Review
Chemistry, Physical
Lulu Zhang, Jun Huang
Summary: This Opinion article addresses the challenges in measuring and interpreting the electric double layer (EDL) at Pt(111)/aqueous solution interfaces using classical electrochemical methods. The article discusses discrepancies in measuring double layer capacitance, examines assumptions and limitations of the Frumkin-Melik-Gaikazyan (FMG) model, and compares the capacitance values derived from cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The article aims to contribute to a better understanding of the EDL at Pt(111)/aqueous solution interfaces.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Review
Chemistry, Physical
Katharina Doblhoff-Dier, Marc T. M. Koper
Summary: The electric double layer is a fundamental concept in electrochemistry, but its exact structure remains unresolved. This study discusses the current knowledge and gaps in understanding the structure of the Pt(111) double layer near the potential of zero charge (pzc). By analyzing various models, it is suggested that water adsorption at the interface plays an important role in interpreting capacitance features observed near the pzc. However, the deviations from Gouy-Chapman diffuse layer theory in low electrolyte concentration require further investigation.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Physical
Hualin Zhan, Richard Sandberg, Fan Feng, Qinghua Liang, Ke Xie, Lianhai Zu, Dan Li, Jefferson Zhe Liu
Summary: Machine learning can be used to establish a physics-based nanocircuit model, allowing for the prediction and evaluation of electrical characteristics in nanoporous ionic systems. This approach provides insights into ion dynamics in nanoporous electrodes, such as nonideal cyclic voltammetry and dynamic, pore-size-dependent surface conductance.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Selwyn Hanselman, Federico Calle-Vallejo, Marc T. M. Koper
Summary: Surface platinum hydride structures on Pt(111) play a potentially important role in electrocatalysis and cathodic corrosion. Using thermodynamic methods and density functional theory, multiple surface hydride structures on Pt(111) were compared. These structures contain multiple monolayers of hydrogen that can bind subsurface or reconstruct the surface. Stable configurations share one monolayer of subsurface H stacking between the top two Pt layers. Our work provides insight into the operando surface state during low-potential reduction reactions on Pt(111) and shows a plausible precursor for cathodic corrosion.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Huichen Xie, Zheng Li, Jian Zhu, Hao Li, Qing Yang, Yang Yang, Can Li
Summary: The deposition of Pt co-catalysts solely on Au nanoparticles has been found to enhance the activity of plasmonic photocatalytic reactions and improve charge separation efficiency.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Huichen Xie, Zheng Li, Jian Zhu, Hao Li, Qing Yang, Yang Yang, Can Li
Summary: Chemical processes induced by surface plasmon resonance have attracted attention in the field of photocatalysis. This study reports the selective deposition of Pt co-catalysts on Au nanoparticles, resulting in improved activity of plasmonic photocatalysts. The results reveal that Pt solely on Au NPs provides higher photocatalytic activity due to enhanced charge separation efficiency.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Review
Chemistry, Physical
Timur Aslyamov
Summary: The properties of the electric double layer (EDL) play a crucial role in various scientific and technological applications. This review focuses on publications that investigate electrolyte behavior in contact with rough electrodes. The surface geometry of the electrodes directly affects ion distributions, leading to key effects such as increased accumulated charge, changes in the dependence of differential capacitance on applied potential, and a constant phase element contribution to impedance. The review also highlights the limitations of current approaches and suggests potential solutions for improvement.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Article
Chemistry, Physical
Yue Wang, Yifei Sun, Yubin Dong, Guocai Tian
Summary: The microscopic structures of ionic liquids ([Emmim]TFSI and [Emim]TFSI) on a flat Au(111) surface were studied using molecular dynamics simulations. The results show that the substitution of hydrogen on C1 by methyl groups in the imidazole ring increases the interaction between the particles. Different interaction energies of various particles lead to changes in anion conformation and cation orientation, ultimately affecting the images on Au(111) differently in the two systems. These findings provide a new perspective for studying double layer structures and deepen the understanding of interface behavior of ionic liquids.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Multidisciplinary Sciences
Kasinath Ojha, Katharina Doblhoff-Dier, Marc T. M. Koper
Summary: This study presents detailed measurements of the double-layer capacitance at the Pt(111)-electrolyte interface near the potential of zero charge (PZC). Strong deviations from traditional Gouy-Chapman-Stern behavior are observed at low electrolyte concentrations, independent of the nature of the electrolyte ions. The capacitance further away from PZC and the trends for increasing ion concentration show ion-specific effects related to ion size or hydration strength. A model is formulated to explain the structure of the electric double layer at the Pt(111)-electrolyte interface, going beyond the Gouy-Chapman-Stern theory.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Benjamin Bobin Ye, Zhen-Gang Wang
Summary: Recent mean-field theories predict spontaneous surface charge separation in room-temperature ionic liquid electric double-layer capacitors without applied potential. In this study, a coarse-grained molecular model is constructed to directly simulate the behavior of the ionic liquid, revealing the importance of image charge interactions and enhanced in-plane ordering on electrodes, which are not considered by mean-field theories.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Electrochemistry
Huan Yin, Hui Shao, Barbara Daffos, Pierre-Louis Taberna, Patrice Simon
Summary: The charge mechanisms in TiC-derived nanoporous carbons synthesized at different temperatures were studied using EQCM. The results showed that the microstructure of the carbon materials influenced the charge storage mechanism.
