期刊
ACS CATALYSIS
卷 5, 期 11, 页码 6509-6523出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b01554
关键词
hydrodeoxygenation; ruthenium; TiO2; biofuels upgrading; DFT
资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0011983]
- DOE EPSCoR Grant [DE-FG02-07ER46373]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- U.S. DOE, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- National Science Foundation [ACI5681053575]
- agency of the United States Government
- Center of Advanced Computing and Data Systems (CACDS) at the University of Houston
- U.S. Department of Energy (DOE) [DE-FG02-07ER46373, DE-SC0011983] Funding Source: U.S. Department of Energy (DOE)
Catalytic reduction of pyrolyzed biomass is required to remove oxygen and produce transportation fuels, but limited knowledge of how hydrodeoxygenation (HDO) catalysts work stymies the rational design of more efficient and stable catalysts, which in turn limits deployment of biofuels. This work reports results from a novel study utilizing both isotopically labeled phenol (which models the most recalcitrant components of biofuels) with D2O and DFT calculations to provide insight into the mechanism of the highly efficient HDO catalyst, Ru/TiO2. The data point to the importance of interface sites between Ru nanopartides and the TiO2 support and suggest that water acts as a cocatalyst favoring a direct deoxygenation pathway in which the phenolic OH is replaced directly with H to form benzene. Rather than its reducibility, we propose that the amphoteric nature of TiO2 facilitates H-2 heterolysis to generate an active site water molecule that promotes the catalytic C-O bond scission of phenol. This work has clear implications for efforts to scale-up the hydrogen-efficient conversion of wood waste into transportation fuels and biochemicals.
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