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机构地区:[1]浙江大学生物质化工教育部重点实验室,浙江大学化学工程与生物工程学院,浙江杭州310027 [2]浙江工业大学药学院,浙江杭州310014
出 处:《高校化学工程学报》2016年第2期391-397,共7页Journal of Chemical Engineering of Chinese Universities
基 金:国家自然科学基金(21106134,21276230,21476211);浙江省自然科学基金(LY14B060003);浙江省重点科技创新团队(2011R50002)
摘 要:为了解决镍基催化剂在酸性环境下易被酸腐蚀的问题,分别以金属Fe、Mn和Mo作为助剂,以经Na BH4处理的活性炭作为疏水性载体,采用等体积浸渍法制备了一系列镍基催化剂,并将其应用于苯酐、乙酰丙酸、丁烯二酸酐、丁二酸酐和偏苯三酸酐等酸性介质的加氢反应中,以研究金属助剂和疏水性载体对镍基催化剂抗酸性能和催化性能的影响。结果表明,与Raney Ni相比,Fe和Ni含量分别为5%(wt)和15%(wt)、疏水性活性炭负载的催化剂(5Fe-15Ni/AC-Na BH4)具有非常突出的催化活性和抗酸稳定性,在酸性反应环境中重复使用多次仍表现了很好的催化性能。这归因于载体的疏水表面能够阻止产生的水与催化剂表面的接触,使金属活性中心氢离子的活度降低,从而减少了金属镍的腐蚀。此外,XRD和TEM表征结果证明催化剂中形成了Fe-Ni合金,这有利于Ni在载体表面的分散,也有效地延缓了催化剂的失活。In order to improve activity and acid-resistance of hydrogenation catalysts, a series of nickel-based catalysts doped with Fe, Mn, Mo and supported by Na BH4-reduced activated carbon(AC-Na BH4) were prepared via an incipient wetness method. They were applied for the hydrogenation of phthalic anhydride, levulinic acid, maleic anhydride, succinic anhydride and trimellitic anhydride. The results show that the Fe doped catalyst containing 5%(wt) Fe and 15%(wt) Ni(5Fe-15Ni/AC-Na BH4) has satisfactory activity and stability, which can be attributed to the hydrophobic surface of AC-Na BH4 that prevents the resulted water from contacting metal surface. This makes the decrease of H+ concentration which eventually reduces Ni corrosion. Furthermore, XRD and TEM analysis prove the formation of Fe-Ni alloy, which is beneficial to the disperse of nickel particles and can effectively inhibit nickel corrosion.
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