Article
Chemistry, Multidisciplinary
Samuel Faucher, Matthias Kuehne, Volodymyr B. Koman, Natalie Northrup, Daichi Kozawa, Zhe Yuan, Sylvia Xin Li, Yuwen Zeng, Takeo Ichihara, Rahul Prasanna Misra, Narayana Aluru, Daniel Blankschtein, Michael S. Strano
Summary: Researchers utilized an experimental platform based on single-walled carbon nanotubes to study water under extreme nanoscale confinement. The changes in Raman radial breathing mode were shown to reflect the increase in interior mechanical modulus caused by liquid water filling under restricted conditions, with diameter-dependent patterns observed.
Review
Chemistry, Multidisciplinary
Jingjing Dai, Hongbo Zhang
Summary: The confinement effect in micro/meso-porous crystalline materials plays a crucial role in catalytic reactions, providing shape selectivity and modulating the surface electron distribution of active species, thereby affecting catalytic reactivity, selectivity, and stability. This systematic review offers valuable insights for researchers aiming to design excellent porous crystalline catalysts based on the concept of confinement effect in heterogeneous catalysis.
Article
Multidisciplinary Sciences
Haoran Qu, Archith Rayabharam, Xiaojian Wu, Peng Wang, Yunfeng Li, Jeffrey Fagan, Narayana R. Aluru, YuHuang Wang
Summary: Research has shown that single-wall carbon nanotubes can separate n-hexane from cyclohexane through nanopores, despite the fact that the kinetic diameters of these molecules are larger than the pore size. Simulations and experiments have revealed that n-hexane molecules can stretch inside the nanotube pores, challenging current understanding of nanopore selectivity.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Fenfa Yao, Mingyue Xia, Qing Zhang, Qiuqin Wu, Osamu Terasaki, Junfeng Gao, Chuanhong Jin
Summary: The confinement effect induced conformational evolution of one-dimensional (1D) phosphorus atomic chains encapsulated inside carbon nanotubes (CNTs) has been studied. The study shows that as the inner diameter of CNTs increases, the phosphorus chains change from monoatomic linear chain to (P8P2)n chains. These encapsulated (P8P2)n chains exhibit excellent structural stability and can serve as potential building blocks for nano-electronic and molecular electronic devices.
Article
Physics, Multidisciplinary
A. Mueller, A. L. D. Kilcoyne, S. Schippers, R. A. Phaneuf
Summary: This paper provides an overview of experimental investigations into the photoionization and fragmentation of fullerenes and endohedral fullerenes by absorption of a single short-wavelength photon. The study focused on the behavior of the Xe@C-60(+) molecular ion and discovered new reaction channels, recovering about 70% of the expected oscillator strength for the encapsulated Xe atom in the investigated energy range. The results are in agreement with previous relativistic R-matrix calculations.
Article
Chemistry, Multidisciplinary
Samuel Faucher, Matthias Kuehne, Hananeh Oliaei, Rahul Prasanna Misra, Sylvia Xin Li, Narayana R. Aluru, Michael S. Strano
Summary: Recent measurements have shown that fluids under extreme confinement, such as water in narrow carbon nanotubes, deviate significantly from theoretical descriptions. In this study, precise replicas of carbon nanotubes filled with water were generated and analyzed using Raman spectroscopy. The results revealed the presence of submicron vapor-like and liquid-like domains in partially filled nanodroplet states, and a Clausius-Clapeyron-type model was used to calculate the heats of condensation of water inside different diameter carbon nanotubes. The findings suggest the potential of molecular engineering of nanoconfined liquid/vapor interfaces for water treatment or membrane distillation.
Article
Chemistry, Multidisciplinary
A. Prekob, L. Vanyorek, Z. Fejes
Summary: The study found that the BCNT support exhibited higher selectivity towards benzhydrol during the hydrogenation of benzophenone, possibly due to the presence of covalently bonded nitrogen atoms that can inhibit over-hydrogenation processes.
