Article
Multidisciplinary Sciences
Yong Chen, Satoshi Takeya, Amadeu K. Sum
Summary: Clathrate hydrates are ordered structures stabilized by hydrophobic interactions between water and guest molecules. In this study, an alternative method is proposed to understand the complex structures of clathrate hydrates, revealing the diverse crystalline hydrogen-bonded networks that can be formed. The topological dual relations between clathrate hydrate networks and tetrahedrally close-packed structures provide insights into their nucleation, phase transition, and co-existence mechanisms. Molecular dynamics simulations are employed to explore the intrinsic structural relationships of clathrate hydrates and other unrelated ordered materials.
NATURE COMMUNICATIONS
(2023)
Article
Engineering, Chemical
Yu Wei, Nobuo Maeda
Summary: The memory effect in gas hydrate nucleation refers to the phenomenon that gas hydrates form easier or faster in water with a history of gas hydrate formation. Despite several proposed hypotheses, the cause of the memory effect remains a mystery. This study examines the impact of guest gas supersaturation on the memory effect.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Chemistry, Physical
Dean Eaton, Ivan Saika-Voivod, Richard K. Bowles, Peter H. Poole
Summary: The authors tested the theoretical free energy surface (FES) for two-step nucleation (TSN) by comparing it to numerical results from Monte Carlo simulations, finding that the theory successfully predicted FES over a range of thermodynamic conditions. This demonstrates that Iwamatsu's extension of classical nucleation theory provides an excellent framework for understanding the thermodynamics of TSN.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Energy & Fuels
Gustavo A. B. Sandoval, Marcio Couto Ozorio, Monica F. Naccache, Paulo R. de Souza Mendes, Amadeu K. Sum, Leandro Valim, Adriana Teixeira
Summary: This work presents a rheological analysis of cyclopentane hydrates formed in water-in-oil emulsions, investigating the influence of parameters such as pretreatment temperatures and cooling/heating rates. The study shows that the resulting hydrate slurry exhibits elasticity and shear thinning behavior, likely caused by breakdown of hydrate structures and alignment of hydrate agglomerates to the flow.
Article
Chemistry, Multidisciplinary
Feng Zhang, Hao Ni, Yi Wang, Fujun Xia, Baojun Wei, Xuefeng Liu
Summary: By using classical molecular dynamics simulations, the mechanical stability of CO2-N2 heteroclathrate hydrates (CNHHs) under uniaxial loading was investigated. The ratio of CO2 to N2 in the large and small water cages was found to have a crucial effect on the mechanical properties and fracture behaviors of CNHHs. The occupancy of small cages by CO2 was identified as a decisive factor affecting fracture position, leading to brittle or ductile fracture behavior. These findings provide insights into the deformation and fracture mechanisms of heteroclathrate hydrates and the impact of CO2 sequestration on the stability of gas hydrate reservoirs.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Physical
A. R. Finney, M. Salvalaglio
Summary: Molecule- and particle-based simulations are used to test classical nucleation theory. The variational approach to Markov processes is applied to determine the suitability of different reaction coordinates for studying crystallization from supersaturated colloid suspensions. The results show that collective variables that correlate with the number of particles in the condensed phase, the system potential energy, and approximate configurational entropy are the most appropriate order parameters.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Multidisciplinary Sciences
Navneet Singh, A. K. Sood, Rajesh Ganapathy
Summary: This study reports the observation of an intermediate hexatic phase during the melting of colloidal crystals on a sphere by tuning interparticle interactions in situ. Unlike in flat space, the melting process on a sphere exhibits the characteristics of ideal melting.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Multidisciplinary
Xiaofang Lv, Jie Zhang, Yi Zhao, Yang Liu, Jiawen Xu, Qianli Ma, Shangfei Song, Shidong Zhou
Summary: Through experimental study on the growth characteristics of NGH in an oil-water emulsion system, it was found that pressure, flow rate, and water cut affect the hydrate induction time, gas consumption, consumption rate, and hydrate volume fraction, obtaining important experimental rules. The induction time decreases with increasing pressure, flow rate, and water cut, while gas consumption and hydrate volume fraction increase with pressure and water cut, and decrease with flow rate.
