Ji Chenghan, Yu Hang, Lu Junhe, Ren Yi, Lv Lu, Zhang Weiming
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China.
Department of Environmental Science and Engineering, Nanjing Agricultural University, Nanjing 210095, China.
ACS Appl Mater Interfaces. 2021 May 26;13(20):23833-23842. doi: 10.1021/acsami.1c05204. Epub 2021 May 11.
Adsorption as a desalination approach has the advantages of energy efficiency, low cost, and operational convenience, but its practical application is limited by low desalination capacity, consumption/disposal of strong acids/bases as regeneration reagents, and poor reusability. Herein, we synthesized a thermo-regenerable salt absorbent by grafting ethylenediaminetetraacetic acid (EDTA) onto a metal-organic framework (MOF), MOF-808-EDTA, which could rapidly adsorb NaCl within 30 min from saline water at 25 °C with a desalination capacity as high as 9.4 mmol/g. Moreover, the saturated adsorbent could be facilely regenerated in 80 °C water. Fourier transform infrared spectroscopy and derivative thermogravimetry revealed that temperature-regulated proton transfer between amino and carboxyl groups was the mechanism of thermo-regeneration. EDTA on MOF-808-EDTA appears in a zwitterionic state in water at room temperature, which allowed simultaneous adsorption of Na and Cl. At elevated temperature, it returned to a nonionic state accompanied by the desorption of ions. A similar temperature-dependent adsorption-regeneration process was also observed for other salts, including LiCl, KCl, CaCl, and MgCl. Column experiments of brackish groundwater showed that 1 g of MOF-808-EDTA could produce ∼106 mL of fresh water (total dissolved solids < 600 mg/L) without significant capacity loss after 10 successive adsorption-regeneration cycles. This study is the first to propose an EDTA-based MOF for desalination and indicates the potential of MOF-808-EDTA as a green adsorbent for sustainable water desalination.
吸附作为一种海水淡化方法,具有能源效率高、成本低和操作方便等优点,但其实际应用受到海水淡化能力低、使用强酸/强碱作为再生试剂以及可重复使用性差的限制。在此,我们通过将乙二胺四乙酸(EDTA)接枝到金属有机框架(MOF)上合成了一种热再生盐吸附剂,即MOF-808-EDTA,它能够在25℃下于30分钟内从盐水中快速吸附NaCl,海水淡化能力高达9.4 mmol/g。此外,饱和吸附剂可在80℃的水中轻松再生。傅里叶变换红外光谱和导数热重分析表明,氨基和羧基之间的温度调节质子转移是热再生的机制。MOF-808-EDTA上的EDTA在室温下于水中以两性离子状态存在,这使得Na和Cl能够同时被吸附。在升高温度时,它会恢复到非离子状态并伴随着离子的解吸。对于其他盐,包括LiCl、KCl、CaCl和MgCl,也观察到了类似的温度依赖性吸附-再生过程。微咸地下水的柱实验表明,1 g MOF-808-EDTA在连续10次吸附-再生循环后可产生约106 mL淡水(总溶解固体<600 mg/L),且容量无明显损失。本研究首次提出了一种基于EDTA的用于海水淡化的MOF,并表明了MOF-808-EDTA作为可持续海水淡化绿色吸附剂的潜力。