State Key Laboratory of Pollution Control and Resource Reuse, Jiangsu Key Laboratory of Vehicle Emissions Control, School of the Environment, Nanjing University, Nanjing 210023, PR China.
State Key Laboratory of Pollution Control and Resource Reuse, Jiangsu Key Laboratory of Vehicle Emissions Control, School of the Environment, Nanjing University, Nanjing 210023, PR China.
Sci Total Environ. 2019 May 1;663:673-685. doi: 10.1016/j.scitotenv.2019.01.392. Epub 2019 Jan 31.
Liquid phase catalytic reduction of bromate with supported noble metals as the catalysts is a promising method to remove bromate in water. Magnetic supports provide a feasible way to recover catalysts whose surface properties also strongly influence the catalytic efficiency. In this study, Pd nanoparticles supported on core-shell structured magnetites with varied shells (e.g., carbon, SiO, polypyrrole, polyaniline, polydopamine and chitosan) were prepared and catalytic reduction of bromate on the catalysts was investigated. The results showed that in comparison with other catalysts Pd/(FeO@polyaniline) exhibited a higher catalytic efficiency due to its higher point of zero charge and surface hydrophilicity. In parallel, bromate reduction on Pd/(FeO@polyaniline) followed the Langmuir-Hinshelwood model, confirming the crucial role of bromate adsorption. At pH 5.6 and a catalyst dosage of 0.05 g/L, 0.4 mM bromate could be completely reduced into bromide within 120 min. Furthermore, the magnetic catalysts could be effectively separated and recovered under an external magnetic field within 3 min. The results of catalyst reuse showed that after five consecutive catalytic reduction cycles Pd/(FeO@polyaniline) retained 87% of its fresh catalyst activity. The present findings indicate that Pd/(FeO@polyaniline) with polyaniline as the shell is a highly active, stable and recyclable catalyst for liquid phase catalytic hydrogenation of pollutants in water.
负载型贵金属催化剂液相催化还原法是一种去除水中溴酸盐的有前景的方法。磁性载体为回收催化剂提供了一种可行的方法,其表面性质也强烈影响催化效率。本研究制备了具有不同壳层(如碳、SiO、聚吡咯、聚苯胺、聚多巴胺和壳聚糖)的核壳结构磁铁矿负载的钯纳米粒子,并研究了催化剂上的溴酸盐催化还原。结果表明,与其他催化剂相比,Pd/(FeO@polyaniline) 由于具有更高的零电荷点和表面亲水性,表现出更高的催化效率。同时,Pd/(FeO@polyaniline) 上的溴酸盐还原遵循 Langmuir-Hinshelwood 模型,证实了溴酸盐吸附的关键作用。在 pH 5.6 和催化剂用量为 0.05 g/L 的条件下,0.4 mM 的溴酸盐在 120 min 内可完全还原为溴化物。此外,在 3 min 内,磁性催化剂可在外磁场的作用下有效分离和回收。催化剂重复使用的结果表明,经过五次连续的催化还原循环,Pd/(FeO@polyaniline) 仍保留了 87%的新鲜催化剂活性。本研究结果表明,以聚苯胺为壳层的 Pd/(FeO@polyaniline) 是一种高效、稳定且可回收的水相催化还原污染物的催化剂。