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1、DOI:10.1002/cctc.201000126TheMechanismofWaterOxidation:FromElectrolysisviaHomogeneoustoBiologicalCatalysis[a][b][c][a][b]HolgerDau,*ChristianLimberg,*TobiasReier,MarcelRisch,StefanRoggan,and[c]PeterStrasser*7242010Wiley-VCHVerlagGmbH&Co.KGaA,WeinheimChem
2、CatChem2010,2,724–761Strivingfornewsolarfuels,thewateroxidationreactioncur-catalyticmanganese–calciumcomplexofphotosyntheticwaterrentlyisconsideredtobeabottleneck,hamperingprogressinoxidation.Recentdevelopmentsinhomogeneouswater-oxida-thedevelopmentofappl
3、icabletechnologiesfortheconversiontioncatalysisareoutlinedwithafocusonthediscoveryofoflightintostorablefuels.Thisreviewcomparesandunifiesmononuclearruthenium(andnon-ruthenium)complexesthatviewpointsonwateroxidationfromvariousfieldsofcatalysisefficientlyme
4、diateO2evolutionfromwater.Wateroxidationinresearch.Thefirstpartdealswiththethermodynamicefficien-photosynthesisisthesubjectofaconcisepresentationofcyandmechanismsofelectrochemicalwatersplittingbymetalstructureandfunctionofthenaturalparagon—themanga-oxides
5、onelectrodesurfaces,explainingtherecentconceptofnese–calciumcomplexinphotosystemII—forwhichideascon-thepotential-determiningstep.Subsequently,novelcobaltcerningredox-potentialleveling,protonremoval,andOOoxide-basedcatalystsforheterogeneous(electro)cataly
6、sisarebondformationmechanismsarediscussed.Thelastparthigh-discussed.Thesemaysharestructuralandfunctionalpropertieslightscommonthemesandunifyingconcepts.withsurfaceoxides,multinuclearmolecularcatalystsandtheIntroductiontensified,asitcanserveasanimportantin
7、spirationandbenchmarkforthedevelopmentofartificialwater-oxidationInrecentyears,theincreasedinterestindirectconversionofcatalysts.solarenergyintostorablefuelshasledtointensifiedresearchHereinwewilldiscussandcompareconceptsandrecent[1]effortswithrespecttoar
8、tificialphotosynthesis.Asuccessfulfindingonthemechanismofwateroxidationobtainedintheimitationofthenaturalenergy-storingprocessrequiresthefollowingseparateresearchcommunities:combinationofseveraldistinctprocesses,inc