Article
Chemistry, Physical
Xiaohu Yang, Hanqing Gu, Qiwen Sun, Wenming Zhang, Zhanyu Li
Summary: As a promising competitor for large-scale energy storage components in the future, aluminum batteries have gained attention. However, the sensitivity to air and corrosiveness of nonaqueous electrolytes hinder the development of aluminum ion batteries. Aluminum batteries meet the needs of green development and are a key research focus.
ENERGY STORAGE MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Hongxia Hao, Ellen M. Adams, Sarah Funke, Gerhard Schwaab, Martina Havenith, Teresa Head-Gordon
Summary: Transport mechanisms of solvated protons in reverse micelles containing NaAOT or CTABr were studied using reactive force field simulations. The proton hopping events were found to be suppressed for NaAOT and completely ceased for CTABr. The sluggish proton dynamics in both charged reverse micelles were attributed to the expulsion of hydronium and chloride ions from the interface, resulting in increased pH of the acid pools compared to nonionic reverse micelles. The localized oscillatory hopping dominated in the charged micelles, especially for CTABr, where the proton residence time was significantly increased.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Jicai Liang, Hao Wei, Kaifeng Yu, Chengjiang Lin, Hongfei Li, Mingming Ding, Xiaozheng Duan
Summary: The study utilizes coarse-grained molecular dynamics simulations to investigate the structural and dynamic properties of ionic solutions, highlighting the impact of ion solvation, electrostatic correlations, and applied electric fields on the systems. The research reveals nontrivial microscopic molecular features such as solvent reorganization, ion clustering, and ion diffusion, offering insights into physicochemical properties of ion-containing liquids and contributing to the development of ion-containing materials.
Article
Chemistry, Multidisciplinary
Hongxia Hao, Ellen M. Adams, Sarah Funke, Gerhard Schwaab, Martina Havenith, Teresa Head-Gordon
Summary: Through reactive force field simulations, this study analyzed the transport mechanisms of solvated protons in 1 M hydrochloric acid confined within reverse micelles (RMs) containing either the negatively charged surfactant sodium bis(2-ethylhexyl) sulfosuccinate (NaAOT) or the positively charged surfactant cetyltrimethylammonium bromide (CTABr). The findings suggest that the proton hopping events are further suppressed in NaAOT RMs compared to nonionic RMs, while the Grotthuss mechanism ceases altogether in CTABr RMs. The slow proton dynamics in both charged RMs can be attributed to the expulsion of hydronium and chloride ions from the interface, increasing the pH of the acid pools.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Viktor Rozsa, Giulia Galli
Summary: The interaction between ions and water at high pressure and temperature has significant effects on geochemical properties. However, the average structural and vibrational properties of water are weakly affected by ions at extreme conditions, and the presence of ions only slightly increases the ionic conductivity of the liquid and moderately reduces the dielectric constant.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Shahrazad M. A. Malek, Victor Kwan, Ivan Saika-Voivod, Styliani Consta
Summary: The interactions between water and ions within droplets are critical in the chemical reactivity of atmospheric and man-made aerosols. Computational evidence shows that in supercooled aqueous nanodroplets, a lower density core of tetrahedrally coordinated water expels ions to the denser subsurface. At room temperature, the radial distribution in the droplet core varies depending on the ion's nature.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Yulia V. Novakovskaya
Summary: The stationary nonempirical simulations of [Na(H2O)n]+ clusters with n in the range of 28-51 reveal the interrelated structural and energetic peculiarities of the sodium ion hydration structures. The differences and correlations between the stationary and averaged dynamically changing configurations are quantified. The coordination neighborhoods of the sodium ion are predicted depending on its local fraction in actual specimens.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Austin O. Atsango, Tobias Morawietz, Ondrej Marsalek, Thomas E. Markland
Summary: The transport of excess protons and hydroxide ions in water is crucial for many important chemical and biological processes. Traditional simulation methods are prohibitively expensive for accurately modeling the associated transport mechanisms. In this study, machine-learned potentials (MLPs) are developed to simulate the transport of excess protons and hydroxide ions at a fraction of the cost of traditional methods, while still reproducing the trends observed in ab initio simulations. These simulations provide insights into the role of hypercoordination in the transport mechanism of hydroxide ions and support the asymmetry in diffusion between excess protons and hydroxide ions.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Medicinal
