Shanghai Research Institute of Petrochemical Technology SINOPEC, Shanghai 201208, China.
Department of Chemistry, Fudan University, Shanghai, 200233, China.
Sci Rep. 2016 Jul 5;6:28898. doi: 10.1038/srep28898.
Hydrogenation of levulinic acid (LA) and its esters to produce γ-valerolactone (GVL) and 2-methyl tetrahydrofuran (2-MTHF) is a key step for the utilization of cellulose derived LA. Aiming to develop a commercially feasible base metal catalyst for the production of GVL from LA, with satisfactory activity, selectivity, and stability, Al2O3 doped Cu/SiO2 and Cu/SiO2 catalysts were fabricated by co-precipitation routes in parallel. The diverse physio-chemical properties of these two catalysts were characterized by XRD, TEM, dissociative N2O chemisorptions, and Py-IR methods. The catalytic properties of these two catalysts were systematically assessed in the continuous hydrogenation of ethyl levulinate (EL) in a fixed-bed reactor. The effect of acidic property of the SiO2 substrate on the catalytic properties was investigated. To justify the potential of its commercialization, significant attention was paid on the initial activity, proper operation window, by-products control, selectivity, and stability of the catalyst. The effect of reaction conditions, such as temperature and pressure, on the performance of the catalyst was also thoroughly studied. The development of alumina doped Cu/SiO2 catalyst strengthened the value-chain from cellulose to industrially important chemicals via LA and GVL.
将戊二酸(LA)及其酯加氢转化为γ-戊内酯(GVL)和 2-甲基四氢呋喃(2-MTHF)是利用纤维素衍生的 LA 的关键步骤。为了开发一种用于从 LA 生产 GVL 的商业可行的基础金属催化剂,具有令人满意的活性、选择性和稳定性,采用共沉淀法平行制备了 Al2O3 掺杂的 Cu/SiO2 和 Cu/SiO2 催化剂。通过 XRD、TEM、解离 N2O 吸附和 Py-IR 方法对这两种催化剂的不同物理化学性质进行了表征。在固定床反应器中连续加氢乙基戊酸酯(EL),系统评估了这两种催化剂的催化性能。考察了 SiO2 载体的酸性对催化性能的影响。为了证明其商业化的潜力,我们还特别关注催化剂的初始活性、合适的操作窗口、副产物控制、选择性和稳定性。还深入研究了反应条件(如温度和压力)对催化剂性能的影响。氧化铝掺杂 Cu/SiO2 催化剂的开发加强了从纤维素到工业重要化学品的价值链,途经 LA 和 GVL。