Issue 1, 2024

Highly dispersed Pd-based pseudo-single atoms in zeolites for hydrogen generation and pollutant disposal

Abstract

Atomically dispersed metal catalysts with excellent activity and stability are highly desired in heterogeneous catalysis. Herein, we synthesized zeolite-encaged Pd-based pseudo-single atoms via a facile and energy-efficient ligand-protected direct H2 reduction method. Cs-corrected scanning transmission electron microscopy, extended X-ray absorption, and pair distribution function measurements reveal that the metal species are close to atomic-level dispersion and completely confined within the intersectional channels of silicalite-1 (S-1) zeolite with the MFI framework. The Pd@S-1-H exhibits excellent activity and stability in methane combustion reactions with a complete combustion temperature of 390 °C, and no deactivation is observed even after 100 h on stream. The optimized bimetallic 0.8Pd0.2Ni(OH)2@S-1-H catalyst exhibits an excellent H2 generation rate from FA decomposition without any additives, affording a superhigh turnover frequency up to 9308 h−1 at 333 K, which represents the top activity among all of the best heterogeneous catalysts under similar conditions. Significantly, zeolite-encaged metal catalysts are first used for Cr(VI) reduction coupled with formic acid (FA) dehydrogenation and show a superhigh turnover number of 2980 mol(Cr2O72−) mol(Pd)−1 at 323 K, surpassing all of the previously reported catalysts. This work demonstrates that zeolite-encaged pseudo-single atom catalysts are promising in efficient hydrogen storage and pollutant disposal applications.

Graphical abstract: Highly dispersed Pd-based pseudo-single atoms in zeolites for hydrogen generation and pollutant disposal

Supplementary files

Article information

Article type
Edge Article
Submitted
02 11 2023
Accepted
28 11 2023
First published
30 11 2023
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2024,15, 379-388

Highly dispersed Pd-based pseudo-single atoms in zeolites for hydrogen generation and pollutant disposal

K. Zhang, N. Wang, Y. Meng, T. Zhang, P. Zhao, Q. Sun and J. Yu, Chem. Sci., 2024, 15, 379 DOI: 10.1039/D3SC05851D

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