三维有序大孔钙钛矿型La_(1–x)K_xNiO_3催化剂提高炭烟催化燃烧活性:K取代的作用（英文）
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摘要
催化炭烟燃烧的本质是典型的固体(炭烟颗粒)-固体(催化剂)-气体(O_2和NO)三相深度氧化反应.因此炭烟燃烧性能不仅与催化剂的本征活性有关,同时也与催化剂和炭烟颗粒之间的接触效率有关.钙钛矿型(ABO_3)氧化物具有高热稳定性和高催化活性,在钙钛矿型氧化物中A位通常为稀土元素,B位通常为过渡金属元素,钙钛矿的A,B位离子都可以被半径相近的其他元素部分取代,而且物相结构不发生变化.我们组前期研究发现,用碱金属部分取代钙钛矿型氧化物中的A位,可以有效提高其催化活性.同时发现三维有序大孔(3DOM)结构可以有效的增加催化剂与碳烟颗粒的接触效率.基于此,本文利用胶体晶体模板法成功制备了3DOM La_(1-x)K_xNiO_3钙钛矿型催化剂,并采用SEM,TEM,HRTEM,Elements mapping,XRD,Raman,XPS和H_2-TPR等手段对其物理化学性能进行了表征,进一步探讨K取代对3DOM La_(1–x)K_xNiO_3催化剂炭烟催化燃烧性能的影响.SEM和TEM照片显示,制备的3DOM La_(1–x)K_xNiO_3催化剂孔道三维有序贯通,孔径均一,孔壁厚度均匀,每个大孔下面展示清晰可见的小孔窗,大孔孔径大约为260 nm,这有利于炭烟颗粒在气流的协助下进入催化剂的孔道之内,从而提高炭烟与催化剂之间的接触效率.3DOM结构催化剂具有大的比表面积(24?27 m~2g~(–1)),且K的取代对其比表面积无太大的影响.XRD和Raman谱证实了催化剂的钙钛矿结构,且K能够取代La并进入钙钛矿氧化物的晶格中.XPS和H_2-TPR表征发现,K取代La之后,B位的Ni元素的价态有所提升,表面活性氧物种密度增加,其中3DOM La_(0.95)K_(0.05)NiO_3催化剂具有最高的Ni~(4+)的含量和活性氧含量.3DOM La_(1–x)K_xNiO_3催化剂展示了高的炭烟燃烧催化性能,且K的取代能够明显促进其催化炭烟燃烧活性.在松散接触条件下,催化剂炭烟催化燃烧活性的顺序为:3DOM La_(0.95)K_(0.05)NiO_3>3DOM La_(0.90)K_(0.10)NiO_3>3DOM La_(0.80)K_(0.20)NiO_3>3DOM La_(0.99)K_(0.01)NiO_3>3DOM LaNiO_3>particle–type LaNiO_3.其中,3DOM La_(0.95)K_(0.05)NiO_3催化剂展示了最高的炭烟燃烧催化性能,其T_(50)和S_(CO2)值分别为338°C和98.2%,这与Pt基催化剂活性相当.另外,对炭烟催化燃烧性能的影响因素进行了探讨:一方面,三维有序大孔结构有效提高催化剂活性;另一方面,K元素的取代提高了Ni的价态,从而提升了表面活性氧物种数量,这对炭烟催化燃烧起着至关重要的作用.
Three-dimensional ordered macroporous(3DOM)La_(1-x)K_xNiO_3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy,transmission electron microscopy,high-resolution transmission electron microscopy,energy-dispersive X-ray scattering elemental mapping,X-ray diffraction,Raman and X-ray photoelectron spectroscopy,and temperature-programmed reduction of H_2.Further,their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction.K substitution into the LaNiO_3 lattice led to remarkably improved catalytic activity of this catalyst in soot combustion.Amongst various catalysts,La_(0.95)K_(0.05)NiO_3 exhibited the highest activity in soot combustion(with its T_(50) and S_(CO_2) values being 338°C and 98.2%,respectively),which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst.K-substitution improves the valence state of Ni and increases the number of oxygen vacancies,thereby leading to increased density of surface-active oxygen species.The active oxygen species play a vital role in catalyzing the elimination of soot.The perovskite-type La_(1-x)K_xNiO_3 nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.
Three-dimensional ordered macroporous(3DOM)La_(1-x)K_xNiO_3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy,transmission electron microscopy,high-resolution transmission electron microscopy,energy-dispersive X-ray scattering elemental mapping,X-ray diffraction,Raman and X-ray photoelectron spectroscopy,and temperature-programmed reduction of H_2.Further,their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction.K substitution into the LaNiO_3 lattice led to remarkably improved catalytic activity of this catalyst in soot combustion.Amongst various catalysts,La_(0.95)K_(0.05)NiO_3 exhibited the highest activity in soot combustion(with its T_(50) and S_(CO_2) values being 338°C and 98.2%,respectively),which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst.K-substitution improves the valence state of Ni and increases the number of oxygen vacancies,thereby leading to increased density of surface-active oxygen species.The active oxygen species play a vital role in catalyzing the elimination of soot.The perovskite-type La_(1-x)K_xNiO_3 nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.
引文
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