(Multivariate)-Metal–Organic Framework for Highly Efficient Antibiotic Capture from Aquatic Environmental Matrices

Abstract

Contamination of aquatic environments by pharmaceuticals used by modern societies has become a serious threat to human beings. Among them, antibiotics are of particular concern due to the risk of creating drug-resistant bacteria and, thus, developing efficient protocols for the capture of this particular type of drug is mandatory. Herein, we report a family of three isoreticular MOFs, derived from natural amino acids, that exhibit high efficiency in the removal of a mixture of four distinct families of antibiotics, such as fluoroquinolones, penicillins, lincomycins, and cephalosporins, as solid-phase extraction (SPE) sorbents. In particular, a multivariate (MTV)-MOF, prepared using equal percentages of amino acids L-serine and L-methionine, also exhibits outstanding recyclability, surpassing the benchmark material activated carbon. The good removal performance of the MTV-MOF was rationalized by means of single-crystal X-ray diffraction. These results highlight the situation of MOFs as a real and promising alternative for the capture of antibiotics from environmental matrices, especially wastewater streams.

Exploring the Role of Amino Acid-Derived Multivariate Metal–Organic Frameworks as Catalysts in Hemiketalization Reactions

“…Looking at such modeled crystal structure of 3 , the two “arms” decorated with serine and methylcysteine derivatives, respectively, show different orientations, with the methylcysteine one being more distended, within the largest octagonal pores, and the serine one bent and confined in the smallest channels developing along the a crystallographic axis (Figures b,c and S3). Here, it is worth noting that MTV-MOFs, as already underlined in our previous works, ,,, show as a thrilling feature an impressive flexibility of the functional arms confined within the pores, exhibiting different conformations depending on the target molecules captured in pores. Thus, loaded reactants of a given catalytic reaction might have an effect on the final conformation adopted by the flexible aminoacidic arms decorating the pores.…”

“…So far, we have observed a successful transfer from the complexity of composition to the improvement of performance in water remediation. 14,18,26,27 18 On this basis and with the background inspiration of the active centers of enzymes, where different organic functionalities are able to act synergistically to interact, adapt, and efficiently catalyze the transformation of specific substrates, the aim of this investigation has been to explore within a family of isoreticular MOFs the role and influence of the presence and absence of functional channels decorated with more than one distinct amino acid residue in catalysis. To this end, we have focused on the use of two previously reported MOFs, with formulas {Sr II The addition of alcohols to the carbonyl group of aldehydes and ketones is an essential reaction in nature 31 and industrial synthesis 32 since the electronic density of the carbonyl group is completely switched from electron-rich to electron-poor.…”

“…One of our main research lines has been devoted to exploring the development of MTV-MOFs with oxamidato-based ligands derived from amino acids, with the main aim to take advantage of the heterogeneity of composition and the intrinsic flexibility of the residues decorating the MTV-MOF channels toward more complex applications. So far, we have observed a successful transfer from the complexity of composition to the improvement of performance in water remediation. ,,, In particular, an MTV-MOF {Ca II Cu 6 II [( S , S )-methox] 1.43–1.46 [( S , S )-serimox] 1.57–1.54 (OH) 2 (H 2 O)}·30H 2 O (where methox = bis­[( S )-methionine]­oxalyl diamide and serimox = bis­[( S )-serine]­oxalyl diamide) with functional channels decorated with approximately 50% of hydroxyl groups and 50% thioalkyl ones derived from natural amino acids L-serine and L-methionine, respectively, has proven very efficient in the simultaneous capture of contaminants with inorganic and organic nature . Also, this has been further validated with an isoreticular MTV-MOF {Sr II Cu 6 II [( S , S )-methox] 1.50 [( S , S )-mecysmox] 1.50 (OH) 2 (H 2 O)}·36H 2 O (where methox = bis­[( S )-methylcysteine]­oxalyl diamide), which outperforms single-component MOFs in the removal of emergent neonicotinoid contaminants from water …”

Nanoarchitectonics Design Strategy of Metal–Organic Framework and Bio-Metal–Organic Framework Composites for Advanced Wastewater Treatment through Adsorption

“…Here, we elucidate an overview of the latest advancements in adsorption techniques in MOFbased materials and their effectiveness in mitigating pharmaceutical pollution. At the latest, Negro et al 169 have developed a multivariate MOF (MTV-MOF) that effectively removes a mixture of antibiotics such as ciprofloxacin, clindamycin, ceftriaxone, and amoxicillin by using solid-phase extraction (SPE) sorbents. The MTV-MOF is synthesized using L-serine and L-methionine at equal percentages.…”

Isomerización de alquenos catalizada por rutenio sin ligando e hidrólisis de acetales catalizada por aminoácidos en redes metalorgánicas

“…Hasta ahora, se ha observado una transferencia exitosa de la complejidad de la composición a la mejora del rendimiento en la remediación de agua. 288,292,299,300 En particular, un MTV-MOF {Ca II Cu II = bis[(S)-serina] oxalil diamida) con canales funcionales decorados con aproximadamente un 50% de grupos hidroxilo y un 50% de grupos tioalquilo derivados de los aminoácidos naturales L-serina y L-metionina, respectivamente, han demostrado ser muy eficaces en la captura simultánea de contaminantes de naturaleza inorgánica y orgánica. 288 Además, esto se ha validado aún más con un MTV-MOF isorreticular {Sr II Cu II 6[(S,S)-metoxi]1.50[(S,S)-Mecysmox]1.50(OH)2(H2O)}•36H2O (donde metox = bis[(S)-metionina]oxalil diamida), que superan a los MOF de un solo componente en la eliminación de contaminantes neonicotinoides emergentes en agua.…”