Kosuke Kawama, Yusaku Fukushima, Mitsunori Ikeguchi, Masateru Ohta, Takashi Yoshidome
Summary: In this study, a deep learning model is proposed to rapidly estimate the distribution functions and position of water molecules around proteins, with a prediction time more than two orders of magnitude faster than traditional methods. The predicted results show good agreement with the actual distribution functions obtained using traditional methods.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2022)
Article
Chemistry, Multidisciplinary
Takakazu Seki, Chun-Chieh Yu, Kuo-Yang Chiang, Alessandro Greco, Xiaoqing Yu, Fumiki Matsumura, Mischa Bonn, Yuki Nagata
Summary: In typical aqueous systems, multiple ion species are co-solvated, and these ions at the water-air interface can have significant impacts on chemical reactivity, aerosol formation, climate, and water odor. Through sum-frequency generation spectroscopy, researchers have quantified the relative surface activity of two co-solvated ions and found that hydrophobic ions tend to be speciated to the water interface due to the presence of hydrophilic ions. The speciation of ions at electrolyte solution interfaces is determined by the solvation energy difference between the ions and the intrinsic surface propensity of ions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Datian Li, Weiqing Liu, Wenhao Chen, Baoshuo Han, Xiaobo Xu, Qingqing Chang, Zhuoyu Yang, Yixiao Wang
Summary: A new model is established to reveal the storage mechanism of multivalent metal ions, especially Al3+ ions, in aqueous batteries. The results obtained in this work have great significance for understanding the role of multivalent cations on metal oxide surfaces in aqueous batteries and can be extended to other fields such as supercapacitors, photovoltaics, and photocatalysis.
ELECTROCHIMICA ACTA
(2023)
Article
Chemistry, Multidisciplinary
Yanxin Shang, Shi Chen, Nan Chen, Yuejiao Li, Jingning Lai, Yue Ma, Jun Chen, Feng Wu, Renjie Chen
Summary: Aqueous batteries are gaining attention for their safety and low cost. However, their narrow electrochemical stability window and limited working temperature range have posed challenges. This study introduces a new solvent that can break the water hydrogen bond network and enhance the stability of the electrolyte, resulting in a wider stability window and lower freezing point. The electrolyte also demonstrates good cycling performance at high temperatures.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Chemistry, Physical
Qingqing Tu, Wenwen Liu, Meng Jiang, Wenjuan Wang, Qing Kang, Pengcheng Wang, Weijia Zhou, Feimeng Zhou
Summary: A NiFe-LDH catalyst with partially crystalline characteristics was synthesized, showing high catalytic activity and stability during seawater electrolysis. The presence of more boundaries in the partially crystalline NiFe-LDH contributes to its higher catalytic efficiency and stability in alkalized seawater.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Engineering, Environmental
Chao Meng, Weidong He, Zhen Kong, Zhenyan Liang, Huaping Zhao, Yong Lei, Yongzhong Wu, Xiaopeng Hao
Summary: This study demonstrates a new strategy of tuning the electrolyte solvation structure and electrode interface to achieve highly reversible zinc plating/stripping. The introduction of acetonitrile as a co-solvent attenuates the solvation of Zn2+ and water activity, leading to an adaptive zinc-electrolyte interface. This electrolyte engineering significantly prevents undesired reactions and improves the cycling stability and rate performance of zinc-ion batteries in various systems.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Eva Zunzunegui-Bru, Elisabeth Gruber, Stefan Bergmeister, Miriam Meyer, Fabio Zappa, Massimiliano Bartolomei, Fernando Pirani, Pablo Villarreal, Tomas Gonzalez-Lezana, Paul Scheier
Summary: In this study, helium clusters around SF6+ and SF5+ ions were investigated using a combination of experimental and theoretical approaches. The analysis of ion yields and molecular dynamics calculations revealed the existence of stable configurations at specific sizes for the helium clusters interacting with the ions. This research provides new insights into the energetics and structure of He-N-SF6+ and He-N-SF5+ clusters.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Gabriel L. S. Rodrigues, Elias Diesen, Johannes Voss, Patrick Norman, Lars G. M. Pettersson
Summary: The desorption of a carbon monoxide molecule from a Ru(0001) surface was investigated using X-ray Absorption Spectra (XAS) and computational methods (TP-DFT and TD-DFT). The study revealed that the CO molecule exhibits gas-phase character at a distance of 2.3 Å from the surface. The C 1s XAS is insensitive to changes in the C-O bond length, while the O 1s excitation is sensitive to stretching of the CO bond. The study demonstrated that the TD-DFT method, using common exchange-correlation functionals and finite-size clusters, can accurately describe the spectral evolution of the 1s → π* transition with correct spin and gas-to-chemisorbed chemical shifts.
