Wang Hao, Jing Mengmeng, Wu Yan, Chen Weiliang, Ran Yao
School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, PR China.
School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, PR China.
J Hazard Mater. 2018 Jul 5;353:53-61. doi: 10.1016/j.jhazmat.2018.03.053. Epub 2018 Mar 29.
A series of CuNiFe layered double hydroxides (LDHs) with various Cu/Ni molar ratios were synthesized as catalysts for Fenton degradation of phenol. It is found that Cu, Cu, Ni, Ni and Fe are present on LDHs, owing to an electron transfer from Ni to Cu via metal-oxo-metal bridges. At lower Cu/Ni ratios, the highly dispersed MO octahedra and the electron donation effect of Ni facilitate such electron transfer and thus increase the percentage of Cu. The catalytic activity increases with the decrease in Cu/Ni ratio. The most active CuNiFe LDH can mineralize 98.9% phenol at ambient pH and less excessive HO dosage ( [Formula: see text] /M = 37). Even at the HO dosage close to the theoretical value, around 90% phenol can be mineralized. The structure-activity correlation indicates Cu which can readily react with HO to produce hydroxyl radicals may dominate the reaction. The regeneration of Cu could be achieved by the electron transfer between Cu and Ni in LDHs. Moreover, Fe can also act as Fenton-like active sites. The special structure of CuNiFe LDHs could offer surface-enriched and easily regenerated Cu species, leading to the complete mineralization of phenol and the efficient use of HO.
合成了一系列具有不同铜/镍摩尔比的铜镍铁层状双氢氧化物(LDHs)作为苯酚芬顿降解的催化剂。研究发现,由于通过金属-氧-金属桥从镍到铜的电子转移,铜、铜、镍、镍和铁存在于层状双氢氧化物上。在较低的铜/镍比下,高度分散的MO八面体和镍的电子给予效应促进了这种电子转移,从而增加了铜的百分比。催化活性随着铜/镍比的降低而增加。最具活性的铜镍铁层状双氢氧化物在环境pH值和较少过量的过氧化氢用量([公式:见原文]/M = 37)下可使98.9%的苯酚矿化。即使在过氧化氢用量接近理论值时,约90%的苯酚也可被矿化。结构-活性关系表明,能够与过氧化氢容易反应生成羟基自由基的铜可能主导该反应。铜的再生可通过层状双氢氧化物中铜和镍之间的电子转移来实现。此外,铁也可作为类芬顿活性位点。铜镍铁层状双氢氧化物的特殊结构可提供表面富集且易于再生的铜物种,从而实现苯酚的完全矿化和过氧化氢的高效利用。