Insight into the chemical adsorption properties of CO molecules supported on Au or Cu and hybridized Au-CuO nanoparticles | |
Luo, Jingjie; Liu, Yuefeng; Niu, Yiming; Jiang, Qian; Huang, Rui; Zhang, Bingsen; Su, Dangsheng; Liu, YF; Zhang, BS; Su, DS (reprint author), Chinese Acad Sci, Shenyang Natl Lab Mat Sci SYNL, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China.; Su, DS (reprint author), Chinese Acad Sci, Dalian Natl Lab Clean Energy DNL, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China. | |
2017-10-21 | |
发表期刊 | ROYAL SOC CHEMISTRY
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ISSN | 2040-3364 |
卷号 | 9期号:39页码:15033-15043 |
摘要 | Although nanosized Au clusters have been well developed for many applications, fundamental understanding of their adsorption/activation behaviors in catalytic applications is still lacking, especially when other elements provide promotion or hybridization functions. Au hybridized with Cu element is a highly investigated system; Cu is in the same element group as Au and thus displays similar physicochemical properties. However, their hybrids are not well understood in terms of their chemical states and adsorption/ activation properties. In this work, typical gamma-Al2O3-supported Au and CuO as well as Au-CuO nanoparticles were prepared and characterized to explore their adsorption/activation properties in depth using CO as a probe molecule using advanced techniques, such as XPS, HR-TEM, temperature programmed experiments and operando DRIFT combined with mass spectra. It was found that gold and copper can both act as active sites during CO adsorption and activation. The CO-TPD and operando DRIFT results also revealed that CO molecules were able to react with surface oxygenated species, resulting in the direct formation of CO2 over the three samples in the absence of gaseous O-2. The gold step sites (Austep) participated more readily in the reaction, especially under gaseous O-2-free conditions. During adsorption, CO molecules were more preferentially adsorbed on Au-0 sites at lower temperature comparing with those on the Cu-0 sites. However, competitive adsorption occurred between CO adsorbed on Au-0 and Cu-0 with increased reaction temperature, and the synergy between the Au and Cu compositions was too strong to suppress the adsorption and activation of the CO molecules. The dynamic adsorption equilibrium over 120 degrees C to 200 degrees C resulted in the appearance of a hysteresis performance platform.; Although nanosized Au clusters have been well developed for many applications, fundamental understanding of their adsorption/activation behaviors in catalytic applications is still lacking, especially when other elements provide promotion or hybridization functions. Au hybridized with Cu element is a highly investigated system; Cu is in the same element group as Au and thus displays similar physicochemical properties. However, their hybrids are not well understood in terms of their chemical states and adsorption/ activation properties. In this work, typical gamma-Al2O3-supported Au and CuO as well as Au-CuO nanoparticles were prepared and characterized to explore their adsorption/activation properties in depth using CO as a probe molecule using advanced techniques, such as XPS, HR-TEM, temperature programmed experiments and operando DRIFT combined with mass spectra. It was found that gold and copper can both act as active sites during CO adsorption and activation. The CO-TPD and operando DRIFT results also revealed that CO molecules were able to react with surface oxygenated species, resulting in the direct formation of CO2 over the three samples in the absence of gaseous O-2. The gold step sites (Austep) participated more readily in the reaction, especially under gaseous O-2-free conditions. During adsorption, CO molecules were more preferentially adsorbed on Au-0 sites at lower temperature comparing with those on the Cu-0 sites. However, competitive adsorption occurred between CO adsorbed on Au-0 and Cu-0 with increased reaction temperature, and the synergy between the Au and Cu compositions was too strong to suppress the adsorption and activation of the CO molecules. The dynamic adsorption equilibrium over 120 degrees C to 200 degrees C resulted in the appearance of a hysteresis performance platform. |
部门归属 | [luo, jingjie ; liu, yuefeng ; niu, yiming ; huang, rui ; zhang, bingsen ; su, dangsheng] chinese acad sci, shenyang natl lab mat sci synl, inst met res, 72 wenhua rd, shenyang 110016, liaoning, peoples r china ; [liu, yuefeng ; jiang, qian ; su, dangsheng] chinese acad sci, dalian natl lab clean energy dnl, dalian inst chem phys, 457 zhongshan rd, dalian 116023, peoples r china |
学科领域 | Chemistry, Multidisciplinary ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied |
资助者 | China Postdoctoral Science Foundation [2016M600221]; National Natural Science Foundation of China [91645117, 21606243, 21473223, 91545119, 21773269]; Youth Innovation Promotion Association CAS [2015152] |
收录类别 | SCI |
语种 | 英语 |
WOS记录号 | WOS:000412940000032 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/79038 |
专题 | 中国科学院金属研究所 |
通讯作者 | Liu, YF; Zhang, BS; Su, DS (reprint author), Chinese Acad Sci, Shenyang Natl Lab Mat Sci SYNL, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China.; Su, DS (reprint author), Chinese Acad Sci, Dalian Natl Lab Clean Energy DNL, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China. |
推荐引用方式 GB/T 7714 | Luo, Jingjie,Liu, Yuefeng,Niu, Yiming,et al. Insight into the chemical adsorption properties of CO molecules supported on Au or Cu and hybridized Au-CuO nanoparticles[J]. ROYAL SOC CHEMISTRY,2017,9(39):15033-15043. |
APA | Luo, Jingjie.,Liu, Yuefeng.,Niu, Yiming.,Jiang, Qian.,Huang, Rui.,...&Su, DS .(2017).Insight into the chemical adsorption properties of CO molecules supported on Au or Cu and hybridized Au-CuO nanoparticles.ROYAL SOC CHEMISTRY,9(39),15033-15043. |
MLA | Luo, Jingjie,et al."Insight into the chemical adsorption properties of CO molecules supported on Au or Cu and hybridized Au-CuO nanoparticles".ROYAL SOC CHEMISTRY 9.39(2017):15033-15043. |
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