物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2013年
1期
157-166
,共10页
丁志忠%董永春*%李冰%李淼
丁誌忠%董永春*%李冰%李淼
정지충%동영춘*%리빙%리묘
聚四氟乙烯纤维%金属配合物%配位结构%光催化%Fenton反应%染料降解
聚四氟乙烯纖維%金屬配閤物%配位結構%光催化%Fenton反應%染料降解
취사불을희섬유%금속배합물%배위결구%광최화%Fenton반응%염료강해
Polytetrafluoroethylene fiber%Metal ic complex%Coordination structure%Photocatalysis%Fenton reaction%Dye degradation
使用聚丙烯酸接枝改性聚四氟乙烯(PAA-g-PTFE)纤维分别与Fe3+及其与Cu2+的混合物反应制备改性PTFE纤维铁和铁铜双金属配合物,并分别使用傅里变换叶红外(FTIR)光谱和紫外-可见(UV-Vis)漫反射光谱(DRS)对两种配合物的化学结构和光吸收性能进行表征.然后将两种配合物分别作为非均相光Fenton反应催化剂应用于典型偶氮染料活性蓝222氧化降解反应中,考察和比较了二者在不同pH介质中对降解反应的催化作用.结果表明,在有或无Cu2+的存在条件下,一个Fe3+能够与三个PAA-g-PTFE表面的6个羧基发生反应形成配合物,并且它们在紫外和可见光区表现出好的光吸收特性.当两种金属离子共存时Cu2+比Fe3+更容易与PAA-g-PTFE发生配位反应形成铁铜双金属配合物.在可见光辐射下PAA-g-PTFE铁配合物对不同pH水溶液中染料降解反应均表现出显著的催化作用,但是溶液pH的升高不利于配合物催化活性的发挥.而配合物中铁离子含量提高特别是引入Cu2+作为助金属离子能够较大幅度地改善其在高pH范围内的催化活性和重复利用性.
使用聚丙烯痠接枝改性聚四氟乙烯(PAA-g-PTFE)纖維分彆與Fe3+及其與Cu2+的混閤物反應製備改性PTFE纖維鐵和鐵銅雙金屬配閤物,併分彆使用傅裏變換葉紅外(FTIR)光譜和紫外-可見(UV-Vis)漫反射光譜(DRS)對兩種配閤物的化學結構和光吸收性能進行錶徵.然後將兩種配閤物分彆作為非均相光Fenton反應催化劑應用于典型偶氮染料活性藍222氧化降解反應中,攷察和比較瞭二者在不同pH介質中對降解反應的催化作用.結果錶明,在有或無Cu2+的存在條件下,一箇Fe3+能夠與三箇PAA-g-PTFE錶麵的6箇羧基髮生反應形成配閤物,併且它們在紫外和可見光區錶現齣好的光吸收特性.噹兩種金屬離子共存時Cu2+比Fe3+更容易與PAA-g-PTFE髮生配位反應形成鐵銅雙金屬配閤物.在可見光輻射下PAA-g-PTFE鐵配閤物對不同pH水溶液中染料降解反應均錶現齣顯著的催化作用,但是溶液pH的升高不利于配閤物催化活性的髮揮.而配閤物中鐵離子含量提高特彆是引入Cu2+作為助金屬離子能夠較大幅度地改善其在高pH範圍內的催化活性和重複利用性.
사용취병희산접지개성취사불을희(PAA-g-PTFE)섬유분별여Fe3+급기여Cu2+적혼합물반응제비개성PTFE섬유철화철동쌍금속배합물,병분별사용부리변환협홍외(FTIR)광보화자외-가견(UV-Vis)만반사광보(DRS)대량충배합물적화학결구화광흡수성능진행표정.연후장량충배합물분별작위비균상광Fenton반응최화제응용우전형우담염료활성람222양화강해반응중,고찰화비교료이자재불동pH개질중대강해반응적최화작용.결과표명,재유혹무Cu2+적존재조건하,일개Fe3+능구여삼개PAA-g-PTFE표면적6개최기발생반응형성배합물,병차타문재자외화가견광구표현출호적광흡수특성.당량충금속리자공존시Cu2+비Fe3+경용역여PAA-g-PTFE발생배위반응형성철동쌍금속배합물.재가견광복사하PAA-g-PTFE철배합물대불동pH수용액중염료강해반응균표현출현저적최화작용,단시용액pH적승고불리우배합물최화활성적발휘.이배합물중철리자함량제고특별시인입Cu2+작위조금속리자능구교대폭도지개선기재고pH범위내적최화활성화중복이용성.
Polyacrylic acid grafted polytetrafluoroethylene (PAA-g-PTFE) fibers were coordinated with Fe3 + ions and with a mixture of Cu2 + and Fe3 + ions to prepare PAA-g-PTFE Fe and Cu-Fe bimetal ic complexes. The chemical structures and light adsorption properties of the complexes were characterized using Fourier transform infrared (FTIR) spectrometry and UV-Vis diffuse reflection spectroscopy (DRS), respectively. The complexes were used as heterogeneous photo-Fenton catalysts in the oxidative degradation of the azo dye, Reactive Blue 222, in different pH aqueous media. The results indicate that Fe3 + coordinates with six carboxyl groups grafted on the surface of PAA-g-PTFE in the presence or absence of Cu2+ion, and improved light adsorption properties are achieved in the UV and visible regions. When both metal ions coexist in solution, the Cu2+ion coordinates more easily with PAA-g-PTFE than Fe3+to produce a PAA-g-PTFE Cu-Fe bimetal ic complex. Moreover, PAA-g-PTFE Fe significantly increases the degradation of Reactive Blue 222 in the pH range 3-9 under visible irradiation. However, at high pH conditions (>7) the catalytic ability is reduced. Increasing the Fe content, and especial y incorporating Cu2+ions in the complex, dramatical y improves the catalytic reusability at high pH value.