Carbon supported nano-metal catalysts are expected to improve CO2 reduction selectivity and efficiency due to the addition of more active sites and enhancement of electron transport ability. In this study, HKUST-1 was pyrolyzed and decorated with Pt to prepare Pt–Cu/C catalysts. The catalytic effect of the catalysts with different Pt contents in the CO2 photoeletrochemical reduction reaction (CO2PRR) were compared. The total carbon atom conversion rate in CO2PRR experiments using Pt–Cu/C catalysts first increased to a peak when using 1.6 wt% Pt–Cu/C catalyst and then decreased with the increase of Pt content. The 1.6 wt% Pt–Cu/C catalyst showed good hydrogen evolution reaction (HER) inhibiting ability compared with other Pt–Cu/C catalysts. Density functional theory (DFT) calculations were conducted to give an insight into the CO2PRR mechanism on some possible active sites in Pt–Cu/C catalysts. The result demonstrated that HER was more likely to be inhibited on the Cu/Pt active surface and at the same time CO2PRR was promoted.
Chenjie Han,Yeqing Lyu,Shaona Wang,Biao Liu,Yi Zhang,Jan J. Weigand,Hao Du,Jun Lu
Using ethanol electrocatalytic oxidation reaction (EOR) with a lower reaction potential to replace oxygen evolution reaction (OER) and integrating hydrogen evolution reaction (HER) have a promising development prospect for more energy-saving electrolytic hydrogen production. However, the main challenges of EOR are insufficient catalytic activity, high overpotential, and slow kinetics. Active sites on the electrocatalysts surface are occupied by alkali metal ion hydrate clusters by noncovalent interactions, which is considered to be one of the major causes of these challenges. To reduce the effect of the noncovalent interactions on the catalytic activity of the electrocatalyst, copper is chosen and doped in the form of a single atom in the electrocatalyst (Pt@Cu/C) to increase the electrocatalyst conductivity and make the anode contain more positive charge in this study. Then, alkali metal ion hydrate clusters are difficult to adsorb at the active site of Pt@Cu/C. The EOR electrocatalytic activity of Pt@Cu/C is up to 8184 mA mg Pt −1 , which is ≈4.8 times as high as that of Pt/C. The two-electrode hydrogen production device using Pt@Cu/C as anode for coupled EOR&HER requires a smaller voltage of 0.60 V to reach 10 mA cm −2 compared with that of Pt/C (0.76 V).
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