Article
Chemistry, Multidisciplinary
Wanjun Xu, Shuaijun Pan, Benjamin B. Noble, Zhixing Lin, Sukhvir Kaur Bhangu, Chan-Jin Kim, Jingqu Chen, Yiyuan Han, Irene Yarovsky, Frank Caruso
Summary: This article reports on flexible metal-phenolic networks (MPNs) that exhibit stimuli-responsive behavior to various solute guests. The responsive behavior of the MPNs is primarily determined by the competitive coordination of metal ions to phenolic ligands with multiple coordination sites and solute guests. The embedding of glucose molecules into the dynamic MPNs leads to the reconfiguration of the metal-organic networks and changes in their physicochemical properties for targeted applications. This study expands the library of stimuli-responsive flexible metal-organic materials and enhances the understanding of intermolecular interactions between metal-organic materials and solute guests, which is crucial for the rational design of responsive materials for various applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Saurav Bhattacharya, Uttara Basu, Mohamed Haouas, Pei Su, Michael Forrester Espenship, Fei Wang, Albert Sole-Daura, Dereje H. Taffa, Michael Wark, Josep M. Poblet, Julia Laskin, Emmanuel Cadot, Ulrich Kortz
Summary: This paper reports the synthesis, structure, and characterization of neutral palladium-oxo clusters (POCs), specifically the Pd-16, Pd-16Cl, and Pd-24 compounds. These compounds exhibit novel chemical properties based on their different structural units. Comprehensive characterization of these compounds was conducted in the solid, solution, and gas phases.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Biochemistry & Molecular Biology
Rosaria Bruno, Teresa F. Mastropietro, Giovanni De Munno, Donatella Armentano
Summary: Self-assembly using pi center dot center dot center dot pi stacking interactions between aromatic groups of ligands was utilized to create a rare nanoporous supramolecular metal-organic framework with chiral hydrophobic and hydrophilic pores. The encoded chiral information from enantiopure building blocks was transferred to the final supramolecular structure, resulting in efficient enantioselective separation capabilities.
Article
Chemistry, Multidisciplinary
Wen-Qi Tang, Ying-Jie Zhao, Ming Xu, Jin-Ya Xu, Sha-Sha Meng, Yun-Dong Yin, Qing-Hua Zhang, Lin Gu, Da-Huan Liu, Zhi-Yuan Gu
Summary: Control over the stacking modes of metal-organic framework (MOF) nanosheets can lead to excellent gas chromatographic separations. Different solvents can induce twisted stacking of nanosheets, while alkanes may result in untwisted stacking.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Tobias Schnitzer, Eno Paenurk, Nils Trapp, Renana Gershoni-Poranne, Helma Wennemers
Summary: Despite the challenges in forming networks from peptidic ligands, a peptide-metal framework consisting of helical oligoproline ligands and Zn/K (or Zn/Rb) has been successfully created in this study. The crystal network contains pleated nanosheets with metal ions aligned in strings, with the unique architecture derived from under-appreciated London dispersion interactions between the ligands. The secondary structure of the peptidic ligand plays an important role in the creation of new MOF architectures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Sarah E. E. Morgan, Morgan L. L. Willis, Golnaz Dianat, Gregory W. W. Peterson, John J. J. Mahle, Gregory N. N. Parsons
Summary: This study presents a novel mechanism for rapid synthesis of UiO-66-NH2 using common low-boiling-point solvents, enabling scalable fabrication of composite fabrics. The choice of solvents and segregated spray method facilitates rapid MOF nucleation on fiber surface and reduces energy and time required for post-processing. The MOF fabric demonstrates superior protective capability by blocking permeation of the chemical warfare agent.