Article
Energy & Fuels
Parisa Naeiji, Mengdi Pan, Manja Luzi-Helbing, Saman Alavi, Judith M. Schicks
Summary: A study was conducted to investigate the dissociation behavior of methane hydrates under different temperature and pressure conditions. Both experimental and simulated data showed that the behavior differed above and below the freezing point of water. At temperatures near or below freezing, CH4 hydrates exhibited self-preservation behaviors due to the formation of a quasi-liquid or amorphous phase at the outer layers of the hydrate crystal. Above the freezing point, dissociation appeared to initiate at the surface of the hydrate phase.
Article
Chemistry, Physical
Manju Sharma, Satyam Singh
Summary: This study investigates the enhanced CO2 sequestration in natural gas hydrates using DFT calculations and molecular dynamics simulations, through the formation of stable dual cages and Y-shaped clusters in the presence of flue and noble gases.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Hyung Joong Kim, Jong Hoon Kim, Jong Seok Jeong, Chang youn Moon, Sahn Nahm, Ki Min Nam, Jucheol Park, Young Heon Kim
Summary: In this study, the nucleation and crystallization of Bi particles on c-Bi2S3 and a-Bi12TiO20 matrices were investigated using in situ transmission electron microscopy (TEM) analysis. It was found that the growth process followed a two-step nucleation mechanism and was influenced by the matrix, leading to different morphologies and atomic structures of Bi particles on different matrices.
Article
Multidisciplinary Sciences
A. Escobar, M. Ledesma-Motolinia, J. L. Carrillo-Estrada, F. Donado
Summary: In this study, we investigated the two-step crystallization process of a magnetic active 2D-granular system placed on different lens concaveness and under the action of an alternating magnetic field. We found that the depth of the parabolic potential plays a significant role in the two-step features of the crystallization process. The initial formation of an amorphous aggregate in the central region of the lens is followed by the evolution to an ordered crystalline structure due to effective temperature and perturbations caused by free particles. The size of the nucleus and the shape of the aggregates are influenced by the depth of the parabolic potential.
SCIENTIFIC REPORTS
(2023)
Review
Energy & Fuels
Yogendra Kumar, Jitendra S. Sangwai
Summary: Immediate measures are needed to store large quantities of anthropogenic CO2 in geological and oceanic reservoirs to address global warming and climate change. This article discusses the long-term viability, environmental sustainability, and economic potential of CO2 sequestration in the form of hydrates into oceanic and subsea sediments. The analysis shows that CO2 is denser than seawater at depths above 2800 m, providing an additional barrier for CO2 escape.
Article
Energy & Fuels
Zhenchao Li, Yajun Deng, Shihang Rao, Hailong Lu
Summary: Molecular dynamics simulations were used to investigate the formation and distribution of hydrates in kaolinite slit pores with methane gas bubbles adsorbed on one surface. The results indicate that hydrates nucleate in the solution in pores and then grow into hydrate shells around methane gas bubbles, hindering methane diffusion. Additionally, the adsorption of methane on siloxane surfaces promotes its dissolution, benefiting hydrate formation. However, in siloxane-siloxane pores, the strong adsorption of siloxane surface forms layer-like bubbles with low methane concentration, inhibiting hydrate formation.
Article
Multidisciplinary Sciences
Yang Sun, Feng Zhang, Mikhail Mendelev, Renata M. Wentzcovitch, Kai-Ming Ho
Summary: Studies have found that the nucleation mechanism for the Earth's inner core involves the metastable body-centered cubic (bcc) phase of iron, which has a higher nucleation rate than the hexagonal close-packed (hcp) phase. This suggests that the bcc phase is likely the first step in inner core formation, rather than direct nucleation of the hcp phase. This discovery is important in solving the inner core nucleation paradox and provides insights into the structure and anisotropy of the present inner core.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Multidisciplinary
Hans-Georg Steinruck, Chuntian Cao, Yuchi Tsao, Christopher J. Takacs, Oleg Konovalov, Jenel Vatamanu, Oleg Borodin, Michael F. Toney
ENERGY & ENVIRONMENTAL SCIENCE
(2018)
Article
Chemistry, Physical
Dengpan Dong, Jenel P. Vatamanu, Xiaoyu Wei, Dmitry Bedrov
JOURNAL OF CHEMICAL PHYSICS
(2018)
Article
