3D多级孔炭负载铜催化剂及其合成碳酸二甲酯性能研究

Study on 3D-interconnected hierarchical porous carbon supported Cu catalyst and its properties in dimethyl carbonate synthesis

以ɑ-纤维素和NaHCO3为原料,采用生物质发泡法制得大孔、介孔和微孔共存的三维(3D)多级孔炭(HPC);以硝酸铜为铜源,通过调变铜负载量制得3D多级孔炭负载铜催化剂(y Cu/HPC),并考察其催化甲醇氧化羰基化合成碳酸二甲酯性能。实验结果表明:当铜负载量(质量分数)为10%时,10Cu/HPC催化剂在DMC合成反应中时空收率(STYDMC)和转换频率(TOF)分别达1778 mg/(g·h)和13.8 s^(-1)。N2吸附、XRD、TEM等表征表明:3D多级孔结构不但有利于铜物种的高度分散,同时可加快底物分子的传质速率,从而提升催化活性。

Usingɑ-cellulose and NaHCO3 as raw materials,three-dimensional(3D)-interconnected hierarchical porous carbon(HPC)with macroporous,mesoporous and microporous coexistence was obtained by the biomass foaming method.Then copper nitrate was used as the copper source,a three-dimensional(3D)-interconnected hierarchical porous carbon(HPC)supported Cu catalyst(yCu/HPC)was prepared by adjusting the copper loading amount,and its catalytic performance for methanol oxidative carbonylation was investigated.The experimental results showed that when the copper load(mass fraction)was 10%,the space-time yield(STYDMC)and conversion frequency(TOF)of 10Cu/HPC catalyst in the synthesis reaction of dimethyl carbonate(DMC)reached 1778 mg/(g·h)and 13.8 s^(-1)respectively.N2 adsorption,XRD,TEM and other characterizations showed that the 3D-interconnected hierarchical porous carbon was not only conducive to the high dispersion of copper species,but also accelerated the mass transfer rate of substrate molecules,thus improving the catalytic activity.