Sustainable methanol production via CO_(2) hydrogenation leads to increased interest in the understanding of active phase of Cu/ZnO/Al_(2)O_(3)(CZA) catalyst. Model catalysts of ZnO/Cu(111) with structures varied from...Sustainable methanol production via CO_(2) hydrogenation leads to increased interest in the understanding of active phase of Cu/ZnO/Al_(2)O_(3)(CZA) catalyst. Model catalysts of ZnO/Cu(111) with structures varied from two-dimensional planar to three-dimensional nanoparticles were prepared by atomic layer deposition(ALD) method. By combing scanning tunneling microscopy(STM) and X-ray photoelectron spectroscopy(XPS) at near-ambient pressure of CO_(2) hydrogenation, we reveal that the submonolayer ZnO/Cu(111) transformed into Cu-Zn alloy under 10 mbar CO_(2)/H_(2) at 493 K, and underwent a partial reoxidation during evacuation. The dynamic phase transformation of ZnO/Cu(111) may partly explain the existence of differences and apparently contradictory theories to account for the origin of active phase in CZA catalysts.展开更多
Fun dame ntal un derstandi ng of chemistry confined to nano space remains a challe nge since molecules en capsulated in confined microe nviron merits are difficult to be characterized.Here,we show that CO adsorptio n ...Fun dame ntal un derstandi ng of chemistry confined to nano space remains a challe nge since molecules en capsulated in confined microe nviron merits are difficult to be characterized.Here,we show that CO adsorptio n on Pt(111)8nfined un der mono layer hexago nal boron nitride(h-BN)can be dynamically imaged using near ambient pressure seanning tunneling microscope(NAP-STM)and thanks to tunneling transparency of the top h-BN layer.The observed CO superstructures on Pt(111)in different CO atmospheres allow to derive surface coverages of CO adlayers,which are higher in the 8nfined nano space between h-BN and Pt(111)than those on the ope n Pt surface un der the same conditions.Dynamic NAP-STM imaging data together with theoretical calculations confirm confinement-induced molecule enrichment effect within the 2D nano space,which reveals new chemistry aroused by the confined nano reactor.展开更多
基金financially supported by the National Natural Science Foundation of China (No. 91845109, No. 21872169)。
文摘Sustainable methanol production via CO_(2) hydrogenation leads to increased interest in the understanding of active phase of Cu/ZnO/Al_(2)O_(3)(CZA) catalyst. Model catalysts of ZnO/Cu(111) with structures varied from two-dimensional planar to three-dimensional nanoparticles were prepared by atomic layer deposition(ALD) method. By combing scanning tunneling microscopy(STM) and X-ray photoelectron spectroscopy(XPS) at near-ambient pressure of CO_(2) hydrogenation, we reveal that the submonolayer ZnO/Cu(111) transformed into Cu-Zn alloy under 10 mbar CO_(2)/H_(2) at 493 K, and underwent a partial reoxidation during evacuation. The dynamic phase transformation of ZnO/Cu(111) may partly explain the existence of differences and apparently contradictory theories to account for the origin of active phase in CZA catalysts.
基金the National Natural Science Foundation of China(Nos.21688102,21621063,91545204,and 21703274)the Ministry of Science and Technology of China(No.2016YFA0200200)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17020000).
文摘Fun dame ntal un derstandi ng of chemistry confined to nano space remains a challe nge since molecules en capsulated in confined microe nviron merits are difficult to be characterized.Here,we show that CO adsorptio n on Pt(111)8nfined un der mono layer hexago nal boron nitride(h-BN)can be dynamically imaged using near ambient pressure seanning tunneling microscope(NAP-STM)and thanks to tunneling transparency of the top h-BN layer.The observed CO superstructures on Pt(111)in different CO atmospheres allow to derive surface coverages of CO adlayers,which are higher in the 8nfined nano space between h-BN and Pt(111)than those on the ope n Pt surface un der the same conditions.Dynamic NAP-STM imaging data together with theoretical calculations confirm confinement-induced molecule enrichment effect within the 2D nano space,which reveals new chemistry aroused by the confined nano reactor.
