低温下Pt/Al2O3和Pd/Al2O3光辅助乙二醇水相重整制氢研究

Low temperature light-assisted hydrogen production from aqueous reforming ethylene glycol over Pt/Al2O3 and Pd/Al2O3 catalysts

  • 摘要: 采用浸渍还原法制备了氧化铝负载的Pt和Pd纳米颗粒催化剂,用于光辅助乙二醇水相重整制氢反应。结果表明,光照能够有效降低乙二醇水相重整制氢的活化能,Pt/Al2O3比Pd/Al2O3具有更高的H2转换频率(TOF)和更低的CO选择性。采用XRD、TEM、UV-vis等技术对催化剂的结构和形貌进行了表征,原位漫反射红外光谱(DRIFTS)表明,光照能促进乙二醇分子O-H键的断裂。理论计算表明,Pt/Al2O3催化乙二醇重整制氢反应产物中较低的CO选择性主要归因于CO在Pt表面较小的反应能垒,能够较快与H2O解离的O反应生成CO2

     

    Abstract: Al2O3 supported Pt and Pd nanoparticle catalysts were prepared by impregnation-reduction method, and employed in the photocatalytic aqueous-phase reforming of ethylene glycol. Light illumination can decrease the reaction activation energy remarkably. Pt/Al2O3 exhibits much higher H2 turnover frequency (TOF) and lower CO selectivity than Pd/Al2O3 catalyst. Their morphology and structure were characterized by XRD, TEM, UV-vis techniques. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) indicates light can promote the cleavage of O-H bonds of ethylene glycol molecule. DFT calculation suggests the lower CO selectivity over Pt/Al2O3 catalyst can be attributed to the low energy barriers of reaction in the step of CO+O→CO2.

     

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