Chemistry, Physical
Jenel Vatamanu, Oleg Borodin, Dmitry Bedrov
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2018)
Article
Chemistry, Physical
Jonathan H. Raberg, Jenel Vatamanu, Stephen J. Harris, Christina H. M. van Oversteeg, Axel Ramos, Oleg Borodin, Tanja Cuk
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2019)
Article
Multidisciplinary Sciences
Cun Wang, Lidan Xing, Jenel Vatamanu, Zhi Chen, Guangyuan Lan, Weishan Li, Kang Xu
NATURE COMMUNICATIONS
(2019)
Article
Chemistry, Physical
Jiawei Chen, Jenel Vatamanu, Lidan Xing, Oleg Borodin, Huiyang Chen, Xiongcong Guan, Xiang Liu, Kang Xu, Weishan Li
ADVANCED ENERGY MATERIALS
(2020)
Article
Chemistry, Physical
Long Chen, Jiaxun Zhang, Qin Li, Jenel Vatamanu, Xiao Ji, Travis P. Pollard, Chunyu Cui, Singyuk Hou, Ji Chen, Chongyin Yang, Lin Ma, Michael S. Ding, Mounesha Garaga, Steve Greenbaum, Hung-Sui Lee, Oleg Borodin, Kang Xu, Chunsheng Wang
ACS ENERGY LETTERS
(2020)
Article
Nanoscience & Nanotechnology
Longsheng Cao, Dan Li, Travis Pollard, Tao Deng, Bao Zhang, Chongyin Yang, Long Chen, Jenel Vatamanu, Enyuan Hu, Matt J. Hourwitz, Lin Ma, Michael Ding, Qin Li, Singyuk Hou, Karen Gaskell, John T. Fourkas, Xiao-Qing Yang, Kang Xu, Oleg Borodin, Chunsheng Wang
Summary: The study introduces an aqueous zinc battery with a solid-electrolyte interphase that enables excellent performance in various tests, demonstrating its potential for practical applications in energy storage.
NATURE NANOTECHNOLOGY
(2021)
Article
Chemistry, Physical
Mingzhu Liu, Jenel Vatamanu, Xinli Chen, Lidan Xing, Kang Xu, Weishan Li
Summary: By combining theoretical and experimental approaches, this study identified the direct reaction between water and PF6- as the main source of corrosive HF in Li-ion batteries. This hydrolysis process is accelerated by high voltage, highlighting the need for effective mitigation strategies to stabilize LiPF6-based electrolytes for high voltage LIBs. Clarifying this important electrolyte failure mechanism points to the potential for improved battery performance and longevity.
ACS ENERGY LETTERS
(2021)
Article
Chemistry, Applied
Xuehuan Luo, Lidan Xing, Jenel Vatamanu, Jiawei Chen, Jiakun Chen, Mingzhu Liu, Cun Wang, Kang Xu, Weishan Li
Summary: The degradation of electrolytes in lithium-ion batteries caused by dissolved manganese (II) species has been recently identified. The use of A12C4 as an additive helps deactivate the catalytic activity of manganese (II) ions, improving the thermal stability of the electrolyte and enhancing cycling performance of the batteries. The strong binding effect of A12C4 reduces the charge density of manganese (II) ions, preventing their destruction of the electrolyte structure and improving overall stability.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Chemistry, Physical
Zekai Ma, Jiawei Chen, Jenel Vatamanu, Oleg Borodin, Dmitry Bedrov, Xianggui Zhou, Wenguang Zhang, Weishan Li, Kang Xu, Lidan Xing
Summary: A non-flammable hybrid electrolyte with a wide electrochemical stability window of 4.7 V and supporting fast ion transport at temperatures as low as -50 degrees C has been proposed, demonstrating high Coulombic efficiency in lithium-ion batteries at room temperature and remaining operational under extreme low temperatures.
ENERGY STORAGE MATERIALS
(2022)
Article
Multidisciplinary Sciences
Lin Ma, Jenel Vatamanu, Nathan T. Hahn, Travis P. Pollard, Oleg Borodin, Valeri Petkov, Marshall A. Schroeder, Yang Ren, Michael S. Ding, Chao Luo, Jan L. Allen, Chunsheng Wang, Kang Xu
Summary: Research shows that using methanol as an electrolyte solvent in rechargeable zinc metal batteries improves performance and stability, effectively solving issues in the battery, and has good cycle life at extreme temperatures.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Green & Sustainable Science & Technology
Chongyin Yang, Jiale Xia, Chunyu Cui, Travis P. Pollard, Jenel Vatamanu, Antonio Faraone, Joseph A. Dura, Madhusudan Tyagi, Alex Kattan, Elijah Thimsen, Jijian Xu, Wentao Song, Enyuan Hu, Xiao Ji, Singyuk Hou, Xiyue Zhang, Michael S. S. Ding, Sooyeon Hwang, Dong Su, Yang Ren, Xiao-Qing Yang, Howard Wang, Oleg Borodin, Chunsheng Wang
Summary: The global electrification of transportation and the increasing demand for grid energy storage are driving the growth of batteries worldwide. However, the supply chain of Li-ion batteries is facing challenges in sourcing essential and scarce materials. Therefore, there is a growing incentive to develop more sustainable battery chemistries.
