Bare nanoscale zero-valent iron (NZVI) particles in aqueous suspensions aggregate into micron to submicron sizes. The transport process of enlarged aggregates or multi-sized aggregates is different from that of nanoparticles. In this work, we performed aggregate size distribution analysis of NZVI suspension using a laser grain size analyzer and conducted a series of continuous injection column experiments with different injected NZVI concentrations. The results show that aggregates in NZVI suspensions range from submicron to submillimeter size and are mainly distributed around 5–9 μm and 50–100 μm. Quantitative calculation of iron transport and retention showed that the retained iron linearly correlates with injected concentration. The cross-section images revealed that clogging weakened from inlet to outlet. Furthermore, larger aggregates (>40 μm) appeared more often in the rising-declining stages of breakthrough curves, whereas small aggregates (<30 μm) dominated the steady stage. Indeed, relatively preferential flow facilitated the transport and discharge of both large and small iron aggregates. Straining of glass beads especially for the large iron aggregates resulted in a decline in breakthrough. Moreover, the blocking of attached and plugged iron prevented later retention of iron, resulting in a certain concentration of iron in the effluents. Our study provides greater insight into the transport of NZVI.
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