Doping palladium with tellurium for the highly selective electrocatalytic reduction of aqueous CO2 to CO,Chemical Science

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Doping palladium with tellurium for the highly selective electrocatalytic reduction of aqueous CO2 to CO
Chemical Science ( IF 7.6 ) Pub Date : 2017-11-06 00:00:00 , DOI: 10.1039/c7sc03018e
Hengcong Tao _{1,

2,

3,

4} , Xiaofu Sun _{5,

6,

7,

8,

9} , Seoin Back _{10,

11,

12,

13} , Zishan Han _{1,

2,

3,

4} , Qinggong Zhu _{5,

6,

7,

8,

9} , Alex W. Robertson _{14,

15,

16,

17} , Tao Ma _{1,

2,

3,

4} , Qun Fan _{1,

2,

3,

4} , Buxing Han _{5,

6,

7,

8,

9} , Yousung Jung _{10,

11,

12,

13} , Zhenyu Sun _{1,

2,

3,

4}

Affiliation

State Key Laboratory of Organic-Inorganic Composites
Beijing University of Chemical Technology
Beijing 100029
China
Beijing National Laboratory for Molecular Sciences
Key Laboratory of Colloid and Interface and Thermodynamics
Institute of Chemistry
Chinese Academy of Sciences
Beijing 100190
Graduate School of EEWS
Korea Advanced Institute of Science and Technology (KAIST)
Daejeon 34141
Republic of Korea
Department of Materials
University of Oxford
Oxford
UK

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.

中文翻译：

碲掺杂钯用于高选择性电催化将含水的CO ₂还原为CO

设计高选择性和高能效的电催化剂以最小化在电化学还原含水CO _2中的竞争性放氢反应仍然是一个挑战。在这项研究中，我们报告说，用少量Te掺杂Pd可以有选择地将CO ₂转化为低过电势的CO。Pd / Te摩尔比为1：0.05的PdTe /几层石墨烯（FLG）催化剂在-0.8 V时显示最大CO法拉第效率（相对于可逆氢电极RHE），CO分电流密度为4.4 mA cm ^-2时和-1.0 V时的CO形成转换频率为0.14 s ^-1（vs.RHE），分别比Pd / FLG催化剂高3.7倍，4.3倍和10倍。密度泛函计算表明，Te原子优先结合在Pd的平台位上，从而抑制了不希望有的氢的释放，而CO ₂在Pd的高指数位上发生了吸附和活化，从而产生了CO。

更新日期：2017-11-15

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