Performance of activated carbon supported nickel catalysts in the pyrolysis of waste plastics to produce carbon nanotubes
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摘要: 以椰壳炭、竹炭和木炭三种活性炭为载体，采用浸渍法制备炭负载金属镍的催化剂，考察其在废塑料裂解制备碳纳米管过程中的催化反应性能；采用X射线衍射、扫描电镜、透射电镜、拉曼光谱仪、同步热分析仪、比表面积分析仪等手段分析了催化剂和产物碳纳米管的形貌和结构。结果表明，椰壳活性炭为载体制备的镍基催化剂上碳纳米管产量最高、石墨化程度最好。以椰壳活性炭为载体制备的镍基催化剂为例，研究了反应温度和镍负载量对其催化性能的影响。Abstract: A series of Ni based catalysts are prepared through impregnation method with coconut shell, bamboo charcoal and charcoal activated carbons as the support; their catalytic performance in the pyrolysis of waste plastics to produce carbon nanotubes was comparatively investigated. The structure and morphology of the catalyst and carbon nanotubes were characterized by X-ray diffraction, scanning electron microscope, transmission electron microscope, Raman spectroscopy, thermogravimetric analysis and nitrogen physisorption. The results show that carbon nanotubes with the highest yield and the best quality can be produced by using the nickel catalyst supported on coconut shell activated carbon (Ni/CSAC). In addition, the effect of reaction temperature and nickel loading on the catalytic performance of Ni/CSAC in the pyrolysis of waste plastics was considered.
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图 2 催化剂的SEM照片
Figure 2 SEM images of nickel catalysts supported on (a) coconut shell activated carbon (Ni/CSAC), (b) bamboo charcoal activated carbon (Ni/BCAC), and (c) charcoal activated carbons (Ni/CAC)
图 4 催化剂的N2吸附-脱附等温线(a)和用DFT方法计算的孔径分布图(b)
Figure 4 N2 adsorption-desorption isotherms (a) and the corresponding DFT pore size distribution curves (b) of various catalysts
图 6 反应后催化剂的程序升温氧化
Figure 6 Temperature program oxidation (TPO) profiles of the spent catalysts
图 7 反应过后催化剂的SEM和TEM照片
Figure 7 SEM and TEM images of the spent catalysts
(a) and (b): Ni/CSAC-CNTs; (c) and (d): Ni/BCAC-CNTs; (e) and (f): Ni/CAC-CNTs
图 9 新鲜催化剂(a)和反应后催化剂(b)的Raman谱图
Figure 9 Raman spectra of the fresh catalysts (a) and spent catalysts (b)
图 10 温度(a)和Ni负载量(b)对CNTs产量的影响
Figure 10 Effect of temperature (a) and Ni loading (b) on the yield of CNTs for the pyrolysis of waste plastics over the Ni/CSAC catalyst
表 1 不同催化剂的比表面积和孔结构特征
Table 1 Surface area and pore-structure characteristic of various catalysts
Sample ABET/ (m2·g-1) Amicro/ (m2·g-1) Ameso/ (m2·g-1) vtotal/ (m3·g-1) vmicro/ (m3·g-1) vmeso/ (m3·g-1) Amicro/ Ameso vmicro/ vmeso Ni/CSAC 545 288 257 0.389 0.149 0.240 1.121 0.621 Ni/BCAC 255 53 202 0.243 0.026 0.217 0.262 0.120 Ni/CAC 969 352 617 0.963 0.183 0.780 0.571 0.235 
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