Catalytic performance of PdCl2/Cu-HMS: Influence of hydrophobicity and structure of molecular sieves

Catalytic performance of PdCl2/Cu-HMS: Influence of hydrophobicity and structure of molecular sieves
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PdCl2/Cu-HMS的催化性能:疏水性和分子筛结构的影响

DOI:
10.1016/j.apsusc.2014.01.001
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发表时间:
2014-03
影响因子:
6.7
通讯作者:
Jiang, Pingping
Jiang, Pingping
中科院分区:
材料科学1区
文献类型:
--
作者:
Zhang, Pingbo;Zhou, Yan;Fan, Mingming;Jiang, Pingping

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分别以甲基三氯硅烷和苯基三氯硅烷为原料,通过简单的硅烷化反应合成了表面疏水化的PdCl 2/Si-Cu-HMS-m材料。通过红外光谱、粉末X射线衍射、氮气吸附-脱附、水滴接触角测定等手段对复合材料进行了表征。结果表明,改性后的Cu-HMS保留了介孔结构,并提高了疏水性。然而,硅烷化试剂对催化剂性能有显著影响。实验结果表明,PdCl 2/Si-Cu-HMS-CH 3对乙醇气相氧化羰基化合成碳酸二乙酯(DEC)具有较高的催化活性,与PdCl 2/Si-Cu-HMS-Ben催化剂相比,PdCl 2/Si-Cu-HMS-CH 3催化剂的空间位阻较小,但疏水性较弱,表明催化剂的催化性能与副产物水和分子筛结构有关,但后者是催化体系中的主要因素。此外,还提出了分子筛结构是影响催化剂性能的主要因素的可能机理。
Surface hydrophobically modified PdCl2/Si-Cu-HMS-m materials were successfully synthesized via a simple silylation process using methyltrichlorosilane and phenyltrichlorosilane respectively. They were characterized by a series of techniques including FT-IR, powder XRD, nitrogen adsorption–desorption, and the contact angle measurement of the water droplet. It was demonstrated that the mesoporous structure of Cu-HMS was retained after modification and that hydrophobicity was enhanced. However, silylation agents had a significant influence on catalytic performance. The experimental results indicated that PdCl2/Si-Cu-HMS-CH3showed a high catalytic activity for the gas phase oxidative carbonylation of ethanol to diethyl carbonate (DEC) and a small steric hindrance but a weak hydrophobicity in comparison with PdCl2/Si-Cu-HMS-Ben catalyst, demonstrating that catalytic performance was relative to both by-product water and structure of molecular sieves catalyst, but the latter was a main factor in the catalytic system. In addition, a probable mechanism has been proposed to explain this result that structure of molecular sieves was the main factor of influencing catalytic performance.
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