CO_(2) hydrogenation into valuable chemical products has attracted intensive research interest in recent years,with product selectivity control remaining an important topic that requires fine tuning of the catalytic s...CO_(2) hydrogenation into valuable chemical products has attracted intensive research interest in recent years,with product selectivity control remaining an important topic that requires fine tuning of the catalytic structure and mechanistic understanding.Herein we report our study of anionic phosphorus-regulated indium oxide In_(2)O_(3)(P-In_(2)O_(3))nanocatalyst materials for CO_(2) hydrogenation and achieve nearly fullrange selectivity control between methanol and CO products by means of tuning the P content.In situ DRIFTS experiments and XPS characterization reveal the importance of P anion regulation in controlling the CO_(2) hydrogenation pathways,with an increase in the P content resulting in a decrease in the reducibility of In_(2)O_(3) that alters CO_(2) adsorption configuration by blocking and weakening oxygen vacancy(OV)sites for methanol generation and in the meantime creates new sites predominantly active for CO generation.This study demonstrates excellent control of the product selectivity property by regulating the catalyst composition with P anions and provides mechanistic discussions,which offers a new,effective strategy in CO_(2) hydrogenation catalyst research.展开更多
基金the Ohio Development Services Agency(R-16-04)for the financial support of this study.
文摘CO_(2) hydrogenation into valuable chemical products has attracted intensive research interest in recent years,with product selectivity control remaining an important topic that requires fine tuning of the catalytic structure and mechanistic understanding.Herein we report our study of anionic phosphorus-regulated indium oxide In_(2)O_(3)(P-In_(2)O_(3))nanocatalyst materials for CO_(2) hydrogenation and achieve nearly fullrange selectivity control between methanol and CO products by means of tuning the P content.In situ DRIFTS experiments and XPS characterization reveal the importance of P anion regulation in controlling the CO_(2) hydrogenation pathways,with an increase in the P content resulting in a decrease in the reducibility of In_(2)O_(3) that alters CO_(2) adsorption configuration by blocking and weakening oxygen vacancy(OV)sites for methanol generation and in the meantime creates new sites predominantly active for CO generation.This study demonstrates excellent control of the product selectivity property by regulating the catalyst composition with P anions and provides mechanistic discussions,which offers a new,effective strategy in CO_(2) hydrogenation catalyst research.
