Turning on Low-Temperature Catalytic Conversion of Biomass Derivatives through Teaming Pd<sub>1</sub> and Mo<sub>1</sub> Single-Atom Sites
Yu Tang, George Yan, Shiran Zhang, Yuting Li, Luan Nguyen, Yasuhiro Iwasawa, Tomohiro Sakata, Christopher M. Andolina, Judith C. Yang, Philippe Sautet, Franklin Tao
Abstract
On-purpose atomic scale design of catalytic sites, specifically active and selective at low temperature for a target reaction, is a key challenge. Here, we report teamed Pd 1 and Mo 1 single-atom sites that exhibit high activity and selectivity for anisole hydrodeoxygenation to benzene at low temperatures, 100–150 °C, where a Pd metal nanoparticle catalyst or a MoO 3 nanoparticle catalyst is individually inactive. The catalysts built from Pd 1 or Mo 1 single-atom sites alone are much less effective, although the catalyst with Pd 1 sites shows some activity but low selectivity. Similarly, less dispersed nanoparticle catalysts are much less effective. Computational studies show that the Pd 1 and Mo 1 single-atom sites activate H 2 and anisole, respectively, and their combination triggers the hydrodeoxygenation of anisole in this low-temperature range. The Co 3 O 4 support is inactive for anisole hydrodeoxygenation by itself but participates in the chemistry by transferring H atoms from Pd 1 to the Mo 1 site. This finding opens an avenue for designing catalysts active for a target reaction channel such as conversion of biomass derivatives at a low temperature where neither metal nor oxide nanoparticles are.