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创新型铁/钙原位浸渍介孔活性炭对低温水中砷的吸附及腐殖酸存在的影响。

Arsenic adsorption by innovative iron/calcium in-situ-impregnated mesoporous activated carbons from low-temperature water and effects of the presence of humic acids.

机构信息

School of Energy and Civil Engineering, Harbin University of Commerce, Harbin, 150028, China.

Department of Nephropathy, First Affiliated Hospital of Harbin Medical University, Harbin, Heilongjiang, 150001, China.

出版信息

Chemosphere. 2020 Jul;250:126275. doi: 10.1016/j.chemosphere.2020.126275. Epub 2020 Feb 21.

Abstract

Innovative iron/calcium in-situ-impregnated mesoporous activated carbons (GL100 and GL200) have been prepared by iron/calcium in-situ-impregnation and Multistage Depth-Activation. Arsenic adsorption kinetics, isotherms, thermodynamics, and re-usability were investigated. Effects of surface-absorbed (ST-HA) and dissolved states humic acid (DHA) on the arsenic adsorption were also determined. Results suggested in-situ iron/calcium impregnation caused the well-development of mesoporous structures during ranges of 2.0-5.0 nm in GL100 and 5.0-50 nm in GL200, respectively. The increase of iron/calcium ensured surface basicity and high ash contents on GL100/GL200, and As(III)/As(V) can be better adsorbed in neutral conditions with higher kinetics in comparison with regular mesoporous carbon XHIT. Maximum adsorption capacities of As(III)/As(V) by GL100 and GL200 were 2.985/3.385 mg/g and 2.516/2.807 mg/g, respectively. Arsenic desorption and carbon re-usability of GL100/200 was improved. As(III)(As (V)) adsorption capacities by GL100 and GL200 were 2.437(1.672) mg/g and 1.740(1.308) mg/g, respectively, after eight cycles. Arsenic adsorption capacities on GL100 were proved to be promoted with the presence of low-level of ST-HA or DHA, and be inhibited at a high-level. As(V) was bound more strongly than As(III) in the presence of ST-HA. As(III)/As(V) uptakes increased slightly and decrease gradually to 1.75/1.86 mg/g in the presence of DHA (0-10 mg DOC/L). Physisorption and chemisorption mechanisms dominant in arsenic adsorption on GL100 in presence of humic acid, forming inner-sphere complexation with metallic oxide, functional groups on carbon surface and humic acid structure, or ternary surface complexation via cationic metal ions as cation bridge.

摘要

创新性的铁/钙原位浸渍介孔活性炭 (GL100 和 GL200) 是通过铁/钙原位浸渍和多阶段深度活化制备的。研究了砷的吸附动力学、等温线、热力学和可重复使用性。还确定了表面吸附 (ST-HA) 和溶解态腐殖酸 (DHA) 对砷吸附的影响。结果表明,原位铁/钙浸渍在 GL100 的 2.0-5.0nm 和 GL200 的 5.0-50nm 范围内分别导致介孔结构的良好发展。铁/钙的增加确保了 GL100/GL200 的表面碱性和高灰分含量,与常规介孔碳 XHIT 相比,在中性条件下可以更好地吸附 As(III)/As(V),并且动力学更高。GL100 和 GL200 对 As(III)/As(V)的最大吸附容量分别为 2.985/3.385mg/g 和 2.516/2.807mg/g。GL100/200 的砷解吸和碳可重复使用性得到了提高。GL100 和 GL200 经过八次循环后,As(III)(As(V))的吸附容量分别为 2.437(1.672)mg/g 和 1.740(1.308)mg/g。研究表明,低水平的 ST-HA 或 DHA 存在会促进 GL100 上的砷吸附,而高水平的 ST-HA 或 DHA 存在则会抑制砷的吸附。在 ST-HA 存在下,As(V)比 As(III)结合得更牢固。在 DHA(0-10mgDOC/L)存在下,As(III)/As(V)的摄取量略有增加,然后逐渐下降至 1.75/1.86mg/g。在腐殖酸存在下,GL100 上砷的吸附主要通过物理吸附和化学吸附机制,形成金属氧化物、碳表面官能团和腐殖酸结构内的内球络合,或通过阳离子金属离子作为阳离子桥的三元表面络合。

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