Article
Chemistry, Multidisciplinary
Marjan Darwish, Camila Mafla-Gonzalez, Belmin Kolenovic, Adrianna Deremer, Daniel Centeno, Tianchi Liu, Deok-Yang Kim, Thomas Cattabiani, Thomas J. Drwiega, Ish Kumar, Clive Li, Christian Traba
Summary: This study reports the synthesis of gold, silver, and copper nanoparticles using argon plasma reduction of cations. The results demonstrate that this method is a rapid, green, and versatile approach for the synthesis of both noble and non-noble metal nanoparticles.
Article
Chemistry, Physical
R. Gustavo J. Chacon, Fabiano S. Rodembusch, Brunno L. Albuquerque, Wellington D. G. Goncalves, Jonder Morais, Daniel L. Baptista, Allan de Moraes Lisboa, Adriano Feil, Dario Eberhardt, Jose Espeso, Jairton Dupont
Summary: In this study, a photocatalytic device based on gold nanoparticles coated with an ionic liquid was developed for hydrogen evolution reactions via methanol photo reforming and photocatalytic water-splitting. The device prepared through magnetron sputtering exhibited direct Au-TiO2 interactions and the presence of the ionic liquid enhanced the photocatalytic performance. The results showed high apparent quantum yield values for hydrogen evolution using the prepared materials.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Polymer Science
Yongqi Yang, Xiawei Li, Youjun Yan, Rongkai Pan, Jun Liu, Meng Lian, Xin Luo, Guangyao Liu
Summary: Poly(ionic liquids) (PILs) demonstrate improved durability, processability, and mechanical stability compared to ionic liquids. In this study, PIL nanoparticles with various morphologies were successfully synthesized using polymer self-assembly method. This efficient approach for preparing functionalized PIL nano-objects with controlled morphologies represents significant progress in the field.
Article
Chemistry, Physical
Geeta Durga, Pooja Kalra, Vinay Kumar Verma, Kanjur Wangdi, Anuradha Mishra
Summary: Ionic liquids have established themselves as a preferred solvent in synthetic chemistry, particularly in polymer chemistry. They are versatile solvents used for polymeric reactions and can also be polymerized to enhance their inherent properties, finding applications in various fields such as electrochemical devices, nanocomposites, optoelectronics, and more. This comprehensive review covers both aspects of ILs as a solvent in polymeric reactions and their polymeric form, poly(ionic liquids), presenting their diverse potential applications.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Physical
Stephanie Boullanger, Emmanuel Contal, Cedric C. Buron, Lydie Viau
Summary: Pyrrole-functionalized imidazolium surfactants with different alkyl chain lengths were synthesized and their aggregation properties in water were investigated. It was found that these surfactants exhibited lower critical micellar concentration compared to their non-functionalized analogues. The structure of the aggregates formed and the preparation of water-stable polypyrrole nanoparticles were also studied.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Physical
Xuefeng Pan, Zdravko Kochovski, Yong-Lei Wang, Radwan M. Sarhan, Eneli Haerk, Siddharth Gupta, Sasho Stojkovikj, Gumaa A. El-Nagar, Matthew T. Mayer, Robin Schuermann, Jerome Deumer, Christian Gollwitzer, Jiayin Yuan, Yan Lu
Summary: In this study, a straightforward and scalable synthetic route was developed to fabricate poly(ionic liquid) (PIL) homopolymer nanovesicles (NVs) with tunable particle size and shell thickness. By increasing the monomer concentration, the morphology of the NVs changed from hollow structures to dense spheres and then to directional worms. The internal morphology transformation of NVs was investigated using simulations, which revealed a correlation between PIL chain length and NVs shell thickness. The functionalized PIL NVs were employed as electrocatalysts for CO2 electroreduction and exhibited enhanced selectivity towards C1 products due to strong electronic interactions with ultra-small copper nanoparticles (CuNPs).
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Physical
Yong-Ya Zhang, Nan Zhang, Peng Peng, Rui Wang, Yan Jin, Ya-Kun Lv, Xin Wang, Wei Wei, Shuang-Quan Zang
Summary: By utilizing divinyl functionalized ionic liquids, Ru nanoparticles supported on nitrogen-doped carbon frameworks were synthesized, showing excellent stability and efficiency for hydrogen production via water splitting. The optimized catalyst exhibited low overpotential and Tafel slope, and maintained stability even after 10,000 cycles, demonstrating promising industrial applications. This work not only presents a facile method for preparing efficient Ru-based catalysts, but also provides insights for synthesizing highly dispersed metallic nanoparticles for specific applications.
