Highly dispersed Pd-based pseudo-single atoms in zeolites for hydrogen generation and pollutant disposal
Kai Zhang1, Ning Wang4(王宁)*, Yali Meng1, Tianjun Zhang5, Pu Zhao1, Qiming Sun1,2 （孙启明）*, Jihong Yu3
1Innovation Center for Chemical Science, College of Chemistry, Chemical Engineering, and Materials Science, Soochow University, Suzhou, 215123, P. R. China.
2Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, 215123, Jiangsu, P. R. China
3State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, International Center of Future Science, College of Chemistry, Jilin University, Changchun 130012, P. R. China.
4Institute of Sustainable Energy and Resources, College of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, P. R. China.
5College of Chemistry and Materials Science, Hebei University, Baoding 071002, P. R. China
Chem. Sci., 2024, 15, 379–388
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.
链接：//pubs.rsc.org/en/content/articlelanding/2024/sc/d3sc05851d
