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The B r J B r e l ec t rode r eac t ion w i t h t r i b r o m i d e c o m p l e x f o r m a t i o n r eac t ion in t he so lu t ion , a chemica l e l ec t roche mi cal (C-E) t ype reac t ion , has b e e n i n v e s t i g a t e d in o rde r to d e t e r m i n e t he ef fec t of t he c h e m i c a l r eac t i on on t he e l ec t rode kine t ics . I t is s h o w n t h a t the c h e m i c a l r eac t ion has l i t t le effect on t he e l ec t rode k ine t i c s at ve ry s low h o m o g e n e o u s r eac t ion ra tes , b u t ha s a m o r e d ras t i c ef fec t o n t h e e l ec t rode k ine t i c s at fas te r h o m o g e n e o u s r eac t ion rates . Also, t h e k ine t i c s at t he e l ec t rode are a f fec ted b y c h a n g e s in t he c o n c e n t r a t i o n s of t h e ac t ive spec ies (Br~, Br, a n d Br.~ ) in t he b u l k so lu t ion as a c o n s e q u e n c e of t h e coup l ing effect of t he c h e m i c a l r eac t ion on t he e l ec t rode k ine t ics . T h e B r J B r e l e c t r o d e r e a c t i o n is a v e r s i o n of a c h e m i c a l e l e c t r o c h e m i c a l (C-E) r e a c t i o n in w h i c h t h e h o m o g e n e o u s c h e m i c a l s t ep in r e a c t i o n [2] p r e c e d e s t h e cha rge t r a n s f e r s t ep in r e a c t i o n [1] Br2 + 2eredu~'~n 2 B r [1] u~idation Br2 + B r k t Br3[2] % T h i s r e a c t i o n ha s a t t r a c t e d c o n s i d e r a b l e a t t e n t i o n in t h e p a s t c o u p l e of yea r s (t-5) b e c a u s e i t s e r v e s as o n e of t h e p r i n c i p a l e l e c t r o d e r e a c t i o n s of t h e Zn/Br2 s e c o n d a r y b a t t e r y s y s t e m t h a t is b e i n g c o n s i d e r e d for u s e in l a r g e s c a l e e n e r g y s to r age . I n f o r m a t i o n a b o u t t h i s r e a c t i o n is d e s i r e d to a id in t h e d e s i g n a n d o p t i m i z a t i o n of t h e Zn/Br2 ba t t e ry . T h e e q u i l i b r i u m c o n s t a n t for r e a c t i o n [2], Ke,, w h e r e K~q = kf/k~, is o n l y 17.0 l i t e r s / too l (6). As a resu l t , s ignif i c a n t c o n c e n t r a t i o n s of Br2, Br , a n d Br.~wil l c o m m o n l y b e p r e s e n t in t h e e l e c t r o l y t e . F o r t h a t m a t t e r , a n y det a i l e d m o d e l for p r e d i c t i n g t h e c u r r e n t p o t e n t i a l cha rac t e r i s t i c s of t h e B r J B r e l e c t r o d e m u s t i n c l u d e t h e e f fec t s of t h e h o m o g e n e o u s c o m p l e x a t i o n r eac t ion . I n t h e pas t , s o m e i n v e s t i g a t o r s (7) h a v e j u s t i f i ed t h e e x c l u s i o n of t he c h e m i c a l r e a c t i o n by a s s u m i n g t h e c o m p l e x a t i o n k i n e t ics to b e v e r y rap id . In o t h e r words , t h e y c o n s i d e r e d t h i s r e a c t i o n to b e e s s e n t i a l l y a t e q u i l i b r i u m a t al l p o i n t s in t h e e l e c t r o l y t e a n d for t h i s r e a s o n a s s u m e d t h a t t h e c h e m i c a l r e a c t i o n h a d no e f fec t on t h e e l e c t r o d e k ine t i c s . O t h e r i n v e s t i g a t o r s (8, 9) we re ab l e to a c c o u n t for t h e effec t of t h e c h e m i c a l r e a c t i o n on t h e e l e c t r o d e k i n e t i c s b y c o n s i d e r i n g t h e e q u i l i b r i u m c o n s t a n t of t h e c h e m i c a l rea c t i o n to b e i n d e p e n d e n t of d i s t a n c e f r o m t h e e l e c t r o d e s u r f a c e . W i t h t h e l a t t e r a p p r o a c h , N e w m a n (9) d e m o n s t r a t e d w i t h t h e CuSO4-H2SO4 s y s t e m t h a t t h e i n c o m p l e t e d i s s o c i a t i o n of t h e h o m o g e n e o u s b i s u l f a t e r e a c t i o n d i d h a v e a d r a m a t i c e f f e c t on t h e l i m i t i n g c u r r e n t s as a r e s u l t of c h a n g e s in t h e ion ic s t r e n g t h of t h e s o l u t i o n d u e * Electrochemical Society Active Member. to t h e m i g r a t i o n of d i s s o c i a t e d spec i e s . H o w e v e r , for cases w i t h m o d e r a t e or s low h o m o g e n e o u s k ine t i c s , t he a s s u m p t i o n t h a t t h e h o m o g e n e o u s r e a c t i o n is a t equ i l i b r i u m a t al l p o i n t s in t h e e l e c t r o l y t e is n o l o n g e r v a l i d . T h e r e f o r e , a m o r e rea l i s t i c a p p r o a c h m u s t b e a d o p t e d to a c c o u n t for t h e e f f e c t of t h i s h o m o g e n e o u s r e a c t i o n o n t h e e l e c t r o d e k ine t i c s . Th i s i n v o l v e s t r e a t i n g t h e c h e m i cal r e a c t i o n as a r e a c t i o n w i t h a f in i te ra te , w h e r e t h e p s e u d o e q u i l i b r i u m c o n s t a n t for t h i s s y s t e m , K'(~), is de f i ned as

The Effect of the Tribromide Complex Reaction on the Oxidation/Reduction Current of the Br2 / Br − Electrode