g-C3N4 anchored Cu(Ⅰ)highly selective catalytic synthesis of 2,4,4,4-tetrachlorobutyronitrile using CCl4 and acrylonitrile
CuCNn(n=1,2,3)catalysts with different Cu loading amounts were prepared by thermal condensation using urea and Cu(NO3)2·3H2O as precursors,The structures and morphology of the catalysts were characterized by XRD,FTIR,XPS,BET,SEM and TEM.The catalytic performance of Cu/CNn with different Cu loading amounts was compared in the atom transfer radical addition(ATRA)reaction of CCl4 with acrylonitrile(AN)to synthesize 2,4,4,4-tetrachlorobutanitrile(TBN).The results showed that the Cu/CN1 exhibited excellent catalytic performance.Using acetonitrile(MeCN)as a solvent,n(Cu/CN1)∶n(AN)=1∶1000,120℃,for 12h,the selectivity and yield of TBN can reach 96.5%and 83.3%,respectively.As a heterogeneous catalyst,Cu/CN can be reused only after filtration treatment,and its catalytic activity can still be stably maintained after 7 times of use.Based on the relevant experimental results,the oxidation-reduction cycle ATRA reaction mechanism of CCl4 and AN catalyzed by Cu/CN was proposed.The results of experiments revealed the synergistic mechanism of Cu and g-C3N4,providing a new idea for the development of efficient catalytic systems for CCl4 deep processing.
2,4,4,4-tetrachloronitrileg-C3N4Cu/CN catalystatom transfer radical addition(ATRA)
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