MATERIALS TODAY CHEMISTRY
(2021)
Article
Chemistry, Physical
Dingding Yao, Haiping Yang, Qiang Hu, Yingquan Chen, Hanping Chen, Paul T. Williams
Summary: In this study, carbon nanotubes were produced from post-consumer mixed waste plastics using a pyrolysis-catalysis process, with the Ni-Fe/MCM41 catalyst displaying the highest catalytic activity. The order of catalytic activity was related to differences in catalyst pore volume and catalyst reducibility, with the formation of a Ni-Fe alloy suggested to be crucial for the promotion of carbon nanotube formation. By-product production of hydrogen at large quantities could be utilized as process fuel.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
A. Bautista Hernandez, Wilfredo Ibarra Hernandez, F. Severiano, E. Garcia Hernandez, E. Chigo Anota, M. Salazar Villanueva
Summary: The structural and electronic properties of Zn-m@C-60 and Zn-m@C-70 endohedral metallofullerenes (m = 1-5) were investigated using DFT calculations. Despite having higher binding energies, these endohedral metallofullerenes are energetically stable. Encapsulating Zn-4 and Zn-5 clusters inside C-60 and C-70 fullerenes leads to structural transformations and electronic changes, improving their absorption of visible and ultraviolet light. These properties have potential applications in areas such as heavy metal encapsulation, electronic device design, gas sensors, and solar cells.
SURFACES AND INTERFACES
(2021)
Article
Chemistry, Applied
Leticia Forrer Sosa, Victor Teixeira da Silva, Priscilla M. de Souza
Summary: Carbon nanotubes supported nickel catalysts were evaluated for the hydrogenation of levulinic acid to gamma-valerolactone. The catalysts prepared from nickel nitrate and nickel hydroxide salts showed higher activity compared to those prepared from nickel acetate salts, likely due to better metal dispersion.
Article
Chemistry, Multidisciplinary
Jie Tang, Tingting Ge, Wenxuan Wang, Chao Liu, Jiahui Huang
Summary: Studying the modulation of nanoclusters at an atomic scale is crucial for understanding the correlation between properties and catalytic performance. In this study, we synthesized and characterized Pd-n (n = 2-5) nanoclusters coordinated with di-1-adamantylphosphine. Pd-5 nanoclusters exhibited the highest catalytic performance (conversion = 99.3%, selectivity = 95.3%) for the hydrogenation of cinnamaldehyde to hydrocinnamaldehyde, with XPS identifying Pd & delta;+ as the key active component. The objective of this work was to explore the relationship among the number of Pd atoms, their electronic structure, and catalytic activity.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Magdalena Kierkowicz, Elzbieta Pach, Julio Fraile, Concepcion Domingo, Belen Ballesteros, Gerard Tobias
Summary: This study investigates the impact of annealing temperature on the structure and morphology of single-walled carbon nanotubes (CNTs), finding that the fraction of end-closed CNTs increases with temperature and the filling yield of encapsulated payload also rises. Thermal treatment does not affect the tubular structure of CNTs, and insight is provided into the efficacy of filling from the molten phase at different annealing temperatures.
Article
Chemistry, Physical
Bin-Hao Chen
Summary: The adsorption properties of hydrogen molecules in twisted double-walled carbon nanotubes were investigated, and it was found that the amount of stored hydrogen and the kinetic diameter of hydrogen molecules are influenced by the degree of twisting. Additionally, the adsorption heat was found to depend on the extent of twisting.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Applied
Song Lv, Liya Ma, Xinyu Shen, Hua Tong
Summary: Porous carbon nanotubes are a promising electrode material for supercapacitors, with high specific surface area and excellent electrochemical performance. Factors affecting their growth have been identified, and discussions on the relationships between their morphology and structure have been made.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Chemistry, Applied
Rongju Zhong, Jingmei Tao, Xu Yang, Zhihua Fu, Hongmei Yang, Zhoumeng Pu, Rui Bao, Yichun Liu, Jianhong Yi
Summary: This study investigates the influence of oxygen-containing functional groups (OCFGs) on the filling rate of CNTs by filling Cu nanoparticles into acid-treated CNTs. The results show that excessive OCFGs can hinder the filling rate of CNTs, providing a new perspective for the application of CNTs in composite preparation and related fields.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Biochemistry & Molecular Biology
Ottavia Bellotto, Slavko Kralj, Michele Melchionna, Paolo Pengo, Matic Kisovec, Marjetka Podobnik, Rita De Zorzi, Silvia Marchesan
Summary: This study investigated the self-assembling behavior of distinct stereoisomers of Ile-Phe and Phe-Ile in PBS to form hydrogels, confirming peptide purity and identity through NMR, mass spectrometry, and crystalline XRD data. One stereoisomer was found to exhibit fast kinetics and the highest elastic modulus, making it the only gelator in the study to self-organize into stable hydrogels with distinctive features.