Article
Chemistry, Multidisciplinary
Jared I. Bowman, Cabell B. Eades, Maria A. Vratsanos, Nathan C. Gianneschi, Brent S. Sumerlin
Summary: Polymerization-induced self-assembly (PISA) is a powerful technique for producing block copolymer nanostructures, and ultrafast photoiniferter PISA can be used to quickly create various nanostructures.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Polymer Science
Qunying Wang, Sergey Popov, Veronika Strehmel, Jochen S. Gutmann, Bernd Strehmel
Summary: A series of cyanines with varying methine chain lengths and terminal groups were reacted with a specific cation after excitation in the NIR region, resulting in the generation of free radicals and conjugate acids. This study investigated the efficiency of free radical and cationic polymerization, as well as their combination as a hybrid system. By using NIR-LED exposure and varying the sensitizers, different photopolymerization efficiencies were achieved. The results showed that the combination of free radical and cationic polymerization can work effectively in hybrid systems.
Article
Polymer Science
Oscar Ramirez, Matias Leal, Ximena Briones, Marcela Urzua, Sebastian Bonardd, Cesar Saldias, Angel Leiva
Summary: This study reports the synthesis of hybrid nanocomposites with catalytic activity by combining polymer nanofibers and gold nanoparticles. The nanofibers were obtained through electrospinning blends of a poly (ionic liquid) and its precursor polymer. The results showed that the nanofiber characteristics depended on the proportion of polymer in the blends. The obtained nanofibers were used to synthesize gold nanoparticles on their surface, which significantly improved the performance of the nanofibers in ion adsorption and catalytic reactions.
Article
Polymer Science
Honggang Mei, Bingjie Zhao, Huaming Wang, Sixun Zheng
Summary: The preparation of crosslinked PDCPD nanoparticles via ROMP-induced self-assembly approach was reported in this communication. The morphology of the obtained nanoparticles varied from spherical, cylindrical to planar depending on the molecular weights of Macro-CTAs, the concentrations of DCPD and the natures of solvents. The ROMPISA method provides a new and efficient approach to prepare crosslinked polymer nanoparticles.
MACROMOLECULAR RAPID COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Arifa Shaheen, Arun Dhanagar, Rabia Arif
Summary: The interaction between anionic quantum dots (QDs) and a gemini surfactant [C(16)Im-3OH-ImC(16)]Br-2 in water resulted in luminescent self-assemblies. The surfactant self-associates into micelles before engaging with the QDs. The addition of the surfactant to the QD solution led to the formation of supramolecular and vesicle structures, with self-assembled QDs inside the spherical vesicles exhibiting luminescence.
Review
Chemistry, Multidisciplinary
Csilla Gyorgy, Steven P. Armes
Summary: It is well-known that polymerization-induced self-assembly (PISA) is a powerful technique for synthesizing colloidal dispersions of diblock copolymer nanoparticles. This review article aims to summarize the advances in PISA syntheses in non-polar media since the last review article in 2016. The article discusses PISA syntheses using RAFT polymerization in various non-polar solvents and examines the morphological transitions and rheological properties of the formed nanoparticles.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Satoru Masubuchi, Masato Sakano, Yuma Tanaka, Yusai Wakafuji, Takato Yamamoto, Shota Okazaki, Kenji Watanabe, Takashi Taniguchi, Jincai Li, Hirotaka Ejima, Takao Sasagawa, Kyoko Ishizaka, Tomoki Machida
Summary: This paper presents a dry pick-and-flip assembly technique for angle-resolved photoemission spectroscopy (ARPES) of van der Waals heterostructures. By altering the glass transition temperature of polymers, the flipping assembly of 2D heterostructures is achieved.
SCIENTIFIC REPORTS
(2022)
Article
Biochemistry & Molecular Biology
Francisco Jose Alguacil, Jose Ignacio Robla
Summary: This study investigated the solvent extraction of gold(III) from HCl media using pseudo-protic ionic liquids (PPILs) dissolved in toluene as the extractant phase. Three PPILs were generated from commercially available amines and 1 M HCl solution. The interaction coefficients (e) for the pair AuCl4-, H+ in the systems involving the three PPILs were estimated using the Specific Interaction Theory. Gold(III) was recovered from the metal-loaded organic phases using sodium thiocyanate solutions, and gold was finally recovered as zero-valent gold (ZVG) nanoparticles.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Applied
Tugce Gunay Semerci, Arianna Melillo, Yasemin Cimen Mutlu, Hermenegildo Garcia
Summary: Simulated sunlight driven overall water splitting was achieved using porphyrin-based PCN-222 metalorganic frameworks with various transition metals. PCN-222(Zn) exhibited the highest H2 evolution reaction (HER) efficiency, surpassing porphyrinic MOFs with Pt. In addition, oxygen evolution was detected in a quasi stoichiometric ratio to H2. Transient absorption spectroscopy measurements provided evidence for charge separation and oxidation of H2O by positive holes. This study offers insights for the development of noble metal-free photocatalysts for water splitting and future experiments for uphill reactions.
