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Chem Sci. 2017 Nov 6;9(2):483-487. doi: 10.1039/c7sc03018e. eCollection 2018 Jan 14.

Doping palladium with tellurium for the highly selective electrocatalytic reduction of aqueous CO2 to CO.

Author information

1
State Key Laboratory of Organic-Inorganic Composites , Beijing University of Chemical Technology , Beijing 100029 , China . Email: sunzy@mail.buct.edu.cn.
2
Beijing National Laboratory for Molecular Sciences , Key Laboratory of Colloid and Interface and Thermodynamics , Institute of Chemistry , Chinese Academy of Sciences , Beijing 100190 , China . Email: hanbx@iccas.ac.cn.
3
Graduate School of EEWS , Korea Advanced Institute of Science and Technology (KAIST) , Daejeon 34141 , Republic of Korea . Email: ysjn@kaist.ac.kr.
4
Department of Materials , University of Oxford , Oxford , OX1 3PH , UK.

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.

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