摘要
分别采用化学镀法和浸渍法制备Ni_(3)P/SiO_(2)和Ni/SiO_(2)催化剂,并将其与介质阻挡放电等离子体协同催化甲烷干重整制合成气(H_(2)+CO)反应。对所制备的催化剂进行X射线粉末衍射、X射线光电能谱、N_(2)物理吸附-脱附和CO_(2)程序升温脱附表征和催化甲烷干重整性能评价。相较于Ni/SiO_(2),Ni_(3)P/SiO_(2)具有更大的比表面积和更多缺电子态的Ni^(δ+)位点,以及对CO_(2)较强的吸附能力。催化性能评价结果表明,当等离子体输出功率20 W时,Ni_(3)P/SiO_(2)具有比Ni/SiO_(2)更优的甲烷干重整催化活性和稳定性,这可能是Ni_(3)P/SiO_(2)表面较多的Ni^(δ+)位点促进了反应物分子的吸附活化。对Ni_(3)P/SiO_(2)催化剂制备条件和反应条件考察结果表明,Ni负载质量分数为15%的催化剂前体在400℃下H_(2)气氛中还原2 h所得的Ni_(3)P/SiO_(2)性能最优。该催化剂在等离子体输出功率20 W、进料气体积空速15000 mL/(gcat·h)、CO_(2)/CH_(4)体积比为1的最佳反应条件下,CH_(4)和CO_(2)转化率分别为70.9%、62.5%,H_(2)和CO选择性分别为76%、87%,能量利用率为4.46 mmol/kJ。
Ni_(3)P/SiO_(2)and Ni/SiO_(2)catalysts were prepared by the eletroless plating method and impregnation method respectively,and were used in the synergistic catalysis for dry reforming of methane to synthesis gas(H_(2)+CO)reaction aided by a dielectric barrier discharge plasma.The prepared catalysts were characterized by means of X-ray powder diffraction,X-ray photoelectron spectroscopy,N_(2)-physisorption and CO_(2)-temperature-programmed desorption,as well as the performance evaluation of catalytic methane dry reforming.Compared with Ni/SiO_(2),Ni_(3)P/SiO_(2)has a larger specific surface area,more electron-deficient Ni^(δ+)sites,and stronger adsorption capacity for CO_(2).The evaluation of catalytic performance shows that at the plasma output power of 20 W,Ni_(3)P/SiO_(2)has better catalytic activity and stability for methane dry reforming than Ni/SiO_(2),probably because there are more Ni^(δ+)sites on the surface of Ni_(3)P/SiO_(2),which can promote the adsorption and activation properties of reactant molecules.The preparation and reaction conditions of Ni_(3)P/SiO_(2)catalyst are investigated.The results show that using catalyst precursor with the Ni loading of 15%(mass fraction),Ni_(3)P/SiO_(2)prepared by reduction under 400℃in H_(2)atmosphere for 2 hours has the highest performance.Under the optimal reaction conditions:plasma discharge power of 20 W,feed gas space velocity of 15000 mL/(g cat·h),and V CO_(2)/V CH_(4)=1,the conversions of CH_(4)and CO_(2)are 70.9%and 62.5%,and the selectivities to H_(2)and CO are 76%and 87%,respectively;the energy efficiency is 4.46 mmol/kJ.
作者
王荣
徐波
郑兆宇
王安杰
刘颖雅
孙志超
王瑶
WANG Rong;XU Bo;ZHENG Zhaoyu;WANG Anjie;LIU Yingya;SUN Zhichao;WANG Yao(State Key Laboratory of Fine Chemical Engineering,Dalian University of Technology,Dalian 116024,China)
出处
《石油学报（石油加工）》
EI
CAS
CSCD
北大核心
2023年第5期1033-1045,共13页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家自然科学基金项目(21972014,22172015)资助。
作者简介
第一作者:王荣,女,硕士研究生,从事等离子体催化研究,Tel:0411-84986015,E-mail:2640075557@qq.com;通讯联系人:王瑶,女,教授,博士,从事反应过程强化研究,Tel:0411-84986015,E-mail:wangyao@dlut.edu.cn。
