沉淀沉积法制备活性炭负载铜基催化剂及其氧化羰基化

Preparation and oxycarbonylation of activated carbon supported copper-based catalyst by deposition-precipitation method

摘要: 采用沉淀沉积法制备了活性炭负载的铜基催化剂,并用其催化甲醇直接气相氧化羰基化合成碳酸二甲酯(DMC)。通过催化活性评价以及XRD、H₂-TPR、SEM等表征考察了铜源、还原剂、沉淀剂、铜负载量等制备条件对催化剂性能的影响。结果表明,采用醋酸铜作为铜源、葡萄糖作为还原剂、负载量为17.1%时制备的Cu₂O/AC催化剂合成DMC活性最佳,在MeOH/CO/O₂体积比=5:11:1、SV=6 625 h^-1的条件下,催化剂最高时空收率可达99.36 mg/(g·h), DMC的选择性为83.13%。

Abstract: The activated carbon supported copper-based catalyst was prepared by deposition-precipitation method and used to catalyze the direct vapor-phase oxycarbonylation of methanol to dimethyl carbonate (DMC). The effect of preparation conditions(such as copper salt, reductant, precipitant and loading amount ect) on the catalytic performance were investigated by XRD, H₂-TPR and SEM techniques. The result showed that under the condition of MeOH/CO/O₂(volume ratio)=5:11:1, SV=6 625 h^-1, Cu₂O /AC catalyst (Cu(CH₃COO)₂·H₂O as precursor, glucose as reductant, Cu₂O loading amount of 17.1%) showed satisfactory catalytic performance for DMC synthesis. The STY reached 99.36 mg/(g·h) and the selectivity of DMC was about 83.13%.