Indexed by:
Journal Papers
First Author:
Zhang, Xiaoyu
Correspondence Author:
Nie, XW (reprint author), Dalian Univ Technol, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Sch Chem Engn, Dalian 116024, Peoples R China.; Qu, ZP (reprint author), Dalian Univ Technol, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn, Dalian 116024, Peoples R China.
Co-author:
Wang, Hui,Meng, Linlin,Nie, Xiaowa,Qu, Zhenping
Date of Publication:
2020-04-27
Journal:
ACS APPLIED ENERGY MATERIALS
Included Journals:
SCIE
Document Type:
J
Volume:
3
Issue:
4
Page Number:
3465-3476
ISSN No.:
2574-0962
Key Words:
reconstruction; Cu2O-CuO mixed oxide; DFT calculations; oxygen
dissociated adsorption; bidentate nitrate
Abstract:
Cubic cuprous oxide is applied in the selective catalytic oxidation of ammonia to nitrogen (NH3-SCO) to investigate the effect of structure evolution on catalytic performance. Different structures (Cu2O, Cu2O-CuO, and CuO) that formed progressively during the reconstruction process with time are discovered by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and other characterization methods. The optimal CuO-Cu2O exhibits the best catalytic performance, which has T-100% = 210 degrees C and above 80% N-2 selectivity. Combining the experimental method and the density functional theory (DFT), the oxygen molecule is adsorbed in the form of a stable molecular state on Cu2O particles, while the dissociative adsorption of O-2 occurs over the mixed CuO-Cu2O and pure CuO phases. It is found that O-2 is more likely to be dissociated and activated on CuO-Cu2O with E-ads = -7.15 eV. There are three kinds of intermediate species (monodentate, bidentate, and bridging nitrate) observed. The formation of key bidentate nitrate species facilitates NH3 conversion and N-2 formation, but the other intermediate species have a negative effect on NH3 oxidation.
Translation or Not:
no
