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首页> 外文期刊>Chemistry: A European journal >Glucose- and Cellulose-Derived Ni/C-SO3H Catalysts for Liquid Phase Phenol Hydrodeoxygenation
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Glucose- and Cellulose-Derived Ni/C-SO3H Catalysts for Liquid Phase Phenol Hydrodeoxygenation

机译：葡萄糖和纤维素衍生的Ni / C-SO3H液相苯酚加氢脱氧催化剂

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摘要

Sulfonated carbons were explored as functionalized supports for Ni nanoparticles to hydrodeoxygenate (HDO) phenol. Both hexadecane and water were used as solvents. The dual-functional Ni catalysts supported on sulfonated carbon (Ni/C-SO3H) showed high rates for phenol hydrodeoxygenation in liquid hexadecane, but not in water. Glucose and cellulose were precursors to the carbon supports. Changes in the carbons resulting from sulfonation of the carbons resulted in variations of carbon sheet structures, morphologies and the surface concentrations of acid sites. While the C-SO3H supports were active for cyclohexanol dehydration in hexadecane and water, Ni/C-SO3H only catalysed the reduction of phenol to cyclohexanol in water. The state of 3-5 nm grafted Ni particles was analysed by in situ X-ray absorption spectroscopy. The results show that the metallic Ni was rapidly formed in situ without detectable leaching to the aqueous phase, suggesting that just the acid functions on Ni/C-SO3H are inhibited in the presence of water. Using in situ IR spectroscopy, it was shown that even in hexadecane, phenol HDO is limited by the dehydration step. Thus, phenol HDO catalysis was further improved by physically admixing C-SO3H with the Ni/C-SO3H catalyst to balance the two catalytic functions. The minimum addition of 7 wt% C-SO3H to the most active of the Ni/C-SO3H catalysts enabled nearly quantitative conversion of phenol and the highest selectivity (90%) towards cyclohexane in 6 h, at temperatures as low as 473 K, suggesting that the proximity to Ni limits the acid properties of the support.
机译：磺化碳被用作Ni纳米粒子加氢脱氧（HDO）苯酚的功能化载体。十六烷和水均用作溶剂。负载在磺化碳上的双功能Ni催化剂（Ni / C-SO3H）在液体十六烷中显示出较高的苯酚加氢脱氧率，而在水中则没有。葡萄糖和纤维素是碳载体的前体。由碳的磺化引起的碳的变化导致碳片结构，形态和酸位的表面浓度的变化。尽管C-SO3H载体对于在十六烷和水中的环己醇脱水具有活性，但Ni / C-SO3H仅催化水中苯酚还原为环己醇。通过原位X射线吸收光谱分析了3-5nm接枝的Ni颗粒的状态。结果表明，金属镍是在原位快速形成的，而没有可检测到的浸出到水相中，这表明在水的存在下，仅能抑制Ni / C-SO3H上的酸功能。使用原位红外光谱表明，即使在十六烷中，苯酚HDO也会受到脱水步骤的限制。因此，通过将C-SO3H与Ni / C-SO3H催化剂物理混合以平衡两种催化功能，可以进一步改善苯酚HDO催化作用。在活性最强的Ni / C-SO3H催化剂中最少添加7 wt％的C-SO3H，可在低至473 K的温度下在6小时内对苯酚进行几乎定量的转化，并向环己烷具有最高的选择性（90％），这表明与镍的接近限制了载体的酸性质。

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