有机小分子在纳米氢氧化镍膜电极上催化氧化的非线性动力学行为分析

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1、STUDlESOFNONLINEARKINETICBEHAVlORSINTHEELECTROCATALYTlC0XlDAT10NOFSMALLORGANICMOLECULESONNANO—STRUCTUREDNICKELHYDROXIDEFILM(NNHF)ELECTRODEABSTRACTElectrochemicaloscillations，aspatiotemporalphenomenonunderconditionsofkeepingfarawayfromequilibrium，havebeenobservedinanumberofelect

2、rochemicalprocesses，includingelectrodissolutionofmetals，electrodepositionofmetals，electrocatalyticoxidationofsmallorganicmolecules，andSOon．Theprofoundstudyofelectrochemicaloscillationshasimportantscientificmeaningforrecognizingtheoscillatoryphenomena，developingthekineticsofelec

3、trodeprocesses，enrichingtheresearchcontentofnonlinearkinetics，andpromotingthedevelopmentoftheoryandexperimentalmethodsconcemedinphysicalchemistry．Inthiswork，weaimat(i)findingnewelectrochemicaloscillatorssystematicallybymeansofourcyclic。voltammetry—basedcriterionestablishedrecen

4、tly,and(ii)studyingtheoscillatorymechanismatthemolecularlevelbyinsituspectroelectrochemicalmethods．Asweallknowthatthestudyofelectrocatalyticoxidationofsmallorganicmoleculesissignificantbothforfundamentalresearchasmodelsystemsandforpotentialapplicationinthefuelcells．Thestudyofos

5、cillatorymechanismishelpfulindeepeningthewholeunderstandingoftheelectrocatalyticprocesses，becauseacompleteelectrocatalyticmachanismshouldbealsoapplicabletodescriptionoftheoscillations。OscillationsonnoblemetalslikePthavebeenwidelystudiedforaboutahalfcentury．However,noreportsappe

6、arintheliteratureuptodateonoscillationswiththeelectrodeofnickelhydroxide，thoughthiselectrodeiswidelyusedinorganicelectrosynthesisandelectroanalysis．Inthisthesis，severalnewoscillatorshavebeenfoundwiththehelpofthecyclic·—voltammetry·-basedcriterionintheelectrooxidationofvariouski

7、ndsofsmallorganicmoleculesonanano—structurednickelhydroxidefilm(NYHF)electrode，whichwasdepositedonamechanicallyroughednickeldiskundercathodicgalvanostaticconditions．Bytakingcurrentorpotentialscanning，wefoundthatbothcurrentandpotentialoscillationscanoccurduringtheoxidationofprim

8、aryalcoholsoramines，whileonlycurrentoscillationsappear