ELECTROCHEMISTRY COMMUNICATIONS
(2022)
Article
Nanoscience & Nanotechnology
Fang-Yu Lin, Pei-Yuan Lee, Tien-Fu Chu, Chang- Peng, Gou-Jen Wang
Summary: The study introduces a Pt/Au alloy electrode for enzyme-free glucose detection in a neutral environment with excellent specificity and sensitivity, showing feasibility for clinical applications.
INTERNATIONAL JOURNAL OF NANOMEDICINE
(2021)
Article
Biochemistry & Molecular Biology
Pawel Krukowski, Takuma Hattori, Megumi Akai-Kasaya, Akira Saito, Hideji Osuga, Yuji Kuwahara
Summary: The light emission properties of helicene molecules on Au(111) surfaces were investigated using tunneling-current-induced light-emission technique. Plasmon-originated light emission was observed on the helicene/Au(111) surface, but suppressed at the edges of the Au(111) terraces where the molecules were adsorbed. To overcome this, C-60 layers were used as decoupling buffer layers. The multilayers of helicene molecules on C-60 showed strong luminescence modulated by the molecular electronic states.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Multidisciplinary
Yue Wang, Guocai Tian
Summary: The microstructure and electronic structure of different ionic liquids lead to interesting universal laws in the electrical double layers. The morphology of anions on electrode surface varies due to geometric differences, and the energy levels are influenced by the electronegativity of central atoms. Stronger interactions between particles and electrodes result in unique patterns and thinner effective EDL, impacting the differential capacitance values.
Article
Chemistry, Physical
Kareem M. Gameel, Mohamed K. Elshazly, Ahmed Huzayyin, Francis Dawson
Summary: We present a computational model based on density functional theory (DFT) calculations to calculate the interfacial capacitance of low-dimensional materials in contact with a bulk substrate. The model incorporates key electrostatic and quantum mechanical components and introduces a material-agnostic formalism based on classical electromagnetic theory. Case studies on monolayer and bilayer graphene adsorbed on a silica substrate show that the predicted electrostatic capacitance of the interfaces is field-independent and aligns well with experimental measurements, offering a better understanding of the electrochemical behavior of nanoscopic interfaces.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Review
Electrochemistry
Soumya Mukherjee, Shujin Hou, Sebastian A. Watzele, Batyr Garlyyev, Weijin Li, Aliaksandr S. Bandarenka, Roland A. Fischer
Summary: Taking into account the United Nations Sustainable Development Goal 7 on affordable and clean energy, metal-organic frameworks (MOFs) and derived materials have attracted research interest in electrocatalysis. This review summarizes recent advances in MOF-based electrocatalysts exclusively prepared through indirect post-treatments.
