One‐step synthesis of ultra‐small amount of Pd‐Alloyed Zinc Nanosheets for efficient electrochemical CO₂ reduction to CO

AbstractThe practicality of the electrochemical CO2 reduction technique depends on the development of cost‐effective, robust, and highly selective catalysts. To achieve this goal, we have engineered self‐supported 3D electrodes composed of Pd‐Zn nanosheets (NSs) for CO2 electrochemical reduction to CO with minimal Pd content. This innovative electrode with an increased surface area was created using an electrodeposition method employing a dynamic hydrogen bubble template. By precisely adjusting the Pd content, we improved the thickness, porosity, and surface area of the electrodes, resulting in a CO2‐to‐CO selectivity reaching as high as 88.5 %, with an average of at least 80 % sustained over 10 hours. This remarkable improved activity can be attributed to the synergistic effects of an appropriate Pd/Zn atomic ratio as well as to the large surface area of nanosheets structures with rich edge active sites. Furthermore, to get around the limitations of CO2 mass transfer, reactions were done at high pressures conditions ranging from 3 to 9.5 bar; this strategic approach yielded an outstanding partial current density of −304.6 mA cm−2 for CO. These noteworthy findings establish concepts for constructing effective and earth‐abundant CO‐producing electrocatalysts.