Band Position‐Independent Piezo‐Electrocatalysis for Ultrahigh CO₂ Conversion

Piezo-electrocatalysis as an emerging mechano-to-chemistry energy conversion technique opens multiple innovative opportunities and draws great interest over the past decade. However, the two potential mechanisms in piezo-electrocatalysis, i.e., screening charge effect and energy band theory, generally coexist in the most piezoelectrics, making the essential mechanism remain controversial. Here, for the first time, the two mechanisms in piezo-electrocatalytic CO2 reduction reaction (PECRR) is distinguished through a narrow-bandgap piezo-electrocatalyst strategy using MoS2 nanoflakes as demo. With conduction band of -0.12 eV, the MoS2 nanoflakes are unsatisfied for CO2 -to-CO redox potential of -0.53 eV, yet they achieve an ultrahigh CO yield of ≈543.1 µmol g-1 h-1 in PECRR. Potential band position shifts under vibration are still unsatisfied with CO2 -to-CO potential verified by theoretical investigation and piezo-photocatalytic experiment, further indicating that the mechanism of piezo-electrocatalysis is independent of band position. Besides, MoS2 nanoflakes exhibit unexpected intense "breathing" effect under vibration and enable the naked-eye-visible inhalation of CO2 gas, independently achieving the complete carbon cycle chain from CO2 capture to conversion. The CO2 inhalation and conversion processes in PECRR are revealed by a self-designed in situ reaction cell. This work brings new insights into the essential mechanism and surface reaction evolution of piezo-electrocatalysis.