Article
Chemistry, Multidisciplinary
Yanchao Wu, Yong Zhang, Yuan Chen, Hui Tang, Mi Tang, Shuaifei Xu, Kun Fan, Chenyang Zhang, Jing Ma, Chengliang Wang, Wenping Hu
Summary: In recent years, the emerging pi-d conjugated coordination polymers (CCPs) have attracted increasing attention for various applications. The study proposed two Ni-based CCPs with N and S as co-chelating atoms, which exhibited high electrical conductivity and stability, resulting in high capacity, excellent cyclability, and high rate capability in sodium-ion batteries (SIBs). These results enrich the CCPs field and stimulate further investigations of CCPs with heterochelating atoms for various applications.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Wanjun Xu, Shuaijun Pan, Benjamin B. Noble, Jingqu Chen, Zhixing Lin, Yiyuan Han, Jiajing Zhou, Joseph J. Richardson, Irene Yarovsky, Frank Caruso
Summary: This study reports the synthesis of site-selective coordinated metal-phenolic networks using flavonoids as coordination modulators. The tuning of different coordination sites allows for easy control of the physicochemical properties of the materials, expanding our understanding of metal-phenolic chemistry and providing new design routes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
J. Gao, H-M Yu, M. Wu, Q. Chen, Y. Yang, Y. Qu, M. Sun, J-C Qin, L. Ma, Y-W Yang
Summary: This study developed a stimuli-responsive theranostic nanoplatform with well-defined architectures for tumor treatment, featuring computed tomography imaging guidance, tumorous microenvironment-triggered drug release, and effective chemo-photothermal synergistic therapy capabilities. The system allows controlled drug release in response to multiple stimuli, demonstrating potential for prolonged treatment in clinical investigations.
MATERIALS TODAY CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Estefania Tiburcio, Yongkun Zheng, Marta Mon, Nuria Martin, Jesus Ferrando Soria, Donatella Armentano, Antonio Leyva Perez, Emilio Pardo
Summary: This study reports the gram-scale preparation of Ag-2(0) subnanometer clusters within a metal-organic framework, which exhibits high catalytic activity for the catalytic Buchner ring expansion reaction.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Despoina Andriotou, Sylvain Duval, Christophe Volkringer, Angel M. Arevalo-Lopez, Pardis Simon, Herve Vezin, Thierry Loiseau
Summary: The reactivity of 2,3-pyridine-dicarboxylic acid and 2,5-pyridine-dicarboxylic acid as complexing agents towards the niobium(IV) tetrachloride precursor has been investigated, resulting in the isolation of four crystalline coordination complexes. The complexes exhibit stable coordination structures formed by the interaction between the ligands and the niobium(IV) center.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Despoina Andriotou, Sylvain Duval, Christophe Volkringer, Angel M. Arevalo-Lopez, Pardis Simon, Herve Vezin, Thierry Loiseau
Summary: The reactivity of 2,3-pyridine-dicarboxylic and 2,5-pyridine-dicarboxylic acids as ligands towards the niobium(IV) tetrachloride precursor was studied, resulting in the formation of four crystalline mononuclear coordination complexes with different molecular arrangements. Each complex showed an eightfold coordination of the niobium(IV) center and exhibited unique structural characteristics. Magnetic measurements, EPR and XPS were used to analyze the d(1) configuration of the niobium(IV) centers, revealing an anti-ferromagnetism transition at very low temperatures for certain complexes.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Yury Torubaev, Ivan Skabitsky, Anton Rozhkov, Bartomeu Galmes, Antonio Frontera, Vadim Yu Kukushkin
Summary: The study revealed that cocrystallization of iodine(i)-based perfluoroarenes with palladium acetate cluster resulted in significant noncovalent interactions, as confirmed by single-crystal X-ray diffractometry. In the structures, aromatic rings were coupled with the cluster through lone pair-pi-(Ar-F)-hole interactions, while iodine-containing arenes were engaged in halogen bonding with carboxylate O centers. The electron-rich PdO4 plane behaved as a nucleophile providing oxygen lone pairs, complementing the pi-acidic surface of the arenes in circular stacking.
INORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Multidisciplinary
Xing Ma, Hang Liu, Weijie Yang, Guangyang Mao, Lirong Zheng, Hai-Long Jiang
Summary: A general and facile strategy for the construction of high-loading single-atom catalysts with a tunable coordination microenvironment has been developed based on metal-organic frameworks. The well-accessible and atomically dispersed metal sites possess close proximity to photosensitive units, greatly accelerating charge transfer and promoting photocatalysis. The optimized Ni-1-S/MOF with a unique Ni(I) microenvironment presents excellent photocatalytic H-2 production activity, surpassing other counterparts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Zhixing Lin, Jiajing Zhou, Yijiao Qu, Shuaijun Pan, Yiyuan Han, Rene P. M. Lafleur, Jingqu Chen, Christina Cortez-Jugo, Joseph J. Richardson, Frank Caruso
Summary: The study introduces a novel fluorescence labeling strategy using luminescent metal-phenolic networks (MPNs) which can produce customized fluorescent coatings on various particles with stability and strong fluorescence, showing negligible cytotoxicity to cells. This approach has great potential for diverse applications in the fields of life sciences and physical sciences.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Nanoscience & Nanotechnology
Cristina Negro, Hector Martinez Perez-Cejuela, Ernesto Francisco Simo-Alfonso, Waseem Iqbal, Jose Manuel Herrero-Martinez, Donatella Armentano, Jesus Ferrando-Soria, Emilio Pardo
Summary: The contamination of aquatic environments by pharmaceuticals used by modern societies, especially antibiotics, poses a serious threat to humans due to the potential for creating drug-resistant bacteria. This study reports a family of three isoreticular MOFs derived from natural amino acids that show high efficiency in removing a mixture of different families of antibiotics. A specific MOF, called MTV-MOF, prepared using equal percentages of L-serine and L-methionine, not only exhibits outstanding recyclability but also outperforms activated carbon. The successful removal performance of MTV-MOF is explained by single-crystal X-ray diffraction, highlighting the potential of MOFs as a promising alternative for capturing antibiotics from wastewater streams.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Review
Chemistry, Multidisciplinary
Paula Escamilla, Walter D. Guerra, Antonio Leyva-Perez, Donatella Armentano, Jesus Ferrando-Soria, Emilio Pardo
Summary: Since the emergence of metal-organic frameworks (MOFs), a wide range of exciting properties and applications have been reported, mainly due to their porous nature and rich host-guest chemistry. However, the potential rewards offered by other important features of MOFs have been largely unexplored. This feature outlines recent advances in using highly robust and crystalline oxamato- and oxamidato-based MOFs as reactors for the in situ preparation of well-defined catalytically active single atom catalysts (SACS), subnanometer metal nanoclusters (SNMCs), and supramolecular coordination complexes (SCCs).
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Ana Rubio-Gaspar, Sergio Navalon, Sergio Tatay, Francisco G. Cirujano, Carmen Fernandez-Conde, Natalia M. Padial, Carlos Marti-Gastaldo
Summary: Compared to indirectly modifying the framework, synthetic control of cluster composition allows direct access to catalytic activities without specific metal combinations. In this study, the aminolysis reaction of epoxides was tested using isostructural mesoporous frameworks with five combinations of homometallic and heterobimetallic metal-oxo trimers (Fe3, Ti3, TiFe2, TiCo2, and TiNi2). Only the TiFe2 nodes displayed activities comparable to benchmark catalysts based on grafting of strong acids, which arise from the combination of Lewis Ti4+ and Bronsted Fe3+-OH acid sites. The applicability of MUV-101(Fe) in the synthesis of beta-amino alcohols was demonstrated, including the gram-scale synthesis of propranolol, a natural beta-blocker listed as an essential medicine by the World Health Organization, with excellent yield and selectivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Victor Zatko, Regina Galceran, Marta Galbiati, Julian Peiro, Florian Godel, Lisa-Marie Kern, David Perconte, Fatima Ibrahim, Ali Hallal, Mairbek Chshiev, Benjamin Martinez, Carlos Frontera, Lluis Balcells, Piran R. Kidambi, John Robertson, Stephan Hofmann, Sophie Collin, Frederic Petroff, Marie-Blandine Martin, Bruno Dlubak, Pierre Seneor
Summary: 2D materials can be manipulated by proximity effects to modify their electronic structure, allowing for the creation of unique properties in interfaces and heterostructures. In this study, we investigate the possibility of using a ferromagnetic insulator-graphene electrode to design a magnetic tunnel junction. Through the observation of tunnel magnetoresistance, we confirm the emergence of spin polarization in proximitized graphene layers, which is induced by a spin-dependent splitting of the Dirac band structure. This opens up opportunities for utilizing 2D quantum materials in spintronics applications, such as memory cells and logic circuits.
