Article
Chemistry, Multidisciplinary
Raffaella Breglia, Daniele Perilli, Cristiana Di Valentin
Summary: This paper investigates the potential electrocatalysts for oxygen evolution and reduction reactions by embedding several transition metal atoms in N-doped graphene using hybrid density functional theory (DFT) calculations. The study finds that Ni and Fe are the most promising systems for the reactions based on overpotential values. Additionally, considering low-spin configurations changes the order of activity between different electrocatalytic systems.
MATERIALS TODAY CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Kolleboyina Jayaramulu, Michael Horn, Andreas Schneemann, Haneesh Saini, Aristides Bakandritsos, Vaclav Ranc, Martin Petr, Vitalie Stavila, Chandrabhas Narayana, Blazej Scheibe, Stepan Kment, Michal Otyepka, Nunzio Motta, Deepak Dubal, Radek Zboril, Roland A. Fischer
Summary: The study demonstrates the covalent attachment of an amine functionalized metal-organic framework to carboxylate functionalized graphene, resulting in a hybrid material with high capacitance and cycling stability. An asymmetric supercapacitor was successfully constructed using this hybrid material, showing comparable performance to commercial devices such as Pb-acid and Ni/MH batteries. The amide linkage plays a key role in forming a p-conjugated structure, facilitating charge transfer and enhancing capacitance and cycling stability.
ADVANCED MATERIALS
(2021)
Article
Multidisciplinary Sciences
Chengjun Kang, Zhaoqiang Zhang, Shibo Xi, He Li, Adam K. Usadi, David C. Calabro, Lisa Saunders Baugh, Yuxiang Wang, Dan Zhao
Summary: This study reports a CO2 capture mechanism of doped covalent organic frameworks (COFs), which significantly increases the CO2 adsorption capacity. This discovery provides new insights into developing chemistry for CO2 capture and conversion.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Multidisciplinary
Si-Guo Wu, Long-Fei Wang, Ze-Yu Ruan, Shan-Nan Du, Silvia Gomez-Coca, Zhao-Ping Ni, Eliseo Ruiz, Xiao-Ming Chen, Ming-Liang Tong
Summary: In this study, a rare cationic metal-organic framework with hysteretic spin-crossover behavior and redox-programmable capability is reported. The stepwise spin-crossover dynamics can be manipulated by chemical redox reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Dan Chen, Weiben Chen, Guang Zhang, Shen Li, Weihua Chen, Guolong Xing, Long Chen
Summary: This study successfully synthesized two highly ordered N-rich COFs by designing a novel heptazine monomer and condensing it with aromatic amines, one of which showed significantly enhanced photocatalytic performance under mild conditions compared to the pristine photocatalyst.
Article
Chemistry, Multidisciplinary
Wen-Ya Zhi, Yu-Ting Liu, Si-Li Shan, Cheng-Jie Jiang, Huan Wang, Jia-Xing Lu
Summary: In this study, Cu/Cu2O@NG materials were prepared using a simple MOFs-derivatized strategy for efficient CO2 electroreduction. The synergistic effect between Cu/Cu2O and NG significantly enhanced CO2 adsorption capacity and active site abundance, leading to improved catalytic performance in producing C-2-C-3 products.
