Castro Isabel U, Stüber Frank, Fabregat Azael, Font Josep, Fortuny Agustí, Bengoa Christophe
Departament d'Enginyeria Química, Escola Tècnica Superior d'Enginyeria Química, Universitat Rovira i Virgili, Av. Països Catalans 26, 43007 Tarragona, Catalonia, Spain.
J Hazard Mater. 2009 Apr 30;163(2-3):809-15. doi: 10.1016/j.jhazmat.2008.07.054. Epub 2008 Jul 19.
Supported Cu(II) polymer catalysts were used for the catalytic oxidation of phenol at 30 degrees C and atmospheric pressure using air and H(2)O(2) as oxidants. Heterogenisation of homogeneous Cu(II) catalysts was achieved by adsorption of Cu(II) salts onto polymeric matrices (poly(4-vinylpyridine), Chitosan). The catalytic active sites were represented by Cu(II) ions and showed to conserve their oxidative activity in heterogeneous catalysis as well as in homogeneous systems. The catalytic deactivation was evaluated by quantifying released Cu(II) ions in solution during oxidation, from where Cu-PVP(25) showed the best leaching levels no more than 5 mg L(-1). Results also indicated that Cu-PVP(25) had a catalytic activity (56% of phenol conversion when initial Cu(II) catalytic content was 200 mg L(Reaction)(-1)) comparable to that of commercial catalysts (59% of phenol conversion). Finally, the balance between activity and copper leaching was better represented by Cu-PVP(25) due to the heterogeneous catalytic activity had 86% performance in the heterogeneous phase, and the rest on the homogeneous phase, while Cu-PVP(2) had 59% and CuO/gamma-Al(2)O(3) 68%.
负载型铜(II)聚合物催化剂用于在30℃和大气压下,以空气和过氧化氢为氧化剂催化氧化苯酚。通过将铜(II)盐吸附到聚合物基质(聚(4-乙烯基吡啶)、壳聚糖)上实现均相铜(II)催化剂的多相化。催化活性位点由铜(II)离子表示,并且显示出在多相催化以及均相体系中都保留其氧化活性。通过量化氧化过程中溶液中释放的铜(II)离子来评估催化失活,由此铜-聚(4-乙烯基吡啶)(25)显示出最佳的浸出水平,不超过5mg/L。结果还表明,铜-聚(4-乙烯基吡啶)(25)具有与商业催化剂相当的催化活性(当初始铜(II)催化含量为200mg/L(反应)-1时,苯酚转化率为56%)(苯酚转化率为59%)。最后,由于多相催化活性在多相相中具有86%的性能,其余在均相相中,而铜-聚(4-乙烯基吡啶)(2)具有59%,氧化铜/γ-氧化铝具有68%,铜-聚(4-乙烯基吡啶)(25)在活性和铜浸出之间的平衡表现得更好。