Strain-Regulated Pd/Cu Core/Shell Icosahedra for Tunable Syngas Electrosynthesis from CO2

Introducing surface strain into catalysts would optimize the adsorption energy and surface electronic structure, but it is rarely used in the carbon dioxide reduction reaction (CO2RR) to regulate syngas. Herein, we have demonstrated a new class of Pd/Cu core/shell icosahedra (ico) with a tensile-strained Cu shell for efficient syngas production with tunable compositions from the CO2RR for the first time. By tuning the composition of Pd/Cu from 2.2 to 4.3 and 6.1, the molar ratio of H2/CO in syngas on Pd/Cu core/shell ico could be tuned from 1/1 to 2/1 and 3/1, respectively. The variable selectivity of the CO2RR on Pd/Cu core/shell ico originated from the tensile-strained Cu shell, which synergistically optimizes the binding energy of the intermediate and the electronic structure of catalysts. The work reveals how surface strain regulation accelerates electrocatalytic performance at the molecular level, providing new strategies to regulate CO2RR performance.