Article
Chemistry, Multidisciplinary
Arianna Melillo, Antonio Franconetti, Mercedes Alvaro, Belen Ferrer, Hermenegildo Garcia
Summary: This study investigates the role of transition metal nanoparticle catalysts in the hydrogenation of multiple bonds. The results demonstrate that metal nodes of MIL-101(Cr) and UiO-66 can promote the hydrogenation of polarized X=Y double bonds in the absence of metal nanoparticles. The catalytic activity is dependent on the composition of the metal node and the organic linker.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Review
Chemistry, Applied
Kayhaneh Berijani, Ali Morsali, Hermenegildo Garcia
Summary: Metal-organic frameworks (MOFs) are a type of porous materials with diverse applications. Recently, there has been increasing interest in synthesizing MOFs with multimodal pores, which can enhance the performance of MOFs in different applications.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Review
Energy & Fuels
Saravanan Nagappan, Malarkodi Duraivel, Vijayakumar Elayappan, Nallal Muthuchamy, Balaji Mohan, Amarajothi Dhakshinamoorthy, Kandasamy Prabakar, Jae-Myung Lee, Kang Hyun Park
Summary: Recently, metal-organic frameworks (MOFs)-based cathode materials have gained significant attention for their high surface area, controlled architecture, porosity, and tunability. By altering the synthesis techniques, the performance of MOF-based cathodes can be improved for specific battery applications. The review article provides a comprehensive overview of the uniqueness and history of MOF-based cathodes, their advantages and disadvantages, various synthesis approaches, and their use in different battery applications.
Article
Chemistry, Multidisciplinary
Sara Oudi, Ali Reza Oveisi, Saba Daliran, Mostafa Khajeh, Amarajothi Dhakshinamoorthy, Hermenegildo Garcia
Summary: Researchers designed and synthesized a porphyrin-based covalent organic framework (COF) called Porph-UOZ-COF. The COF exhibited outstanding catalytic performance under visible-light, without the need for additives or metals, and could be reused. This study demonstrates the potential of COFs as metal-free catalysts for tandem reactions.
Article
Chemistry, Physical
Alberto Garcia-Baldovi, Lu Peng, Amarajothi Dhakshinamoorthy, Abdullah M. Asiri, Ana Primo, Hermenegildo Garcia
Summary: Ni nanoparticles (approximate to 8 nm) strongly grafted on N-doped graphitic carbon matrix, supported by chitosan, were used as catalyst for H2 storage/release on N-ethylcarbazole (EC). The addition of minute amounts (18 ppm) of Pt significantly increased the H2 storage/release activity of Ni@(N)C due to effect of Pt promoting H spill over the Ni NPs. After four cycles, (Pt)Ni@(N)C exhibited some fatigue in the H2 storage/release of the same EC batch, but no changes were observed in the XRD, TEM and XPS characterization of the catalyst.
CATALYSIS COMMUNICATIONS
(2023)
Article
Energy & Fuels
Arianna Melillo, Maria Cabrero-Antonino, Belen Ferrer, Amarajothi Dhakshinamoorthy, Herme G. Baldovi, Sergio Navalon
Summary: In this study, a series of novel MOF-on-MOF composites were prepared and their photocatalytic activity in overall water splitting under simulated sunlight irradiation was examined. Among these composites, UiO-66(Zr)-NH2@UiO-66(Ce) exhibited promising photocatalytic activity. The enhanced activity of UiO-66(Zr)-NH2@UiO-66(Ce) was attributed to its appropriate energy band diagram and ability for photoinduced charge separation, as revealed by various spectroscopic measurements.
