Thermal Unequilibrium of PdSn Intermetallic Nanocatalysts: From In Situ Tailored Synthesis to Unexpected Hydrogenation Selectivity

Chen, Minda; Yan, Yu; Gebre, Mebatsion; Ordonez, Claudio; Liu, Fudong; Qi, Long; Lamkins, Andrew; Jing, Dapeng; Dolge, Kevin; Zhang, Biying; Heintz, Patrick; Shoemaker, Daniel P.; Wang, Bin; Huang, Wenyu

doi:10.1002/anie.202106515

Thermal Unequilibrium of PdSn Intermetallic Nanocatalysts: From In Situ Tailored Synthesis to Unexpected Hydrogenation Selectivity

Journal Article · Fri Jul 16 00:00:00 EDT 2021 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202106515· OSTI ID:1817653

Chen, Minda ^[1]; Yan, Yu ^[2]; Gebre, Mebatsion ^[3]; Ordonez, Claudio ^[1]; Liu, Fudong ^[4]; Qi, Long ^[5]; Lamkins, Andrew ^[1]; Jing, Dapeng ^[6]; Dolge, Kevin ^[1]; Zhang, Biying ^[1]; Heintz, Patrick ^[1]; Shoemaker, Daniel P. ^[3]; ^[2]; ^[7]

Iowa State Univ., Ames, IA (United States)
Univ. of Oklahoma, Norman, OK (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States)
Univ. of Central Florida, Orlando, FL (United States). Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC)
Ames Lab., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States). Materials Analysis and Research Lab.
Ames Lab., and Iowa State Univ., Ames, IA (United States)

Effective control on chemoselectivity in the catalytic hydrogenation of C=O over C=C bonds is uncommon with Pd-based catalysts because of the favored adsorption of C=C bonds on Pd surface. Here we report a unique orthorhombic PdSn intermetallic phase with unprecedented chemoselectivity toward C=O hydrogenation. We observed the formation and metastability of this PdSn phase in situ. During a natural cooling process, the PdSn nanoparticles readily revert to the favored Pd₃Sn₂ phase. Instead, using a thermal quenching method, we prepared a pure-phase PdSn nanocatalyst. Furthermore, PdSn shows an >96% selectivity toward hydrogenating C=O bonds of various α,β-unsaturated aldehydes, highest in reported Pd-based catalysts. Further study suggests that efficient quenching prevents the reversion from PdSn- to Pd₃Sn₂-structured surface, the key to the desired catalytic performance. Density functional theory calculations and analysis of reaction kinetics provide an explanation for the observed high selectivity.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE

Grant/Contract Number:: AC02-06CH11357; AC02-07CH11358; SC0013897; SC0018284

OSTI ID:: 1817653

Alternate ID(s):: OSTI ID: 1808608
OSTI ID: 1814768
OSTI ID: 1814797
OSTI ID: 1818354

Report Number(s):: IS--J 10,555

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 33 Vol. 60; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (44)