Article
Electrochemistry
Xing Ding, Daniel Scieszka, Sebastian Watzele, Song Xue, Batyr Garlyyev, Richard W. Haid, Aliaksandr S. Bandarenka
Summary: Efficient electrocatalysis is a crucial solution to recent energy challenges, although the prediction and explanation of the influence of seemingly inert electrolyte components on activity have posed significant complications in this field. This study uses a unique laser-induced current transient technique to investigate different electrocatalytic systems and answer the fundamental question of how inactive electrolytes can drastically change activity.
Review
Electrochemistry
Xing Ding, Theophilus Kobina Sarpey, Shujin Hou, Batyr Garlyyev, Weijin Li, Roland A. Fischer, Aliaksandr S. Bandarenka
Summary: Understanding processes, phenomena, and mechanisms at the electrode/electrolyte interface is crucial for optimizing electrochemical systems. The introduction of sub-microsecond laser pulses has simplified the investigation of the electrochemical interface, and the laser-induced current transient and laser-induced potential transient techniques have proven to be valuable tools.
Article
Chemistry, Physical
Xaver Lamprecht, Iman Evazzade, Iago Ungerer, Ludek Hromadko, Jan M. Macak, Aliaksandr S. Bandarenka, Vitaly Alexandrov
Summary: In this study, the degradation mechanisms of a model Na2Ni[Fe(CN)6] functional electrode in aqueous electrolytes are elucidated through density functional theory calculations and experiments. Besides solution pH and cation concentration, anion adsorption is identified as the main driving force for electrode dissolution. The nature of adsorbed anions can control the mass and charge transfer mechanisms during metal cation intercalation as well as the electrode degradation rate. The findings of this study provide practical guidelines for electrolyte optimization and can be extrapolated to the entire family of PBAs operating in aqueous media.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Song Xue, Ru Liu, Yadi Cheng, Sebastian Watzele, Xiangju Song, Mengke Liu, Yajing Zhang, Guanghu He, Oded Nir, Minghua Huang, Heqing Jiang
Summary: Monopolar membrane-assisted electrolyzers enable water electrolysis using acid-alkali asymmetric electrolytes. It works by utilizing the chemical potential gradient between the asymmetric electrolytes, which modifies the reversible hydrogen electrode potential and reduces the necessary external potential. The performance of this electrolyzer depends on various factors and when coupled with advanced electrocatalysts, it achieves high current density and outperforms conventional water electrolyzers.
JOURNAL OF POWER SOURCES
(2023)
Article
Energy & Fuels
Kun-Ting Song, Christian M. Schott, Peter M. Schneider, Sebastian A. Watzele, Regina M. Kluge, Elena L. Gubanova, Aliaksandr S. Bandarenka
Summary: In this work, the hydrogen evolution reaction (HER) catalyzed by polycrystalline Pt (Pt(pc)) and Pt5Gd disc electrodes was studied, and they were characterized using rotating disc electrode (RDE) and electrochemical impedance spectroscopy techniques simultaneously. Pt5Gd exhibited higher HER activities than Pt in acidic and alkaline media due to strain and ligand effects. The mechanistic study revealed that the Volmer-Tafel pathway dominated the HER in the Pd/C nanostructured catalysts.
JOURNAL OF PHYSICS-ENERGY
(2023)
Article
Chemistry, Physical
Mohammad R. Nouri, Regina M. Kluge, Richard W. Haid, Jill Fortmann, Alfred Ludwig, Aliaksandr S. Bandarenka, Vitaly Alexandrov
Summary: A study shows that tunneling current fluctuations in electrochemical scanning tunneling microscopy (EC-STM) can map the electrocatalytic activity of surfaces with high spatial resolution. By using electron transport calculations, the study examines tunneling at Pt surfaces under the conditions of the oxygen reduction reaction. The results suggest that detecting reaction intermediates at electrified interfaces in operando conditions is possible based on tunneling noise amplitudes.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Applied
Thorsten O. O. Schmidt, Richard W. W. Haid, Elena L. L. Gubanova, Regina M. M. Kluge, Aliaksandr S. S. Bandarenka
Summary: To advance the design of electrocatalytically active catalysts, understanding the nature of active sites is crucial. The complexity of factors such as material composition, site coordination, electrolyte effects, and the support material makes the identification of active sites challenging. In-situ experiments, such as electrochemical scanning tunneling microscopy (EC-STM), play a significant role in identifying active centers while the reaction takes place. This technique has been successfully used to determine active sites on palladium (Pd) surfaces under strain effects and on graphite-based surfaces considering the effects of coordination.
