The catalytic properties of non-reducible metal oxides have intrigued continuous interest in the past dec-ades.Often time,catalytic studies of bulk non-reducible oxides focused on their high-temperature appli-cations owing to their weak interaction with small molecules.Hereby,combining ambient-pressure scanning tunneling microscopy(AP-STM),AP X-ray photoelectron spectroscopy(AP-XPS)and density functional theory(DFT)calculations,we studied the activation of CO and CO2 on ZnO,a typical non-reducible oxide and major catalytic material in the conversion of C1 molecules.By visualizing the chem-ical processes on ZnO surfaces at the atomic scale under AP conditions,we showed that new adsorbate structures induced by the enhanced physisorption and the concerted interaction of physisorbed mole-cules could facilitate the activation of CO and CO2 on ZnO.The reactivity of ZnO towards CO could be observed under AP conditions,where an ordered(2×1)-CO structure was observed on ZnO(1010).Meanwhile,chemisorption of CO2 on ZnO(1010)under AP conditions was also enhanced by physisorbed CO2,which minimizes the repulsion between surface dipoles and causes a(3×1)-CO2 structure.Our study has brought molecular insight into the fundamental chemistry and catalytic properties of ZnO sur-faces under realistic reaction conditions.

Yunjian Ling;Jie Luo;Yihua Ran;Yunjun Cao;Wugen Huang;Jun Cai;Zhi Liu;Wei-Xue Li;Fan Yang;Xinhe Bao

State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China;University of Chinese Academy of Sciences,Beijing 100039,China;School of Chemistry and Materials Science,Hefei National Laboratory for Physical Sciences at Microscales,University of Science and Technology of China,Hefei 230026,Anhui,China;School of Physical Science and Technology,ShanghaiTech University,Shanghai 201210,China

能源化学

[1]Yunjian Ling;Jie Luo;Yihua Ran;Yunjun Cao;Wugen Huang;Jun Cai;Zhi Liu;Wei-Xue Li;Fan Yang;Xinhe Bao-.Dynamic chemical processes on ZnO surfaces tuned by physisorption under ambient conditions)[J].能源化学,2022(09):258-264

intrigued,physisorbed

Dynamic,chemical,processes,ZnO,surfaces,tuned,physisorption,under,ambient,conditions,catalytic,properties,reducible,metal,oxides,have,continuous,interest,past,dec,ades,Often,studies,bulk,focused,their,high,temperature,appli,cations,owing,weak,interaction,small,molecules,Hereby,combining,pressure,scanning,tunneling,microscopy,AP,STM,ray,photoelectron,spectroscopy,XPS,density,functional,theory,DFT,calculations,studied,activation,typical,major,material,conversion,C1,By,visualizing,atomic,scale,showed,that,new,adsorbate,structures,induced,enhanced,concerted,could,facilitate,reactivity,towards,observed,where,ordered,was,Meanwhile,chemisorption,also,which,minimizes,repulsion,between,dipoles,causes,Our,study,has,brought,molecular,insight,into,fundamental,chemistry,realistic,reaction

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