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Au/Ni雙金屬納米顆粒的制備及其催化制氫活性
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國家自然科學(xué)基金面上項目（5127188）


Preparation and Catalytic Activity of Au/Ni Bimetallic Nanoparticles for Hydrogen Generation from the Hydrolysis Reaction of Alkaline NaBH4 Solution
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    摘要:

    采用化學(xué)共還原法制備了聚乙烯吡咯烷酮(PVP)保護(hù)的Au/Ni雙金屬納米顆粒，采用UV-Vis、TEM對所合成的納米顆粒進(jìn)行了表征，研究了雙金屬納米顆粒的化學(xué)組成對其催化水解NaBH4制氫活性的影響。結(jié)果表明：所制備的Au/Ni雙金屬納米顆粒的平均粒徑為2.9~4.2 nm，Au/Ni雙金屬納米顆粒的催化活性高于Au和Ni單金屬納米顆粒的活性，Au50Ni50雙金屬納米顆粒的催化活性最高，30 ℃時其催化活性數(shù)值達(dá)到550 mol-H2·h-1·mol-M-1。XPS和密度泛函理論(DFT)的結(jié)果都表明：Au/Ni雙金屬納米顆粒優(yōu)異的催化性能可歸因于電荷轉(zhuǎn)移效應(yīng)，Ni原子與Au原子之間發(fā)生的電子轉(zhuǎn)移使得Au原子帶負(fù)電而Ni原子帶正電，荷電的Au和Ni原子成為催化反應(yīng)的活性中心。Au50Ni50雙金屬納米顆粒催化水解NaBH4制氫的活化能為61.9 kJ/mol。

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    Poly(N-vinyl-2-pyrrolidone) (PVP)-protected Au/Ni bimetallic nanoparticles (BNPs) were prepared using a chemical reduction method. The obtained BNPs were characterized by Ultraviolet-visible spectrophotometry (UV-Vis) and transmission electron microscopy (TEM). The effects of metal compositions on the hydrolysis reaction of the alkaline NaBH4 solution were studied. The results indicate that the prepared Au/Ni BNPs have an average size of 2.9~4.2 nm. The activities of BNPs are much higher than that of Au and Ni monometallic nanoparticles (MNPs). Among all the MNPs and BNPs, Au/Ni BNPs with atomic ratio of 50/50 display the highest catalytic activity, showing a high hydrogen release rate of 550 mol-H2·h-1·mol-M-1 at 30 oC. The catalytic activity of the Au/Ni BNPs higher than that of corresponding MNPs can be ascribed to electronic charge transfer effects. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) show that Au atoms are indeed negatively charged, while the Ni atoms have positive charges due to the electron donation from the Ni atoms to Au atoms. The positively charged Ni atoms and negatively charged Au atoms act as catalytic active sites for the hydrolysis reaction of the alkaline NaBH4 solution. Au50Ni50 BNPs display a low apparent activation energy of 61.9 kJ/mol.

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王小鳳,曹迎楠,孫少瑞,黃自力,張海軍,張少偉. Au/Ni雙金屬納米顆粒的制備及其催化制氫活性[J].稀有金屬材料與工程,2015,44(3):753~758.[Wang Xiaofeng, Cao Yingnan, Sun Shaorui, Huang Zili, Zhang Haijun, Zhang Shaowei. Preparation and Catalytic Activity of Au/Ni Bimetallic Nanoparticles for Hydrogen Generation from the Hydrolysis Reaction of Alkaline NaBH4 Solution[J]. Rare Metal Materials and Engineering,2015,44(3):753~758.]
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  • 收稿日期:2014-03-20
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  • 在線發(fā)布日期: 2015-05-29
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