Confined Pyrolysis within Metal-Organic Frameworks to Form Uniform Ru3 Clusters for Efficient Oxidation of Alcohols

Shufang Ji; Yuanjun Chen; Qiang Fu; Yifeng Chen; Juncai Dong; Wenxing Chen; Zhi Li; Yu Wang; Lin Gu; Wei He; Chen Chen; Qing Peng; Yu Huang; Xiangfeng Duan; Dingsheng Wang; Claudia Draxl; Yadong Li

doi:10.1021/jacs.7b05018

Confined Pyrolysis within Metal-Organic Frameworks to Form Uniform Ru₃ Clusters for Efficient Oxidation of Alcohols

Shufang Ji
, Yuanjun Chen
, Qiang Fu
, Yifeng Chen
, Juncai Dong
, Wenxing Chen
, Zhi Li
, Yu Wang
, Lin Gu
, Wei He
, Chen Chen
, Qing Peng
, Yu Huang
, Xiangfeng Duan
, Dingsheng Wang^*
, Claudia Draxl
, Yadong Li

^*Corresponding author for this work

Tsinghua University
Humboldt University of Berlin
CAS - Institute of High Energy Physics
Chinese Academy of Sciences
CAS - Institute of Physics
University of California at Los Angeles

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

336 Citations (Scopus)

Abstract

Here we report a novel approach to synthesize atomically dispersed uniform clusters via a cage-separated precursor preselection and pyrolysis strategy. To illustrate this strategy, well-defined Ru₃(CO)₁₂ was separated as a precursor by suitable molecular-scale cages of zeolitic imidazolate frameworks (ZIFs). After thermal treatment under confinement in the cages, uniform Ru₃ clusters stabilized by nitrogen species (Ru₃/CN) were obtained. Importantly, we found that Ru₃/CN exhibits excellent catalytic activity (100% conversion), high chemoselectivity (100% for 2-aminobenzaldehyde), and significantly high turnover frequency (TOF) for oxidation of 2-aminobenzyl alcohol. The TOF of Ru₃/CN (4320 h^-1) is about 23 times higher than that of small-sized (ca. 2.5 nm) Ru particles (TOF = 184 h^-1). This striking difference is attributed to a disparity in the interaction between Ru species and adsorbed reactants.

Original language	English
Pages (from-to)	9795-9798
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	139
Issue number	29
DOIs	https://doi.org/10.1021/jacs.7b05018
Publication status	Published - 26 Jul 2017
Externally published	Yes

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Ji, S., Chen, Y., Fu, Q., Chen, Y., Dong, J., Chen, W., Li, Z., Wang, Y., Gu, L., He, W., Chen, C., Peng, Q., Huang, Y., Duan, X., Wang, D., Draxl, C., & Li, Y. (2017). Confined Pyrolysis within Metal-Organic Frameworks to Form Uniform Ru₃ Clusters for Efficient Oxidation of Alcohols. Journal of the American Chemical Society, 139(29), 9795-9798. https://doi.org/10.1021/jacs.7b05018

@article{d4a82ab0b2b6478e99c3baeb3c2d4a30,

title = "Confined Pyrolysis within Metal-Organic Frameworks to Form Uniform Ru3 Clusters for Efficient Oxidation of Alcohols",

abstract = "Here we report a novel approach to synthesize atomically dispersed uniform clusters via a cage-separated precursor preselection and pyrolysis strategy. To illustrate this strategy, well-defined Ru3(CO)12 was separated as a precursor by suitable molecular-scale cages of zeolitic imidazolate frameworks (ZIFs). After thermal treatment under confinement in the cages, uniform Ru3 clusters stabilized by nitrogen species (Ru3/CN) were obtained. Importantly, we found that Ru3/CN exhibits excellent catalytic activity (100\% conversion), high chemoselectivity (100\% for 2-aminobenzaldehyde), and significantly high turnover frequency (TOF) for oxidation of 2-aminobenzyl alcohol. The TOF of Ru3/CN (4320 h-1) is about 23 times higher than that of small-sized (ca. 2.5 nm) Ru particles (TOF = 184 h-1). This striking difference is attributed to a disparity in the interaction between Ru species and adsorbed reactants.",

author = "Shufang Ji and Yuanjun Chen and Qiang Fu and Yifeng Chen and Juncai Dong and Wenxing Chen and Zhi Li and Yu Wang and Lin Gu and Wei He and Chen Chen and Qing Peng and Yu Huang and Xiangfeng Duan and Dingsheng Wang and Claudia Draxl and Yadong Li",

