石墨烯催化苯醌加氢制备氢醌.pdf

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1、2015年9月化学研究460第26卷第5期CHEMICALRESEARCHhttp：／／hxya．cbpt．cnki．net钯／石墨烯催化苯醌加氢制备氢醌杨敬贺，郁清涛，毛立群(河南大学化学化工学院，河南开封475004)摘要：采用微波辅助加热还原法合成了钯／石墨烯(Pd／G)、钯／活性炭(Pd／AC)、钯／石墨(Pd／Graphite)和钯／二氧化硅(Pd／SiO)，并使用透射电子显微镜观测了钯的形貌及在载体上的分散性．将负载型钯催化剂用于苯醌加氢反应，结果显示，Pd／G催化剂的活性最高，苯醌的转

2、化率达到99，氢醌的选择性为100，并且循环7次后催化剂仍保持着较高的转化率和选择性。结构表征表明，石墨烯担载的钯纳米粒子的粒径约为5nm，无明显团聚．实验进一步考察了反应溶剂(甲醇、乙醇、丙酮、正丙醇、异丙醇、正丁醇)对Pd／G催化苯醌加氢反应的影响，结果表明该反应对溶剂较为敏感，其中甲醇和丙酮较适宜作为反应溶剂．当以甲醇作为溶剂时，苯醌的转化率为98，氢醌选择性为99；以丙酮为溶剂时，苯醌转化率为98，氢醌选择性为9O．研究工作表明，作为载体，石墨烯对钯催化剂的催化效果起着稳定和增强作用．关键词

3、：钯纳米粒子；石墨烯；苯醌加氢；氢醌中图分类号：O625．3文献标志码：A文章编号：1008—1011(2015)05—0460—04Pd／Graphenecatalytichydrogenationofbenzoquinonet0hydr0quin0neYANGJinghe，YUQingtao，MAOLiqun(CollegeofChemistryandChemicalEngineering，HenanUniversity，Kaireng475004，Henan，China)Abstract：In

4、thepresentstudy，weexploitedGasasupportforpalladiumnanoparticlesbymi—crowaveassistedreductionofpalladiumacetatewithgrapheneunderhydrogenatmosphere．Inthesamemethod，wealsoemployedgraphite，activecarbonandsilicaascarrierforsynthesispalladiumgraphite(Pd／Grap

5、hite)，palladiumactivecarbon(Pd／AC)andpalladiumsilica(Pd／SiO2)．Thehydrogenationofbenzoquinonereactionhasbeenselectedasmodelreactionfore—valuatingG—basedpalladiumcatalysts(Pd／G)，andthemorphologyanddispersionofpalla—diumonthecarrierwereobservedbyTEM．Weuti

6、lizedthesupportedpalladiumcatalystsforbenzoquinonehydrogenationreaction．TheresultsimplythatthePd／Gcatalystshowsthehigh—estactivity．Theconversionofbenzoquinonereached999／6andtheselectivitytohydroquinonewas100．Inaddtion，thecatalyticperformanceofPd／Gcatal

7、ystremainedhighevenaftersevenreactioncycles．Structuralcharacterizationindicatespalladiumnanoparticleswithanaver—agesizeof5nmwereuniformlydistributedontheGsupportandtheydidn’tshowobviousag—gregation．Thestudyalsofoundthatthespeciesofsolvent(methanol，etha

8、nol，acetone，n—pro—panol，isopropanol，咒一butano1)hadagreatinfluenceoncatalytichydrogenationofbenzoqui—noneusingPd／Gascatalysts．Methanolandacetonewassuitablesolventforthisreaction．Whenusingmethanolassolvent，theconversionandselectivitywere98