Synthesis of Robust MOF-Derived Cu/SiO2 Catalyst with Low Copper Loading via Sol–Gel Method for the Dimethyl Oxalate Hydrogenation Reaction,ACS Catalysis

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Synthesis of Robust MOF-Derived Cu/SiO2 Catalyst with Low Copper Loading via Sol–Gel Method for the Dimethyl Oxalate Hydrogenation Reaction
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-03-13 00:00:00 , DOI: 10.1021/acscatal.8b00501
Run-Ping Ye _{1,

2,

3} , Ling Lin ₁ , Chong-Chong Chen _{1,

2} , Jin-Xia Yang ₁ , Fei Li _{1,

2} , Xin Zhang ₁ , De-Jing Li _{1,

4} , Ye-Yan Qin ₁ , Zhangfeng Zhou ₁ , Yuan-Gen Yao ₁

Affiliation

The insufficient catalytic stability of Cu-based catalysts is still its bottleneck in industrial application, and it is widely studied how to synthesize highly stable Cu-based catalysts. Herein, we have developed a MOF-derived preparation of robust Cu/SiO₂ catalyst for the efficient hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG). The sol–gel method was used to in situ load the HKUST-1 into SiO₂ support with only a copper loading of 7.83%. The advantages of MOF-derived Cu/SiO₂ catalyst are that copper species could escape from severe coating by silica matrix and expose more active sites with small particles sizes (4.2 nm). Furthermore, it is inclined to generate more stable Cu₂O reduced from Cu–O–Si units by using MOF as precursor. As a result, more than 95.0% selectivity of EG with a long lifetime of 220 h was achieved over the Cu/SiO₂-MOF catalyst. On the contrary, when using the copper nitrate as the copper precursor, the prepared Cu/SiO₂-CN catalyst with similar copper loading exhibited much lower catalytic activity because that copper species were encapsulated into SiO₂ network and difficult to be available for reactants. Therefore, using MOF as copper precursor solves the problem of high-dispersed copper species but inactive by coating with SiO₂ matrix.

中文翻译：

溶胶-凝胶法合成草酸低MOF衍生的稳健的Cu / SiO ₂催化剂用于草酸二甲酯加氢反应

铜基催化剂的催化稳定性不足仍是工业应用中的瓶颈，如何合成高稳定性的铜基催化剂已被广泛研究。在这里，我们已经开发了MOF衍生的坚固的Cu / SiO ₂催化剂，用于将草酸二甲酯（DMO）有效氢化为乙二醇（EG）。溶胶-凝胶法用于将HKUST-1原位负载在SiO ₂载体上，铜负载量仅为7.83％。MOF衍生的Cu / SiO ₂催化剂的优势在于，铜物种可能会从二氧化硅基质的严重涂层中逸出，并暴露出具有较小粒径（4.2 nm）的更多活性位。此外，倾向于产生更稳定的Cu _2。通过使用MOF作为前体，将O从Cu–O–Si单元中还原。结果，与Cu / SiO ₂ -MOF催化剂相比，具有超过220小时的长寿命的EG的选择性超过95.0％。相反，当使用硝酸铜作为铜前体时，制得的具有相似铜负载量的Cu / SiO ₂ -CN催化剂显示出低得多的催化活性，因为铜物质被包封在SiO ₂网络中并且难以用作反应物。因此，使用MOF作为铜前驱物解决了铜物种高度分散但通过涂覆SiO ₂基体而失活的问题。

更新日期：2018-03-13

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