TOPICS IN CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Leon Katzenmeier, Manuel Goesswein, Leif Carstensen, Johannes Sterzinger, Michael Ederer, Peter Mueller-Buschbaum, Alessio Gagliardi, Aliaksandr S. Bandarenka
Summary: The interface between metallic lithium and solid-state electrolytes is investigated to understand the charge and mass transport mechanisms and the underlying mechanisms of charge accumulation. This is crucial for developing high-performance solid-state batteries.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Physical
Thorsten O. Schmidt, Andre Wark, Richard W. Haid, Regina M. Kluge, Shinya Suzuki, Kazuhide Kamiya, Aliaksandr S. Bandarenka, Jun Maruyama, Egill Skulason
Summary: This study successfully mimics the water oxidation reaction of Photosystem II by developing manganese oxide nanosheets as affordable and abundant electrocatalysts. Detailed investigation reveals that the detected activity at the nanosheet edges is crucial for the enhanced performance of the catalyst.
ADVANCED ENERGY MATERIALS
(2023)
Article
Electrochemistry
Goektug Yesilbas, Chun-Yu Chou, Aliaksandr S. Bandarenka
Summary: This article presents a physical impedance model that accurately describes the impedance spectra of graphite electrodes in a coin-cell assembly. The model parameters are analyzed to verify its effectiveness. Additionally, the authors propose using double layer capacitance values to determine if the normalized values align with expectations.
Article
Chemistry, Physical
Mohammad R. Nouri, Regina M. Kluge, Richard W. Haid, Jill Fortmann, Alfred Ludwig, Aliaksandr S. Bandarenka, Vitaly Alexandrov
Summary: Recently, it has been proposed that tunneling current fluctuations in electrochemical scanning tunneling microscopy can be used to map the electrocatalytic activity of surfaces with high spatial resolution. This study investigates tunneling at Pt surfaces during the oxygen reduction reaction and reveals that the tunneling barrier is influenced by the chemical identity of adsorbed reaction intermediates and the orientation of water species' dipole moment. Theoretical results combined with EC-STM measurements suggest that detecting reaction intermediates at electrified interfaces is possible based on tunneling noise amplitudes, and this study aims to stimulate further explorations of tunneling-based electron-proton transfers for quantum electrocatalysis.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Xaver Lamprecht, Iman Evazzade, Iago Ungerer, Ludek Hromadko, Jan M. Macak, Aliaksandr S. Bandarenka, Vitaly Alexandrov
Summary: In this study, the mechanism of degradation of model Na2Ni[Fe(CN)(6)] functional electrodes in aqueous electrolytes was investigated using density functional theory calculations and experiments. It was found that anion adsorption plays a significant role in electrode dissolution, with weakly adsorbing anions impeding degradation and strongly adsorbing anions accelerating it.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Review
Chemistry, Physical
Haiting Yu, Christian Schott, Thorsten Schmidt, Peter M. Schneider, Kun-Ting Song, Qiwei Zhang, Andrea Capogrosso, Lewin Deville, Elena Gubanova, Aliaksandr S. Bandarenka
Summary: Electrocatalysis plays a crucial role in transitioning to a renewable energy society. In this manuscript, the recent progress in the observation of active sites in various electrocatalysts and reactions is analyzed using operando microscopies. These techniques allow for real-time identification and comprehensive observation of electrocatalytic behavior, providing insights into reaction steps and correlating activity with catalyst properties.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Regina M. Kluge, Richard W. Haid, Alexander Riss, Yang Bao, Knud Seufert, Thorsten O. Schmidt, Sebastian A. Watzele, Johannes Barth, Francesco Allegretti, Willi Auwarter, Federico Calle-Vallejo, Aliaksandr S. Bandarenka
Summary: This study focuses on the catalytic design of oxygen reduction reaction, determining the composition and geometric configuration of optimal catalytic active sites through a combination of experiments and models. The lattice compression resulting from alloying Pt with 3d transition metals gradually increases the generalized coordination number of surface Pt atoms, making (111) terraces highly active.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
