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Magnetic multi-walled carbon nanotubes (MWCNTs) were prepared to support Pd/Fe nanoparticles, inhibit the aggregation and passivation, and achieve magnetic separation to avoid the environmental risk of nanoparticles. Rapid adsorption of initial contaminant, steady dechlorination, and gradual desorption of final product was observed. The micromorphology, chemical structure, and components of the nanohybrids were comprehensively characterized by a series of analysis technologies, such as EDX, XRD, SEM, TEM, and XPS. The interactions between the nanohybrids compositions were discussed according to the characterization and experimental data. The whole insight of 2,4-dichlorophenol (2,4-DCP) adsorption- dechlorination-desorption was studied in detail, including the pathways, influence factors, dechlorination kinetics and selectivity. Weak acidity (pH = 5.0 and 6.5) favored the 2,4-DCP removal …