Silica-Encapsulated Pt-Sn Intermetallic Nanoparticles: A Robust Catalytic Platform for Parahydrogen-Induced Polarization of Gases and Liquids Zhao, Evan W.; Maligal-Ganesh, Raghu; Xiao, Chaoxian Angewandte Chemie, Vol. 129, Issue 14 https://doi.org/10.1002/ange.201701314	journal	March 2017
Silica-Encapsulated Pt-Sn Intermetallic Nanoparticles: A Robust Catalytic Platform for Parahydrogen-Induced Polarization of Gases and Liquids Zhao, Evan W.; Maligal-Ganesh, Raghu; Xiao, Chaoxian Angewandte Chemie International Edition, Vol. 56, Issue 14 https://doi.org/10.1002/anie.201701314	journal	March 2017
From Oxide-Supported Palladium to Intermetallic Palladium Phases: Consequences for Methanol Steam Reforming Lorenz, Harald; Rameshan, Christoph; Bielz, Thomas ChemCatChem, Vol. 5, Issue 6 https://doi.org/10.1002/cctc.201200712	journal	February 2013
Facile and Convenient Method of Deuterium Gas Generation Using a Pd/C-Catalyzed H2–D2 Exchange Reaction and Its Application to Synthesis of Deuterium-Labeled Compounds Kurita, Takanori; Aoki, Fumiyo; Mizumoto, Takuto Chemistry - A European Journal, Vol. 14, Issue 11 https://doi.org/10.1002/chem.200701245	journal	April 2008
Selective Hydrogenation and H-D Exchange of Unsaturated Hydrocarbons on Pd(100)-P(1×1)-H(D) Guo, X. C.; Madix, R. J. Journal of Catalysis, Vol. 155, Issue 2 https://doi.org/10.1006/jcat.1995.1215	journal	September 1995
EXAFS Studies of Supported Rh–Sn Catalysts for Citral Hydrogenation Sordelli, Laura; Psaro, Rinaldo; Vlaic, Gilberto Journal of Catalysis, Vol. 182, Issue 1 https://doi.org/10.1006/jcat.1998.2348	journal	February 1999
Outstanding Performances of Magnesia-Supported Platinum–Tin Catalysts for Citral Selective Hydrogenation Recchia, Sandro; Dossi, Carlo; Poli, Nicola Journal of Catalysis, Vol. 184, Issue 1 https://doi.org/10.1006/jcat.1999.2485	journal	May 1999
On the Stability and Recyclability of Supported Metal–Ligand Complex Catalysts: Myths, Misconceptions and Critical Research Needs Jones, Christopher W. Topics in Catalysis, Vol. 53, Issue 13-14 https://doi.org/10.1007/s11244-010-9513-9	journal	May 2010
Metal-support effects on the intramolecular selectivity of crotonaldehyde hydrogenation over platinum Vannice, M. Journal of Catalysis, Vol. 115, Issue 1 https://doi.org/10.1016/0021-9517(89)90007-9	journal	January 1989
Catalytic denitrification of water with palladium-based catalysts supported on activated carbons Lemaignen, L.; Tong, C.; Begon, V. Catalysis Today, Vol. 75, Issue 1-4 https://doi.org/10.1016/S0920-5861(02)00042-1	journal	July 2002
Hydrogenation of carvone on Pt–Sn/Al2O3 catalysts Torres, Gerardo C.; Ledesma, Sandra D.; Jablonski, Estanislao L. Catalysis Today, Vol. 48, Issue 1-4 https://doi.org/10.1016/S0920-5861(98)00359-9	journal	January 1999
Effects of thiophene on CO adsorption and crotonaldehyde hydrogenation over silica-supported Pd$z.sbnd;Cu catalysts Ashour, S. Journal of Molecular Catalysis A: Chemical, Vol. 123, Issue 1 https://doi.org/10.1016/S1381-1169(97)00045-9	journal	August 1997
Palladium-based alloy and monometallic catalysts for gas phase hydrogenation of crotonaldehyde: effects of alloying and alloy crystallite size Iwasa, Nobuhiro; Takizawa, Masanori; Arai, Masahiko Applied Catalysis A: General, Vol. 283, Issue 1-2 https://doi.org/10.1016/j.apcata.2005.01.015	journal	April 2005
Chemoselective hydrogenation of carbonyl compounds over heterogeneous catalysts Mäki-Arvela, P.; Hájek, J.; Salmi, T. Applied Catalysis A: General, Vol. 292 https://doi.org/10.1016/j.apcata.2005.05.045	journal	September 2005
Origin of different deactivation of Pd/SnO2 and Pd/GeO2 catalysts in methanol dehydrogenation and reforming: A comparative study Lorenz, Harald; Zhao, Qian; Turner, Stuart Applied Catalysis A: General, Vol. 381, Issue 1-2 https://doi.org/10.1016/j.apcata.2010.04.015	journal	June 2010
Tuning catalytic selectivity of liquid-phase hydrogenation of furfural via synergistic effects of supported bimetallic catalysts Chen, Bingfeng; Li, Fengbo; Huang, Zhijun Applied Catalysis A: General, Vol. 500 https://doi.org/10.1016/j.apcata.2015.05.006	journal	July 2015
