| 双溶剂法制备CuCl@MIL-101(Cr)配位型吸附剂及其脱硫性能 |
| Preparation of CuCl@MIL-101(Cr) by Double-Solvent Method and Investigation on Adsorptive Desulfurization Performance |
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| 摘要: 分别以CuCl2和维生素C为Cu（Ⅱ）源和绿色还原剂，MIL-101（Cr）为多孔载体，采用双溶剂法直接将CuCl2引入MIL-101（Cr）孔道内并全部还原成CuCl，成功实现了在金属有机骨架材料上构筑Cu（Ⅰ）活性位。结果表明，双溶剂法不会影响载体MIL-101（Cr）的结构，引入的铜物种全部被选择性地还原成CuCl。当CuCl负载量为2.85 mmol·g-1时，吸附剂对噻吩的吸附性能达到最佳，饱和吸附量为0.175 mmol·g-1，明显高于载体MIL-101（Cr）的0.112 mmol·g-1。本策略实现了在温和条件下高效可控地制备Cu（Ⅰ）功能化吸附剂，其丰富的Cu（Ⅰ）位点和高孔隙率使得该吸附剂具有较好的吸附脱硫性能。 |
| 关键词: 脱硫 吸附 π作用 金属有机骨架 还原 |
| 基金项目: 国家自然科学基金（No.21722606、21676138和21878149）和中国博士后科学基金（No.51201370）资助。 |
| Abstract: Herein, a representative metal-organic framework (MOF), MIL-101(Cr), with a large specific surface area and good hydrothermal stability, has been chosen as porous support. The introducing of Cu(Ⅱ) precursor and reduction to Cu(Ⅰ) were sequentially occurred in the pores of MIL-101(Cr) via double-solvent method (DSM) in which the CuCl2 was directly used for reduction and vitamin C was employed as a green reductant. The DSM is effective in preparing Cu(Ⅰ) sites on support MIL-101(Cr). By using the DSM, it can ensure that the structure of support material was maintained on account of mild operating conditions and all copper species in MIL-101(Cr) were reduced to Cu (Ⅰ). When CuCl content was 2.85 mmol·g-1, the obtained Cu(Ⅰ)-containing materials exhibited a thiophene adsorption capacity (up to 0.175 mmol·g-1), obviously higher than that of pristine MIL 101(Cr) (0.112 mmol·g-1). This method thus offers a useful, controllable and green approach to form Cu(Ⅰ) sites within MOFs under relatively facile conditions. The resultant adsorbents exhibit obviously enhanced adsorptive desulfurization performance because of the specific interaction between Cu(Ⅰ) and thiophenic sulfur compounds. |
| Keywords: desulfurization adsorption π interactions metal-organic frameworks reduction |
| 投稿时间：2020-08-14 修订日期：2020-11-16 |
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| 李玉霞,李帅帅,刘晓勤,孙林兵.双溶剂法制备CuCl@MIL-101(Cr)配位型吸附剂及其脱硫性能[J].无机化学学报,2021,37(2):259-266. |
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