Band Position‐Independent Piezo‐Electrocatalysis for Ultrahigh CO2 Conversion

Abstract 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 CO 2 reduction reaction (PECRR) is distinguished through a narrow‐bandgap piezo‐electrocatalyst strategy using MoS 2 nanoflakes as demo. With conduction band of −0.12 eV, the MoS 2 nanoflakes are unsatisfied for CO 2 ‐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 CO 2 ‐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, MoS 2 nanoflakes exhibit unexpected intense “breathing” effect under vibration and enable the naked‐eye‐visible inhalation of CO 2 gas, independently achieving the complete carbon cycle chain from CO 2 capture to conversion. The CO 2 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.