Intra-crystalline mesoporous zeolite encapsulation-derived thermally robust metal nanocatalyst in deep oxidation of light alkanes

Peng, Honggen; Dong, Tao; Yang, Shenyou; Chen, Hao; Yang, Zhenzhen; Liu, Wenming; He, Chi; Wu, Peng; Tian, Jinshu; Peng, Yue; Chu, Xuefeng; Wu, Daishe; An, Taicheng; Wang, Yong; Dai, Sheng

doi:10.1038/s41467-021-27828-x

Title: Intra-crystalline mesoporous zeolite encapsulation-derived thermally robust metal nanocatalyst in deep oxidation of light alkanes

Journal Article · Thu Jan 13 00:00:00 EST 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-27828-x· OSTI ID:1844855

^[1]; Dong, Tao ^[1]; Yang, Shenyou ^[1]; Chen, Hao ^[2];

^[2]; Liu, Wenming ^[1];

^[3];

^[4]; Tian, Jinshu ^[5];

^[6]; Chu, Xuefeng ^[6]; Wu, Daishe ^[1];

^[7]; Wang, Yong ^[8];

^[2]

Nanchang Univ. (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Xi’an Jiaotong University, Shaanxi (China)
East China Normal Univ. (ECNU), Shanghai (China)
Zhejiang Univ. of Technology, Hangzhou (China)
Tsinghua Univ., Beijing (China)
Guangdong University of Technology, Guangzhou (China)
Washington State Univ., Pullman, WA (United States)

Zeolite-confined metal nanoparticles (NPs) have attracted much attention owing to their superior sintering resistance and broad applications for thermal and environmental catalytic reactions. However, the pore size of the conventional zeolites is usually below 2 nm, and reactants are easily blocked to access the active sites. Herein, a facile in situ mesoporogen-free strategy is developed to design and synthesize palladium (Pd) NPs enveloped in a single-crystalline zeolite (silicalite-1, S-1) with intra-mesopores (termed Pd@IM-S-1). Pd@IM-S-1 exhibited remarkable light alkanes deep oxidation performances, and it should be attributed to the confinement and guarding effect of the zeolite shell and the improvement in mass-transfer efficiency and active metal sites accessibility. The Pd–PdO interfaces as a new active site can provide active oxygen species to the first C–H cleavage of light alkanes. This work exemplifies a promising strategy to design other high-performance intra-crystalline mesoporous zeolite-confined metal/metal oxide catalysts for high-temperature industrial thermal catalysis.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China; Natural Science Foundation of Jiangxi Province; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1844855

Journal Information:: Nature Communications, Vol. 13, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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