Review
Chemistry, Inorganic & Nuclear
Peiyun Zhou, Junjun Lv, Xiubing Huang, Yunfeng Lu, Ge Wang
Summary: In recent years, Metal-Organic Frameworks (MOFs) have been applied as promising electrocatalysts, but their catalytic activity and electronic conductivity remain unsatisfactory. This review summarizes the research efforts to optimize the intrinsic activity and electronic conductivity of MOFs-based electrocatalytic materials. It discusses strategies to enhance the activity of active sites and increase the number of accessible active sites based on the reaction mechanisms of various electrochemical processes. It also outlines strategies to improve electronic conductivity through the design and construction of MOFs derivatives.
COORDINATION CHEMISTRY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Geraudys Mora-Barzaga, Felipe J. Valencia, Matias Carrasco, Rafael Gonzalez, Martin G. Parlanti, Enrique N. Miranda, Eduardo M. Bringa
Summary: The thermal conductivity of amorphous carbon nanostructures, including nanowires and nanotubes, was investigated using classical Molecular Dynamics simulations and compared with experimental results. It was found that the thermal conductivity of nanotubes increases with decreasing wall thickness, which can be explained by the variation in elastic modulus of the nanostructures.
Review
Polymer Science
Fei Xin, Qiang Lyu
Summary: This review summarizes recent research on the thermal characteristics of hydrogels and their applications in electronic devices. The thermal stability, thermoresponsiveness and thermal conductivity of hydrogels are discussed in detail. Methods such as introducing soluble ions and organic solvents, forming ionogels, modifying polymer chains and incorporating nanomaterials can improve the thermal stability of hydrogels under extreme environments. Moreover, the thermoresponsive capacity of hydrogels is influenced by the composition, concentration, crosslinking degree and hydrophilic/hydrophobic characteristics of copolymers. The thermal conductivity of hydrogels plays a vital role in electronics applications and can be enhanced by adding nanocomposites.
Article
Engineering, Environmental
Fenyang Tian, Shuo Geng, Lin He, Yarong Huang, Akhmat Fauzi, Weiwei Yang, Yequn Liu, Yongsheng Yu
Summary: Transition metal phosphides, specifically PSS-PPy/Ni-Co-P, have been shown to exhibit highly efficient hydrogen evolution reaction performance in neutral-pH electrolyte, with remarkable activity and stability achieved through conductivity, hydrophilicity, and electronic structure optimization. This research paves the way for the design of low-cost, high-efficiency, and stable electrocatalysts for HER in neutral-pH electrolyte.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Xiaoshu He, Zhijun Feng, Ling Zhou, Xing Xu
Summary: The dual-conductive coated NCA material showed excellent performance at high rate, with significantly increased capacity and improved cycling stability. The coating also demonstrated enhanced capacity retention at elevated temperatures.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Materials Science, Ceramics
Zhengxin Guan, Jun Li, Han Wu, Xiaohong Chen, Wei Ou-Yang
Summary: Metal-organic frameworks (MOFs) have been widely used in various fields due to their unique features. However, their poor electrical conductivity has hindered their application in field emission (FE) vacuum electronic devices. This study successfully grows a novel conductive MOF, Cu-CAT, on graphite paper to achieve excellent field emission performance.
CERAMICS INTERNATIONAL
(2022)
Review
Polymer Science
Wenhua Gao, Qiyuan Tu, Ping Wang, Jinsong Zeng, Jinpeng Li, Bin Wang, Jun Xu, Kefu Chen, Zhen Zhang, Noureddine Abidi, Lucian A. Lucia
Summary: The challenge of energy depletion and environmental pollution calls for the development of green and sustainable materials in the form of nanocellulose (NC) derived from abundant and renewable resources. Conductive polymers (CPs)/NC composites have gained significant attention as functional electronic devices. This mini review provides an overview of nanocellulose, CPs, the preparation strategy of CPs/NC conducive composites, and the factors influencing electrical conductivity. Different CPs/NC composite systems and their applications are discussed, including sensors, supercapacitors, and lithium-ion batteries. Current challenges, existing problems, and future perspectives of CPs/NC conductive composites are also proposed.