Pd-SnO2/Al2O3 heteroaggregate nanocatalysts for selective hydrogenations of p-nitroacetophenone and p-nitrobenzaldehyde Liu, Miaomiao; Tang, Weiqiang; Xu, Yisheng Applied Catalysis A: General, Vol. 549 https://doi.org/10.1016/j.apcata.2017.10.004	journal	January 2018
Effect of the support on tin distribution in Pd–Sn/Al2O3 and Pd–Sn/SiO2 catalysts for application in water denitration Garron, Anthony; Lázár, Károly; Epron, Florence Applied Catalysis B: Environmental, Vol. 59, Issue 1-2 https://doi.org/10.1016/j.apcatb.2005.01.002	journal	July 2005
Carbon-supported PdSn and Pd3Sn2 anodes for glucose electrooxidation in alkaline media Brouzgou, A.; Song, S.; Tsiakaras, P. Applied Catalysis B: Environmental, Vol. 158-159 https://doi.org/10.1016/j.apcatb.2014.03.051	journal	October 2014
Promotion of Sn on the Pd/AC catalyst for the selective hydrogenation of cinnamaldehyde Zhao, Jia; Xu, Xiaoliang; Li, Xiaonian Catalysis Communications, Vol. 43 https://doi.org/10.1016/j.catcom.2013.09.019	journal	January 2014
Toward Phase and Catalysis Control: Tracking the Formation of Intermetallic Nanoparticles at Atomic Scale Ma, Tao; Wang, Shuai; Chen, Minda Chem, Vol. 5, Issue 5 https://doi.org/10.1016/j.chempr.2019.02.026	journal	May 2019
Bromine-promoted PtZn is very effective for the chemoselective hydrogenation of crotonaldehyde Galloway, E.; Armbruster, M.; Kovnir, K. Journal of Catalysis, Vol. 261, Issue 1 https://doi.org/10.1016/j.jcat.2008.11.003	journal	January 2009
The relationship between the structural properties of bimetallic Pd–Sn/SiO2 catalysts and their performance for selective citral hydrogenation Vicente, Aurélie; Lafaye, Gwendoline; Especel, Catherine Journal of Catalysis, Vol. 283, Issue 2 https://doi.org/10.1016/j.jcat.2011.07.010	journal	October 2011
Interfacial energy of solid In2Bi intermetallic phase in equilibrium with In–Bi eutectic liquid at 72 °C equilibrating temperature Akbulut, S.; Ocak, Y.; Maraşlı, N. Materials Characterization, Vol. 59, Issue 8 https://doi.org/10.1016/j.matchar.2007.08.028	journal	August 2008
Preparation and characterization of Pd2Sn nanoparticles Page, Katharine; Schade, Christina S.; Zhang, Jinping Materials Research Bulletin, Vol. 42, Issue 12 https://doi.org/10.1016/j.materresbull.2007.05.010	journal	December 2007
Common Pitfalls of Catalysis Manuscripts Submitted to Chemistry of Materials Schüth, Ferdi; Ward, Michael D.; Buriak, Jillian M. Chemistry of Materials, Vol. 30, Issue 11 https://doi.org/10.1021/acs.chemmater.8b01831	journal	May 2018
Single-Atom Alloy Pd–Ag Catalyst for Selective Hydrogenation of Acrolein Aich, Payoli; Wei, Haojuan; Basan, Bridget The Journal of Physical Chemistry C, Vol. 119, Issue 32 https://doi.org/10.1021/acs.jpcc.5b01357	journal	July 2015
A Ship-in-a-Bottle Strategy To Synthesize Encapsulated Intermetallic Nanoparticle Catalysts: Exemplified for Furfural Hydrogenation Maligal-Ganesh, Raghu V.; Xiao, Chaoxian; Goh, Tian Wei ACS Catalysis, Vol. 6, Issue 3 https://doi.org/10.1021/acscatal.5b02281	journal	February 2016
Individual Heat of Adsorption of Adsorbed CO Species on Palladium and Pd–Sn Nanoparticles Supported on Al ₂ O ₃ by Using Temperature-Programmed Adsorption Equilibrium Methods Jbir, Imen; Couble, Julien; Khaddar-Zine, Sihem ACS Catalysis, Vol. 6, Issue 4 https://doi.org/10.1021/acscatal.5b02749	journal	March 2016
Selective Hydrogenation of Crotonaldehyde to Crotyl Alcohol over Metal Oxide Modified Ir Catalysts and Mechanistic Insight Tamura, Masazumi; Tokonami, Kensuke; Nakagawa, Yoshinao ACS Catalysis, Vol. 6, Issue 6 https://doi.org/10.1021/acscatal.6b00400	journal	May 2016
Bimetallic Silica-Supported Catalysts Based on Ni−Sn, Pd−Sn, and Pt−Sn as Materials in the CO Oxidation Reaction Araña, J.; Ramirez de la Piscina, P.; Llorca, J. Chemistry of Materials, Vol. 10, Issue 5 https://doi.org/10.1021/cm970728n	journal	April 1998
