Promoted the reduction of Cu2+ to enhance CuOCeO2 catalysts for CO preferential oxidation in H2-rich streams: Effects of preparation methods and copper precursors
作者:
Wang, Jing;Pu, Hongping* ;Wan, Gengping;Chen, Kezhen;Lu, Jichang;...
期刊:
International Journal of Hydrogen Energy ,2017年42(34):21955-21968 ISSN:0360-3199
通讯作者:
Pu, Hongping;Luo, Yongming
作者机构:
[He, Sufang; Luo, Yongming; Chen, Kezhen; Pu, Hongping; Luo, YM; Lu, Jichang; Wan, Gengping; Wang, Jing; Lei, Yanqiu; Zhong, Liping] Kunming Univ Sci & Technol, Fac Environm Sci & Engn, Kunming 650500, Yunnan, Peoples R China.;[Wang, Jing] Hengyang Normal Univ, Coll Life Sci & Environm, Hengyang 421008, Peoples R China.;[Wan, Gengping] Hainan Univ, Res Ctr Anal & Measurement, Haikou 570228, Hainan, Peoples R China.;[He, Sufang] Kunming Univ Sci & Technol, Res Ctr Anal & Measurement, Kunming 650093, Yunnan, Peoples R China.
通讯机构:
[Pu, HP; Luo, YM] K;Kunming Univ Sci & Technol, Fac Environm Sci & Engn, Kunming 650500, Yunnan, Peoples R China.
关键词:
Catalysts;Copper;Crystallite size;Gas fuel purification;Oxidation;CO preferential oxidation;Copper precursors;Copper species;CuO-CeO2;Synthesis method;Catalyst activity
摘要:
A series of CuO–CeO<inf>2</inf>catalyst samples synthesized by using various methods (CuCe-SF-N, CuCe-UGC-N, CuCe-SG-N and CuCe-ST-N) and copper precursors (CuCe-SF-N, CuCe-SF-C, CuCe-SF-A and CuCe-SF-S) were estimated for CO preferential oxidation in H<inf>2</inf>-rich streams. It was found that both synthesis routes and copper precursors have an important effect on catalytic behaviors of CuO–CeO<inf>2</inf>catalyst. Compared to CuCe-UGC-N, CuCe-SG-N and CuCe-ST-N, CuCe-SF-N exhibits the lowest temperature and the widest temperature window for 100% CO conversion (about 50 °C), which should be attributed to synergistic effects of smaller crystallite size, the formation of more Cu<sup>+</sup>species together with the high ratio of Ce<sup>3+</sup>/(Ce<sup>3+</sup>+Ce<sup>4+</sup>). Among the four catalysts prepared with different Cu precursors (CuCe-SF-N, CuCe-SF-C, CuCe-SF-A and CuCe-SF-S), the corresponding CO conversions of them are in the order of CuCe-SF-N >CuCe-SF-A >CuCe-SF-C »CuCe-SF-S. The lowest catalytic activity of CuCe-SF-S should be due to the presence of SO<inf>4</inf><sup>2−</sup>species covered on the surface of the catalyst, which not only results in the formation of the less Cu active species but inhibits the interaction between Cu species and CeO<inf>2</inf>. In addition, the optimal CuCe-SF-N catalyst displays relative stability during the 200 h time-on-stream test even in the presence of H<inf>2</inf>O and CO<inf>2</inf>. ©2017 Hydrogen Energy Publications LLC
语种:
英文
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A solvent-free method to rapidly synthesize CuO-CeO2 catalysts to enhance their CO preferential oxidation: Effects of Cu loading and calcination temperature
作者:
Wang, Jing;Zhong, Liping;Lu, Jichang;Chen, Ran;Lei, Yanqiu;...
期刊:
Molecular Catalysis ,2017年443:241-252 ISSN:2468-8231
通讯作者:
He, Sufang;Luo, Yongming
作者机构:
[He, Sufang; Luo, Yongming; Chen, Ran; Chen, Kezhen; Lu, Jichang; Han, Caiyun; Wan, Gengping; He, SF; Luo, YM; Wang, Jing; Zhong, Liping; Lei, Yanqiu] Kunming Univ Sci & Technol, Fac Environm Sci & Engn, Kunming 650500, Yunnan, Peoples R China.;[Wang, Jing] Hengyang Normal Univ, Coll Life Sci & Environm, Hengyang 421008, Peoples R China.;[He, Sufang] Kunming Univ Sci & Technol, Res Ctr Anal & Measurement, Kunming 650093, Yunnan, Peoples R China.;[Wan, Gengping] Hainan Univ, Res Ctr Anal & Measurement, Haikou 570228, Hainan, Peoples R China.
通讯机构:
[He, SF; Luo, YM] K;Kunming Univ Sci & Technol, Fac Environm Sci & Engn, Kunming 650500, Yunnan, Peoples R China.
关键词:
Calcination;Catalyst activity;Catalysts;Copper oxides;Energy conservation;Gelation;Nitrogen compounds;Sol-gel process;Sol-gels;Solvents;Urea;Calcination temperature;Catalytic performance;CO preferential oxidation;Cu loadings;CuO-CeO2;Optimal calcination;Solvent free;Surfactant template;Cerium compounds
摘要:
A facile and solvent-free route has been developed to rapidly synthesize CuO-CeO2 catalysts within 30 min. The effect of calcination temperature on catalytic performances is more significant than Cu loading, and the optimal calcination temperature and Cu loading are 700 °C and 7.5 wt.%, respectively. The optimal catalyst 7.5CuCe-SF-700 exhibits the highest CO conversion and the corresponding temperature window for full CO conversion is as wide as 50 °C. According to the characterization results of XRD, N2 adsorption-desorption, H2-TPR, TEM, HR-TEM, STEM, EDS, Raman and XPS, it can be concluded that the high-performances of CuO-CeO2 catalyst should be attributed to synergistic effects of high dispersion Cu species and CeO2, and the presence of more reduced copper species as the active site in the catalyst. 7.5CuCe-SF-700 exhibits excellent stability for CO-PROX during the 200 time-on-stream test under actual reaction conditions (with 15% CO2 and 10% H2O). In addition, surfactant template, urea gelation/co-precipitation and sol-gel methods were used to synthesize CuO-CeO2 catalysts so as to compare them with 7.5CuCe-SF-700, and the results exhibit not only 7.5CuCe-SF-700 is superior to the former three catalysts but also our synthesis route is more simple, controllable, solvent-free, time-saving and energy-saving.
语种:
英文
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