新型钌和钴配合物的制备及其光解水制氢的分析-preparation of new ruthenium and cobalt complexes and analysis of hydrogen production by photolysis of water.docx

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2018-06-03 发布于上海
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新型钌和钴配合物的制备及其光解水制氢的分析-preparation of new ruthenium and cobalt complexes and analysis of hydrogen production by photolysis of water.docx

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新型钌和钴配合物的制备及其光解水制氢的分析-preparation of new ruthenium and cobalt complexes and analysis of hydrogen production by photolysis of water

AbstractAbstractVisiblelight-drivenwatersplittingintohydrogenasacleanandsustainablehydrogenproductionmethodhasattractedmoreandmoreattentionsofscientists.Inthisarticle,webuilttwophotocatalytichydrogenproductionsystem:basedonthebipyridinerutheniumcomplexessensitizedtitaniumdioxideheterogeneousphotocatalytichydrogenproductionsystemandacobalt-basedcatalysthomogeneousphotocatalytichydrogenproductionsystem.Twobipyridinerutheniumcomplexes(PS1,PS2)weresynthesizedandcharacterizedbyMS,elementalanalysis,IR,NMR,UV-visiblespectrumandcyclicvoltammogram.TwobipyridinerutheniumcomplexesweresensitizedonPt-TiO2ascompositephotosensitivecatalysttobuildheterogeneousphotocatalytichydrogenproductionsysteminwater,ascorbicacidusedasanelectrondonor.Undertheoptimalcondition,itshowedthatthemaximumcumulativehydrogenproductionwas375.8μmolandthemaximumrateofhydrogenevolutionwas11903.3μmol/g/hover5hirradiationinthewatersystemwithPS1(20mg)sensitizedonPt-TiO2ascompositephotosensitivecatalyst,ascorbicacid(1.0g)assacrificialelectrondonor,pH=5.3.Thecycleexperimentshowedthelong-termstabilityofthecompositephotosensitivecatalyst.ThereasonofreactionsystemdeactivationspeculatedthatphotosensitiverutheniumcomplexdyedesorptionfromthesurfaceofTiO2.Threecobalt-basedphotocatalyst(C1,C2,C3)weresynthesizedandcharacterizedbyIR,NMR,singlecrystaldiffraction,UV-visiblespectroscopyandcyclicvoltammetry.Thecobaltcomplex(C1,C2,C3)wereusedasphoto-catalysttobuildphotocatalyticH2productionhomogeneoussystemwithEosinYdye(EY2-)asthephotosensitizer,TEAorTEOAaselectrondonor,acetonitrile/watermixedsolventassolvent.Undertheoptimalcondition([Cat.]2×10-5M、EY2-1×10-4M、10%TEA，v/v、pH=10.0、MeCN/H2O=1:1,v/v),itshowedthatthemaximumamountofH2generatedforthecobaltcomplexC1was352TON(vs.catalyst)after3hoursirradiationofvisiblelight.Keywords:rutheniumcomplexes;dye-sensitizedTiO2;cobaltcatalyst;photocatalytichydrogenproductionII目录目录摘要...................................................................................................................