<p>Electrosynthetic techniques are gaining prominence
across the fields of chemistry, engineering and energy science. However, most
works within the direction of synthetic heterogeneous electrocatalysis focus on
water electrolysis and CO<sub>2</sub> reduction. In this work, we moved to
expand the scope of this technology by developing a synthetic scheme which
couples CO<sub>2</sub> and NH<sub>3</sub> at a gas-liquid-solid triple-phase
boundary to produce species with C-N bonds. Specifically, by bringing in CO<sub>2</sub>
from the gas phase and NH<sub>3</sub> from the liquid phase together over solid
copper catalysts, we have succeeded in forming formamide and acetamide products
for the first time. In a subsequent complementary step, we have combined
electrochemical analysis and a newly developed <i>operando </i>spectroelectrochemical
method, capable of probing the aforementioned triple phase boundary, to extract
an initial level of mechanistic analysis regarding the reaction pathways of
these reactions and the current system’s limitations. We believe that the
development and understanding of this set of reaction pathways will play an
exceptionally significant role in expanding the community’s understanding of
on-surface electrosynthetic reactions as well as push this set of inherently
sustainable technologies towards widespread applicability. </p>
Triple phase boundary and power density enhancement in PEMFCs of a Pt/C electrode with double catalyst layers