Bifunctional Catalytic System Effective for Oxidative Dehydrogenation of 1-Butene and n -Butane Using Pd-Based Intermetallic Compounds Furukawa, Shinya; Endo, Masahiro; Komatsu, Takayuki ACS Catalysis, Vol. 4, Issue 10 https://doi.org/10.1021/cs500920p	journal	September 2014
Liquid-Phase Hydrogenation of Crotonaldehyde over Platinum- and Palladium-Based Catalysts Campo, Betiana C.; Volpe, María A.; Gigola, Carlos E. Industrial & Engineering Chemistry Research, Vol. 48, Issue 23 https://doi.org/10.1021/ie901217r	journal	October 2009
Shape-Controlled Conversion of β-Sn Nanocrystals into Intermetallic M -Sn ( M = Fe, Co, Ni, Pd) Nanocrystals Chou, Nam Hawn; Schaak, Raymond E. Journal of the American Chemical Society, Vol. 129, Issue 23 https://doi.org/10.1021/ja069032y	journal	June 2007
Electrooxidation of Methanol at SnO _x –Pt Interface: A Tunable Activity of Tin Oxide Nanoparticles Zhou, Wei-Ping; An, Wei; Su, Dong The Journal of Physical Chemistry Letters, Vol. 3, Issue 22 https://doi.org/10.1021/jz3015925	journal	October 2012
Controlled selectivity for palladium catalysts using self-assembled monolayers Marshall, Stephen T.; O’Brien, Marykate; Oetter, Brittany Nature Materials, Vol. 9, Issue 10 https://doi.org/10.1038/nmat2849	journal	September 2010
Solvent-mediated charge separation drives alternative hydrogenation path of furanics in liquid water Zhao, Zheng; Bababrik, Reda; Xue, Wenhua Nature Catalysis, Vol. 2, Issue 5 https://doi.org/10.1038/s41929-019-0257-z	journal	April 2019
Hydrogenation of cinnamaldehyde to hydrocinnamaldehyde over Pd nanoparticles deposited on nitrogen-doped mesoporous carbon Nagpure, Atul S.; Gurrala, Lakshmiprasad; Gogoi, Pranjal RSC Advances, Vol. 6, Issue 50 https://doi.org/10.1039/C6RA04154J	journal	January 2016
Kinetics, energetics, and size dependence of the transformation from Pt to ordered PtSn intermetallic nanoparticles Chen, Minda; Han, Yong; Goh, Tian Wei Nanoscale, Vol. 11, Issue 12 https://doi.org/10.1039/C8NR10067E	journal	January 2019
The nature of the active sites of Pd–Ga catalysts in the hydrogenation of CO ₂ to methanol Manrique, Raydel; Rodríguez-Pereira, Jhonatan; Rincón-Ortiz, Sergio A. Catalysis Science & Technology, Vol. 10, Issue 19 https://doi.org/10.1039/D0CY00956C	journal	January 2020
Synthesis, characterization and sensing properties of nano-SnO ₂ supported on SBA-15 as highly sensitive semiconductor gas sensors Yang, Jun; Hidajat, Kus; Kawi, Sibudjing J. Mater. Chem., Vol. 19, Issue 2 https://doi.org/10.1039/b807539e	journal	January 2009
Selective Hydrogenation of α,β-Unsaturated Aldehydes Gallezot, P.; Richard, D. Catalysis Reviews, Vol. 40, Issue 1-2 https://doi.org/10.1080/01614949808007106	journal	February 1998
The direct measurement of temperature changes within freeze-fracture specimens during rapid quenching in liquid coolants Costello, M. J.; Corless, J. M. Journal of Microscopy, Vol. 112, Issue 1 https://doi.org/10.1111/j.1365-2818.1978.tb01151.x	journal	January 1978
Thermal unequilibrium of strained black CsPbI ₃ thin films Steele, Julian A.; Jin, Handong; Dovgaliuk, Iurii Science, Vol. 365, Issue 6454 https://doi.org/10.1126/science.aax3878	journal	July 2019

Similar Records

Thermal Unequilibrium of PdSn Intermetallic Nanocatalysts: From In Situ Tailored Synthesis to Unexpected Hydrogenation Selectivity

Journal Article · Thu Jul 15 20:00:00 EDT 2021 · Angewandte Chemie · OSTI ID:1808607

Chemisorption and diffusion of atomic hydrogen in and on cluster models of Pd, Rh, and bimetallic PdSn, RhSn, and RhZn catalysts

Journal Article · Tue Nov 06 23:00:00 EST 1990 · Journal of the American Chemical Society; (United States) · OSTI ID:5757660

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
alpha
beta-unsaturated aldehydes
heterogeneous catalysis
intermetallic phases
metastable compounds
nanoparticles

Thermal Unequilibrium of PdSn Intermetallic Nanocatalysts: From In Situ Tailored Synthesis to Unexpected Hydrogenation Selectivity

Citation Formats

References (44)

Similar Records

Related Subjects