TY - JOUR
T1 - MOF-Encapsulating Metal-Acid Interfaces for Efficient Catalytic Hydrogenolysis of Biomass-Derived Aromatic Aldehydes
AU - Deng, Qiang
AU - Zhu, Jiawei
AU - Zhong, Yao
AU - Li, Xiang
AU - Wang, Jun
AU - Cai, Jianxin
AU - Zeng, Zheling
AU - Zou, Ji Jun
AU - Deng, Shuguang
N1 - Funding Information:
The authors appreciate the support from the National Natural Science Foundation of China (21878138, 91200157, 21706112) and the Postdoctoral Science Foundation of China (2017M622104, 2018T110660).
Publisher Copyright:
©
PY - 2021/8/23
Y1 - 2021/8/23
N2 - Developing an efficient and selective catalyst for C-O hydrogenolysis of biomass-derived aromatic aldehydes, such as 5-methylfurfural (MF), 5-hydroxymethylfurfural (HMF), and vanillin (VA), is highly significant for the synthesis of biofuel and fine chemicals. Herein, metal-organic framework (MOF)-encapsulating metal-acid interfaces (Pd@UiO-CH2SO3H, Pd@UiO-PhSO3H) were first reported. Compared with traditionally supported catalysts (Pd/UiO-SO3H, Pd/UiO-NH2), Pd-acid-interface-encapsulated MOFs show much higher activity and selectivity for MF to 2,5-dimethylfuran (DMF), HMF to DMF, and VA to 2-methoxy-4-methylphenol (MMP) reactions. In particular, Pd@UiO-SO3H shows the best catalytic performance with 89.0 and 86.0% DMF yield from MF and HMF and a 99.4% MMP yield from VA based on its suitable hydrophilicity, high hydrogen activation ability, and abundant Pd-SO3H interface active sites. According to the catalytic performance of Pd/UiO-NH2 and the results of an ATR-IR test, the acidic sites on the Pd-acid interface can accelerate the activation of the hydroxyl group for these hydrogenolysis reactions. This work provides an effective design strategy for the preparation of MOF-encapsulating metal-acid interfaces and shows the powerful synergistic effect of hydrogenation and acid catalysis.
AB - Developing an efficient and selective catalyst for C-O hydrogenolysis of biomass-derived aromatic aldehydes, such as 5-methylfurfural (MF), 5-hydroxymethylfurfural (HMF), and vanillin (VA), is highly significant for the synthesis of biofuel and fine chemicals. Herein, metal-organic framework (MOF)-encapsulating metal-acid interfaces (Pd@UiO-CH2SO3H, Pd@UiO-PhSO3H) were first reported. Compared with traditionally supported catalysts (Pd/UiO-SO3H, Pd/UiO-NH2), Pd-acid-interface-encapsulated MOFs show much higher activity and selectivity for MF to 2,5-dimethylfuran (DMF), HMF to DMF, and VA to 2-methoxy-4-methylphenol (MMP) reactions. In particular, Pd@UiO-SO3H shows the best catalytic performance with 89.0 and 86.0% DMF yield from MF and HMF and a 99.4% MMP yield from VA based on its suitable hydrophilicity, high hydrogen activation ability, and abundant Pd-SO3H interface active sites. According to the catalytic performance of Pd/UiO-NH2 and the results of an ATR-IR test, the acidic sites on the Pd-acid interface can accelerate the activation of the hydroxyl group for these hydrogenolysis reactions. This work provides an effective design strategy for the preparation of MOF-encapsulating metal-acid interfaces and shows the powerful synergistic effect of hydrogenation and acid catalysis.
KW - Adsorption configuration
KW - Aromatic aldehydes
KW - C-O hydrogenolysis
KW - C=O hydrogenation
KW - Pd@UiO-SOH
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U2 - 10.1021/acssuschemeng.1c02998
DO - 10.1021/acssuschemeng.1c02998
M3 - Article
AN - SCOPUS:85113747478
VL - 9
SP - 11127
EP - 11136
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
SN - 2168-0485
IS - 33
ER -
