pH值调控构建的纳米Ni-W催化剂用于纤维素氢解制多元醇的研究（英文）  

Preparation of nano-scale nickel-tungsten catalysts by pH value control and applicati on in hydrogenolysis of cellulose to polyols

作　　者：肖竹钱 毛建卫[1,2] 计建炳[3] 沙如意[1,2] 范煜[1,2] 邢闯[1,2] XIAO Zhu-qian MAO Jian-wei JI Jian-bing SHA Ru-yi FAN Yu XING Chuang(Zhejiang Provincial Collaborative Innovation Center of Agricultural Biological Resources Biochemical Manufacturing, Hangzhou 310023, China Zhejiang Provincial Key Laboratory of Chemical and Biological Processing Technology of Farm Products, Hangzhou 310023, China College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China)

机构地区：[1]浙江省农业生物资源生化制造协同创新中心,浙江杭州310023 [2]浙江省农产品化学与生物加工技术重点实验室,浙江杭州310023 [3]浙江工业大学化学工程学院,浙江杭州310014

出　　处：《燃料化学学报》2017年第6期641-650,共10页Journal of Fuel Chemistry and Technology

基　　金：supported by Scientific Research Project of Zhejiang Provincial Collaborative Innovation Center of Agricultural Biological Resources Biochemical Manufacturing(2016KF0035);Science and Technology Project of Zhejiang Province(2017C37049)~~

摘　　要：采用等体积浸渍法制备了双金属Ni-W催化剂,并研究了制备过程中前驱体溶液pH值对活性的影响。柠檬酸和氢氧化钾分别作为酸碱调节剂将前驱体溶液pH值调节至0.83、1.00、3.09、5.00、7.03、8.97和11.0。纤维素氢解反应结果表明,当前驱体溶液的pH值为1.00时,在氢压为5.0 MPa、温度为518 K的反应条件下,得到低碳(C_(2,3))多元醇的总收率为74.5%。此外,通过BET和SEM表征了催化剂的物理性质。其比表面积为330-450 m2/g,且在高温煅烧下SBA-15仍保持良好的水热稳定性。TEM和SEM-EDX结果显示,催化剂粒子在载体表面分散性较好,但也有少量的聚集现象。XRD表征表明,NiO等物种的还原程度明显受到pH值的影响,且镍、钨物种的相态也存在着显著不同。The Ni-W/SBA-15 catalysts prepared by incipient-wetness impregnation method and controlled by the pH value were developed. Potassium hydroxide and citric acid regarded as the pH value regulators were added to the solution before impregnation to provide an acidic or basic condition at different pH values （0. 83, 1.00, 3.09, 5.00, 7.03, 8.97 and 11.0）. The 74. 5% yield of total low carbon （C. 3） polyols including ethylene glycol （EG） , 1,2-propylene glycol （1,2-PG） and glycerol （Gly） was obtained over 10%Ni-20%W/SBA-15 catalyst prepared at pH value of 1. 00 and 518 K under H2 pressure of 5. 0 MPa. Furthermore, the physical properties of this series of nickel-tungsten catalysts were characterized by BET and SEM. The results demonstrated that the catalysts showed excellent thermal stability and the surface area was mainly in range of 330-450 m^2 /g . The particles had a good dispersion on the surface of SBA-15 but some aggregations were existed which could be characterized by TEM and SEM-EDX. However, the reduction of metallic oxides especially for NiO was obviously influenced by pH value control and some metallic species characterized by XRD. According to XRD results, the impregnation pH value influenced the reduction of NiO and the phase states of nickel and tungsten species.

关 键 词：纤维素 氢解 pH值调控 镍-钨催化剂 多元醇 

分 类 号：TQ352.1[化学工程]