Temperature-Controlled Selectivity of Hydrogenation and Hydrodeoxygenation in the Conversion of Biomass Molecule by the Ru 1 /mpg-C 3 N 4 Catalyst

Tian Sheng, Ziyun Wang, Wanbing Gong, Wenxing Chen, Quanchen Feng, Qi Xu, Chun Chen, Chen Chen, Qing Peng, Lin Gu, Huijun Zhao, Peijun Hu, Dingsheng Wang, Yadong Li

Research output: Contribution to journalArticle

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Abstract

Hydrogenation and hydrodeoxygenation are significant and distinct approaches for the conversion of biomass and biomass-derived oxygenated chemicals into high value-added chemicals and fuels. However, it remains a great challenge to synthesize catalysts that simultaneously possess excellent hydrogenation and hydrodeoxygenation performance. Herein, we report a catalyst made of isolated single-atom Ru supported on mesoporous graphitic carbon nitride (Ru 1 /mpg-C 3 N 4 ), fabricated by a wet impregnation method. The as-prepared Ru 1 /mpg-C 3 N 4 catalyst shows excellent hydrogenation and hydrodeoxygenation performance. First-principles calculations reveal that the Ru atom is mobilized, and the active site is induced by adsorption of the reactants. A systematic reaction mechanism is proposed, suggesting that vanillyl alcohol is the deoxygenation prohibited product, while 2-methoxy-p-cresol is the deoxygenation allowed product. Thus, the excellent selectivity for the hydrogenation or hydrodeoxygenation of vanillin at different temperatures results from switching between the two types of products. © 2018 American Chemical Society.
Original languageEnglish
Pages (from-to)11161-11164
JournalJournal of the American Chemical Society
Volume140
Issue number36
Early online date30 Aug 2018
DOIs
Publication statusPublished - 12 Sep 2018

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Hydrogenation
Biomass
Catalysts
Molecules
Temperature
Bioconversion
Atoms
Carbon nitride
Impregnation
Adsorption
Catalytic Domain
Alcohols

Cite this

Sheng, Tian ; Wang, Ziyun ; Gong, Wanbing ; Chen, Wenxing ; Feng, Quanchen ; Xu, Qi ; Chen, Chun ; Chen, Chen ; Peng, Qing ; Gu, Lin ; Zhao, Huijun ; Hu, Peijun ; Wang, Dingsheng ; Li, Yadong. / Temperature-Controlled Selectivity of Hydrogenation and Hydrodeoxygenation in the Conversion of Biomass Molecule by the Ru 1 /mpg-C 3 N 4 Catalyst. In: Journal of the American Chemical Society. 2018 ; Vol. 140, No. 36. pp. 11161-11164.
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abstract = "Hydrogenation and hydrodeoxygenation are significant and distinct approaches for the conversion of biomass and biomass-derived oxygenated chemicals into high value-added chemicals and fuels. However, it remains a great challenge to synthesize catalysts that simultaneously possess excellent hydrogenation and hydrodeoxygenation performance. Herein, we report a catalyst made of isolated single-atom Ru supported on mesoporous graphitic carbon nitride (Ru 1 /mpg-C 3 N 4 ), fabricated by a wet impregnation method. The as-prepared Ru 1 /mpg-C 3 N 4 catalyst shows excellent hydrogenation and hydrodeoxygenation performance. First-principles calculations reveal that the Ru atom is mobilized, and the active site is induced by adsorption of the reactants. A systematic reaction mechanism is proposed, suggesting that vanillyl alcohol is the deoxygenation prohibited product, while 2-methoxy-p-cresol is the deoxygenation allowed product. Thus, the excellent selectivity for the hydrogenation or hydrodeoxygenation of vanillin at different temperatures results from switching between the two types of products. {\circledC} 2018 American Chemical Society.",
author = "Tian Sheng and Ziyun Wang and Wanbing Gong and Wenxing Chen and Quanchen Feng and Qi Xu and Chun Chen and Chen Chen and Qing Peng and Lin Gu and Huijun Zhao and Peijun Hu and Dingsheng Wang and Yadong Li",
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Sheng, T, Wang, Z, Gong, W, Chen, W, Feng, Q, Xu, Q, Chen, C, Chen, C, Peng, Q, Gu, L, Zhao, H, Hu, P, Wang, D & Li, Y 2018, 'Temperature-Controlled Selectivity of Hydrogenation and Hydrodeoxygenation in the Conversion of Biomass Molecule by the Ru 1 /mpg-C 3 N 4 Catalyst', Journal of the American Chemical Society, vol. 140, no. 36, pp. 11161-11164. https://doi.org//10.1021/jacs.8b06029

