Hydrogenation of acetylene over supported metal catalysts. Part 3.—[14C]tracer studies of the effects of added ethylene and carbon monoxide on the reaction catalysed by silica-supported palladium, rhodium and iridium Al-Ammar, Asad S.; Webb, Geoffrey Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 75, Issue 0 https://doi.org/10.1039/f19797501900	journal	January 1979

Similar Records

Molecular Rhodium Complexes Supported on the Metal-Oxide-Like Nodes of Metal Organic Frameworks and on Zeolite HY: Catalysts for Ethylene Hydrogenation and Dimerization

Journal Article · 2017 · ACS Applied Materials and Interfaces · OSTI ID:1469880

Bernales, Varinia; Yang, Dong; Yu, Jun; +4 more

Time-Resolved Structural Characterization of Formation and Break-up of Rhodium Clusters Supported in Highly Dealuminated Y Zeolite

Journal Article · 2009 · J. Phys. Chem. C · OSTI ID:1007093

Liang, Ann J; Gates, Bruce C

Tracking Rh Atoms in Zeolite HY: First Steps of Metal Cluster Formation and Influence of Metal Nuclearity on Catalysis of Ethylene Hydrogenation and Ethylene Dimerization

Journal Article · 2016 · Journal of Physical Chemistry Letters · OSTI ID:1298393

Yang, Dong; Xu, Pinghong; Browning, Nigel D.; +1 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Supported rhodium complexes
Zeolite
Acetylene semi-hydrogenation
Electronic structure effect
density functional theory

Title: Atomically dispersed zeolite-supported rhodium complex: Selective and stable catalyst for acetylene semi-hydrogenation

Citation Formats

References (53)

Similar Records

Related Subjects