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Molecular nitrogen promotes catalytic hydrodeoxygenation

DOI: 10.1038/s41929-019-0368-6 DOI Help

Authors: Haohong Duan (University of Oxford; Tsinghua University) , Jin-Cheng Liu (Tsinghua University) , Ming Xu (Peking University) , Yufei Zhao (University of Oxford; Beijing University of Chemical Technology) , Xue-Lu Ma (Tsinghua University) , Juncai Dong (Beijing Synchrotron Radiation Facility) , Xusheng Zheng (National Synchrotron Radiation Laboratory) , Jianwei Zheng (The Wolfson Catalysis Centre, University of Oxford) , Christopher Allen (University of Oxford; Diamond Light Source Ltd) , Mohsen Danaie (Diamond Light Source) , Yung-Kang Peng (University of Hong Kong) , Titipong Issariyakul (SCG Packaging Public Company Limited) , Dongliang Chen (Beijing Synchrotron Radiation Facility) , Angus Kirkland (University of Oxford; Diamond Light Source) , Jean-Charles Buffet (University of Oxford) , Jun Li (Tsinghua University; Southern University of Science and Technology, China) , Shik Chi Edman Tsang (University of Oxford) , Dermot O'Hare (University of Oxford)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Catalysis , VOL 345

State: Published (Approved)
Published: October 2019
Diamond Proposal Number(s): 16969 , 17397

Abstract: Although molecular dinitrogen (N2) is widely used as a carrier or inert gas for many catalytic reactions, it is rarely considered as a catalytic promoter. Here, we report that N2 could be used to reduce the activation energy for catalytic hydrodeoxygenation over ruthenium-based catalysts. Specifically, we report a 4.3-fold activity increase in the catalytic hydrodeoxygenation of p-cresol to toluene over a titanium oxide supported ruthenium catalyst (Ru/TiO2) by simply introducing 6 bar N2 under batch conditions at 160 °C and 1 bar hydrogen. Detailed investigations indicate that N2 can be adsorbed and activated on the metallic ruthenium surface to form hydrogenated nitrogen species, which offer protic hydrogen to lower the activation energy of direct carbonaromatic–oxygen bond scission and the hydrogenation of hydroxy groups. Thus, by employing different ruthenium catalysts, including Ru/TiO2, Ru/Al2O3, Ru/ZrO2 and Ru/C, we demonstrate that N2 promotion of hydrodeoxygenation can be regarded as a general strategy.

Journal Keywords: Catalytic mechanisms; Heterogeneous catalysis; Porous materials

Subject Areas: Chemistry

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: E01-JEM ARM 200CF

Added On: 06/11/2019 11:01

Discipline Tags:

Physical Chemistry Catalysis Chemistry

Technical Tags:

Microscopy Electron Microscopy (EM) Scanning Transmission Electron Microscopy (STEM)