RESUMEN
The two-electron oxygen reduction reaction in acid is highly attractive to produce H2O2, a commodity chemical vital in various industry and household scenarios, which is still hindered by the sluggish reaction kinetics. Herein, both density function theory calculation and in-situ characterization demonstrate that in dual-atom CoIn catalyst, O-affinitive In atom triggers the favorable and stable adsorption of hydroxyl, which effectively optimizes the adsorption of OOH on neighboring Co. As a result, the oxygen reduction on Co atoms shifts to two-electron pathway for efficient H2O2 production in acid. The H2O2 partial current density reaches 1.92 mA cm-2 at 0.65 V in the rotating ring-disk electrode test, while the H2O2 production rate is as high as 9.68 mol g-1 h-1 in the three-phase flow cell. Additionally, the CoIn-N-C presents excellent stability during the long-term operation, verifying the practicability of the CoIn-N-C catalyst. This work provides inspiring insights into the rational design of active catalysts for H2O2 production and other catalytic systems.
RESUMEN
The production of value-added chemicals from CO2 electroreduction, using renewable energy, provides an appealing route to achieve the goal of carbon neutrality. Challenges remain in designing and understanding of high-performance catalysts with restructuring behavior under electrochemical conditions. Here, the intrinsic performance enhancement of an Au-complex derived carbon nanotube-supported Au nanoclusters catalyst was demonstrated for CO2 reduction. This catalyst exhibited impressive activity for yielding CO in both H-cell and flow cell reactors. Experimental results revealed that the synthesis procedure via metal complex reconstructing on proper support induced charge transfer between Au nanoclusters and carbon nanotubes, forming a rather electron-rich state for Au active sites, which greatly contributed to the CO2 activation pathway.