Article
Chemistry, Inorganic & Nuclear
Giuseppe Gentile, Cristian Rosso, Alejandro Criado, Valentina Gombac, Giacomo Filippini, Michele Melchionna, Paolo Fornasiero, Maurizio Prato
Summary: The study developed an efficient heterogeneous catalytic system for driving Knoevenagel condensation reactions between benzaldehydes and malononitrile. The catalyst, CNO-NaOH, showed high reactivity and good tolerance towards functional group variations of the reagents, making it a potential new recyclable structure for organic base catalysis.
INORGANICA CHIMICA ACTA
(2022)
Review
Chemistry, Multidisciplinary
Miriam Marchi, Giuseppe Gentile, Cristian Rosso, Michele Melchionna, Paolo Fornasiero, Giacomo Filippini, Maurizio Prato
Summary: Dual photocatalysis, combining Earth-abundant nickel-based catalytic systems with visible-light-activated photoredox catalysts, has become a powerful tool for functionalization of organic molecules under mild conditions. This relatively new branch of catalysis has inspired interdisciplinary research and established itself as a dominant trend in modern organic synthesis.
Article
Chemistry, Multidisciplinary
Arianna Actis, Michele Melchionna, Giacomo Filippini, Paolo Fornasiero, Maurizio Prato, Enrico Salvadori, Mario Chiesa
Summary: This study assesses the influence of morphology and light-excitation on the number and chemical nature of radical defects in carbon nitride (CN) and derives the spatial distribution of native radicals in CN using magnetic dipole-dipole coupling.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Organic
Giuseppe Gentile, Miriam Marchi, Michele Melchionna, Paolo Fornasiero, Maurizio Prato, Giacomo Filippini
Summary: Dual photocatalysis has become popular for functionalizing organic substrates under mild conditions. Single-atom heterogeneous catalysts (SACs) with carbon nitride-based supports have emerged as a frontier in this research field. This Concept highlights recent advances and applications of carbon nitride-based SACs in light-driven dual-catalytic processes, as well as future opportunities.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Jonathan Filippi, Hamish A. Miller, Lucia Nasi, Maria V. Pagliaro, Andrea Marchionni, Michele Melchionna, Paolo Fornasiero, Francesco Vizza
Summary: This study investigates the performance of a Cobalt@N-doped graphitic carbon core-shell nanohybrid electrocatalyst in a complete cell, and by optimizing the flow rate and potential, it can efficiently produce H2O2 with a high concentration of up to 1 wt%.
MATERIALS TODAY ENERGY
(2022)
Article
Chemistry, Physical
Luka Suhadolnik, Marjan Bele, Miha Cekada, Primoz Jovanovic, Nik Maselj, Anja Loncar, Goran Drazic, Martin Sala, Nejc Hodnik, Janez Kovac, Tiziano Montini, Michele Melchionna, Paolo Fornasiero
Summary: A versatile approach for producing cluster- and single atom-based thin-film electrode composites is described in this article. The TiOxNy-Ir catalyst developed in this study was prepared from sputtered Ti-Ir alloy with 0.8 +/- 0.2 at % Ir in alpha-Ti solid solution. The prepared catalyst exhibited high oxygen evolution reaction activity and has potential applications in electrocatalysis. The article provides a detailed description of the new method and a high-performance thin film catalyst, along with suggestions for future development in this field.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Arianna Actis, Michele Melchionna, Giacomo Filippini, Paolo Fornasiero, Maurizio Prato, Mario Chiesa, Enrico Salvadori
Summary: Time-resolved EPR technique was used to study the formation of well-defined spin triplet excitons in carbon nitride. The mobility of the triplet excitons was revealed through the analysis of temperature-dependent TR-EPR signal. It was found that the energy of the spin triplet is approximately 0.2 eV higher than the conduction band edge, suggesting the inversion of singlet-triplet in carbon nitride materials. This study provides important insights into the response of carbon nitride to light and the nature of photoexcited states.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Giuseppe Sportelli, Gaia Grando, Manuela Bevilacqua, Giacomo Filippini, Michele Melchionna, Paolo Fornasiero
Summary: In this study, the use of graphitic carbon nitride (g-CN) for the photocatalytic radical formylation of anilines is proposed as a sustainable and attractive alternative to current methods. The reaction occurs under mild conditions and employs air as an oxidant. The ability of g-CN to reach an excited state upon visible-light absorption plays a crucial role in triggering the formation of reactive a-amino radical species from anilines.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Giuseppe Gentile, Marc Morant-Giner, Lucia Cardo, Michele Melchionna, Paolo Fornasiero, Maurizio Prato, Giacomo Filippini
Summary: 2H-MoS2 is a promising semiconductor with earth-abundant nature, low toxicity, and low cost. Although it has demonstrated good catalytic activity in various energy-related processes, its application in catalysis for C-C bond forming reactions in organic synthesis remains largely unexplored. The challenges arise from the difficulty of using bulk 2H-MoS2 due to its low surface area, which requires high catalytic loadings for acceptable yields and makes the optimization process expensive and tedious. In this study, we developed a 2H-MoS2-mediated synthesis of valuable bis(indolyl)methane derivatives and optimized the reaction conditions using the Design of Experiments method.
