Phillips Erin V, Tricker Andrew W, Stavitski Eli, Hatzell Marta, Sievers Carsten
School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States.
Independent Researcher, Washington, D.C. 20009, United States.
ACS Sustain Chem Eng. 2024 Aug 5;12(33):12306-12312. doi: 10.1021/acssuschemeng.4c03590. eCollection 2024 Aug 19.
This work demonstrates the mechanocatalytic hydrogenolysis of the ether bond in the lignin model compound benzyl phenyl ether (BPE) and hardwood lignin isolated by hydrolysis with supercritical water. Pd catalysts with 4 wt % loading on AlO and SiO supports achieve 100% conversion of BPE with a toluene production rate of (2.6-2.9) × 10 mol·min. The formation of palladium hydrides under H gas flow contributes to an increase in the turnover frequency by a factor of up to 300 compared to Ni on silica-alumina. While a near-quantitative toluene yield is obtained, some of the phenolic products remain adsorbed on the catalyst.
这项工作展示了木质素模型化合物苄基苯基醚(BPE)中醚键的机械催化氢解以及通过超临界水水解分离得到的阔叶木木质素。负载量为4 wt%的Pd催化剂负载在AlO和SiO载体上,可实现BPE的100%转化,甲苯生成速率为(2.6 - 2.9)×10 mol·min。在氢气气流下形成的氢化钯相比于二氧化硅 - 氧化铝上的镍,使周转频率提高了高达300倍。虽然获得了近乎定量的甲苯产率,但一些酚类产物仍吸附在催化剂上。