STRUCTURAL DYNAMICS-US
(2022)
Article
Chemistry, Multidisciplinary
Rui Shi, Wenjie Liao, Pedro J. Ramirez, Ivan Orozco, Mausumi Mahapatra, Jindong Kang, Adrian Hunt, Iradwikanari Waluyo, Sanjaya D. Senanayake, Ping Liu, Jose A. Rodriguez
Summary: This study investigates the structure and reactivity of potassium oxides in contact with the gold surface, using various techniques. It reveals a significant correlation between the structure, oxidation state, and chemical activity of the alkali oxide.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Alex C. Schilling, Nisa Ulumuddin, Volkan Cinar, Ryan T. Hannagan, Kyle Groden, Yicheng Wang, Laura A. Cramer, Paul L. Kress, Dipna A. Patel, Beverly Vo, Adrian Hunt, Phillip Christopher, Iradwikanari Waluyo, Jean-Sabin McEwen, E. Charles H. Sykes
Summary: This study investigates the behavior of Rh single atoms and small clusters on the 29 Cu2O thin film using a surface science approach. Unlike Pt, Rh atoms and clusters coexist and enable low-temperature CO oxidation through different pathways. DFT calculations quantify the energetics of these pathways, while STM and XPS experiments confirm the findings.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Fernando Garcia-Martinez, Lisa Raemisch, Khadiza Ali, Iradwikanari Waluyo, Rodrigo Castrillo Bodero, Sebastian Pfaff, Ignacio J. Villar-Garcia, Andrew Leigh Walter, Adrian Hunt, Virginia Perez-Dieste, Johan Zetterberg, Edvin Lundgren, Frederik Schiller, J. Enrique Ortega
Summary: By using curved crystals, the effect of A-type and B-type atomic packing of steps on the catalytic CO oxidation on Rh was investigated. The experiments showed that B-steps are more efficient than A-steps.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Ning Rui, Erwei Huang, Jeongjin Kim, Vikram Mehar, Rui Shi, Rina Rosales, Yi Tian, Adrian Hunt, Iradwikanari Waluyo, Sanjaya D. Senanayake, Ping Liu, Jose A. Rodriguez
Summary: Understanding the behavior of CH3O species on the surface is crucial for the efficient production of methanol. Recent research has shown that inverse ZrO2/Cu catalysts are highly active and selective for CO2 to methanol conversion. The use of synchrotron-based XPS and DFT calculations revealed the important role of formate and methoxy intermediates in methanol synthesis. Water vapor can significantly reduce the energy barrier for methanol formation, suggesting a practical method to improve methanol selectivity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Jiayue Wang, Dmitri Kalaev, Jing Yang, Iradwikanari Waluyo, Adrian Hunt, Jerzy T. Sadowski, Harry L. Tuller, Bilge Yildiz
Summary: Exsolution is a recent advancement in fabricating oxide-supported metal nanoparticle catalysts. The kinetics of metal exsolution depends on the kinetics of oxygen release from the host oxide, in addition to the kinetics of metal cation diffusion. This study demonstrates that in the thin-film perovskite SrTi0.65Fe0.35O3 (STF) system, surface oxygen release governs the metal nanoparticle exsolution kinetics. Increasing the oxygen release rate in STF accelerates the Fe0 exsolution kinetics and increases the quantity of exsolved Fe0 over time.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Jesu's Graciani, David C. Grinter, PedroJ. Ramirez, Robert M. Palomino, Fang Xu, Iradwikanari Waluyo, Dario Stacchiola, Javier Fdez Sanz, Sanjaya Senanayake, Jose A. . Rodriguez
Summary: The surface chemistry of alcohol synthesis from CO2 hydrogenation was investigated over a Pt/CeOx/TiO2 catalyst, which showed high selectivity towards methanol and ethanol. The addition of water promoted the formation of C-C bonds and enhanced the production of ethanol.
