石墨相g-c3n4复合光催化剂的制备及其光催化性能研究-preparation and photocatalytic properties of graphite phase g - c3n4 composite photocatalyst.docx

石墨相g-C3N4复合光催化剂的制备及其光催化性能研究是单独g．C3N4的4．1倍，具有较高的光生载流子分离能力。通过模拟太阳光下光催化分解水产氢和降解2，4，6．三氯苯酚(2，4，6-TCP)实验来考察BiOl03／g．C3N4异质结光催化剂在光催化产清洁能源和光催化环境污染控制领域的应用。结果表明，该二维层状BiOIOdg．C3N4异质结催化剂具有优异的光催化活性，其光催化产氢速率和光催化降解2,4，6．TCP活性分别是单独g．C3N4的3．5倍和4．8倍，且具有良好稳定性。其中，2，4，6．TCP光催化降解实验中的活性自由基捕获实验发现，羟基自由基和超氧自由基是该光催化反应中的主要活性物种。结合液质联用(LC．MS)技术对中间产物分析发现，该光催化降解2，4，6．TCP的反应路径为羟基自由基攻击并取代苯环上的氯而逐步脱氯的过程。通过电子自旋共振测试和化学荧光测试发现该异质结光生载流子的迁移方式属于z机制。该复合材料具有较高光催化活性可归因于较大的比表面积，较高的光生载流子分离效率以及体系中保留了具有较强的氧化还原能力的光生电子和空穴。关键词：光催化；石墨相g-C3N4；异质结；Z机制万方数据大连理工大学博士学位论文PreparationofGraphiteg—CaN4BasedPhotocatalystsandTheirPhotocatalyticPerformanceAbstractPhotocatalytictechnologyisoneofgreentechnologies，whichhasbeenwidelyusedinenvironmentalpollutantcontrolandsolarenergyconversion．Graphitecarbonnitride(g—C3N4)，anovelpolymersemiconductorphotocatalyst，hasdrawnmuchattentionforitsuniquepropertiessuchasvisibleresponded，highchemicalinertnessandthermalstability．However，thephotocatalyticactivityofg-C3N4islowduetoitshighphotogeneratedcarriersrecombinationrateandtheweakoxidationabilityofphotogeneratedhole．Asweknow，theheterojuctioncanprovidedrivingforceforthephotogeneratedcarrierseparation，thusimprovethequantumyield．Inthisdissertation，wemainlyfocusondesigninghigh-efficiencyg。C3N4。basedheterojunctiontoenhancethephotocatalyticactivityofg-C3N4，andseveralworkshavebeendoneasfollows：(1)Anovelpolyimide(PI)／g—C3N4heterojunctionwaspreparedthroughafacilechemisorptionapproach．TheP垤-C3N4compositeexhibitedextraordinaryhighphotogeneratedcarrierseparationefficiencyandthehighestphotocurrentdensitywas4timesashighasg-C3N4．2，4-dichlorophenol(2，4一DCP)waschosenasthetargettoinvestigatethephotocatalyticperformanceofthecomposite．AndtheresuksshowedthatthePI／g．C3N4compositessequentiallypresentedhigh—efficiencyphotocatalyticactivityindegradationof2,4-dichlorophenol(2，4．DCP)for4hoursundervisiblelightirradiation．Inparticular．theoptimum2,4·DCPremovalrateofthePI儋-C3N4compositeswithweightratioofPIat30％was98％whichwasalmost3．8timesashighasthatoverg．C3N4．Furthermore，itw