期刊
BIOCHAR
卷 4, 期 1, 页码 -出版社
SPRINGER SINGAPORE PTE LTD
DOI: 10.1007/s42773-022-00161-2
关键词
Sorption; Heavy metal; Synchrotron; Density functional theory; Contaminated water
资金
- National Key Research and Development Program of China [2020YFC1807704]
- National Natural Science Foundation of China [21876027]
- Science and Technology Innovation Project of Foshan, China [1920001000083]
This study successfully removed antimonite from water using biochars derived from crawfish shells, and found that surface complexation was the main mechanism of adsorption. The results of this study showed the potential of biochars for antimonite removal.
Removal of antimonite [Sb(III)] from the aquatic environment and reducing its biotoxicity is urgently needed to safeguard environmental and human health. Herein, crawfish shell-derived biochars (CSB), pyrolyzed at 350, 500, and 650 degrees C, were used to remediate Sb(III) in aqueous solutions. The adsorption data best fitted to the pseudo-second-order kinetic and Langmuir isotherm models. Biochar produced at 350 degrees C (CSB350) showed the highest adsorption capacity (27.7 mg g(-1)), and the maximum 78% oxidative conversion of Sb(III) to Sb(V). The adsorption results complemented with infrared (FTIR), X-ray photoelectron (XPS), and near-edge X-ray absorption fine structure (NEXAFS) spectroscopy analyses indicated that the adsorption of Sb(III) on CSB involved electrostatic interaction, surface complexation with oxygen-containing functional groups (C = O, O = C-O), pi-pi coordination with aromatic C = C and C-H groups, and H-bonding with -OH group. Density functional theory calculations verified that surface complexation was the most dominant adsorption mechanism, whilst pi-pi coordination and H-bonding played a secondary role. Furthermore, electron spin resonance (ESR) and mediated electrochemical reduction/oxidation (MER/MEO) analyses confirmed that Sb(III) oxidation at the biochar surface was governed by persistent free radicals (PFRs) (center dot O-2(-) and center dot OH) and the electron donating/accepting capacity (EDC/EAC) of biochar. The abundance of preferable surface functional groups, high concentration of PFRs, and high EDC conferred CSB350 the property of an optimal adsorbent/oxidant for Sb(III) removal from water. The encouraging results of this study call for future trials to apply suitable biochar for removing Sb(III) from wastewater at pilot scale and optimize the process. [GRAPHICS] .
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