Tian Quanzhi, Bai Yingchu, Pan Yinhai, Yao Shuo, Chen Changshuai, Zhang Haijun, Sasaki Keiko
National Engineering Research Center of Coal Preparation and Purification, China University of Mining and Technology, Xuzhou 221116, China; Department of Earth Resources Engineering, Kyushu University, Fukuoka 819-0395, Japan.
School of Chemical Engineering and Technology, China University of Mining and Technology, Xuzhou 221116, China.
Sci Total Environ. 2022 Dec 10;851(Pt 1):158126. doi: 10.1016/j.scitotenv.2022.158126. Epub 2022 Aug 18.
Effects of aluminate and silicate species on the SeO immobilization using alkali-earth metal oxides and ferrous species have not been clearly elucidated. In the present study, Al and Si species were separately added into MgO/Fe(II) and CaO/Fe(II) reactions containing SeO, studied by toxicity characteristic leaching procedure (TCLP), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), X-ray absorption fine structure (XAFS), and PHREEQC simulation. Approximately 42 % of SeO was reduced to SeO for MgO/Fe(II) reaction in the presence of Al species, being consistent with the case without Al species. The Al species only showed slight inhibition of Se leaching for the MgO/Fe(II) reaction. Most of Se oxyanions were adsorbed onto Mg(OH) through outer-sphere complexation. For CaO/Fe(II) reaction, all of SeO was reduced to SeO with or without Al species. However, the Se leaching amount (3 %) of sample added with Al species (CE3) is much lower than that (12 %) of sample without Al species (CE2). This is mainly because SeO can be sorbed onto the iron-based minerals through binuclear bidentate corner-sharing (C) complexation instead of monodentate mononuclear corner-sharing (V) complexation of the case without Al species. On the other hand, SeO was not reduced to SeO in the presence of silicate, and almost all of Se was leached out for silicate-contained samples except CaO/Fe(II) reaction with the addition of Al species. This is due to the polymerization of Al and Si species under a high-alkalinity environment, thereby stabilizing SeO in the amorphous silicon-aluminum structure and contributing to the decrease of Se leaching.
铝酸盐和硅酸盐物种对使用碱土金属氧化物和亚铁物种固定硒酸盐的影响尚未得到明确阐释。在本研究中,将铝和硅物种分别添加到含硒酸盐的氧化镁/亚铁和氧化钙/亚铁反应体系中,通过毒性特性浸出程序(TCLP)、X射线衍射(XRD)、傅里叶变换红外光谱(FTIR)、热重分析(TGA)、X射线吸收精细结构(XAFS)以及PHREEQC模拟进行研究。在铝物种存在的情况下,氧化镁/亚铁反应中约42%的硒酸盐被还原为亚硒酸盐,这与无铝物种时的情况一致。铝物种对氧化镁/亚铁反应中硒的浸出仅表现出轻微抑制作用。大多数硒氧阴离子通过外层络合吸附在氢氧化镁上。对于氧化钙/亚铁反应,无论有无铝物种,所有的硒酸盐都被还原为亚硒酸盐。然而,添加铝物种的样品(CE3)的硒浸出量(3%)远低于未添加铝物种的样品(CE2)的硒浸出量(12%)。这主要是因为硒酸盐可以通过双核双齿角共享(C)络合吸附在铁基矿物上,而不是像无铝物种时那样通过单齿单核角共享(V)络合。另一方面,在硅酸盐存在的情况下,硒酸盐不会被还原为亚硒酸盐,并且除了添加铝物种的氧化钙/亚铁反应外,含硅酸盐样品中的几乎所有硒都被浸出。这是由于铝和硅物种在高碱度环境下发生聚合,从而将硒酸盐稳定在无定形硅铝结构中,并导致硒浸出量降低。