钴镍双金属催化剂的制备及氨分解制氢性能研究
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摘要
采用水热法制备Co(OH)_2、Ni(OH)_2及不同比例Co-Ni基纳米片,经高温热解后获得Co-Ni双金属纳米催化剂。以氨分解制氢为模型反应,并结合X射线物相分析、扫描电镜以及红外等考察Co-Ni双金属催化剂的结构-性能关系。结果表明,双金属催化剂的氨解性能随着Co含量的提高而提高;基于Co(OH)_2的纳米片的钴基催化剂活性最高,在873 K下的氨分解转化率为98.2%,活化能Ea为40.68 k J/mol。
Bimetallic Co-Ni based alloy catalysts derived from Co-Ni based hydroxide nanosheet with different proportions of Co-Ni were prepared by hydrothermal method and further thermal treatment. The relationship between catalyst structure and catalytic activity for ammonia decomposition to hydrogen was characterized with the help of X-ray diffraction( XRD),scanning electronic microscope( SEM) and infrared spectroscopy( FT-IR). The result suggested that catalytic activity for ammonia decomposition increased with the increase of Co content in the alloyed catalyst. The monimetllic Co catalyst derived from Co(OH)_2 nanosheet yielded the highest catalytic activity and the conversion of ammonia reached 98. 2% at 873 K and 6000 m L/g ·h. At current reaction condition,apparent activation energy was40. 68 k J/mol according to Arrhenius' s equation.
Bimetallic Co-Ni based alloy catalysts derived from Co-Ni based hydroxide nanosheet with different proportions of Co-Ni were prepared by hydrothermal method and further thermal treatment. The relationship between catalyst structure and catalytic activity for ammonia decomposition to hydrogen was characterized with the help of X-ray diffraction( XRD),scanning electronic microscope( SEM) and infrared spectroscopy( FT-IR). The result suggested that catalytic activity for ammonia decomposition increased with the increase of Co content in the alloyed catalyst. The monimetllic Co catalyst derived from Co(OH)_2 nanosheet yielded the highest catalytic activity and the conversion of ammonia reached 98. 2% at 873 K and 6000 m L/g ·h. At current reaction condition,apparent activation energy was40. 68 k J/mol according to Arrhenius' s equation.
引文
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[8]L Wang,Y Yi,Y Zhao,et al. NH3decomposition for H2generation:effects of cheap metals and supports on plasma-catalyst synergy[J].ACS Catal.,2015,5(7):4167-4174.
[9]M Zhang,Y Yang,W Chen,et al. Metal(hydr)oxides@polymer coreshell strategy to metal single-atom materials[J]. J. Am. Chem. Soc.,2017,139:10976-10979.
[10]程遥,郑远辉,王元生,等. Ni(OH)2及Co(OH)2片状纳米晶体的合成与表征[J].电子显微学报,2005,24(5):460-463.
[2]林翎.能源管理与能源节约领域国际标准化工作进展[J].中国标准化,2017(11):39-42.
[3]S Ren,F Huang,J Zheng,et al. Ruthenium supported on nitrogendoped ordered mesoporous carbon as highly active catalyst for NH3decomposition to H2[J]. Int. J. Hydrogen Energy,2017,42(8):5105-5113.
[4]崔会珍.铁基复合纳米催化剂的制备及其催化氨分解的研究[D].济南:山东大学,2016.
[5]T V Choudhary,C Sivadinarayana,D W Goodman. Catalytic ammonia decomposition:COx-free hydrogen production for fuel cell applications[J]. Catal. Lett.,2001,72:197-201.
[6]A S Chellappa,C M Fischer,W J Thomson. Ammonia decomposition kinetics over Ni-Pt/Al2O3for PEM fuel cell applications[J]. Appl.Catal. A,2002,227:231-240.
[7]D V Leybo, A N Baiguzhina, D S Muratov, et al. Effects of composition and production route on structure and catalytic activity for ammonia decomposition reaction of ternary Ni-Mo nitride catalysts[J].Int. J. Hydrogen Energy,2016,41:3854-3860.
[8]L Wang,Y Yi,Y Zhao,et al. NH3decomposition for H2generation:effects of cheap metals and supports on plasma-catalyst synergy[J].ACS Catal.,2015,5(7):4167-4174.
[9]M Zhang,Y Yang,W Chen,et al. Metal(hydr)oxides@polymer coreshell strategy to metal single-atom materials[J]. J. Am. Chem. Soc.,2017,139:10976-10979.
[10]程遥,郑远辉,王元生,等. Ni(OH)2及Co(OH)2片状纳米晶体的合成与表征[J].电子显微学报,2005,24(5):460-463.