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Improved hydrothermal stability of Pd nanoparticles on nitrogen-doped carbon supports

机译:提高了Pd的水热稳定性纳米粒子在nitrogen-doped碳支持

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摘要

Carbon supports have been shown to provide better hydrothermal stability than alumina or silica supports, thus attracting more attention for aqueous-phase biomass conversion reactions. However, sintering and leaching of the metal particles still occur during condensed phase utilization of carbon supported metal catalysts. To further improve the stability of supported metal particles, a simple nitrogen-doped carbon coated SBA-15 was synthesized and systematically characterized. Better stability of supported Pd particles was found from nitrogen incorporation into the carbon support during extended hydrothermal treatment or under continuous flow reaction conditions. With these materials, leaching was negligible and sintering was suppressed. Based on solid-state N-15 and C-13 NMR analysis before and after hydrothermal treatment, the improved dispersion and stability from nitrogen doping was ascribed to pyridine, pyrrole, and imidazolium groups. Relatively small carbon fragments resulting from nitrogen incorporation rendered more silica exposure to water and concomitant hydrolysis, but the stability and activity of Pd particles were preserved. The Pd stability advantage was also observed on nitrogen-doped carbon coatings of silica gel and CMK-3 supports. The enhanced stability of Pd particles on different nitrogen-doped carbon materials was correlated with the synergistic effect of oxygen and nitrogen heteroatoms and the formation of a decorative carbon overlayer on the Pd particles.
机译:碳可以提供更好的支持水热稳定性比氧化铝和二氧化硅支持,从而吸引更多的关注水相生物转化反应。然而,烧结和金属的浸出在凝相粒子仍然发生利用碳支持金属催化剂。以进一步提高稳定性的支持金属粒子,一个简单的nitrogen-doped碳涂布SBA-15合成和系统为特征。从氮结合粒子被发现在扩展到碳支持热液治疗或在连续流动反应条件。浸出是微不足道的和烧结抑制。核磁共振分析前后的热液治疗,改善分散性和稳定性从氮掺杂是归因于吡啶,吡咯,imidazolium组。碳碎片产生的氮公司呈现更多的硅接触水和伴随的水解,但稳定和Pd活性粒子保存了下来。观察nitrogen-doped碳涂层硅胶和CMK-3支持。Pd粒子在不同的稳定nitrogen-doped碳材料是相关的与氧气和协同效应氮杂原子和形成装饰碳覆盖物在Pd粒子。

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