Article
Engineering, Environmental
Chia-Wei Lien, Balaraman Vedhanarayanan, Jian-Hong Chen, Jeng-Yu Lin, Hsiang-Hsi Tsai, Li-Dong Shao, Tsung-Wu Lin
Summary: In this study, a co-solvent-in-deep eutectic solvent system was developed by mixing water and acetonitrile with a typical DES electrolyte. The addition of co-solvents improved the conductivity and flame-retardant properties of the DES, leading to a wide electrochemical stability window. Furthermore, a hydrogel consisting of 1T-MoS2 and reduced graphene oxide was used as electrode materials for supercapacitors, demonstrating high energy density and capacitance retention after cycles.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Simone Di Muzio, Annalisa Paolone, Olga Russina, Fabio Ramondo
Summary: Non-ionic deep eutectic solvents are innovative and alternative solvents that deviate from thermodynamic ideality due to the strength of hydrogen bonds between different components. In this study, we investigated the phase diagram and structural properties of cyclohexanol and phenol mixtures to understand the role of hydrogen bonding in the non-ideality of phenolic and alcoholic compounds. The results showed that the deviations from ideal mixing were smaller compared to a thymol-menthol mixture, and the intermolecular interactions were influenced by both hydrogen bonding and van der Waals contributions.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Review
Chemistry, Multidisciplinary
Xue Tian, Qizhen Zhu, Bin Xu
Summary: Water-in-salt (WIS) electrolytes show great potential for application in supercapacitors due to their wide electrochemical stability window and other advantages, but also face challenges. This Review discusses the working mechanisms, reasons for the wide stability window, improvement strategies, and applications of WIS electrolytes in various types of supercapacitors.
Article
Chemistry, Multidisciplinary
Hu Hong, Jiaxiong Zhu, Yiqiao Wang, Zhiquan Wei, Xun Guo, Shuo Yang, Rong Zhang, Huilin Cui, Qing Li, Dechao Zhang, Chunyi Zhi
Summary: Non-metallic ammonium ion (NH4+) batteries have attracted attention due to their low cost, non-toxicity, and environmental sustainability. This study elucidates the solvation interactions between NH4+ and solvents, and proposes design principles for weakly solvated electrolytes. By constructing a weak hydrogen bonded electrolyte, NH4+ ion batteries exhibit superior rate capability and long-term cycling performance.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jin Han, Alessandro Mariani, Maider Zarrabeitia, Zenonas Jusys, R. Jurgen Behm, Alberto Varzi, Stefano Passerini
Summary: Halide-free, water-in-salt electrolytes composed of potassium acetate (KAc) and zinc acetate (ZnAc2) are investigated for zinc-ion hybrid supercapacitors (ZHSs). Molecular dynamics simulations reveal that water molecules do not interact with each other in concentrated electrolytes, but have bulk-like regions in dilute electrolytes. Among the investigated electrolytes, a 30 m KAc and 1 m ZnAc2 electrolyte (30K1Zn) exhibits the best performance in terms of rechargeability and stability of Zn plating/stripping. ZHSs utilizing 30K1Zn, along with a commercial activated carbon (AC) positive electrode and Zn negative electrode, show a high capacity and excellent cycling stability.
Article
Chemistry, Physical
Xiaochen Shen, Nicholas Sinclair, Christian Kellamis, Burcu Gurkan, Jesse Wainright, Robert Savinell
Summary: This study examines the influence of cation alkyl chain length and anion chemical identity on the characteristics of the hydrogen (H) bonding network in eutectic solvents. The results reveal the changes in solvated ion size and ionic conductivity as a function of the alkyl chain length and electronegativity of the anions.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Analytical
Dotse Selali Chormey, Buse Tugba Zaman, Tulay Borahan Kustanto, Sezin Erarpat Bodur, Suleyman Bodur, Elif Ozturk Er, Sezgin Bakirdere
Summary: This review provides an overview of the harmful effects of endocrine disrupting chemicals (EDCs) on human health and introduces the methods for analyzing EDCs. Recent research has focused on using green chemicals, such as deep eutectic solvents (DESs), for microextraction to ensure environmental safety.