Article
Chemistry, Physical
Yu Zhang, Luca Mascaretti, Michele Melchionna, Olivier Henrotte, Stepan Kment, Paolo Fornasiero, Alberto Naldoni
Summary: A fabrication approach was developed to create TiN/F-doped carbon hybrids with high catalytic activity for H2O2 production. These hybrids showed a maximum H2O2 selectivity of 90% and achieved a H2O2 productivity of 207 mmol g(TiN) (-1) h(-1) at 0.2 V vs RHE. The formation of nanocomposites played a key role in achieving high currents, with increased TiO x N y surface content promoting higher H(2)O(2) selectivity and fluorinated nanocarbon imparting good stability to the electrodes due to their superhydrophobic properties.
Article
Chemistry, Physical
Anna Lenarda, Michele Melchionna, Santeri Aikonen, Tiziano Montini, Paolo Fornasiero, Tao Hu, Michael Hummel, Juho Helaja
Summary: Activated carbons obtained from organosolv lignin were used as catalysts for aerobic oxidative dehydrogenation (ODH) reactions. The relationship between structure and activity was investigated, and the distribution of oxygen functionality was found to play a crucial role. The catalytic activity was associated with C=O surface functionalities, which was confirmed by blocking experiments. The breadth of the catalysts' applicability was explored through selected relevant ODH reactions.
Article
Chemistry, Multidisciplinary
Miriam Marchi, Edoardo Raciti, Sai Manoj Gali, Federica Piccirilli, Hendrik Vondracek, Arianna Actis, Enrico Salvadori, Cristian Rosso, Alejandro Criado, Carmine D'Agostino, Luke Forster, Daniel Lee, Alexandre C. Foucher, Rajeev Kumar Rai, David Beljonne, Eric A. Stach, Mario Chiesa, Roberto Lazzaroni, Giacomo Filippini, Maurizio Prato, Michele Melchionna, Paolo Fornasiero
Summary: The manipulation of carbon nitride (CN) structures through microwave treatment enhances the activity of CN-based photocatalysts for Ni dual photocatalysis. This approach improves the efficiency of C-X (X = N, S, O) couplings in organic synthesis reactions. The formation of carbon vacancies and subsequent evolution into triazole and imine N species play a crucial role in the enhanced reactivity of the material.
Article
Chemistry, Multidisciplinary
Daniel Iglesias, Raul Martin, Miguel A. Alvarez-Sanchez, Irene Badia-Dominguez, Ester Vazquez, M. Carmen Ruiz Delgado, Pilar Prieto, M. Antonia Herrero
Summary: Carbon nanohorns were non-covalently functionalized with two different benzothiadiazoloquinoxalines via Stille cross-coupling reactions and solvent-free microwave irradiation. The organic molecules and nanostructures exhibited close interactions, leading to significant Raman enhancement and making them appealing for various applications. Both experimental physico-chemical characterization and in silico studies were conducted to gain insights into these phenomena. The processability of the hybrids allowed for the preparation of homogeneous films on diverse substrates.
Article
Chemistry, Multidisciplinary
Edoardo Raciti, Sai Manoj Gali, Michele Melchionna, Giacomo Filippini, Arianna Actis, Mario Chiesa, Manuela Bevilacqua, Paolo Fornasiero, Maurizio Prato, David Beljonne, Roberto Lazzaroni
Summary: By using density functional theory calculations and experimental EPR measurements, the study reveals that structural defects on the gCN surface can create distinctive radical defect states that are essential for photo-activity in certain amorphous and reduced gCN structures. These defect types act as binding sites for specific radical precursors, facilitating photo-induced charge transfer and triggering specific photo-chemical processes for desired reactions.
