Defect-Rich Hierarchical Porous UiO-66(Zr) for Tunable Phosphate Removal,Environmental Science & Technology

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Defect-Rich Hierarchical Porous UiO-66(Zr) for Tunable Phosphate Removal
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-09-23 , DOI: 10.1021/acs.est.1c01723
Mohua Li ₁ , Yanbiao Liu ₁ , Fang Li ₁ , Chensi Shen ₁ , Yusuf Valentino Kaneti ₂ , Yusuke Yamauchi _{2,

3} , Brian Yuliarto _{4,

5} , Bo Chen ₆ , Chong-Chen Wang ₇

Affiliation

The introduction of defects into hierarchical porous metal–organic frameworks (HP-MOFs) is of vital significance to boost their adsorption performance. Herein, an advanced template-assisted strategy has been developed to fine-tune the phosphate adsorption performance of HP-MOFs by dictating the type and number of defects in HP-UiO-66(Zr). To achieve this, monocarboxylic acids of varying chain lengths have been employed as template molecules to fabricate an array of defect-rich HP-UiO-66(Zr) derivatives following removal of the template. The as-prepared HP-UiO-66(Zr) exhibits a higher sorption capacity and faster sorption rate compared to the pristine UiO-66(Zr). Particularly, the octanoic acid-modulated UiO-66(Zr) exhibits a high adsorption capacity of 186.6 mg P/g and an intraparticle diffusion rate of 6.19 mg/g·min^0.5, which are 4.8 times and 1.9 times higher than those of pristine UiO-66(Zr), respectively. The results reveal that defect sites play a critical role in boosting the phosphate uptake performance, which is further confirmed by various advanced characterizations. Density functional theory (DFT) calculations reveal the important role of defects in not only providing additional sorption sites but also reducing the sorption energy between HP-UiO-66(Zr) and phosphate. In addition, the hierarchical pores in HP-UiO-66(Zr) can accelerate the phosphate diffusion toward the active sorption sites. This work presents a promising route to tailor the adsorption performance of MOF-based adsorbents via defect engineering.

中文翻译：

用于可调磷酸盐去除的缺陷丰富的分层多孔 UiO-66(Zr)

将缺陷引入分级多孔金属-有机骨架（HP-MOFs）对于提高其吸附性能具有重要意义。在此，开发了一种先进的模板辅助策略，通过确定 HP-UiO-66(Zr) 中缺陷的类型和数量来微调 HP-MOF 的磷酸盐吸附性能。为了实现这一点，不同链长的单羧酸已被用作模板分子，以在去除模板后制造一系列富含缺陷的 HP-UiO-66(Zr) 衍生物。与原始 UiO-66(Zr) 相比，所制备的 HP-UiO-66(Zr) 具有更高的吸附能力和更快的吸附速率。特别是辛酸调节的 UiO-66(Zr) 具有 186.6 mg P/g 的高吸附容量和 6.19 mg/g·min ^0.5的颗粒内扩散速率，分别是原始 UiO-66(Zr) 的 4.8 倍和 1.9 倍。结果表明，缺陷位点在提高磷酸盐吸收性能方面起着关键作用，这一点得到了各种先进表征的进一步证实。密度泛函理论 (DFT) 计算揭示了缺陷不仅提供了额外的吸附位点，而且还降低了 HP-UiO-66(Zr) 和磷酸盐之间的吸附能的重要作用。此外，HP-UiO-66(Zr) 中的分级孔可以加速磷酸盐向活性吸附位点的扩散。这项工作为通过缺陷工程调整基于 MOF 的吸附剂的吸附性能提供了一条有前途的途径。

更新日期：2021-10-06

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