Article
Chemistry, Multidisciplinary
Zhiyu Hu, Zirui Song, Zhaodong Huang, Shusheng Tao, Bai Song, Ziwei Cao, Xinyu Hu, Jiae Wu, Fengrong Li, Wentao Deng, Hongshuai Hou, Xiaobo Ji, Guoqiang Zou
Summary: This research proposes a novel electrolyte for high-voltage aqueous rechargeable energy storage devices, utilizing polyethylene glycol (PEG) and N, N-dimethylformamide (DMF) as co-solvents to reconstruct the hydrogen bond network. The electrolyte achieves a wide electrochemical window and enhances the performance of zinc cells and zinc-ion supercapacitors, significantly improving their cycle life.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Y. Tanaka, K. Ajino, H. Ogawa, H. Mori
Summary: Deep eutectic electrolytes have gained attention in energy-related fields. This study presents a solvent-free synthetic route to ion-conductive polymers by using metal salt/amide-based deep eutectic monomers. The synthesized polymers exhibit high ionic conductivity and can be obtained through photoinduced radical polymerization without the use of volatile organic solvents in an air environment.
MATERIALS TODAY CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Lewis W. Le Fevre, Andinet Ejigu, Rebecca Todd, Andrew J. Forsyth, Robert A. W. Dryfe
Summary: Water-in-salt electrolytes were tested for high-temperature performance with a carbon-based electrode and commercial cell components. Supercapacitors using these electrolytes demonstrated satisfactory operation at 100°C and 120°C, with gravimetric capacitances exceeding 100 F g(-1) at a voltage of 2 V.
CHEMICAL COMMUNICATIONS
(2021)
Article
Electrochemistry
Ming-Kuen Huang, Krishnan Shanmugam Anuratha, Yaoming Xiao, Yen-Pei Chen, Jeng-Yu Lin
Summary: This study investigates the use of hybrid methylsulfonyl methane-based DES electrolytes with the introduction of water and acetonitrile as co-solvents for symmetric supercapacitors. Through systematic optimization of the molar ratio, the hybrid DES electrolytes exhibit improved ionic conductivity and viscosity. The optimized electrolyte demonstrates excellent performance in terms of specific capacitance, energy density, and cycling stability, providing opportunities for the development of low-cost and high-voltage electrolytes for energy storage applications.
ELECTROCHIMICA ACTA
(2022)
Article
Chemistry, Physical
Chong Liang, Wei Zhao, Xutang Liu, Zhijie Jiang, Fei Wang
Summary: In this study, systematic processes were constructed to separate valuable carboxylic acids from lignite. Through distillation, ether extraction, acetone dissolution, and separation by deep eutectic solvent, the target carboxylic acids were successfully separated. The results showed that choline chloride has better separation performance, and the hydrogen bonds formed in the deep eutectic solvent can enhance separation efficiency.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Green & Sustainable Science & Technology
Haiyu Chen, Ailin Wang, Cancan Yan, Shiwei Liu, Lu Li, Qiong Wu, Yue Liu, Yuxiang Liu, Genkuo Nie, Shuangxi Nie, Shuangquan Yao, Hailong Yu
Summary: DESs were synthesized and tested for their solubilisation of two industrial lignins. The results showed that DESs with higher HBD content, shorter carbon chain length and fewer functional groups were more effective in dissolving lignin. DESs containing carboxyl groups were found to be particularly effective in breaking beta-O-4 bonds and solubilizing lignin. High temperature and suitable water content were also observed to promote lignin solubilization. The pretreatment of poplar and maize straw with specific DESs showed good solubilization of lignin, with ChCl/FA(1:3) being the most effective in dissolving poplar lignin and maize straw lignin, achieving lignin solubilization of 82% and 57% respectively. Overall, these findings indicate the great potential of DESs as solvents for lignin dissolution.
Article
Materials Science, Multidisciplinary
Vidhya Selvanathan, Syaza Amira Razali, Jun-ichi Nishida, Masaaki Tomura, Ghulam Muhammad, Huda Abdullah, Akira Watanabe, Md Akhtaruzzaman
Summary: A structurally unique cobalt-based organic complex was successfully synthesized via ionothermal synthesis, demonstrating excellent porous structure, homogeneous distribution of metal ions, and high specific capacitance, energy density, power density, and cycling stability as an electrode material for supercapacitors.
JOURNAL OF MATERIALS RESEARCH AND TECHNOLOGY-JMR&T
(2022)
Review
Chemistry, Multidisciplinary
Mingming Han, Jiang Zhou, Hong Jin Fan
Summary: Breakthroughs in super-concentrated electrolytes have brought aqueous solutions to the forefront of high-safety battery devices. Eutectic mixtures have emerged as a green, safe, low-cost, and electrochemically stable electrolyte system for rechargeable metal-ion batteries (MIBs). This article summarizes the formation mechanisms, physio-chemical properties, and composition-structure-property relationships of eutectic mixtures, with a focus on their advanced functions and applications in MIBs.
