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

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

doi:10.1038/s41467-021-27828-x

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

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

Research output: Contribution to journal › Article › peer-review

92 Scopus citations

Abstract

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.

Original language	English
Article number	295
Journal	Nature Communications
Volume	13
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-27828-x
State	Published - Dec 2022

Funding

Support for this work from the National Natural Science Foundation of China (21976078, 21922606, 21876139, and 21773016), the National Key R&D Program of China (2016YFC0205900), and the Natural Science Foundation of Jiangxi Province (20202ACB213001) is greatly acknowledged by H.P. S.D. was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Dr. An also want to express his thanks for financial support from Guangdong Provincial Key R&D Program (2019B110206002).

Funders	Funder number
Guangdong Provincial Key R&D Program	2019B110206002
U.S. Department of Energy
Basic Energy Sciences
Chemical Sciences, Geosciences, and Biosciences Division
National Natural Science Foundation of China	21773016, 21876139, 21976078, 21922606
Natural Science Foundation of Jiangxi Province	20202ACB213001
National Key Research and Development Program of China	2016YFC0205900

Access to Document

10.1038/s41467-021-27828-x

Cite this

@article{73e480ebbf7546279c41c2412d1ab860,

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

abstract = "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.",

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

note = "Publisher Copyright: {\textcopyright} 2022, This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply.",

year = "2022",

month = dec,

doi = "10.1038/s41467-021-27828-x",

language = "English",

volume = "13",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Research",

number = "1",

}

TY - JOUR

T1 - Intra-crystalline mesoporous zeolite encapsulation-derived thermally robust metal nanocatalyst in deep oxidation of light alkanes

AU - Peng, Honggen

AU - Dong, Tao

AU - Yang, Shenyou

AU - Chen, Hao

AU - Yang, Zhenzhen

AU - Liu, Wenming

AU - He, Chi

AU - Wu, Peng

AU - Tian, Jinshu

AU - Peng, Yue

AU - Chu, Xuefeng

AU - Wu, Daishe

AU - An, Taicheng

AU - Wang, Yong

AU - Dai, Sheng

PY - 2022/12

Y1 - 2022/12

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85123096517&partnerID=8YFLogxK

U2 - 10.1038/s41467-021-27828-x

DO - 10.1038/s41467-021-27828-x

M3 - Article

C2 - 35027532

AN - SCOPUS:85123096517

SN - 2041-1723

VL - 13

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 295

ER -

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

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this