Mechanisms of Zn removal from water by amorphous geopolymer: Molecular-level insights from X-ray absorption spectroscopy, isotope fractionation, and surface complexation modeling

X射线吸收光谱法 吸附 无定形固体 化学 扩展X射线吸收精细结构 无机化学 表面电荷 化学工程 分析化学(期刊) 吸收光谱法 物理化学 结晶学 有机化学 物理 量子力学 工程类
作者
Jinping Tang,Sun Guangyi,Xinbin Feng,Dongdong Liu,Yingxiang Fei,Jing Shang,Y. Zou Finfrock,Peng Liu
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:477: 147175-147175 被引量:2
标识
DOI:10.1016/j.cej.2023.147175
摘要

Porous geopolymers have attracted widespread attention as promising heavy metal adsorbents that can be synthesized from aluminosilicate solid wastes. However, the precise microstructural evidence for adsorbed heavy metals on geopolymers remains unclear due to the insensitivity of conventional characterization techniques on minerals with amorphous structure and surface disorder. Batch adsorption and column experiments coupled with X-ray absorption spectroscopy (XAS), Zn stable isotope, and surface complexation model (SCM) were employed to reveal the Zn removal mechanisms with coal fly ash porous geopolymer (CFAPG) at a molecular scale. The macroscopic kinetic and isothermal adsorption of Zn on CFAPG were well described by the pseudo-second-order model and Bi_Langmuir equation, respectively, indicating the presence of abundant heterogeneous active sites on the CFAPG surface. Two types of active sites on the CFAPG surface were identified by XAS coupled with Zn isotopes in batch experiments at pH ≤ 6.0: one is pH-dependent and associated with tetrahedral zinc coordination, and the other is pH-insensitive and associated with octahedral zinc coordination; these sites were confirmed by the bidentate SCM as the variable charge site (surface complexation, >S-OH) and the permanent negative charge site (cation exchange, >X–), respectively. Furthermore, the important contribution of surface co-precipitation besides surface complexation and cation exchange to the Zn adsorption on CFAPG was identified by XAS coupled with SCM in a flow-through column experiment at pH >6.0. These investigations provide a systemic understanding of the Zn adsorption mechanisms on CFAPG and an SCM reference for the application and prediction of geopolymers in heavy metal-contaminated water remediations.
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