Renewable methane synthesized via
CO2 electroreduction
has the potential to serve as a carbon-neutral medium benefiting from
its high energy density. However, challenges remain in achieving high
selectivity for electromethanation with low energy input. Here, we
found that the adhered ligands on the copper surface can modulate
the local microenvironment to realize high rates for methane electrogeneration.
The designed glutathione-modified copper electrode exhibited an impressive
CO2 to CH4 Faradaic efficiency of 61.7% with
a partial current density of 153.7 mA cm–2, which
was 35-fold higher than that of pristine copper. Operando Raman spectroscopy
experiments suggest that the carboxyl and amino groups of glutathione
ligands play a crucial role in regulating intermediate configurations
and local proton availability. More broadly, these findings offer
routes to alter surface reactivity and create a platform for designing
highly selective CO2 electroreduction catalysts.
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.
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.
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