Tuning metal-support interactions in nickel–zeolite catalysts leads to enhanced stability during dry reforming of methane

Zhang, Junyan; Li, Yuanyuan; Song, Haohong; Zhang, Lihua; Wu, Yiqing; He, Yang; Ma, Lu; Hong, Jiyun; Tayal, Akhil; Marinkovic, Nebojsa; Jiang, De-en; Li, Zhenglong; Wu, Zili; Polo-Garzon, Felipe

doi:10.1038/s41467-024-50729-8

Tuning metal-support interactions in nickel–zeolite catalysts leads to enhanced stability during dry reforming of methane

Journal Article · Thu Oct 03 00:00:00 EDT 2024 · Nature Communications

DOI:https://doi.org/10.1038/s41467-024-50729-8· OSTI ID:2455058

^[1]; ^[1]; ^[2]; Zhang, Lihua ^[3]; Wu, Yiqing ^[1]; He, Yang ^[1]; Ma, Lu ^[4]; Hong, Jiyun ^[5]; Tayal, Akhil ^[4]; ^[6]; ^[2]; Li, Zhenglong ^[7]; ^[1]; ^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Vanderbilt Univ., Nashville, TN (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Columbia Univ., New York, NY (United States)
Zhejiang Univ., Hangzhou (China); Institute of Zhejiang University, Quzhou (China)

Ni-based catalysts are highly reactive for dry reforming of methane (DRM) but they are prone to rapid deactivation due to sintering and/or coking. In this study, we present a straightforward approach for anchoring dispersed Ni sites with strengthened metal-support interactions, which leads to Ni active sites embedded in dealuminated Beta zeolite with superior stability and rates for DRM. The process involves solid-state grinding of dealuminated Beta zeolites and nickel nitrate, followed by calcination under finely controlled gas flow conditions. By combining in situ X-ray absorption spectroscopy and ab initio simulations, it is elucidated that the efficient removal of byproducts during catalyst synthesis is conducted to strengthen Ni–Si interactions that suppress coking and sintering after 100 h of time-on-stream. Transient isotopic kinetic experiments shed light on the differences in intrinsic turnover frequency of Ni species and explain performance trends. This work constructs a fundamental understanding regarding the implication of facile synthesis protocols on metal-support interaction in zeolite-supported Ni sites, and it lays the needed foundations on how these interactions can be tuned for outstanding DRM performance.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

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

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; AC05-00OR22725; SC0012704

OSTI ID:: 2455058

Alternate ID(s):: OSTI ID: 2477953
OSTI ID: 2475729

Report Number(s):: BNL--226342-2024-JAAM

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (38)

