锰、钴配合物光电催化水和有机底物氧化反应的研究-应用化学专业毕业论文

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锰、钴配合物光电催化水和有机底物氧化反应的研究 W a t e r P h o t o — a n d O x i d a t i o n o f a n d S u b s t r a t e s E l e c t r o c a t a l y t i c O r g a n i c b y a n d C o b a l t M a n g a n e s e C o m p l e x e s A b s t r a c t t o c o n v e r t s o l a r i n t o w a t e r n o v e l c h e m i c a l m e t h o d e n e r g y ， e n e r g y L i g h t — d r i v e n s p l i t t i n g ， a o n e r e a l i z e a r t i f i c i a l o f t o t h e is t w o w a y p r o c e s s p h o t o s y n t h e s i s ． T l l i s r e q u i r e s c o u p l i n g w a t e r a n d o f o f r e d u c t i o n o x i d a t i o n t h e h a l f - r e a c t i o n s ， o x i d a t i o n i n v o l v i n g p r o t o n s ． W a t e r o f f o u r e l e c t r o n s a n d f o u r t h e a n is e n e r g y t r a n s f e r r i n g p r o t o n s ， w h i c h u p h i l l r e a c t i o n ， i s t o w a t e r b o t t l e n e c k o f i n t h e r e s e a r c h o f o x i d a t i o n artificialis p h o t o s y n t h e s i s ． T h u s ． t h e k e y t h e e f f e c t i v e t h e s t a b l e r e a c t i o n a n d w a t e r o x i d a t i o n d e v e l o p c a t a l y s t s y s t e m ． M e a n w h i l e ， i f a s a n c o u l d w a t e r b e o x i d a t i o n o f s u b s t r a t e s w i t h o x y g e n r e p l a c e d b y o r g a n i c s o u r c e ， w h i c h two of i n v o l v e s e l e c t r o n s w a t e r w o u l d increase． splitting efficiency transferring，the I n t h e o f o x i d a t i o n o f r e s e a r c h n o n h e m e s u b s t r a t e s ， a o r g a n i c p h o t o c a t a l y t i c M n ( I I ) ( B Q C N ) ( O T f ) 2 ( M n l ， B Q C N c o m p l e x 2 Ⅳ N ' - d i m e t h y l - N , m a n g a n e s e · b a s e d c h a r a c t e r i z e d ． U n d e r a n d s y n t h e s i z e d i l l u m i n a t i o n ， Ⅳ ' - b i s ( 8 一 q u i n o l y l ) c y c l o h e x a n e d i a m i n e ) W a s w a s t h e o f i n s o l u t i o n M n l c a t a l y t i c a c t i v i t y i n v e s t i g a t e d c o n t a i n i n g p h o t o s e n s i t i z e r M n l a n d 【 R u ( I I ) ( b p y ) 3 ] C 1 2 ( b p y = b i p y r i d i n e ) ， e l e c t r o n a c c e p t o r 【 C o ( I I I ) ( N H 3 ) 5 C 1 ] C 1 2 ， c a t a l y s t i n a c i d i c n e u t r a l a l c o h o l a n d a n d c o n d i t i o n s ． M n l o r g a n i c s u b s t r a t e s ( b e n z y l t h i o a n i s o l e ) ， b o Ⅱ l in the a c i d i c t h e o f 7 5 m i d 2 0 w e r e o b t a i n e d T O N s 1 d i s p l a y s reactivity condition，and h i g h e s t w i t h a l c o h o l and h i g h e s t q u a n t u m 0 ． 2 6 ( ( p m a ) 【 = benzyl thioanisole，respectively．Tlleyield(9)of a s t h i o a n i s o l e t h e w a s c a l c u l a t e d ． T h e s e substrate resultsindicatethat the O．5)with o r g a n i c o f metal--based in oxidation earth·-abundant of practicalapplication catalysts photocatalytic w a s i s substrates the intermediate possible．Finally high-valent organicmanganese—OXO characterizedvariousthe w a s m e c h a n i s m methods，and s p e c t r o s c o p i c b y p r o p o s e d plausible o n b a s e d the measurements． experimental t o I n o r d e r t h e w a t e r e l e c t r o c h e m i c a l c a t a l y t i c d e v e l o p p r a c t i c a l ( p h o t o ) a n o d e ， r e a l i z i n g o f c h o s e d i f f e r e n t k i n d s N 4 a n d N 5 a n d o x i d a t i o n ， w e b e a t i n g m a n g a n e s e l i g a n d s c o m p l e x e s 2 t e t r a a m i d o t h e m e t a l — b a s e d e a r t h — a b u n d a n t C o — T A M L ( T A M L m a c r o c y c l i c l i g a n d ) a s a t t h e o f d i f f e r e n t b u f f e r s e l e c t r o c a t a l y t i c c a t a l y s t s ． T h e p H a c t i v i t y c o m p l e x e s h o m o g e n e o u s Was investigated． o f W o r d s ： M a n g a n e s e C o m p l e x ； P h o t o c a t a l y s i s ； O x i d a t i o n O r g a n i c S u b s t r a t e s ； K e y W a t e r O x i d a t i o n ； E I e c t r o c a t a I y s i s 万方数据