Article
Nanoscience & Nanotechnology
Wei Wang, Jianbo Zhu, Dandan Qin, Wenjing Shi, Songting Cai, Yuxin Sun, Haixu Qin, Jian Cao, Qian Zhang, Wei Cai, Jiehe Sui
Summary: Research indicates that controlling the strength of ionized impurity scattering is crucial for achieving desirable thermoelectric performance in high Yb-filled skutterudites.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Materials Science, Multidisciplinary
Chaojun Zhang, Yang Tang, Tianyu Guo, Yizhou Sang, Ding Li, Xiaoling Wang, Orlando J. Rojas, Junling Guo
Summary: The increase in heat generation in electronic devices due to high power density and miniaturization has become a major issue affecting various aspects. Liquid metals with high thermal conductivity are promising for thermal management, but face challenges such as pump-out and surface-spreading. A biogenic supramolecular network is proposed as a diffusion barrier at copper particle-LM interfaces to overcome these challenges and achieve superior thermal conduction. The EGaIn/Cu@TA demonstrates record-high metallic-mediated thermal conductivity and fluidic stability. The incorporation of copper particles enhances heat flow, making it suitable for computer central processing units.
Article
Polymer Science
Xiaohu Chen, Haonan Zhang, Jiashu Cui, Yanen Wang, Mingyang Li, Juan Zhang, Changgeng Wang, Zhisheng Liu, Qinghua Wei
Summary: Composite hydrogels based on PVA, GEL, OSA, GO, and SWNTs were successfully prepared in this study. These hydrogels exhibited excellent self-healing properties and the ability to transmit sensory signals, making them promising for electronic skin applications.
Article
Chemistry, Physical
Fezzeh Pouraghajan, Andrea Thompson, Emilee E. Hunter, Brian Mazzeo, Jake Christensen, Ram Subbaraman, Michael Wray, Dean Wheeler
Summary: This study quantified the changes in effective ionic conductivity and diffusivity, revealing the variations in electronic and ionic resistivity during cell formation and cycling. The results indicate that the chemistry of the electrodes and cycling conditions impact these changes.
JOURNAL OF POWER SOURCES
(2021)
Article
Multidisciplinary Sciences
Jingguo Li, Amol Kumar, Ben A. Johnson, Sascha Ott
Summary: Conductivity in metal-organic frameworks (MOFs) can be achieved through either a band-like or a redox-hopping charge transport mechanism. This study presents direct experimental evidence for redox conductivity in fluorine-doped tin oxide surface-grown thin films of a specific MOF, demonstrating conductivity enhancement of over 10000-fold compared to neutral or completely reduced films.
NATURE COMMUNICATIONS
(2023)
Article
Physics, Multidisciplinary
Zheng Fan, Gui-Qin Li, Gui-Lu Long
Summary: In this study, the quantum transport properties of ZnO devices with different bulk configurations were investigated using numerical methods. The results showed that the transport property at a higher energy range could be tuned by changing the length of central scattering. Substituting some Zn atoms with Cu atoms also had a significant effect on the quantum properties, resulting in different transmission. The doping positions of Cu atoms also influenced the properties of the ZnO devices, as the tuning mechanism relied on the shifting of carrier distributions in the scattering center.
Article
Green & Sustainable Science & Technology
Siyi Chen, Yulian Chen, Xiaojiang Mu, Pengfei Wang, Lei Miao, Sakae Tanemura, Huanfu Cai
Summary: Gel polymer electrolytes (GPE) are a favorable choice for energy storage devices due to their leakage-free nature, interchangeability with separators, increased safety, and superior ionic conductivity compared to all-solid electrolytes. However, the scope of application of GPEs can be limited by factors such as ionic conductivity and operating voltage, which are positively correlated to energy density. This review examines different polymer backbones and the mechanism of ionic conduction in GPE, while summarizing and discussing strategies for enhancing ionic conductivity and energy density through selective presentation of pioneering works. Furthermore, the current challenges and future directions of GPE research for practical applications are encapsulated to guide upcoming endeavors.
SUSTAINABLE MATERIALS AND TECHNOLOGIES
(2023)
Editorial Material
Engineering, Electrical & Electronic
Samuel Graham, Sukwon Choi
Summary: Boron arsenide can be used as a high-thermal-conductivity cooling substrate in gallium nitride power devices.
NATURE ELECTRONICS
(2021)
Article
Chemistry, Physical
Xavier Deraet, Jan Turek, Mercedes Alonso, Frederik Tielens, Bert M. M. Weckhuysen, Monica Calatayud, Frank De Proft
Summary: This paper investigates the adsorption behavior of single late transition metals on a defect-free anatase surface using periodic density functional theory calculations. The results reveal that the interaction strength between the transition metals and the support can be attributed to electron transfer, s-d orbital hybridization effects, or a synergistic effect between both factors. Palladium shows deviating adsorption behavior, which is likely associated with the lower dissociation enthalpy of the Pd-O bond. The reactivity of these systems is evaluated using the Fermi weighted density of states approach, and a model is proposed to predict the adsorption strength of CO on anatase-supported d-metal atoms.