Article
Chemistry, Physical
Linda I. Vogt, Julien J. H. Cotelesage, Natalia V. Dolgova, Curtis Boyes, Muhammad Qureshi, Dimosthenis Sokaras, Samin Sharifi, Simon J. George, Ingrid J. Pickering, Graham N. George
Summary: The sulfur K near-edge X-ray absorption spectroscopy (XAS) and sulfur K beta X-ray emission spectroscopy (XES) of sulfones show significant variability depending on the coordination and organic groups bound to the sulfonyl group. Density functional theory simulations enable accurate reproduction and analysis of the spectra, indicating the potential for ab initio prediction of sulfur X-ray absorption and emission spectra of sulfones. This research demonstrates the use of X-ray spectroscopy as an in situ probe of sulfone chemistry.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
David Degerman, Patrick Lomker, Christopher M. Goodwin, Mikhail Shipilin, Fernando Garcia-Martinez, Christoph Schlueter, Anders Nilsson, Peter Amann
Summary: Operando X-ray photoelectron spectroscopy was used to investigate the surface state of Ni(111) and Ni(211) single crystal surfaces during CO hydrogenation. The results showed that at higher temperatures and hydrogen content, CO moved away from on-top configurations and toward multicoordinated sites on the nickel surface. A nickel carbide was formed in the surface near region, especially at high partial pressures of CO and lower temperatures. The presence of the carbide affected CO bonding, but was reduced during hydrogen-rich conditions and temperatures above 250 degrees C.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Ning Rui, Xuelong Wang, Kaixi Deng, Jorge Moncada, Rina Rosales, Feng Zhang, Wenqian Xu, Iradwikanari Waluyo, Adrian Hunt, Eli Stavitski, Sanjaya D. Senanayake, Ping Liu, Jose A. Rodriguez
Summary: The use of an indium oxide (In2O3)-based catalyst in the hydrogenation of CO2 to methanol shows high selectivity and catalytic activity, significantly increasing the methanol yield. The dynamic nature of the RuO2/In2O3 catalyst structure under CO2 hydrogenation conditions leads to the formation of RuOx-In2O3-x interfacial sites, which promote selective methanol synthesis.
Article
Chemistry, Physical
Sha Tan, Muhammad Mominur Rahman, Zhaohui Wu, Haodong Liu, Shen Wang, Sanjit Ghose, Hui Zhong, Iradwikanari Waluyo, Adrian Hunt, Ping Liu, Xiao-Qing Yang, Enyuan Hu
Summary: Sulfurized polyacrylonitrile (SPAN) has been extensively studied due to its low cost, high capacity, and great reversibility. However, the reaction mechanism of SPAN remains poorly understood. In this study, synchrotron-based pair distribution function (PDF) analysis and soft X-ray absorption spectroscopy (sXAS) were used to investigate the structural and interphasial changes of SPAN. PDF analysis revealed key structural features of SPAN, such as C-S bond, sulfur dimer, and sulfur chain. sXAS showed surface changes of SPAN, including the formation of a negatively charged carbon or fused benzene layer and an electrolyte decomposition layer.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
David Degerman, Christopher M. Goodwin, Patrick Lomker, Fernando Garcia-Martinez, Mikhail Shipilin, Andrei Gloskovskii, Anders Nilsson
Summary: By rapidly switching from high pressure to low pressure, this method allows for the detection of the remnant high pressure surface and the dynamics during re-equilibration. It provides faster and more detailed spectra compared to static operando measurements. However, there are different explanations for the different adsorbate distributions and the faster accumulation of CHx in CO2 and CO hydrogenation reactions.
Article
Chemistry, Physical
Dongha Kim, Adrian Hunt, Iradwikanari Waluyo, Bilge Yildiz
Summary: The segregation and re-incorporation of dopants in perovskite oxides can be influenced by the defect reactions involving cation vacancies and oxygen holes under different potential. Anodic conditions can lead to the re-incorporation of surface dopants into the bulk of the material, improving the oxygen exchange kinetics of the perovskite oxide surface.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Vikram Mehar, Wenjie Liao, Mausumi Mahapatra, Rui Shi, Hojoon Lim, Irene Barba-Nieto, Adrian Hunt, Iradwikanari Waluyo, Ping Liu, Jose A. Rodriguez
Summary: This study investigates the behavior of CsOx nanostructures grown on Au(111) as active centers for CO2 binding and hydrogenation reactions. The results show that CsOx nanostructures exhibit excellent catalytic performance in CO2 hydrogenation, producing formate as an important intermediate.
Article
Chemistry, Multidisciplinary
Jiayue Wang, Kevin B. Woller, Abinash Kumar, Zhan Zhang, Hua Zhou, Iradwikanari Waluyo, Adrian Hunt, James M. LeBeau, Bilge Yildiz
Summary: Ion irradiation is a promising method for controlling the size, composition, and location of metal nanoparticles during exsolution. By using ion sputtering, implantation, and defect generation mechanisms, researchers have successfully reduced the size of exsolved nanoparticles and tailored their composition. Additionally, irradiation creates point defects and defect clusters that serve as nucleation sites for metal exsolution. Nanocatalysts prepared by irradiation-assisted exsolution exhibit superior catalytic activity compared to those produced using conventional methods.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