JOURNAL OF CO2 UTILIZATION
(2021)
Article
Chemistry, Physical
Huiqian Yang, Bo Wang, Yidi Li, Hongmei Du, Jinsheng Zhao, Yu Xie
Summary: Covalent organic frameworks (COFs) with metal complexing ligand COF-phen and COF-bpy have been designed and prepared. They can complex with Sn4+ to form COF-phen-Sn and COF-bpy-Sn. In this study, these metal ion complexed COFs are used as precursors for the preparation of composite materials SnO2 @NCNR-x with nano SnO2 embedded in N-doped carbonaceous materials. SnO2 @NCNR-1 shows high reversible specific capacity as an anode material for LIBs, due to its high specific area, highly dispersed SnO2 nanoparticles, and improved conductivity.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Analytical
Asad Ali, Naseem Iqbal, Tayyaba Noor, Umair Imtiaz
Summary: This study investigates a novel catalyst based on nitrogen-doped carbon and manganese-zinc nanocomposite for the oxygen reduction reaction in an alkaline medium. The nanostructured composite surpasses the commercial platinum/carbon catalyst in terms of material resources and application efficacy, exhibiting lower overpotential and higher activity for oxygen reduction, as well as tolerance to methanol.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Elisabet De Bolos, Marta Martinez-Abadia, Felix Hernandez-Culebras, Alison Haymaker, Kyle Swain, Karol Strutynski, Benjamin L. Weare, Javier Castells-Gil, Natalia M. Padial, Carlos Marti-Gastaldo, Andrei N. Khlobystov, Akinori Saeki, Manuel Melle-Franco, Brent L. Nannenga, Aurelio Mateo-Alonso
Summary: This study reports the synthesis of a crystalline one-dimensional polymer in solution by dynamic covalent chemistry, with the structure of the polymer confirmed by microcrystal electron diffraction, showing how the stacked chains of the polymer generate optimal channels for charge transport.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Engineering, Environmental
Peng Hu, Fengping Xiao, Yifei Wu, Xuming Yang, Na Li, Hongkang Wang, Jianfeng Jia
Summary: In this study, a novel nitrogen-doped graphene/sulfur cathode material was developed. Sulfur was homogeneously incorporated into the graphene-based host through a vapor-infiltration method, and a polydopamine-derived nitrogen-doped carbon layer was coated to improve the sulfur content. The obtained cathode material showed excellent cycle stability in room temperature sodium-sulfur battery.
CHEMICAL ENGINEERING JOURNAL
(2022)
Review
Chemistry, Physical
Lingjun Kong, Ming Liu, Hui Huang, Yunhua Xu, Xian-He Bu
Summary: Metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs) are emerging families of functional materials with immense potential for high-performance electrode materials for metal-ion batteries. Despite their advantages, MOFs/COFs and their derivatives face challenges as cathode materials.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Lei Fang, Gaozhang Gou, Jin Shang, Mingxian Liu, Qinfen Gu, Liangchun Li
Summary: Covalent triazine frameworks (CTFs) can form versatile metal-N single-atom coordination sites as promising catalytic centers. A five-step strategy involving spin states has been established for hierarchical high-throughput screening of M/CTFs (M = Transition metal) as excellent catalysts for nitrogen reduction reaction (NRR). Among the potential candidates, Cr/CTF shows excellent performance for nitrogen fixation with strong inhibition of hydrogen evolution reaction (HER) and good thermodynamic stability, narrow band gap, moderate adsorption energy, large activation energy, and theoretical Faradaic efficiency of 100%.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Zhi-yuan Mei, Genfu Zhao, Chenfeng Xia, Sheng Cai, Qi Jing, Xuelin Sheng, Han Wang, Xiaoxiao Zou, Lilian Wang, Hong Guo, Bao Yu Xia
Summary: A new type of covalent organic frameworks has been developed by assembling cobalt-nitrogen-carbon configurations onto carbon nanotubes using linkers with different electronic effects. This innovative method has resulted in an efficient electrocatalyst for oxygen reduction, which is understood through in situ spectroelectrochemistry and the bond order theorem. The strong interaction between the carbon nanotubes and the linker helps mitigate charge loss at cobalt sites and induces a high spin state, leading to improved oxygen reduction capability. This work provides valuable insights into designing high-performance electrocatalysts by regulating the electronic configuration and charge behavior of active sites.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Energy & Fuels
Mervat Ibrahim, Hani Nasser Abdelhamid, Aya Mohamed Abuelftooh, Saad G. Mohamed, Zhen Wen, Xuhui Sun
Summary: This study presents a method for the synthesis of a triazine covalent organic framework/graphene oxide nanocomposite, which is used to synthesize N-doped carbon/reduced graphene oxide. The in-situ synthesized N-doped carbon/reduced graphene oxide shows superior electrochemical performance and is employed as electrode materials for supercapacitors.