Article
Chemistry, Organic
Javier E. Alfonso-Ramos, Ruben Van Lommel, David Hernandez-Castillo, Frank De Proft, Roy Gonzalez-Aleman, Erik V. Van der Eycken, Gerardo M. Ojeda-Carralero
Summary: 3-Dipolar cycloadditions are commonly used to form five-membered heterocycles, but the cycloadditions involving acyl-isocyanide ylides have not been well explored by the chemical community. In this study, we investigated the mechanistic features of the reaction between acyl-isocyanide ylides and dipolarophiles using density functional theory calculations. We explained the experimental results and predicted opposite regioselectivity for electron-poor and electron-rich dipolarophiles. This study provides insights for the design of new cycloaddition reactions based on the acyl-isocyanide ylides motif.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Organic
Mercedes Alonso, Frank De Proft, Tom Bettens, Paul Geerlings
Summary: Anti-Felkin-Anh diastereoselectivity can be achieved by stretching the ketone with a mechanical pulling force. A mechanochemical Felkin-Anh model is proposed based on the distance between the pulling points. The model is validated by density functional theory calculations and the risk of bond rupture is minimized.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Biochemistry & Molecular Biology
Ana V. Cunha, Remco W. A. Havenith, Jari van Gog, Freija De Vleeschouwer, Frank De Proft, Wouter Herrebout
Summary: In this study, the interaction between the halogen atom X and the aromatic ring in the halogen bond complexes CF(3)Xmiddot middot middot Y and C(2)F(3)Xmiddot middot middot Y (with Y = furan, thiophene, selenophene and X = Cl, Br, I) was investigated using DFT and CCSD(T) methods. It was found that the interaction with the pi-bonds in a perpendicular orientation is stronger than the interaction with the in-plane lone pairs of the heteroatom of the aromatic cycle. The interaction energy is dominated by electrostatic, orbital, and dispersion interactions, and the strength of the interaction follows the trend Cl < Br < I.
Article
Chemistry, Multidisciplinary
Nagy L. Torad, Yuta Tsuji, Azhar Alowasheeir, Masako Momotake, Kazuki Okazawa, Kazunari Yoshizawa, Michio Matsumoto, Masafumi Yamato, Yusuke Yamauchi, Miharu Eguchi
Summary: To increase chemical reaction rates, general solutions include increasing the concentration/temperature and introducing catalysts. In this study, the rate constant of an electrophilic metal coordination reaction is accelerated 23-fold on the surface of layered aluminosilicate (LAS), where the reaction substrate (ligand molecule) induces dielectric polarization owing to the polar and anionic surface. This unique method to accelerate the chemical reaction is expected to expand the range of utilization of LASs, which are chemically inert, abundant, and environmentally friendly. The concept is also applicable to other metal oxides which have polar surfaces, which will be useful for various chemical reactions in the future.
Article
Chemistry, Multidisciplinary
Stephen E. Brown, Ioanna Mantaloufa, Ryan T. Andrews, Thomas J. Barnes, Martin R. Lees, Frank De Proft, Ana V. Cunha, Sebastian D. Pike
Summary: The molecular titanium-oxo cluster [Ti6O6((OPr)-Pr-i)(6)((O2CBu)-Bu-t)(6)] (1) can be activated by UV light to produce a mixed valent (photoreduced) Ti (iii/iv) cluster, along with alcohol and ketone organic products. Mechanistic studies show a two-electron mechanism utilizing the cluster structure for multielectron reactions. The photoreduced products [Ti6O6((OPr)-Pr-i)(4)((O2CBu)-Bu-t)(6)(sol)(2)] can be isolated and characterized, and undergo onward oxidation under air. The redox reactivity described is only possible in a cluster with multiple Ti sites.
Article
Chemistry, Physical
Yuta Tsuji, Masataka Yoshida, Kazunari Yoshizawa, Takashi Kamachi
Summary: The nonoxidative coupling of methane is a focus of research due to its production of ethane and hydrogen. This Concept article proposes a solution to the issues of low conversion at low temperatures and carbon deposition at high temperatures. By considering reaction enthalpy and energy differences, a catalyst search guideline is provided to suppress carbon deposition while maintaining high conversion rates. The alloy MgPt is shown to be a promising candidate that satisfies these requirements. Validation experiments for MgPt's catalytic performance are also discussed.