TRENDS IN CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Xuejun Lu, Li Tao, Keqi Qu, Amardeep Amardeep, Jian Liu
Summary: Eutectic electrolytes are being explored for AZICs due to their high electrochemical stability and environmental-friendly feature. The introduction of heavy water and dimethyl sulfoxide provides double-solvent protection, improving the reversibility of Zn anodes. The optimal duet-insurance eutectic electrolyte exhibits high capacitance and excellent capacitance retention, and can operate at a low temperature.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Haibo Xue, Jose Manuel Vicent-Luna, Shuxia Tao, Geert Brocks
Summary: Lattice defects, especially compound defects, significantly affect the stability of halide perovskite solar cells. The most prominent defects in CsPbI3 are the antisite of Pb substituting Cs under equilibrium conditions, while other compound defects are negligible. However, under nonequilibrium thermal and operating conditions, other complexes such as the Cs substituting Pb antisite and compound vacancies of PbI2 or CsPbI3 units become important. These compound defects mainly lead to shallow or inactive charge carrier traps, indicating the electronic stability of halide perovskites.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Xuejun Lu, Zhenhua Liu, Amardeep Amardeep, Zhenrui Wu, Li Tao, Keqi Qu, Hao Sun, Yulong Liu, Jian Liu
Summary: The design of low-cost and commercialized eutectic electrolytes for zinc-based electrochemical energy storage (ZEES) is still a challenge especially at low temperatures. This study proposes the use of chlorine-functionalized eutectic (Cl-FE) electrolytes to regulate the solvation of zinc and improve the performance of ZEES devices. The introduction of Cl anion-induced eutectic interaction with Zn acetate solutions allows the formation of Cl-FE/DOL-based electrolytes with a unique solvation sheath, leading to restricted side reactions on zinc anodes and high Coulombic efficiency.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Chemical
Mariana C. N. Bessa, Azahara Luna-Triguero, Jose M. Vicent-Luna, Paulo M. O. C. Carmo, Mihalis N. Tsampas, Ana Mafalda Ribeiro, Aliirio E. Rodrigues, Sofia Calero, Alexandre F. P. Ferreira
Summary: Two industrial dual-step pressure swing adsorption (PSA) processes were designed and simulated to obtain high-purity methane, CO2, and syngas from a gas effluent of a CO2 electroreduction reactor using different design configurations. NaX and MFI zeolites were selected from the investigated set for simulation. Case study 1 achieved 90.5% methane purity with a 95.2% recovery, whereas case study 2 obtained methane with a 97.5% purity and 95.3% recovery. Both case studies produced high-purity CO2 (>97%) and syngas with a H-2/CO ratio above 4. However, case study 2 had a significantly higher energy consumption compared to case study 1 (64.9 vs 29.8 W h mol(CH4) (-1)).
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Physical
Gabriela Jajko, Juan Jose Gutierrez Sevillano, Sofia Calero, Waclaw Makowski, Pawel Kozyra
Summary: This study investigated the adsorption of toluene in UiO-66 materials. Toluene is a volatile, aromatic organic molecule that is recognized as the main component of VOCs. The UiO-66 material was found to successfully capture toluene through adjustments to the force field parameters and analysis of occupation profiles and radial distribution functions. These findings provide an understanding of the mechanism of toluene adsorption on UiO-66.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Shrinjay Sharma, Marcello S. S. Rigutto, Richard Baur, Umang Agarwal, Erik Zuidema, Salvador R. G. Balestra, Sofia Calero, David Dubbeldam, Thijs J. H. Vlugt
Summary: Ideal Adsorbed Solution Theory (IAST) is a common method for modeling mixture adsorption isotherms, while the segregated version (SIAST) provides improved adsorbed loadings. We have adopted the concept of SIAST and developed the Segregated Explicit Isotherm (SEI) model which considers both size-effects of co-adsorbed molecules and surface heterogeneities. Compared to IAST and SIAST, SEI does not require an iterative scheme, resulting in faster simulations with excellent agreement with experimental data.
Article
Chemistry, Physical
Shrinjay Sharma, Salvador R. G. Balestra, Richard Baur, Umang Agarwal, Erik Zuidema, Marcello S. Rigutto, Sofia Calero, Thijs J. H. Vlugt, David Dubbeldam
Summary: The RUPTURA code is introduced as a free and open-source software package for gas adsorption simulation, mixture prediction, and isotherm model fitting. It can be combined with the RASPA software to compute breakthrough curves directly from adsorption simulations. The code supports a variety of isotherm models and provides an easy way to obtain the model parameters through the fitting module.
