Pd nanoparticles immobilized on MIL-53(Al) as highly effective bifunctional catalysts for oxidation of liquid methanol to methyl formate

Pd nanoparticles immobilized on MIL-53(Al) as highly effective bifunctional catalysts for oxidation of liquid methanol to methyl formate
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DOI:
10.1007/s12182-019-0334-6
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发表时间:
2019-08
期刊:
影响因子:
5.6
通讯作者:
Jianfang Liu;J. Mu;Rong Qin;Sheng-fu Ji
Jianfang Liu;J. Mu;Rong Qin;Sheng-fu Ji
中科院分区:
工程技术2区
文献类型:
--
作者:
Jianfang Liu;J. Mu;Rong Qin;Sheng-fu Ji

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采用浸渍法制备了不同Pd含量的Pd/MIL-53(Al)多相双功能催化剂。采用XRD、SEM、HRTEM、FT-IR和n2吸附/脱附技术对MIL-53(Al)及其催化剂进行了表征。结果表明,MIL-53(Al)成功合成,催化剂制备过程中及制备后结构基本不变。平均粒径为4.6 nm的钯纳米粒子(NPs)均匀分散在MIL-53(Al)上。该催化剂对液态甲醇选择性氧化制甲酸甲酯具有良好的催化活性。在150℃、2 MPa o2、无溶剂反应5 h的条件下,甲醇的转化率可达60.3%,甲酸甲酯的选择性可达62.2%。此外,Pd/MIL-53(Al)双功能催化剂表现出优异的稳定性,在5个循环后仍保持较高的催化活性。
A series of Pd/MIL-53(Al) heterogeneous bifunctional catalysts with different Pd contents were prepared by an impregnation method. The prepared metal–organic frameworks MIL-53(Al) and catalysts were characterized by XRD, SEM, HRTEM, FT-IR and N2adsorption/desorption techniques. The results showed that MIL-53(Al) was synthesized successfully, and the structure was unchanged during and after the preparation of the catalysts. The Pd nanoparticles (NPs) with an average particle size of 4.6 nm were uniformly dispersed on the MIL-53(Al). The catalyst exhibited good catalytic activity in the selective oxidation of liquid methanol to methyl formate. Under the conditions of 150 °C, 2 MPa O2and solvent-free for 5 h, the conversion of methanol could reach 60.3%, and the selectivity of methyl formate was up to 62.2%. In addition, the Pd/MIL-53(Al) bifunctional catalyst exhibited excellent stability and maintained high catalytic activity after five cycles.