The role of catalyst support on the activity of nickel for reforming methane with CO2 Gadalla, Ahmed M.; Bower, Barbara Chemical Engineering Science, Vol. 43, Issue 11 https://doi.org/10.1016/0009-2509(88)80058-7	journal	January 1988
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Catalyst deactivation: is it predictable? Moulijn, J. A.; van Diepen, A. E.; Kapteijn, F. Applied Catalysis A: General, Vol. 212, Issue 1-2 https://doi.org/10.1016/S0926-860X(00)00842-5	journal	April 2001
Effect of metal particle size on coking during CO2 reforming of CH4 over Ni–alumina aerogel catalysts Kim, Jin-Hong; Suh, Dong Jin; Park, Tae-Jin Applied Catalysis A: General, Vol. 197, Issue 2 https://doi.org/10.1016/S0926-860X(99)00487-1	journal	May 2000
Embedding high loading and uniform Ni nanoparticles into silicalite-1 zeolite for dry reforming of methane Liu, Yang; Chen, Yong; Gao, Zirui Applied Catalysis B: Environmental, Vol. 307 https://doi.org/10.1016/j.apcatb.2022.121202	journal	June 2022
Dynamic trap of Ni at elevated temperature for yielding high-efficiency methane dry reforming catalyst He, Dedong; Wu, Shaojie; Cao, Xiaohua Applied Catalysis B: Environment and Energy, Vol. 346 https://doi.org/10.1016/j.apcatb.2024.123728	journal	June 2024
Activity of different zeolite-supported Ni catalysts for methane reforming with carbon dioxide Luengnaruemitchai, Apanee; Kaengsilalai, Athiya Chemical Engineering Journal, Vol. 144, Issue 1 https://doi.org/10.1016/j.cej.2008.05.023	journal	October 2008
Developing silicalite-1 encapsulated Ni nanoparticles as sintering-/coking-resistant catalysts for dry reforming of methane Xu, Shanshan; Slater, Thomas J. A.; Huang, Hong Chemical Engineering Journal, Vol. 446, Issue Part 5 https://doi.org/10.1016/j.cej.2022.137439	journal	October 2022
Nanostructured Ni-containing spinel oxides for the dry reforming of methane: Effect of the presence of cobalt and nickel on the deactivation behaviour of catalysts de Sousa, Francisco F.; de Sousa, Helvio S. A.; Oliveira, Alcemira C. International Journal of Hydrogen Energy, Vol. 37, Issue 4 https://doi.org/10.1016/j.ijhydene.2011.11.072	journal	February 2012
Acid and redox activity of template-free Al-rich H-BEA * and Fe-BEA * zeolites Sazama, Petr; Wichterlová, Blanka; Sklenák, Štěpán Journal of Catalysis, Vol. 318 https://doi.org/10.1016/j.jcat.2014.06.024	journal	October 2014
Variation of the Si/Al ratio in nanosized zeolite Beta crystals Mintova, S.; Valtchev, V.; Onfroy, T. Microporous and Mesoporous Materials, Vol. 90, Issue 1-3 https://doi.org/10.1016/j.micromeso.2005.11.026	journal	March 2006
Dry Reforming of Methane with Suppressed Carbon Deposition over Cr- and Ni-Loaded Dealuminated β Zeolites Tamura, Kazuya; Murata, Daisuke; Sumi, Tomoka Energy & Fuels, Vol. 37, Issue 23 https://doi.org/10.1021/acs.energyfuels.3c02837	journal	November 2023
Hierarchical Echinus-like Cu-MFI Catalysts for Ethanol Dehydrogenation Pang, Jifeng; Zheng, Mingyuan; Wang, Chan ACS Catalysis, Vol. 10, Issue 22 https://doi.org/10.1021/acscatal.0c03860	journal	November 2020
CH₄ Activation over Perovskite Catalysts: True Density and Reactivity of Active Sites Polo-Garzon, Felipe; Fung, Victor; Zhang, Junyan ACS Catalysis, Vol. 12, Issue 19 https://doi.org/10.1021/acscatal.2c03239	journal	September 2022
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
Dry Reforming of Methane on Rh-Doped Pyrochlore Catalysts: A Steady-State Isotopic Transient Kinetic Study Polo-Garzon, Felipe; Pakhare, Devendra; Spivey, James J. ACS Catalysis, Vol. 6, Issue 6 https://doi.org/10.1021/acscatal.6b00666	journal	May 2016
Dimerization of Linear Butenes on Zeolite-Supported Ni ²⁺ Ehrmaier, Andreas; Liu, Yue; Peitz, Stephan ACS Catalysis, Vol. 9, Issue 1 https://doi.org/10.1021/acscatal.8b03095	journal	November 2018
The Origin of the Special Surface and Catalytic Chemistry of Ga-Rich Ni ₃ Ga in the Direct Dehydrogenation of Ethane He, Yang; Song, Yuanjun; Laursen, Siris ACS Catalysis, Vol. 9, Issue 11 https://doi.org/10.1021/acscatal.9b03402	journal	September 2019
Structure Sensitivity in Steam and Dry Methane Reforming over Nickel: Activity and Carbon Formation Vogt, Charlotte; Kranenborg, Jelle; Monai, Matteo ACS Catalysis, Vol. 10, Issue 2 https://doi.org/10.1021/acscatal.9b04193	journal	December 2019