Article
Chemistry, Multidisciplinary
Belen Lerma-Berlanga, Natalia M. Padial, Marta Galbiati, Isaac Brotons-Alcazar, Josep Albero, Hermenegildo Garcia, Alicia Forment-Aliaga, Carolina R. Ganivet, Carlos Marti-Gastaldo
Summary: The presence of tetrazine units in the organic nodes of UiO-68-TZCD controls the formation of ultrathin coatings of single-wall nanotubes that decorate the surface of the crystal. These crystal hybrids can be prepared straightforwardly in one step and exhibit exceptional stability in water, high surface areas, and good conductivity even at low carbon weight contents.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Cristina Negro, Sergio Sanz-Navarro, Antonio Leyva-Perez, Donatella Armentano, Jesu Ferrando-Soria, Emilio Pardo
Summary: Understanding the host-guest chemistry in MOFs has great potential to develop novel porous materials with improved performances in fields such as heterogeneous catalysis. In this study, a family of three isoreticular MOFs derived from amino acids were synthesized and their catalytic activities in hemiketalization reactions were investigated. The results showed that a multivariate MOF prepared using equal percentages of amino acids exhibited the most efficient catalytic conversions. The good catalytic performance was attributed to the intrinsic heterogeneity of the multivariate MOF.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Estefan Tiburcio, Yongkun Zheng, Cristina Bilanin, Juan Carlos Hernandez-Garrido, Alejandro Vidal-Moya, Judit Oliver-Meseguer, Nuria Martin, Marta Mon, Jesus Fernando-Soria, Donatella Armentano, Antonio Leyva-Perez, Emilio Pardo
Summary: This study reports the characterization of a combination of well-defined Fe3+ isolated single-metal atoms and Ag2 subnanometer metal clusters within a metal-organic framework. The resulting material exhibits superior catalytic activity for the direct conversion of styrene to phenylacetylene.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Physics, Multidisciplinary
Marta Galbiati, Fernando Ramiro-Manzano, Jose Joaquin Perez Grau, Fernando Cantos-Prieto, Jaume Meseguer-Sanchez, Ivona Kosic, Filippo Mione, Ana Pallares Vilar, Andres Cantarero, David Soriano, Efren Navarro-Moratalla
Summary: By using hyperspectral wide-field imaging, researchers revealed a nonmonotonic thickness dependence of the optical properties in magnetic 2D material CrI3. This finding sheds light on the structural conundrum and offers insights into mesoscopic effects in layered materials and light-matter interactions in magnetic 2D materials.
PHYSICAL REVIEW LETTERS
(2023)
Article
Geochemistry & Geophysics
Karina J. J. Lagos, Bojan A. A. Marinkovic, Anja Dosen, Alexis Debut, Karla Vizuete, Victor H. H. Guerrero, Emilio Pardo, Patricia I. I. Ponton
Summary: In this study, iron-rich titanate nanosheets were synthesized from Ecuadorian ilmenite sands through an alkaline hydrothermal treatment. The morphology of the nanosheets changed significantly after 72 hours of treatment at 180 degrees C. Analysis confirmed that the nanostructures were iron-rich layered titanates, but incomplete conversion of the precursor was observed.
Article
Chemistry, Multidisciplinary
Natalia M. Padial, Clara Chinchilla-Garzon, Neyvis Almora-Barrios, Javier Castells-Gil, Javier Gonzalez-Platas, Sergio Tatay, Carlos Marti-Gastaldo
Summary: Titanium-organic frameworks have intrinsic photoactivity and high stability, but the hydrolysis of Ti4+ cations limits their systematic design. Researchers have used heterobimetallic clusters as building units to design titanium frameworks with tunable porosity and interpenetration, achieving the highest reported gravimetric surface area for titanium(IV) MOFs.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Enrique Burzuri, Maria Jose Martinez-Perez, Carlos Marti-Gastaldo, Marco Evangelisti, Samuel Manas-Valero, Eugenio Coronado, Jesus I. Martinez, Jose Ramon Galan-Mascaros, Fernando Luis
Summary: In this article, a novel 2D heterometallic oxalate complex is presented as a potential candidate for quantum spin liquid (QSL) material. It exhibits strong antiferromagnetic correlations and the absence of magnetic ordering, making it an appealing QSL candidate.
Article
Chemistry, Multidisciplinary
Javier Castells-Gil, Neyvis Almora-Barrios, Belen Lerma-Berlanga, Natalia M. Padial, Carlos Marti-Gastaldo
Summary: Research on metal-organic frameworks is moving towards more sophisticated concepts that use chemical complexity to encode their function or access new properties. The combination of different metals in these frameworks is still underexplored due to the challenges of controlling nucleation or post-synthetic incorporation. This is especially challenging for titanium-organic frameworks due to difficulties in controlling titanium chemistry in solution.
