Heterogeneous Catalytic Interface Engineering of Oxygen Vacancies on Cu–Zn Sites for Low-Temperature Methanol Synthesis

Despite the synthesis of methanol from CO 2 -containing syngas at low temperature represents an efficient route for chemical energy storage, the limited activity and stability of Cu/ZnO-based catalysts remain major obstacles. Here, we demonstrate that the introduction of Ba induces oxygen-vacancy-mediated heterogeneous catalytic interfaces at Cu–Zn sites, markedly enhancing both the activity and durability of low-temperature methanol synthesis. By precisely regulating the concentration of interfacial oxygen vacancies, a turnover frequency (TOF) as high as 21.2 × 10 –3 s –1 and a methanol space-time yield (STY) of 655.17 g kg cat –1 h –1 are achieved. Simultaneously, Ba incorporation increases the exposed Cu 0 surface area, improves Cu dispersion, suppresses Cu particle sintering, and enriches surface basic sites. Density functional theory calculations further reveal that oxygen vacancies preferentially form at the Cu–Zn interfacial region and act as the primary active sites for low-temperature methanol synthesis. These findings establish that interfacial oxygen-vacancy engineering is an effective strategy for advancing methanol production at low temperatures.