Investigation on Cu2O Surface Reconstruction and Catalytic Performance of NH3-SCO by Experimental and DFT Studies
发表时间：2020-06-01
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- 论文类型：
- 期刊论文
- 第一作者：
- Zhang, Xiaoyu
- 通讯作者：
- 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.
- 合写作者：
- Wang, Hui,Meng, Linlin,Nie, Xiaowa,Qu, Zhenping
- 发表时间：
- 2020-04-27
- 发表刊物：
- ACS APPLIED ENERGY MATERIALS
- 收录刊物：
- SCIE
- 文献类型：
- J
- 卷号：
- 3
- 期号：
- 4
- 页面范围：
- 3465-3476
- ISSN号：
- 2574-0962
- 关键字：
- reconstruction; Cu2O-CuO mixed oxide; DFT calculations; oxygen dissociated adsorption; bidentate nitrate
- 摘要：
- 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.
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- 否