JOURNAL OF ENERGY STORAGE
(2022)
Article
Chemistry, Physical
Rui Zeng, Jun Zhang, Hao-Bo Guan, Sheng-Guang Wang, Tao Qin, Yun-Lei Hou, Dong-Lin Zhao
Summary: In this study, controllable self-assembled flower-like FeS/C@rGO nanocomposites were successfully constructed, which improved the electrochemical performance of iron sulfide in lithium-ion batteries by increasing the contact area between the active material and the electrolyte and enhancing Li+ transmission efficiency. Furthermore, N-doped carbon and rGO effectively inhibited the volume growth and aggregation of FeS nanosheets, resulting in a stable structure and outstanding rate performance of FeS/C@rGO.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Chemistry, Multidisciplinary
Rabindranath Lo, Anna Masinova, Maximilian Lamanec, Dana Nachtigallova, Pavel Hobza
Summary: The effect of solvent on the stability of non-covalent complexes, including hydrogen-, halogen-, and dispersion-bonded complexes, was investigated using previously published datasets. Results showed that the charge transfer within the complex determined whether it was stabilized or destabilized in solvent.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Marketa Paloncyova, Martin Srejber, Petra Cechova, Petra Kuhrova, Filip Zaoral, Michal Otyepka
Summary: RNA-based therapies have shown promise in various applications. Encapsulation of RNA into lipid nanoparticles allows for safe and targeted delivery. Simulations of pH-sensitive RNA-carrying nanoparticles reveal their self-assembly process and internal structure, providing insights into their composition and potential interactions for improving RNA-based medicine.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Multidisciplinary
Kalyan Biswas, Diego Soler, Shantanu Mishra, Qiang Chen, Xuelin Yao, Ana Sanchez-Grande, Kristjan Eimre, Pingo Mutombo, Cristina Martin-Fuentes, Koen Lauwaet, Jose M. Gallego, Pascal Ruffieux, Carlo A. Pignedoli, Klaus Mullen, Rodolfo Miranda, Jose I. Urgel, Akimitsu Narita, Roman Fasel, Pavel Jelinek, David Ecij
Summary: This study explores three families of nanographenes (A, B, and C) and finds that open-shell nanographenes exhibit the strongest magnetic exchange coupling, especially near the transition from closed-shell to open-shell states. Experimental results confirm the predictions, and two specific nanographenes show record values of magnetic exchange coupling measured on the Au(111) surface, close to 200 meV. This research provides insights for designing carbon nanomaterials with robust magnetic ground states.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Federico Frezza, Frederik Schiller, Ales Cahlik, Jose Enrique Ortega, Johannes V. Barth, Andres Arnau, Maria Blanco-Rey, Pavel Jelinek, Martina Corso, Ignacio Piquero-Zulaica
Summary: In this study, quinoidal ligands were reacted with single cobalt atoms on an Au(788) surface in ultra-high vacuum, resulting in the formation of cobalt-quinoid chains. The electronic structure of these chains was investigated using angle-resolved photoemission spectroscopy, and their narrow bandgap structure was revealed using low-temperature scanning tunneling microscopy/spectroscopy. Theoretical calculations confirmed that the observed electronic bands originated from the efficient hybridization of cobalt and molecular orbitals. This work provides a foundation for the systematic search of similar one-dimensional π-d hybridized metal-organic chains with tunable electronic and magnetic properties.
Article
Chemistry, Multidisciplinary
Michal Langer, Lukas Zdrazil, Miroslav Medved, Michal Otyepka
Summary: The establishment of structure-photoluminescence (PL) relationships in carbon dots (CDs) is still a challenge. The core, surface, and molecular states are the main sources of PL, but their interaction and effects on each other are not well understood. By performing TD-DFT calculations, researchers found that different structural arrangements support the communication between PL centers. This study provides insights for designing CDs with desired surface/core characteristics.
News Item
Chemistry, Multidisciplinary
P. Jelinek
Summary: An organic quantum magnet has been created by synthesizing short chains of porphyrin derivatives on a surface and manipulating atoms using a scanning probe microscope tip.
Article
Chemistry, Multidisciplinary
Kewei Sun, Orlando J. Silveira, Yujing Ma, Yuri Hasegawa, Michio Matsumoto, Satoshi Kera, Ondrej Krejci, Adam S. Foster, Shigeki Kawai
Summary: Substituting carbon with silicon in organic molecules and materials is a challenging task, but in this study, the researchers successfully synthesized one- and two-dimensional covalent organic frameworks with atomically precise Si substitution. The structures were characterized using high-resolution scanning tunnelling microscopy and photoelectron spectroscopy, and it was found that each Si atom in a hexagonal C4Si2 ring was covalently linked to one terminal Br atom.
Article
Chemistry, Multidisciplinary
Alejandro Jimenez-Martin, Federico Villalobos, Benjamin Mallada, Shayan Edalatmanesh, Adam Matej, Juan M. Cuerva, Pavel Jelinek, Araceli G. Campana, Bruno de la Torre
Summary: We present a new on-surface synthetic approach for incorporating five-membered rings into conjugated polymers, resulting in low-bandgap fulvalene-bridged bisanthene polymers. The formation of non-benzenoid units is controlled by annealing parameters, which facilitate the transformation of diethynyl bridges into fulvalene moieties. The atomically precise structures and electronic properties are characterized using STM, nc-AFM, STS, and supported by DFT calculations. The narrow frontier electronic gaps of 1.2 eV observed on Au(111) suggest the potential of this strategy in tuning optoelectronic properties by integrating five-membered rings at specific sites in other conjugated polymers.
