The Reactivity and Deactivation Mechanism of Ru@C Catalyst over Hydrogenation of Aromatics to Cyclohexane Derivatives
The Reactivity and Deactivation Mechanism of Ru@C Catalyst over Hydrogenation of Aromatics to Cyclohexane Derivatives
复制标题
Ru@C催化剂芳烃加氢制环己烷衍生物的反应活性及失活机理
DOI：
10.1002/slct.202000311
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发表时间：
2020-04
期刊：
影响因子：
2.1
通讯作者：
Lingjun Chou
中科院分区：
文献类型：
--
作者：
Huahua Zhao;Huanling Song;Jun Zhao;Jian Yang;Liang Yan;Lingjun Chou
报道了具有不同Ru纳米颗粒尺寸的碳载纳米Ru催化剂用于芳烃（邻苯二甲酸二辛酯、二甲苯、对苯二胺、肉桂酸和硝基苯）加氢制备相应的附加值环己烷衍生物。与乙二醇还原法和浸渍法制备的Ru@ C-EG和Ru@C-IM相比，采用简单沉积-沉淀法制备的Ru@C-DP具有更小的Ru纳米颗粒（NP）（2.0 nm）、更高的Ru分散度（60.2%）和更大的Ru比表面积（220.1 m2·gRu−1）。 Ru@C-DP具有优异的活性，芳香族转化率≥ 99%，环己烷衍生物选择性≥ 99%，这归因于其较小的Ru NP尺寸，表明存在尺寸依赖性效应。此外，与工业Ru@C-ID催化剂相比，Ru@C-DP在芳烃加氢反应中表现出显著的重复使用性能。催化剂经过多次加氢循环后，由于反应物/产物分子堵塞孔道、部分氧化和Ru纳米粒子聚集等原因，催化剂失去了一定的活性。
Nano Ru supported on carbon catalysts with different Ru nanoparticle sizes were reported for the aromatics (dioctyl phthalate, xylene,p‐phenylenediamine, cinnamic acid and nitrobenzene) hydrogenation to the corresponding value‐added cyclohexane derivatives. Ru@C–DP prepared by facile deposition‐precipitation strategy, exhibited the smaller Ru nanoparticle (NP) size 2.0 nm, higher Ru dispersion degree (60.2%) and larger Ru specific surface area (220.1 m2⋅gRu−1) than Ru@C‐EG and Ru@C–IM synthesized with ethylene glycol reduction and impregnation method, respectively. Ru@C–DP possessed excellent activity with aromatic conversion ≥ 99% and cyclohexane derivative selectivity ≥ 99%, which was attributed to its smaller Ru NP size, suggesting the presence of a size‐dependent effect. Moreover, compared with the commercial Ru@C–ID catalyst, Ru@C–DP showed remarkable reusability in aromatic hydrogenation. After the several hydrogenation recycles, the catalyst lost some activity mainly account for the pore blocking by reactant/product molecules, part oxidation and aggregation of Ru NPs.
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