NATURE SUSTAINABILITY
(2023)
Review
Chemistry, Multidisciplinary
Oleg Borodin, Xiaoming Ren, Jenel Vatamanu, Arthur von Wald Cresce, Jaroslaw Knap, Kang Xu
ACCOUNTS OF CHEMICAL RESEARCH
(2017)
Article
Chemistry, Physical
Fei Wang, Oleg Borodin, Michael S. Ding, Mallory Gobet, Jenel Vatamanu, Xiulin Fan, Tao Gao, Nico Edison, Yujia Liang, Wei Sun, Steve Greenbaum, Kang Xu, Chunsheng Wang
Article
Chemistry, Physical
Sergey Yu. Ketkov, Sheng-Yuan Tzeng, Elena A. Rychagova, Anton N. Lukoyanov, Wen-Bih Tzeng
Summary: Metallocenes, including methylcobaltocene, play important roles in various fields of chemistry. The ionization energy and vibrational structure of (Cp ')(Cp)Co can be influenced by introducing methyl substituents. The mass-analyzed threshold ionization spectrum and DFT calculations provide accurate information about the properties and transformations of (Cp ')(Cp)Co.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Review
Chemistry, Physical
Qifeng Mu, Jian Hu
Summary: Polymer mechanochemistry has experienced a renaissance due to the rapid development of mechanophores and principles governing mechanochemical transduction or material strengthening. It has not only provided fundamental guidelines for converting mechanical energy into chemical output, but also found applications in engineering and smart devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Da Hye Yang, Francesco Ricci, Fredrik L. Nordstrom, Na Li
Summary: Through systematic evaluation of the oiling-out behavior of procaine, we identified both stable and metastable liquid-liquid phase separation, and established phase diagrams to assist in rational selection of crystallization strategies.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Vikki Anand Varma, Simmie Jaglan, Mohd Yasir Khan, Sujin B. Babu
Summary: Designing engineering structures like nanocages, shells, and containers through self-assembly of colloids is a challenging problem. This work proposes a simple model for the subunit, which leads to the formation of monodispersed spherical cages or containers. The model with only one control parameter can be used to design cages with the desired radius.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Hainan Jiang, Yaolong He, Xiaolin Li, Zhiyao Jin, Huijie Yu, Dawei Li
Summary: The cycling lifespan and coulombic efficiency of lithium-ion batteries are crucial for high C-rate applications. The Li-ion concentration plays a crucial role in determining the mechanical integrity and structural stability of electrodes. This study focuses on graphite as the working electrode and establishes an experimental system to investigate the mechanical properties of composite graphite electrode at different C-rates. Considering the effect of Li-ion concentration in stress analysis is found to be significant.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Zhiye Wang, Yunchuan Li, Mingjun Sun
Summary: This study investigates the influence of intramolecular pi-pi interactions on the electronic transport capabilities of molecules. By designing and analyzing three pi-conjugated molecules, the researchers observe that different pi-conjugated structures have varying effects on electron transport. The findings provide a theoretical foundation for designing single-molecule electronic devices with multiple electron channels based on intramolecular pi-pi interactions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Yuandong Xu, Haoyang Feng, Chaoyang Dong, Yuqing Yang, Meng Zhou, Yajun Wei, Hui Guo, Yaqing Wei, Jishan Su, Yingying Ben, Xia Zhang
Summary: Hollow MoS2 cubes and spheres were successfully synthesized using a one-step hydrothermal method with the hard template method. The hollow MoS2 cubes exhibited higher specific capacitance and energy density compared to the hollow MoS2 spheres. The symmetrical supercapacitors assembled with these hollow structures showed good performance and high capacity retention after multiple cycles. These findings suggest that controlling the pore structure and surface characteristics of MoS2 is crucial for enhancing its electrochemical properties.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Ainhoa Oliden-Sanchez, Rebeca Sola-Llano, Joaquin Perez-Pariente, Luis Gomez-Hortiguela, Virginia Martinez-Martinez
Summary: The combination of photoactive molecules and inorganic structures is important for the development of advanced materials in optics. In this study, bulky dyes were successfully encapsulated in a zeolitic framework, resulting in emission throughout the visible spectrum.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Miaomiao Zhang, Cunyuan Pei, Qiqi Xiang, Lintao Liu, Zhongxu Dai, Huijuan Ma, Shibing Ni