Temperature-Controlled Selectivity of Hydrogenation and Hydrodeoxygenation in the Conversion of Biomass Molecule by the Ru 1 /mpg-C 3 N 4 Catalyst. / Sheng, Tian; Wang, Ziyun; Gong, Wanbing; Chen, Wenxing; Feng, Quanchen; Xu, Qi; Chen, Chun; Chen, Chen; Peng, Qing; Gu, Lin; Zhao, Huijun; Hu, Peijun; Wang, Dingsheng; Li, Yadong.

In: Journal of the American Chemical Society, Vol. 140, No. 36, 12.09.2018, p. 11161-11164.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Temperature-Controlled Selectivity of Hydrogenation and Hydrodeoxygenation in the Conversion of Biomass Molecule by the Ru 1 /mpg-C 3 N 4 Catalyst

AU - Sheng, Tian

AU - Wang, Ziyun

AU - Gong, Wanbing

AU - Chen, Wenxing

AU - Feng, Quanchen

AU - Xu, Qi

AU - Chen, Chun

AU - Chen, Chen

AU - Peng, Qing

AU - Gu, Lin

AU - Zhao, Huijun

AU - Hu, Peijun

AU - Wang, Dingsheng

AU - Li, Yadong

PY - 2018/9/12

Y1 - 2018/9/12

N2 - Hydrogenation and hydrodeoxygenation are significant and distinct approaches for the conversion of biomass and biomass-derived oxygenated chemicals into high value-added chemicals and fuels. However, it remains a great challenge to synthesize catalysts that simultaneously possess excellent hydrogenation and hydrodeoxygenation performance. Herein, we report a catalyst made of isolated single-atom Ru supported on mesoporous graphitic carbon nitride (Ru 1 /mpg-C 3 N 4 ), fabricated by a wet impregnation method. The as-prepared Ru 1 /mpg-C 3 N 4 catalyst shows excellent hydrogenation and hydrodeoxygenation performance. First-principles calculations reveal that the Ru atom is mobilized, and the active site is induced by adsorption of the reactants. A systematic reaction mechanism is proposed, suggesting that vanillyl alcohol is the deoxygenation prohibited product, while 2-methoxy-p-cresol is the deoxygenation allowed product. Thus, the excellent selectivity for the hydrogenation or hydrodeoxygenation of vanillin at different temperatures results from switching between the two types of products. © 2018 American Chemical Society.

AB - Hydrogenation and hydrodeoxygenation are significant and distinct approaches for the conversion of biomass and biomass-derived oxygenated chemicals into high value-added chemicals and fuels. However, it remains a great challenge to synthesize catalysts that simultaneously possess excellent hydrogenation and hydrodeoxygenation performance. Herein, we report a catalyst made of isolated single-atom Ru supported on mesoporous graphitic carbon nitride (Ru 1 /mpg-C 3 N 4 ), fabricated by a wet impregnation method. The as-prepared Ru 1 /mpg-C 3 N 4 catalyst shows excellent hydrogenation and hydrodeoxygenation performance. First-principles calculations reveal that the Ru atom is mobilized, and the active site is induced by adsorption of the reactants. A systematic reaction mechanism is proposed, suggesting that vanillyl alcohol is the deoxygenation prohibited product, while 2-methoxy-p-cresol is the deoxygenation allowed product. Thus, the excellent selectivity for the hydrogenation or hydrodeoxygenation of vanillin at different temperatures results from switching between the two types of products. © 2018 American Chemical Society.

U2 - /10.1021/jacs.8b06029

DO - /10.1021/jacs.8b06029

M3 - Article

VL - 140

SP - 11161

EP - 11164

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 36

ER -