Article
Biochemistry & Molecular Biology
Lise Vermeersch, Frank De Proft, Vicky Faulkner, Freija De Vleeschouwer
Summary: This study analyzed the governing factors in Lewis acid and non-covalent catalysis of three types of Diels-Alder reactions. The stability of the non-covalent interaction donor-dienophile complex was found to significantly reduce the activation energy. Orbital interactions were shown to be the main driver for catalysis, with electrostatic interactions dominating.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Physical
Lieven Bekaert, Suzuno Akatsuka, Naoto Tanibata, Frank De Proft, Annick Hubin, Mesfin Haile Mamme, Masanobu Nakayama
Summary: Rechargeable batteries are essential in the transition from fossil fuels to renewable energy. Solid-state sodium ion batteries are a promising alternative to lithium-based batteries, offering improvement in safety, lifespan, sustainability, and price. The chemical stability of Na3PS4 solid-state electrolyte with sodium metal electrode has been investigated, providing new design principles for optimizing solid-state electrolytes.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Nicholas Casetti, Javier E. Alfonso-Ramos, Connor W. Coley, Thijs Stuyver
Summary: This article presents an overview of high-throughput screening workflows that combine molecular quantum mechanical modeling and machine learning. It highlights successful applications and provides a brief outlook on further advances in the field.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Organic
Yuta Tsuji, Kazuki Okazawa, Kazunari Yoshizawa
Summary: Face-to-face stacking of aromatic compounds leads to stacked antiaromaticity, while that of antiaromatic compounds leads to stacked aromaticity. Understanding the origin of stacked aromaticity is crucial for realizing it in completely new and different molecular systems. The Huckel method is used to model the face-to-face stacking systems of benzene and cyclobutadiene molecules and discuss their stacked antiaromaticity and stacked aromaticity based on their π-electron energies. By further developing the discussion, clues for realizing stacked aromaticity in synthesizable molecular systems are sought.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Yuta Tsuji, Yuta Yoshioka, Kazuki Okazawa, Kazunari Yoshizawa
Summary: This paper discusses the use of computational and informatics approaches to design efficient metal nanocluster catalysts for ammonia synthesis. It addresses three main challenges: measuring catalytic activity, selecting the best catalyst from numerous candidates, and identifying the thermodynamically stable cluster catalyst structure. The study employs first-principles calculations, Bayesian optimization, and particle swarm optimization to identify a Ti-8 nanocluster as a potential catalyst candidate. The adsorption structures of N-2 and NH3 on Ti(8) indicate significant activation of N-2 and easy desorption of NH3. The research also discovers cluster catalyst candidates that defy the conventional trade-off between strong adsorption of reactants and products.
Article
Chemistry, Physical
Ramon Alain Miranda-Quintana, Alberto Vela, Frank De Proft, Marco Martinez Gonzalez, Jose L. Gazquez
Summary: The hard/soft acid/base (HSAB) principle is fundamental to understanding chemical reactivity preferences. However, the local HSAB principle often fails in making accurate predictions for regioselectivity preferences. By considering both the charge transferred between reacting centers and the charge reorganization within non-reacting parts of the molecule, we propose different reorganization models and corresponding regioselectivity rules.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Nikolay Cherkasov, Shusaku Asano, Yuta Tsuji, Kazuki Okazawa, Kazunari Yoshizawa, Hiroyuki Miyamura, Jun-ichiro Hayashi, Alexander A. Kunitsa, S. David Jackson
Summary: Catalytic reactions of mixed substrates sometimes exhibit different behavior compared to individual substrates. This paper investigates the hydrogenation of propylbenzene in the presence of toluene, which accelerates the reaction rate by 120%. The well-accepted Langmuir-Hinshelwood reaction model cannot explain this acceleration effect. Experimental and computational studies reveal that the acceleration is specific to the liquid phase with the isopropanol solvent, and it is caused by the formation of associates between toluene and propylbenzene on the catalyst surface in the polar environment.
REACTION CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Yasuyuki Yamada, Kentaro Morita, Takuya Sugiura, Yuka Toyoda, Nozomi Mihara, Masanari Nagasaka, Hikaru Takaya, Kiyohisa Tanaka, Takanori Koitaya, Naoki Nakatani, Hiroko Ariga-Miwa, Satoru Takakusagi, Yutaka Hitomi, Toshiji Kudo, Yuta Tsuji, Kazunari Yoshizawa, Kentaro Tanaka
Summary: A biomimetic catalyst based on a mu-nitrido-bridged iron phthalocyanine dimer stacked onto a graphite surface showed high catalytic methane oxidation activity, even at room temperature. The activity was almost 50 times higher than other molecule-based catalysts and comparable to certain natural enzymes in the presence of H2O2. The stacking of the catalyst onto graphite facilitated electron transfer from methane, leading to enhanced catalytic activity.
