A specific defect type of Cu active site to suppress Water-Gas-Shift reaction in syngas conversion to methanol over Cu catalysts

Inspired by the sensitivity of methanol and WGSR to Cu active site types, a specific defect type of Cu active site is proposed to facilitate methanol synthesis and effectively suppress WGSR to produce CO2. In this work, DFT calculations is implemented to investigate the detailed mechanism of syngas-tomethanol and WGSR over Cu catalysts including Cu active type with the point, flatted line, and stepped line defects. The results suggested that WGSR can be regulated by tuning the adsorption and dissociation ability of H2O over different Cu active sites to decrease CO2 selectivity. The relationship of GCN value and d-band center of active center with the activity of methanol and WGSR was proposed to screen out highperformance catalysts. This study provides theoretical basis for designing and optimizing Cu-based catalysts to suppress WGSR leading to lower CO2 selectivity by adjusting Cu active site to meet a specific defect type.

Automated summary

Inspired by the sensitivity of methanol and WGSR to Cu active site types, a specific defect type of Cu active site is proposed to facilitate methanol synthesis and effectively suppress WGSR to produce CO2. DFT calculations were used to investigate the detailed mechanism of syngas-to-methanol and WGSR over Cu catalysts. It was found that the adsorption and dissociation ability of H2O over different Cu active sites can be tuned to regulate WGSR and decrease CO2 selectivity. The relationship between GCN value, d-band center of active center, and the activity of methanol and WGSR was proposed to screen high-performance catalysts. This study provides a theoretical basis for designing and optimizing Cu-based catalysts to suppress WGSR and lower CO2 selectivity by adjusting Cu active sites to specific defect types.