Ou Xiaoxia, Daly Helen, Fan Xiaolei, Beaumont Simon, Chansai Sarayute, Garforth Arthur, Xu Shanshan, Hardacre Christopher
Department of Chemical Engineering, School of Engineering, The University of Manchester, Oxford Road, Manchester M13 9PL, U.K.
Department of Chemistry, University of Durham, South Road, Durham DH1 3LE, U.K.
ACS Catal. 2022 Jul 1;12(13):7598-7608. doi: 10.1021/acscatal.2c01952. Epub 2022 Jun 13.
Catalytic wastewater treatment has rarely been applied to treat high-ionic-strength wastewater (HISWW) as it contains large amounts of catalyst poisons (e.g., Cl). This work investigates the catalytic wet oxidation (CWO) of phenol over a MnCeO catalyst in the presence of high NaCl concentrations where the combination of MnCeO and NaCl promoted the CWO of phenol. Specifically, in the presence of NaCl at a concentration of 200 g L and MnCeO at a concentration of 1.0 g L, phenol (initially 1.0 g L) and total organic carbon (TOC) conversions were ∼98 and 85%, respectively, after a 24 h reaction. Conversely, under the same reaction conditions without NaCl, the catalytic system only achieved phenol and TOC conversions of ∼41 and 27%, respectively. In situ Attenuated Total Reflection infrared spectroscopy identified the nature of the strongly adsorbed carbon deposits with quinone/acid species found on Ce sites and phenolate species on Mn sites in the single oxides and on MnCeO . The presence of high concentrations of NaCl reduced the carbon deposition over the catalyst, promoting surface oxidation of the hydrocarbon and reoxidation of the catalyst, resulting in enhanced mineralization. Moreover, the used MnCeO catalyst in the salt water system was efficiently regenerated via a salt water wash under the reaction conditions, showing the great potential of MnCeO in practical HISWW treatment.
催化废水处理很少用于处理高离子强度废水(HISWW),因为其含有大量催化剂毒物(如Cl)。本研究考察了在高浓度NaCl存在下,MnCeO催化剂上苯酚的催化湿式氧化(CWO),其中MnCeO和NaCl的组合促进了苯酚的CWO。具体而言,在200 g/L的NaCl和1.0 g/L的MnCeO存在下,经过24 h反应后,苯酚(初始浓度为1.0 g/L)和总有机碳(TOC)的转化率分别约为98%和85%。相反,在相同反应条件下但无NaCl时,催化体系仅实现了约41%和27%的苯酚和TOC转化率。原位衰减全反射红外光谱确定了在单一氧化物和MnCeO上,Ce位点上存在的醌/酸类强吸附碳沉积物以及Mn位点上的酚盐类的性质。高浓度NaCl的存在减少了催化剂上的碳沉积,促进了烃的表面氧化和催化剂的再氧化,从而提高了矿化程度。此外,在反应条件下,通过盐水洗涤可有效再生盐水体系中使用过的MnCeO催化剂,这表明MnCeO在实际HISWW处理中具有巨大潜力。