Abstract

To reduce heavy metals (HMs) contamination from tannery sludge, this study investigated the migration behaviour of arsenic (As) and chromium (Cr) at 700–900 °C using CO2 gasification. The HMs enrichment results showed that As contents of ash decreased (6.42→1.87 mg/kg) while Cr contents increased (41.40→78.24 mg/kg) over 700–900 °C. More Si-O bonds and fewer Ca-O bonds with increasing temperature in ash primarily determined this migration behaviour of HMs. Meanwhile, the proportions of toxic As(III) and Cr(VI) declined from 96.02% and 64.26–76.96% and 21.24%, forming As(0) and Cr(III) with less toxicity. This reduction was conducted via two pathways: (i) carbon reduced As(III)/Cr(VI) and (ii) carbon reduced Fe(II)/Fe(III) to Fe(0), then Fe(0) reduced As(III)/Cr(VI) assisted with carbon via Fe(0)→Fe(II)→Fe(III). However, free calcium ions oxidized As(0)/Cr(III) to As(III)/Cr(VI) at 700 ○C. At higher temperatures, silicate glass conversion of ash immobilized free calcium ions and barely oxidized HMs. Furthermore, this study identified the positive effect of increasing temperature on enhancing the stability of HMs in ash by transforming bioavailable HMs into non-bioavailable HMs, which decreased the leaching toxicity and environmental risk. Regarding HMs emissions control and cold gas efficiency, CO2 gasification treatment of tannery sludge is most effective at 800 °C.

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