Summary: The design of a solid electrolyte interphase (SEI) plays a crucial role in improving the electrochemical performance of anode materials. In this study, lithium difluoro(oxalate)borate (LiDFOB) is used as an electrolyte additive to form a protective SEI film on Li3VO4 (LVO) anodes. The addition of LiDFOB results in a dense, uniform, stable, and LiF-richer SEI, which enhances the Li-ion storage kinetics. The generated SEI also prevents further decomposition of the electrolyte and maintains the morphology of LVO anodes during charge/discharge processes. This work demonstrates the effectiveness of LiDFOB as a multi-functional additive for LiPF6 electrolytes and provides insights into SEI construction for high-performance LVO anodes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
B. V. Andryushechkin, T. V. Pavlova, V. M. Shevlyuga
Summary: The atomic structure of the Ag(111)-p(4 x 4)-O phase was reexamined and two phases with the same periodicity were discovered. It was demonstrated that the accepted Ag6 model is incompatible with high-resolution oxygen-sensitive STM images.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
S. L. Romo-Avila, D. Marquez-Ruiz, R. A. Guirado-Lopez
Summary: In this study, we used density functional theory (DFT) calculations to investigate the interaction between model graphene oxide (GO) nanostructures and chlorine monoxide ClO. We aimed to understand the role of this highly oxidizing species in breaking C-C bonds and forming significant holes on GO sheets. Our results showed that C-C bonds in a single graphene oxide sheet can be broken through a simple mechanism involving the dissociation of two chemically attached ClO molecules. The formation of carbonyl groups and holes on the GO surface was also observed. This study provides important insights into the degradation of carbon nanotubes and the stability of GO during the myeloperoxidase (MPO) catalytic cycle.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Alberto Garcia-Fernandez, Birgit Kammlander, Stefania Riva, Hakan Rensmo, Ute B. Cappel
Summary: In this study, the X-ray stability of five different lead halide perovskite compositions (MAPbI3, MAPbCl3, MAPbBr3, FAPbBr3, CsPbBr3) was investigated using photoelectron spectroscopy. Different degradation mechanisms and resistance to X-ray were observed depending on the crystal composition. Overall, perovskite compositions based on the MA+ cation were found to be less stable than those based on FA+ or Cs+. Metallic lead formation was most easily observed in the chloride perovskite, followed by bromide, and very little in MAPbI3. Multiple degradation processes were identified for the bromide compositions, including ion migration, formation of volatile and solid products, as well as metallic lead. CsBr was formed as a solid degradation product on the surface of CsPbBr3.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Timofei Rostilov, Vadim Ziborov, Alexander Dolgoborodov, Mikhail Kuskov
Summary: The shock-loading behavior of nanomaterials is investigated in this study. It is found that shock compaction waves exhibit a distinct two-step structure, with the formation of faster precursor waves that travel ahead of the main compaction waves. The complexity of the shock Hugoniot curve of the tested nanomaterial is described, and the effect of initial porosity on the compressed states is demonstrated.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Alexey A. Markov, Mikhail V. Patrakeev
Summary: The stability of La1/3Sr2/3Fe1-xMnxO3-delta, a perovskite-type oxide, under reducing conditions is dependent on the manganese content. Increasing the manganese content leads to a decrease in stability. The behavior of iron and manganese in the oxide shows distinct differences, which can be attributed to the difference in the enthalpy of oxidation reactions. Additionally, the change in the La/Sr ratio affects the concentration of iron and manganese ions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Mosayeb Naseri, Shirin Amirian, Mehrdad Faraji, Mohammad Abdur Rashid, Maicon Pierre Lourenco, Venkataraman Thangadurai, D. R. Salahub
Summary: Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3, this study assessed the structural stability and investigated the electronic, optical, and thermoelectric properties of a group of two-dimensional perovskite-type materials called perovskenes. The findings revealed that these materials are wide bandgap semiconductors with potential application in UV shielding. Moreover, they exhibit better electrical and thermal conductivity at high temperatures, enabling efficient power generation in thermoelectric devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)