Tuning metal-support interactions in nickel–zeolite catalysts leads to enhanced stability during dry reforming of methane
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.
Authors
- Felipe Polo‐Garzon (ORCID: https://orcid.org/0000-0002-6507-6183)
- Akhil Tayal (ORCID: https://orcid.org/0000-0001-8152-4209)
- De‐en Jiang (ORCID: https://orcid.org/0000-0001-5167-0731)
- Nebojša Marinković (ORCID: https://orcid.org/0000-0003-3579-3453)
- Jiyun Hong (ORCID: https://orcid.org/0000-0002-3631-0559)
- Zili Wu (ORCID: https://orcid.org/0000-0002-4468-3240)
- Haohong Song (ORCID: https://orcid.org/0009-0003-2037-7905)
- Lu‐Fang Ma (ORCID: https://orcid.org/0000-0002-5601-6437)
- Yuanyuan Li (ORCID: https://orcid.org/0000-0003-3074-9672)
- Lihua Zhang (ORCID: https://orcid.org/0000-0003-3331-2345)
- Yiqing Wu (ORCID: https://orcid.org/0000-0002-9746-0163)
- Zhenglong Li (ORCID: https://orcid.org/0000-0001-8811-8625)
- Junyan Zhang
- Yang He (ORCID: https://orcid.org/0000-0002-8530-9132)
Institutions
- Oak Ridge National Laboratory (US)
- Vanderbilt University (US)
- Brookhaven National Laboratory (US)
- SLAC National Accelerator Laboratory (US)
- Quzhou University (CN)
- Zhejiang University (CN)
- Columbia University (US)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-10-03
- DOI
- https://doi.org/10.1038/s41467-024-50729-8
- Citations
- 53
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 6.21
Funders
- U.S. Department of Energy
- Battelle
- UT-Battelle
- Office of Science
- Basic Energy Sciences
- Chemical Sciences, Geosciences, and Biosciences Division
- Oak Ridge National Laboratory
- SLAC National Accelerator Laboratory