Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-04-09 , DOI: 10.1016/j.cej.2022.136276 Yu-Hang Li 1, 2 , Chong-Chen Wang 1, 2 , Xu Zeng 1, 2 , Xue-Zi Sun 1, 2 , Chen Zhao 1, 2 , Huifen Fu 1, 2 , Peng Wang 1, 2
Within this work, a green and facile approach was proposed to modulate NH2-UiO-66 for purpose of obtaining SS-NH2-UiO-66-X (“X” implied the dosage of used SS) using seignette salt (SS). The generation of abundant vacancies with the formation of hierarchical pores boosted their sorption performance for lead (Pb(II)), which strengthened the mass transfer of Pb(II) in SS-NH2-UiO-66-X interior. Particularly, the optimal SS-NH2-UiO-66-5 exhibited good adsorption capacity toward Pb(II) (186.14 mg g−1) and fast diffusion rate (32.1 mg g−1·min0.5) at 25 °C and initial pH = 5.46, which were about 34.2 and 66.9 times higher than those of the pristine NH2-UiO-66, respectively. SS-NH2-UiO-66-5 could selectively capture the Pb(II) from simulated wastewater containing different co-existing ions. The mechanism was proposed that the defect sites played a significant role in boosting the Pb(II) capture performance, which was further affirmed by X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectra (XPS). The density functional theory calculations (DFT calculations) illustrated that the hierarchical pores and rich vacancies enhanced the Pb(II) mobility toward the adsorption active sites and reduced the adsorption energy between SS-NH2-UiO-66-X and Pb(II). This defect engineering approach could be introduced to modulate other Zr-MOFs like MOF-801, UiO-66 and MOF-808, which presented a general strategy to fabricate defective Zr-MOFs for the boosted adsorption performance toward pollutants removal from wastewater.
中文翻译:
Seignette 盐诱导 Zr-MOFs 缺陷促进 Pb(Ⅱ) 吸附:通用策略和机制洞察
在这项工作中,提出了一种绿色且简便的方法来调节 NH 2 -UiO-66,以使用 seignette 盐 (SS)获得 SS-NH 2 -UiO-66-X(“X”表示使用的 SS 的剂量) . 随着分层孔的形成,大量空位的产生提高了它们对铅(Pb(II))的吸附性能,从而加强了Pb(II)在SS-NH 2 -UiO-66-X内部的传质。特别是,最优的 SS-NH 2 -UiO-66-5在 25 °C 和初始温度下对 Pb(II) 表现出良好的吸附能力(186.14 mg g -1)和快速的扩散速率(32.1 mg g -1 ·min 0.5 )。 pH = 5.46,分别是原始 NH 2的 34.2 和 66.9 倍-UiO-66,分别。SS-NH 2 -UiO-66-5 可以选择性地从含有不同共存离子的模拟废水中捕获 Pb(II)。提出的机制是缺陷位点在提高 Pb(II) 捕获性能方面发挥了重要作用,X 射线吸收光谱 (XAS) 和 X 射线光电子能谱 (XPS) 进一步证实了这一点。密度泛函理论计算(DFT计算)表明,分级孔隙和丰富的空位增强了Pb(II)向吸附活性位点的迁移率,降低了SS-NH 2之间的吸附能。-UiO-66-X 和 Pb(II)。这种缺陷工程方法可以用于调节其他 Zr-MOF,如 MOF-801、UiO-66 和 MOF-808,这为制造有缺陷的 Zr-MOF 提供了一种通用策略,以提高对废水中污染物去除的吸附性能。