MOLECULAR SIMULATION
(2023)
Article
Chemistry, Multidisciplinary
Xiucheng Huang, Ana Martin-Calvo, Martijn J. J. Mulder, Sjoerd C. J. van Acht, Juan Jose Gutierrez-Sevillano, Julio C. Garcia-Navarro, Sofia Calero
Summary: This study focuses on the performance of zeolitic imidazolate frameworks (ZIFs) for hydrogen purification from coke oven gases (COG). Molecular simulation is used to compare different ZIF topologies and analyze the separation performance. The findings reveal that ZIFs with smaller pore sizes exhibit better separation of hydrogen from carbon monoxide and nonpolar molecules. The adsorption of carbon dioxide is strongly influenced by the structure's polarizability, while the adsorption of other components depends on their pore sizes. The study provides valuable information for selecting high-performance ZIFs for hydrogen purification.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Rafael M. Madero-Castro, Azahara Luna-Triguero, Andrzej Slawek, Jose Manuel Vicent-Luna, Sofia Calero
Summary: This paper investigates the adsorption of polar working fluids in hydrophobic and hydrophilic zeolites for thermal energy storage applications. Experimental and simulated adsorption isotherms of water and methanol in high-silica HS-FAU, NaY, and NaX zeolites were obtained. The results were used to develop a parameter model for the interaction between methanol and the zeolite and cations. The performance of the adsorbate working fluids for heat storage was evaluated using a mathematical model based on Dubinin-Polanyi adsorption potential theory. The importance of controlling the hydrophilic/hydrophobic nature of zeolites by changing the Al content was highlighted.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Nanoscience & Nanotechnology
Jose Luis Nunez-Rico, Juanjo Cabezas-Gimenez, Vanesa Lillo, Salvador R. G. Balestra, Jose Ramoon Galan-Mascaros, Sofia Calero, Anton Vidal-Ferran
Summary: Metal-organic frameworks (MOFs) with tunable properties and controlled dimensionality have shown promising potential for various applications. The incorporation of chirality into MOFs opens up new strategies for chiral separation, which is crucial in the pharmaceutical industry. In this study, computational modeling and experiments were combined to demonstrate the efficiency, versatility, robustness, and reusability of TAMOF-1-packed HPLC columns as the chiral stationary phase. The in silico studies predicted plausible separations of chiral compounds from different families, and the experimental results confirmed the validity of the models and the high performance of TAMOF-1 columns. The use of in silico screening in chiral chromatography is an unprecedented achievement.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Engineering, Environmental
Dominika O. Wasik, Ana Martin-Calvo, Juan Jose Gutierrez-Sevillano, David Dubbeldam, Thijs J. H. Vlugt, Sofia Calero
Summary: Formic acid production from CO2 can reduce carbon dioxide emissions while synthesizing a versatile product. This study investigated the confinement effects of metal-organic frameworks on CO2 hydrogenation to formic acid through molecular simulations. The results showed that metal-organic frameworks, such as UiO-66, can enhance the production of formic acid by shifting the thermodynamic equilibrium.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Pablo Romero-Marimon, Juan Jose Gutierrez-Sevillano, Sofia Calero
Summary: We examined the impact of aluminum distribution on CO2 adsorption properties in MFI, MOR, and ITW zeolites. Through molecular simulations, we found that CO2 adsorption in MFI is determined by the number rather than the distribution of aluminum atoms. In MOR, the distribution of aluminum in the C-channel plays a crucial role in heat adsorption. ITW zeolite, with its small-pore structure, showed high heat adsorption values only at low aluminum concentrations.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Mike Pols, Victor Brouwers, Sofia Calero, Shuxia Tao
Summary: Machine-learned force fields, trained with an active learning scheme against accurate density functional theory calculations, allow us to investigate defect migration in halide perovskites. We find that halide interstitials migrate faster than halide vacancies, with interstitials having shorter migration paths. Both types of defects migrate faster in CsPbI3 than in CsPbBr3, attributed to the less compact packing of ions in CsPbI3 leading to more frequent defect migration jumps.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Orkun Furat, Donal P. Finegan, Zhenzhen Yang, Matthias Neumann, Sangwook Kim, Tanvir R. Tanim, Peter Weddle, Kandler Smith, Volker Schmidt
Summary: The operating temperature has a significant impact on the degradation behavior of batteries. This study investigates the structural degradation of lithium-ion positive electrodes under different operating temperatures, and finds that particle porosity increases with higher cycling temperature, while particle surface area remains similar across different cycling-temperature aging conditions.