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doi = "10.1021/jacs.7b05018",

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Ji, S, Chen, Y, Fu, Q, Chen, Y, Dong, J, Chen, W, Li, Z, Wang, Y, Gu, L, He, W, Chen, C, Peng, Q, Huang, Y, Duan, X, Wang, D, Draxl, C & Li, Y 2017, 'Confined Pyrolysis within Metal-Organic Frameworks to Form Uniform Ru₃ Clusters for Efficient Oxidation of Alcohols', Journal of the American Chemical Society, vol. 139, no. 29, pp. 9795-9798. https://doi.org/10.1021/jacs.7b05018

TY - JOUR

T1 - Confined Pyrolysis within Metal-Organic Frameworks to Form Uniform Ru3 Clusters for Efficient Oxidation of Alcohols

AU - Ji, Shufang

AU - Chen, Yuanjun

AU - Fu, Qiang

AU - Chen, Yifeng

AU - Dong, Juncai

AU - Chen, Wenxing

AU - Li, Zhi

AU - Wang, Yu

AU - Gu, Lin

AU - He, Wei

AU - Chen, Chen

AU - Peng, Qing

AU - Huang, Yu

AU - Duan, Xiangfeng

AU - Wang, Dingsheng

AU - Draxl, Claudia

AU - Li, Yadong

PY - 2017/7/26

Y1 - 2017/7/26

N2 - Here we report a novel approach to synthesize atomically dispersed uniform clusters via a cage-separated precursor preselection and pyrolysis strategy. To illustrate this strategy, well-defined Ru3(CO)12 was separated as a precursor by suitable molecular-scale cages of zeolitic imidazolate frameworks (ZIFs). After thermal treatment under confinement in the cages, uniform Ru3 clusters stabilized by nitrogen species (Ru3/CN) were obtained. Importantly, we found that Ru3/CN exhibits excellent catalytic activity (100% conversion), high chemoselectivity (100% for 2-aminobenzaldehyde), and significantly high turnover frequency (TOF) for oxidation of 2-aminobenzyl alcohol. The TOF of Ru3/CN (4320 h-1) is about 23 times higher than that of small-sized (ca. 2.5 nm) Ru particles (TOF = 184 h-1). This striking difference is attributed to a disparity in the interaction between Ru species and adsorbed reactants.

AB - Here we report a novel approach to synthesize atomically dispersed uniform clusters via a cage-separated precursor preselection and pyrolysis strategy. To illustrate this strategy, well-defined Ru3(CO)12 was separated as a precursor by suitable molecular-scale cages of zeolitic imidazolate frameworks (ZIFs). After thermal treatment under confinement in the cages, uniform Ru3 clusters stabilized by nitrogen species (Ru3/CN) were obtained. Importantly, we found that Ru3/CN exhibits excellent catalytic activity (100% conversion), high chemoselectivity (100% for 2-aminobenzaldehyde), and significantly high turnover frequency (TOF) for oxidation of 2-aminobenzyl alcohol. The TOF of Ru3/CN (4320 h-1) is about 23 times higher than that of small-sized (ca. 2.5 nm) Ru particles (TOF = 184 h-1). This striking difference is attributed to a disparity in the interaction between Ru species and adsorbed reactants.

UR - https://www.scopus.com/pages/publications/85026308847

U2 - 10.1021/jacs.7b05018

DO - 10.1021/jacs.7b05018

M3 - Article

C2 - 28696113

AN - SCOPUS:85026308847

SN - 0002-7863

VL - 139

SP - 9795

EP - 9798

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 29

ER -

Confined Pyrolysis within Metal-Organic Frameworks to Form Uniform Ru₃ Clusters for Efficient Oxidation of Alcohols

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