Abstract
Designing highly selective and energy-efficient electrocatalysts to minimize the competitive hydrogen evolution reaction in the electrochemical reduction of aqueous CO2 remains a challenge. In this study, we report that doping Pd with a small amount of Te could selectively convert CO2 to CO with a low overpotential. The PdTe/few-layer graphene (FLG) catalyst with a Pd/Te molar ratio of 1 : 0.05 displayed a maximum CO faradaic efficiency of about 90% at -0.8 V (vs. a reversible hydrogen electrode, RHE), CO partial current density of 4.4 mA cm-2, and CO formation turnover frequency of 0.14 s-1 at -1.0 V (vs. a RHE), which were 3.7-, 4.3-, and 10-fold higher than those of a Pd/FLG catalyst, respectively. Density functional calculations showed that Te adatoms preferentially bind at the terrace sites of Pd, thereby suppressing undesired hydrogen evolution, whereas CO2 adsorption and activation occurred on the high index sites of Pd to produce CO.
Highlights
Steady increases in the atmospheric levels of CO2 and increasing energy demands have intensi ed concerns about the adverse CO2 effects on climate change and energy supplies
Density functional calculations showed that Te adatoms preferentially bind at the terrace sites of Pd, thereby suppressing undesired hydrogen evolution, whereas CO2 adsorption and activation occurred on the high index sites of Pd to produce CO
We report that doping Pd nanocrystals with Te signi cantly enhances the electrochemical reduction of aqueous CO2 to CO, affording a much higher CO faradaic efficiency (FE), CO partial current density, mass activity, and formation turnover frequency with respect to the undoped Pd catalyst
Summary
Steady increases in the atmospheric levels of CO2 and increasing energy demands have intensi ed concerns about the adverse CO2 effects on climate change and energy supplies. The PdTe/few-layer graphene (FLG) catalyst with a Pd/Te molar ratio of 1 : 0.05 displayed a maximum CO faradaic efficiency of about 90% at À0.8 V (vs a reversible hydrogen electrode, RHE), CO partial current density of 4.4 mA cmÀ2, and CO formation turnover frequency of 0.14 sÀ1 at À1.0 V (vs a RHE), which were 3.7-, 4.3-, and 10-fold higher than those of a Pd/FLG catalyst, respectively.
Sign-in/Register to view highlights & summary Sign-in/Register to access full text options 
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