ENERGY STORAGE MATERIALS
(2024)
Article
Chemistry, Physical
Junyan Li, Ming Lu, Weijia Zheng, Wei Zhang
Summary: MXenes are two-dimensional materials with unique structures and properties, which have attracted significant scientific interest. Ion intercalation, as an important mechanism, plays a crucial role in regulating the electronic and chemical properties of MXene materials. This review provides an overview of the interaction events between ions and MXenes, including advanced characterization techniques, influencing factors, mechanisms, and functionalization roles of ion intercalation.
ENERGY STORAGE MATERIALS
(2024)
Article
Chemistry, Physical
Zhengtai Zha, Tianjiang Sun, Diantao Li, Tao Ma, Weijia Zhang, Zhanliang Tao
Summary: A novel zwitterion additive is developed to improve the electrochemical performance and cycling stability of aqueous zinc batteries. The zwitterion forms a stable solid electrolyte interphase on the electrode surface, isolating the zinc anode from the electrolytes and enabling fast zinc ion migration. The proposed electrolyte shows promising results in symmetric cells and full cells, with long cycling stability and high capacity retention.
ENERGY STORAGE MATERIALS
(2024)
Article
Chemistry, Physical
Nyung Joo Kong, Myeong Seon Kim, Jae Hyun Park, Jongbok Kim, Jungho Jin, Hyun-Wook Lee, Seok Ju Kang
Summary: Polymeric conducting binders have significant research value as they can serve as both binders and conducting agents, increasing the proportion of active materials in batteries and the volumetric energy density. This study explores the potential of a composite of PEDOT:PSS and polyethylene glycol (PEG) as a high-performing binder for silicon anodes. The addition of PEG polymer enhances the conductivity of PEDOT:PSS and improves the mechanical properties of the silicon anode, resulting in extended cycle endurance. The use of operando optical microscopy allows for direct observation of the binder's operation. Consequently, the bifunctional PEDOT:PSS/PEG binder shows promise for high-performance lithium-ion battery binders.
ENERGY STORAGE MATERIALS
(2024)
Article
Chemistry, Physical
Yangze Huang, Lixuan Zhang, Jiawen Ji, Chenyang Cai, Yu Fu
Summary: This study proposed a novel temperature-dependent viscoelastic liquid electrolyte and a hollow transition bi-metal selenide as the sulfur host material to address the issues in Li-S batteries. The experiments showed promising results in stabilizing the anode and improving cycling performance.
ENERGY STORAGE MATERIALS
(2024)
Article
Chemistry, Physical
Ao Yu, Wei Zhang, Nimanyu Joshi, Yang Yang
Summary: This review provides a comprehensive overview of research progress in ZIB anodes, including protective coating layers on zinc surfaces and intercalated anode materials. By designing protective coating layers and selecting appropriate intercalated anode materials, the inherent limitations of zinc metal anode can be overcome, leading to improved reliability and performance of ZIBs.
ENERGY STORAGE MATERIALS
(2024)
Article
Chemistry, Physical
Xin Wang, Yumiao Tian, Konghua Yang, Chenhui Ma, Wenqiang Lu, Xiaofei Bian, Nan Chen, Heng Jiang, Yan Li, Xing Meng, Pengyue Gao, Dong Zhang, Fei Du
Summary: Researchers developed a new sandwich deposition approach using boron nitride layer as a current collector, which enhances the performance of aqueous zinc-ion batteries.
ENERGY STORAGE MATERIALS
(2024)
Article
Chemistry, Physical
Sang Jun Lee, Dongwoo Kang, Dong Yeol Hyeon, Dong Seok Kim, Suyoon Eom, Su Hwan Jeong, Dong Park Lee, Dawon Baek, Jou-Hyeon Ahn, Gyeong Hee Ryu, Kwi-Il Park, San Moon, Joo-Hyung Kim
Summary: This study utilizes the ice-templating method to create a self-supporting three-dimensional hierarchical porous structure, which effectively inhibits sodium dendrite growth and improves the performance and longevity of sodium-metal batteries.
ENERGY STORAGE MATERIALS
(2024)
Article
Chemistry, Physical
Yifan Yu, Meng Lei, Yangyang Liu, Keyi Chen, Chuanzhong Lai, Jiulin Hu, Chilin Li
Summary: Metal fluorides as conversion-reaction cathodes have advantages such as low cost, environmentally friendly, and high energy density. In this study, a hydroxyl-rich copper fluoride (Cu2(OH)3F) was proposed as a conversion cathode, coupled with an electrolyte additive engineering, to address the poor reversibility issue. The presence of OH in Cu2(OH)3F enables effective suppression of Cu+ dissolution, resulting in better reaction reversibility and kinetics.
ENERGY STORAGE MATERIALS
(2024)