Carbon Dioxide Reforming of Methane To Produce Synthesis Gas over Metal-Supported Catalysts: State of the Art Wang, Shaobin; Lu, G. Q. (Max); Millar, Graeme J. Energy & Fuels, Vol. 10, Issue 4 https://doi.org/10.1021/ef950227t	journal	January 1996
Nickel K-edge x-ray absorption fine structure of lithium nickel oxides Pickering, Ingrid J.; George, Graham N.; Lewandowski, Joseph T. Journal of the American Chemical Society, Vol. 115, Issue 10 https://doi.org/10.1021/ja00063a035	journal	May 1993
Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite Moliner, Manuel; Gabay, Jadeene E.; Kliewer, Chris E. Journal of the American Chemical Society, Vol. 138, Issue 48 https://doi.org/10.1021/jacs.6b10169	journal	November 2016
Effect of the Preparation Method on the State of Nickel Ions in BEA Zeolites. A Study by Fourier Transform Infrared Spectroscopy of Adsorbed CO and NO, Temperature-Programmed Reduction, and X-Ray Diffraction Penkova, Anna; Dzwigaj, Stanislaw; Kefirov, Radoslav The Journal of Physical Chemistry C, Vol. 111, Issue 24 https://doi.org/10.1021/jp071927p	journal	May 2007
Precise Identification of the Infrared Bands of the Polycarbonyl Complexes on Ni–MOR Zeolite by¹²C¹⁶O–¹³C¹⁸O Coadsorption and Computational Modeling Aleksandrov, Hristiyan A.; Zdravkova, Videlina R.; Mihaylov, Mihail Y. The Journal of Physical Chemistry C, Vol. 116, Issue 43 https://doi.org/10.1021/jp304972u	journal	October 2012
Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes Li, Y.; Zakharov, D.; Zhao, S. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8583	journal	June 2015
Enhanced CO2 utilization in dry reforming of methane achieved through nickel-mediated hydrogen spillover in zeolite crystals Zhu, Qiuyan; Zhou, Hang; Wang, Liang Nature Catalysis, Vol. 5, Issue 11 https://doi.org/10.1038/s41929-022-00870-8	journal	November 2022
Zeolite-supported ultra-small nickel as catalyst for selective oxidation of methane to syngas Yasuda, Shuhei; Osuga, Ryota; Kunitake, Yusuke Communications Chemistry, Vol. 3, Issue 1 https://doi.org/10.1038/s42004-020-00375-0	journal	September 2020
A review of dry (CO ₂ ) reforming of methane over noble metal catalysts Pakhare, Devendra; Spivey, James Chem. Soc. Rev., Vol. 43, Issue 22 https://doi.org/10.1039/C3CS60395D	journal	January 2014
Unique chemistries of metal-nitrate precursors to form metal-oxide thin films from solution: materials for electronic and energy applications Cochran, Elizabeth A.; Woods, Keenan N.; Johnson, Darren W. Journal of Materials Chemistry A, Vol. 7, Issue 42 https://doi.org/10.1039/C9TA07727H	journal	January 2019
Advanced zeolite and ordered mesoporous silica-based catalysts for the conversion of CO₂to chemicals and fuels Velty, Alexandra; Corma, Avelino Chemical Society Reviews, Vol. 52, Issue 5 https://doi.org/10.1039/D2CS00456A	journal	January 2023
Solving the structure of reaction intermediates by time-resolved synchrotron x-ray absorption spectroscopy Wang, Qi; Hanson, Jonathan C.; Frenkel, Anatoly I. The Journal of Chemical Physics, Vol. 129, Issue 23 https://doi.org/10.1063/1.3040271	journal	December 2008
Reforming of methane: Effects of active metals, supports, and promoters Al-Fatesh, Ahmed S.; Patel, Naitik; Fakeeha, Anis H. Catalysis Reviews https://doi.org/10.1080/01614940.2023.2211447	journal	May 2023
The Distribution of Active ingredients in Supported Catalysts Prepared by Impregnation Lee, Sheng-Yi; Aris, Rutherford Catalysis Reviews, Vol. 27, Issue 2 https://doi.org/10.1080/01614948508064737	journal	June 1985
CO ₂ Reforming of CH ₄ Bradford, M. C. J.; Vannice, M. A. Catalysis Reviews, Vol. 41, Issue 1 https://doi.org/10.1081/CR-100101948	journal	February 1999
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y. Physical Review B, Vol. 57, Issue 3, p. 1505-1509 https://doi.org/10.1103/PhysRevB.57.1505	journal	January 1998
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
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

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Tuning metal-support interactions in nickel–zeolite catalysts leads to enhanced stability during dry reforming of methane

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