Silicalite-1 Stabilizes Zn-Hydride Species for Efficient Propane Dehydrogenation

Shaojia Song; Kun Yang; Peng Zhang; Zhijie Wu; Jun Li; Hui Su; Sheng Dai; Chunming Xu; Zhenxing Li; Jian Liu; Weiyu Song

doi:10.1021/acscatal.2c00928

Silicalite-1 Stabilizes Zn-Hydride Species for Efficient Propane Dehydrogenation

Shaojia Song
, Kun Yang
, Peng Zhang
, Zhijie Wu
, Jun Li
, Hui Su
, Sheng Dai
, Chunming Xu
, Zhenxing Li
, Jian Liu
, Weiyu Song

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

100 Scopus citations

Abstract

Propane dehydrogenation (PDH) is promising for producing high value-added propylene. The discovery of a more efficient, economical, and nontoxic PDH catalyst is of great importance. Herein, we found zinc hydrides ([ZnH]⁺) as the highly reactive site for PDH. In situ spectroscopy and theoretical studies reveal that [ZnH]⁺ was transformed from zinc hydroxyl ([ZnOH]⁺) sites under reductive conditions. Accordingly, the formation of [ZnH]⁺ can be controlled by adjusting the amount of zinc hydroxyl ([ZnOH]⁺) species by various additives. The optimized Cu-ZnO@S-1 consists of exclusively isolated [ZnOH]⁺ sites, which help produce more [ZnH]⁺ toward optimal PDH activity. Specifically, the catalyst enables 43% propane conversion with >88% propylene selectivity, close to the thermodynamic equilibrium.

Original language	English
Pages (from-to)	5997-6006
Number of pages	10
Journal	ACS Catalysis
Volume	12
Issue number	10
DOIs	https://doi.org/10.1021/acscatal.2c00928
State	Published - May 20 2022
Externally published	Yes

Funding

This work was supported by the National Natural Science Foundation of China (nos. 22178381, 22035009), the National Key R&D Program of China(2021YFA1501301), the National Science Foundation of China University of Petroleum, Beijing (no. ZX20200079), and the State Key Laboratory of Heavy Oil Processing (no. 2021-03).

Keywords

bimetallic catalysts
density functional theory
nonoxidative propane dehydrogenation
zeolite
zinc hydrides

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10.1021/acscatal.2c00928

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@article{c3c25bf48f51484fab1968202843d082,

title = "Silicalite-1 Stabilizes Zn-Hydride Species for Efficient Propane Dehydrogenation",

abstract = "Propane dehydrogenation (PDH) is promising for producing high value-added propylene. The discovery of a more efficient, economical, and nontoxic PDH catalyst is of great importance. Herein, we found zinc hydrides ([ZnH]+) as the highly reactive site for PDH. In situ spectroscopy and theoretical studies reveal that [ZnH]+ was transformed from zinc hydroxyl ([ZnOH]+) sites under reductive conditions. Accordingly, the formation of [ZnH]+ can be controlled by adjusting the amount of zinc hydroxyl ([ZnOH]+) species by various additives. The optimized Cu-ZnO@S-1 consists of exclusively isolated [ZnOH]+ sites, which help produce more [ZnH]+ toward optimal PDH activity. Specifically, the catalyst enables 43\% propane conversion with >88\% propylene selectivity, close to the thermodynamic equilibrium.",

keywords = "bimetallic catalysts, density functional theory, nonoxidative propane dehydrogenation, zeolite, zinc hydrides",

author = "Shaojia Song and Kun Yang and Peng Zhang and Zhijie Wu and Jun Li and Hui Su and Sheng Dai and Chunming Xu and Zhenxing Li and Jian Liu and Weiyu Song",

note = "Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

month = may,

day = "20",

doi = "10.1021/acscatal.2c00928",

language = "English",

volume = "12",

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TY - JOUR

T1 - Silicalite-1 Stabilizes Zn-Hydride Species for Efficient Propane Dehydrogenation

AU - Song, Shaojia

AU - Yang, Kun

AU - Zhang, Peng

AU - Wu, Zhijie

AU - Li, Jun

AU - Su, Hui

AU - Dai, Sheng

AU - Xu, Chunming

AU - Li, Zhenxing

AU - Liu, Jian

AU - Song, Weiyu

PY - 2022/5/20

Y1 - 2022/5/20

N2 - Propane dehydrogenation (PDH) is promising for producing high value-added propylene. The discovery of a more efficient, economical, and nontoxic PDH catalyst is of great importance. Herein, we found zinc hydrides ([ZnH]+) as the highly reactive site for PDH. In situ spectroscopy and theoretical studies reveal that [ZnH]+ was transformed from zinc hydroxyl ([ZnOH]+) sites under reductive conditions. Accordingly, the formation of [ZnH]+ can be controlled by adjusting the amount of zinc hydroxyl ([ZnOH]+) species by various additives. The optimized Cu-ZnO@S-1 consists of exclusively isolated [ZnOH]+ sites, which help produce more [ZnH]+ toward optimal PDH activity. Specifically, the catalyst enables 43% propane conversion with >88% propylene selectivity, close to the thermodynamic equilibrium.

AB - Propane dehydrogenation (PDH) is promising for producing high value-added propylene. The discovery of a more efficient, economical, and nontoxic PDH catalyst is of great importance. Herein, we found zinc hydrides ([ZnH]+) as the highly reactive site for PDH. In situ spectroscopy and theoretical studies reveal that [ZnH]+ was transformed from zinc hydroxyl ([ZnOH]+) sites under reductive conditions. Accordingly, the formation of [ZnH]+ can be controlled by adjusting the amount of zinc hydroxyl ([ZnOH]+) species by various additives. The optimized Cu-ZnO@S-1 consists of exclusively isolated [ZnOH]+ sites, which help produce more [ZnH]+ toward optimal PDH activity. Specifically, the catalyst enables 43% propane conversion with >88% propylene selectivity, close to the thermodynamic equilibrium.

KW - bimetallic catalysts

KW - density functional theory

KW - nonoxidative propane dehydrogenation

KW - zeolite

KW - zinc hydrides

UR - https://www.scopus.com/pages/publications/85140096232

U2 - 10.1021/acscatal.2c00928

DO - 10.1021/acscatal.2c00928

M3 - Article

AN - SCOPUS:85140096232

SN - 2155-5435

VL - 12

SP - 5997

EP - 6006

JO - ACS Catalysis

JF - ACS Catalysis

IS - 10

ER -

Silicalite-1 Stabilizes Zn-Hydride Species for Efficient Propane Dehydrogenation

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Keywords

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