Article
Chemistry, Multidisciplinary
Saravanan Nagappan, Malarkodi Duraivel, SeongHoon Han, Mohammad Yusuf, Manjiri Mahadadalkar, KyeongMun Park, Amarajothi Dhakshinamoorthy, Kandasamy Prabakar, Sungkyun Park, Chang-Sik Ha, Jae-Myung Lee, Kang Hyun Park
Summary: Graphene, a two-dimensional material with a large surface area, is widely used in various fields. Recently, there has been increased focus on developing metal-free graphenes doped with heteroatoms as efficient electrocatalysts for oxygen reduction reactions (ORRs). Our study found that graphene prepared from graphene oxide (GO) by pyrolysis under a nitrogen atmosphere at 900 degrees C showed better ORR activity compared to pristine GO. Various pyrolysis conditions were tested, and the results suggest that the ORR electrocatalytic activity of graphene is influenced by these conditions. The prepared graphenes, particularly G100-1B and G100-2B, displayed promising ORR activity for fuel cell and metal-air battery applications.
Article
Chemistry, Physical
Ruben Ramirez, Arianna Melillo, Silvio Osella, Abdullah M. Asiri, Hermenegildo Garcia, Ana Primo
Summary: A general method is reported to prepare MXene quantum dots (MxQDs) with yields over 20% by liquid-phase laser ablation of the MAX phase. Mechanical and thermal shock by 532 nm laser pulses produces MAX etching and exfoliation to form MXene QDs, avoiding the use of HF. The method is applied to various MAX phases and the MXene size reduction to the nanometric scale allows for control of the band gap. The MXene QDs show high photocatalytic activity for hydrogen evolution.
Article
Nanoscience & Nanotechnology
Arghyadeep Bhattacharyya, Mario Gutierrez, Boiko Cohen, Horatiu Szalad, Josep Albero, Hermenegildo Garcia, Abderrazzak Douhal
Summary: Mixed-metal-organic frameworks (MMOFs) with Ce doping have been studied for their photocatalytic performance. A series of MMOFs isostructural to UiO-66 were synthesized and characterized, and it was found that when the Ce content reached 9%, the highest photocatalytic efficiency was achieved.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Shan Dai, Eva Montero-Lanzuela, Antoine Tissot, Herme G. G. Baldovi, Hermenegildo Garcia, Sergio Navalon, Christian Serre
Summary: In this study, the researchers reported for the first time the efficient synthesis of highly redox active Ce(iv)-MOFs through room temperature synthesis. These Ce(iv)-MOFs showed excellent photocatalytic activities in hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), and Ce-UiO-66-NH2 combined with supported Pt NPs exhibited the highest activity in overall water splitting under simulated sunlight irradiation due to efficient photoinduced charge separation.
Article
Materials Science, Multidisciplinary
Marco Serra, Nikolas Antonatos, Jan Luxa, Luc Lajaunie, Josep Albero, Agata Sabik, Wojciech M. Linhart, Hermenegildo Garcia, Robert Kudrawiec, David Sedmidubsky, Zdenek Sofer
Summary: A NiGa2S4 photodetector was prepared and its photoresponse behavior in different electrolyte solutions was investigated. The results showed that ethanol, as an electron donor, significantly improved the performance of the photodetector and expanded its spectral response range. The dynamics of photogenerated electrons and holes were studied, and the stability of the fueled PEC photodetector was evaluated through long-term tests. This work provides fundamental insight into PEC semiconductor-based photodetectors and offers an extendable strategy for engineering high-performance PEC devices.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Physical
Parisa Alamdari, Farhad Sharif, Saeedeh Mazinani, German Sastre, Hermenegildo Garcia
Summary: Graphene research focuses on altering the structure to improve performance and induce new properties. This study specifically investigates the conversion between hexagon and non-hexagon rings as a tool to control the electronic structure of graphene. The study also explores the possibility of converting pentagon-octagon-pentagon rings to pentagon-heptagon pair rings and examines the influence of heteroatom doping on these transformations.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Christian Mark Pelicano, Jiaxin Li, Maria Cabrero-Antonino, Ingrid F. Silva, Lu Peng, Nadezda V. Tarakina, Sergio Navalon, Hermenegildo Garcia, Markus Antonietti
Summary: We have successfully designed carbon/potassium poly(heptazine imide) heterostructures via a one-step salt-melt assisted condensation method for efficient photocatalysis. By hybridizing adenine-derived carbonaceous material (Ad-carbon) with KPHI, the photocatalytic activity for H-2 evolution and H2O2 production significantly improved. We found that Ad-carbon acts as both an electron acceptor and a photosensitizer, and the intimate heterojunction between Ad-carbon and KPHI promotes charge separation and extends carrier lifetime. Electrocatalysis experiments confirmed that coupling Ad-carbon with KPHI enhances surface reaction kinetics for H-2 evolution and O-2 reduction reactions. The visual evidence of superior charge transport in the hybrid photocatalyst is demonstrated by the uniform distribution of smaller Pt nanoparticles on the carbon regions, which contributes to the increased catalytic activity.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
