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

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

Journal Article · 02 October 2024 · Nature Communications

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

^[1];

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

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^[2]; Li, Zhenglong ^[7];

^[1];

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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

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

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

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