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Hydrogenolysis of Aryl Ether Bond over Heterogeneous Cobalt-Based Catalyst
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-06-15 , DOI: 10.1021/acs.iecr.0c01374 Lijie Zhang 1 , Yongzhao Wang 2 , Li Zhang 1 , Zixin Chi 1 , Yanling Yang 1 , Zhaoxia Zhang 1 , Bingsen Zhang 2 , Jingdong Lin 1 , Shaolong Wan 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-06-15 , DOI: 10.1021/acs.iecr.0c01374 Lijie Zhang 1 , Yongzhao Wang 2 , Li Zhang 1 , Zixin Chi 1 , Yanling Yang 1 , Zhaoxia Zhang 1 , Bingsen Zhang 2 , Jingdong Lin 1 , Shaolong Wan 1
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The development of efficient non-noble metal catalysts is of critical importance for conversion of lignin toward value-added chemicals. The trans-metal Co catalysts and the counterparts promoted with a small amount of Ru were found highly selective for hydrogenolysis of lignin-derived aromatic ethers in decalin at relatively mild conditions. The physical and chemical properties of the as-prepared catalysts were fully investigated by various characterization methods, and Co species was found well dispersed in the reduced catalysts. The experimental results showed that Co/CeO2 could selectively cleave the C–O bonds of diphenyl ether (DPE) to produce benzene and phenol, which can be further converted to cyclohexane and cyclohexanol. Upon 5Co/CeO2, 97% selectivity to those C–O bond ruptured products was achieved, while the direct hydrogenation products including dicyclohexyl ether and cyclohexyl account for only 3%. Moreover, benzene, featured as a typical intermediate product, could reach a maximum yield of 27.4% at around 80% conversion. The addition of a small amount of Ru (0.1 wt % and below) could significantly accelerate the hydrogenolysis reactivity but also result in the declined selectivity of benzene during the reaction due to the stronger hydrogenation ability.
中文翻译：
多相钴基催化剂上芳醚键的氢解
高效非贵金属催化剂的开发对于木质素向增值化学品的转化至关重要。发现在相对温和的条件下，对十氢化萘中木质素衍生的芳族醚的氢解具有很高的选择性，而该过渡金属Co催化剂和少量Ru促进了该催化剂。通过各种表征方法充分研究了所制备催化剂的物理和化学性质，发现Co物种很好地分散在还原的催化剂中。实验结果表明，Co / CeO 2可以选择性地裂解二苯醚（DPE）的C–O键产生苯和苯酚，可以进一步将其转化为环己烷和环己醇。基于5Co / CeO 2，对那些C–O键断裂的产物具有97％的选择性，而直接氢化的产物（包括二环己基醚和环己基）仅占3％。此外，苯是典型的中间产品，在约80％的转化率下，最高收率可达27.4％。少量Ru（0.1wt％及以下）的添加可显着加速氢解反应性，但由于较强的氢化能力，还导致反应期间苯的选择性下降。
更新日期：2020-06-15
中文翻译：
多相钴基催化剂上芳醚键的氢解
高效非贵金属催化剂的开发对于木质素向增值化学品的转化至关重要。发现在相对温和的条件下，对十氢化萘中木质素衍生的芳族醚的氢解具有很高的选择性，而该过渡金属Co催化剂和少量Ru促进了该催化剂。通过各种表征方法充分研究了所制备催化剂的物理和化学性质，发现Co物种很好地分散在还原的催化剂中。实验结果表明，Co / CeO 2可以选择性地裂解二苯醚（DPE）的C–O键产生苯和苯酚，可以进一步将其转化为环己烷和环己醇。基于5Co / CeO 2，对那些C–O键断裂的产物具有97％的选择性，而直接氢化的产物（包括二环己基醚和环己基）仅占3％。此外，苯是典型的中间产品，在约80％的转化率下，最高收率可达27.4％。少量Ru（0.1wt％及以下）的添加可显着加速氢解反应性，但由于较强的氢化能力，还导致反应期间苯的选择性下降。
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