Tri-Coordinated Copper Single Atoms on SAPO-34 Boosts Acetic Acid Production from Methane and Carbon Dioxide

Plasma-driven conversion of CH4 and CO2 into CH3COOH presents a sustainable pathway for greenhouse gas utilization, but the improvement of CH3COOH selectivity remains a bottleneck. Here, we present a catalyst with atomically dispersed Cu species on SAPO-34 zeolites (based on the CHA topology), synergistically enhancing plasma-catalytic conversion of CH4 and CO2 into CH3COOH. Through a simple impregnation method, we obtain Cu1@SAPO-34 single atom catalysts where Cu single atoms (Cu SAs) are anchored to form unique tri-coordinated Cu1-O3 sites that exhibit a strong metal-support interactions between Cu and SAPO-34. These Cu SAs enable a selectivity of CH3COOH (18.36 %) on Cu1@SAPO-34 (5.07 % higher than SAPO-34), with theoretical calculations suggesting that the Cu SAs can help lower the energy required for CH4 activation. By rationally correlating atomic-scale coordination environments with DFT calculations, this work not only promotes a novel strategy for designing the metal coordination environment of SACs but also provides a valuable avenue for applying Cu-based SACs towards enhancing product selectivity.