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Deng, Yuchen

Publications and source records attributed to Deng, Yuchen.

A stable low-temperature H 2 -production catalyst by crowding Pt on α-MoC

The water-gas shift (WGS) reaction is an industrially important source of pure hydrogen (H 2 ) at the expense of carbon monoxide and water. This reaction is of interest for fuel-cell applications, but requires WGS catalysts that are durable and highly active at low temperatures. Here we demonstrate that the structure (Pt 1 Pt n )/α-MoC, where isolated platinum atoms (Pt 1 ) and subnanometre platinum clusters (Pt-n) are stabilized on alpha-molybdenum carbide (α-MoC), catalyses the WGS reaction even at 313 kelvin, with a hydrogen-production pathway involving direct carbon monoxide dissociation identified. We find that it is critical to crowd the α-MoC surface with Pt 1 and Pt n species, which prevents oxidation of the support that would cause catalyst deactivation, as seen with gold/α-MoC, and gives our system high stability and a high metal-normalized turnover number of 4,300,000 moles of hydrogen per mole of platinum. We anticipate that the strategy demonstrated here will be pivotal for the design of highly active and stable catalysts for effective activation of important molecules such as water and carbon monoxide for energy production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Inverse ZrO 2 /Cu as a highly efficient methanol synthesis catalyst from CO 2 hydrogenation

Enhancing the intrinsic activity and space time yield of Cu based heterogeneous methanol synthesis catalysts through CO 2 hydrogenation is one of the major topics in CO 2 conversion into value-added liquid fuels and chemicals. Here we report inverse ZrO 2 /Cu catalysts with a tunable Zr/Cu ratio have been prepared via an oxalate co-precipitation method, showing excellent performance for CO 2 hydrogenation to methanol. Under optimal condition, the catalyst composed by 10% of ZrO 2 supported over 90% of Cu exhibits the highest mass-specific methanol formation rate of 524 g MeOH kg cat -1 h -1 at 220°C, 3.3 times higher than the activity of traditional Cu/ZrO 2 catalysts (159 g MeOH kg cat -1 h -1 ). In situ XRD-PDF, XAFS and AP-XPS structural studies reveal that the inverse ZrO 2 /Cu catalysts are composed of islands of partially reduced 1–2 nm amorphous ZrO 2 supported over metallic Cu particles. The ZrO 2 islands are highly active for the CO 2 activation. Meanwhile, an intermediate of formate adsorbed on the Cu at 1350 cm -1 is discovered by the in situ DRIFTS. This formate intermediate exhibits fast hydrogenation conversion to methoxy. The activation of CO 2 and hydrogenation of all the surface oxygenate intermediates are significantly accelerated over the inverse ZrO 2 /Cu configuration, accounting for the excellent methanol formation activity observed.

36 MATERIALS SCIENCE↗