The global occurrence in water resources of organic micropollutants, such as pesticides and pharmaceuticals, has raised concerns about potential negative effects on aquatic ecosystems and human health. Activated carbons are the most widespread adsorbent materials used to remove organic pollutants from water but they have several deficiencies, including slow pollutant uptake (of the order of hours) and poor removal of many relatively hydrophilic micropollutants. Furthermore, regenerating spent activated carbon is energy intensive (requiring heating to 500-900 degrees Celsius) and does not fully restore performance. Insoluble polymers of β-cyclodextrin, an inexpensive, sustainably produced macrocycle of glucose, are likewise of interest for removing micropollutants from water by means of adsorption. β-cyclodextrin is known to encapsulate pollutants to form well-defined host-guest complexes, but until now cross-linked β-cyclodextrin polymers have had low surface areas and poor removal performance compared to conventional activated carbons. Here we crosslink β-cyclodextrin with rigid aromatic groups, providing a high-surface-area, mesoporous polymer of β-cyclodextrin. It rapidly sequesters a variety of organic micropollutants with adsorption rate constants 15 to 200 times greater than those of activated carbons and non-porous β-cyclodextrin adsorbent materials. In addition, the polymer can be regenerated several times using a mild washing procedure with no loss in performance. Finally, the polymer outperformed a leading activated carbon for the rapid removal of a complex mixture of organic micropollutants at environmentally relevant concentrations. These findings demonstrate the promise of porous cyclodextrin-based polymers for rapid, flow-through water treatment.
Per- and poly fluorinated alkyl substances (PFASs), notably perfluorooctanoic acid (PFOA), contaminate many ground and surface waters and are environmentally persistent. The performance limitations of existing remediation methods motivate efforts to develop effective adsorbents. Here we report a β-cyclodextrin (β-CD)-based polymer network with higher affinity for PFOA compared to powdered activated carbon, along with comparable capacity and kinetics. The β-CD polymer reduces PFOA concentrations from 1 μg L to <10 ng L, at least 7 times lower than the 2016 U.S. EPA advisory level (70 ng L), and was regenerated and reused multiple times by washing with MeOH. The performance of the polymer is unaffected by humic acid, a component of natural organic matter that fouls activated carbons. These results are promising for treating PFOA-contaminated water and demonstrate the versatility of β-CD-based adsorbents.
The cost-effective and energy-efficient removal of organic micropollutants (MPs) from water and wastewater is challenging. The objective of this research was to evaluate the performance of porous β-cyclodextrin polymers (P-CDP) as adsorbents of MPs in aquatic matrixes. Adsorption kinetics and MP removal were measured in batch and flow-through experiments for a mixture of 83 MPs at environmentally relevant concentrations (1 μg L) and across gradients of pH, ionic strength, and natural organic matter (NOM) concentrations. Performance was benchmarked against a coconut-shell activated carbon (CCAC). Data reveal pseudo-second-order rate constants for most MPs ranging between 1.5 and 40 g mg min for CCAC and 30 and 40000 g mg min for P-CDP. The extent of MP removal demonstrates slower but more uniform uptake on CCAC and faster but more selective uptake on P-CDP. Increasing ionic strength and the presence of NOM had a negative effect on the adsorption of MPs to CCAC but had almost no effect on adsorption of MPs to P-CDP. P-CDP performed particularly well for positively charged MPs and neutral or negatively charged MPs with McGowan volumes greater than 1.7 (cm mol)/100. These data highlight advantages of P-CDP adsorbents relevant to MP removal during water and wastewater treatment.
Perfluoroalkyl and polyfluoroalkyl substances (PFAS) are a group of persistent and mobile fluoro-organic chemicals that have been detected in many water supplies, and their recommended safe concentrations in drinking water are as low as 6 ng/L. Current technological advances suggest that amine-containing sorbents can provide alternative solutions to PFAS control in the treatment of municipal water and wastewater at relatively low PFAS concentrations. The objective of this review is to provide critical analysis of the development and application of amine-containing sorbents for PFAS removal. The removal of PFAS by aminated sorbents relies on the combined effects of three main factors: (i) electrostatic interactions with functional groups of the sorbent, (ii) hydrophobic interactions with the sorbent and between PFAS molecules, and (iii) sorbent morphology. The design of next-generation sorbents should take into consideration these three factors and their relative contribution. We also provide an outlook and highlight of the key areas of innovative research needs to develop more efficient sorbents that will enable compliance with the increasingly stringent regulations of PFAS.
A new family of solid polymer electrolytes based upon anionic tetrakis(phenyl)borate tetrahedral nodes and linear bis-alkyne linkers is reported.
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