Article
Chemistry, Multidisciplinary
Debashree Manna, Rabindranath Lo, Dana Nachtigallova, Zdenek Travnicek, Pavel Hobza
Summary: The study investigates the impact of solvent dielectric constant on the dative bond in Lewis electron pair bonding systems. By comparing two systems, H3B <- NH3 and {Zn <-(NH3)}(2+), in solvents with different dielectric constants, and utilizing state-of-the-art computational methods, it is found that the stability of the neutral H3B <- NH3 system increases with solvent polarity, while the positively charged {Zn <-(NH3)}(2+) system shows the opposite trend. These changes are attributed to different charge redistributions in neutral and charged complexes, reflecting the response to the solvent and quantified by changes in solvation energies.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Jonas Heggemann, Yashasvi S. Ranawat, Ondrej Krejci, Adam S. Foster, Philipp Rahe
Summary: This study reveals the microscopic geometry of calcite(104) and the decisive impact of the (2 x 1) reconstruction on adsorbed species such as carbon monoxide, using high-resolution atomic force microscopy data combined with density functional theory and AFM image calculations.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Tao Wang, Paula Angulo-Portugal, Alejandro Berdonces-Layunta, Andrej Jancarik, Andre Gourdon, Jan Holec, Manish Kumar, Diego Soler, Pavel Jelinek, David Casanova, Martina Corso, Dimas G. de Oteyza, Jan Patrick Calupitan
Summary: The coupling of a sterically demanded pentacene derivative on Au(111) into fused dimers connected by non-benzenoid rings was studied using high-resolution scanning tunneling microscopy/spectroscopy and density functional theory. The diradical character of the products was tuned by modifying the coupling section, with the antiaromaticity of cyclobutadiene and its position within the structure playing a significant role. Understanding these structure-property relationships is crucial for designing new complex and functional molecular structures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Aby Cheruvathoor Poulose, Miroslav Medved, Vasudeva Rao Bakuru, Akashdeep Sharma, Deepika Singh, Suresh Babu Kalidindi, Hugo Bares, Michal Otyepka, Kolleboyina Jayaramulu, Aristides Bakandritsos, Radek Zboril
Summary: This study presents a reusable graphene catalyst that can convert glycerol, produced from biomass fermentation, to high-value chemicals at room temperature without solvents. The catalyst shows excellent activity and selectivity for glycerol conversion to solketal, and it can also convert oils to biodiesel.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Alejandro Berdonces-Layunta, Adam Matej, Alejandro Jimenez-Martin, James Lawrence, Mohammed S. G. Mohammed, Tao Wang, Benjamin Mallada, Bruno de la Torre, Adrian Martinez, Manuel Vilas-Varela, Reed Nieman, Hans Lischka, Dana Nachtigallova, Diego Pena, Pavel Jelinek, Dimas G. de Oteyza
Summary: The study demonstrates the sensitivity of graphene nanoribbon zigzag edges to water, showing that water can hydrogenate the central carbon of the zigzag segments. This effect can be reversed by tip manipulation and annealing. The results also show a periodic pattern of spontaneous hydrogenation of gold-supported chiral graphene nanoribbons even at room temperature.
Article
Chemistry, Multidisciplinary
Alejandro Jimenez-Martin, Aurelio Gallardo, Bruno de la Torre
Summary: This study proposes a strategy for tuning the directionality of self-assembly processes in homomolecular organic compounds on inert metal surfaces. The results reveal a halogen-bond geometry transformation induced by a subtle balance of molecule-molecule interaction. Furthermore, the research finds that the halogen-bonded supramolecular assembly can periodically confine electronic quantum states and single atoms.
Article
Chemistry, Physical
Rabindranath Lo, Debashree Manna, Vijay Madhav Miriyala, Dana Nachtigallova, Pavel Hobza
Summary: The stability of dative bond complexes increases with increasing solvent polarity, as the charge transfer increases the dipole moment of the complex. Our research confirms this assumption, but only when the charge transfer is sufficiently large.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
