Time-resolved correlations of the environment, the reaction products, the energy transfer and the material structures during the reaction processes make operando gas and heating TEM more and more attractive in recent years. The time delays existing among parameter measurement locations need to be calibrated for valid correlations. Otherwise, erroneous conclusions would be drawn, such as over/under-estimating the critical temperatures, mismatching the structure and composition relationships to activities, and so on. Herein, we report on a method synchronizing the data from pre-, in- and post-TEM by measuring and calibrating the time delays involved. This method relies on the unique capability of on-chip calorimetry of the gas Nano-Reactor, which is intrinsically synchronized with the TEM imaging and spectroscopy data. The time delay is found to be dependent on the gas flow rate and pressure, and have little dependence on the gas type. A functional relationship fitted between the time delay and the gas flow rate and pressure can automate the time delay calibration and thus synchronize the data from different locations. Based on the investigations, we developed algorithms and scripts to enable the automatic data synchronization in operando gas and heating TEM in both real time experiments and post experiments.
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http://dx.doi.org/10.1016/j.ultramic.2022.113549 | DOI Listing |
Small Methods
January 2025
College of Physics and Energy, Fujian Provincial Key Laboratory of Quantum Manipulation and New Energy Materials, Fujian Normal University, Fuzhou, 350117, China.
The Solid Electrolyte Interphase (SEI) is a nanoscale thickness passivation layer that forms as a product of electrolyte decomposition through a combination of chemical and electrochemical reactions in the cell and evolves over time with charge/discharge cycling. The formation and stability of SEI directly determine the fundamental properties of the battery such as first coulombic efficiency (FCE), energy/power density, storage life, cycle life, and safety. The dynamic nature of SEI along with the presence of spatially inhomogeneous organic and inorganic components in SEI encompassing crystalline, amorphous, and polymeric nature distributed across the electrolyte to the electrolyte-electrode interface, highlights the need for advanced in situ/operando techniques to understand the formation and structure of these materials in creating a stable interface in real-world operating conditions.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China.
Microkinetic modeling of heterogeneous catalysis serves as an efficient tool bridging atom-scale first-principles calculations and macroscale industrial reactor simulations. Fundamental understanding of the microkinetic mechanism relies on a combination of experimental and theoretical studies. This Perspective presents an overview of the latest progress of experimental and microkinetic modeling approaches applied to gas-solid catalytic kinetics.
View Article and Find Full Text PDFAdv Sci (Weinh)
December 2024
Institute of Materials Science, Technische Universität Darmstadt, Peter-Grünberg-Str. 2, D-64287, Darmstadt, Germany.
The design of cathode/electrolyte interfaces in high-energy density Li-ion batteries is critical to protect the surface against undesirable oxygen release from the cathodes when batteries are charged to high voltage. However, the involvement of the engineered interface in the cationic and anionic redox reactions associated with (de-)lithiation is often ignored, mostly due to the difficulty to separate these processes from chemical/catalytic reactions at the cathode/electrolyte interface. Here, a new electron energy band diagrams concept is developed that includes the examination of the electrochemical- and ionization- potentials evolution upon batteries cycling.
View Article and Find Full Text PDFChemSusChem
December 2024
PSI Center for Energy and Environmental Sciences, Paul Scherrer Institute, 5232, Villigen, Switzerland.
Solving the surface (electro-)chemical instability and the fading behavior of high voltage cathode materials cycled above 4.3 V vs Li/Li remains a major challenge for the next generation of high energy density Li-ion batteries. Here, we present a facile, environmentally friendly, cost effective and scalable method to address this problem by uniformly fluorinating the surface of cathode materials with a mild fluorinating agent (CHF) using a gas flow-type reactor.
View Article and Find Full Text PDFNat Commun
December 2024
Department of Inorganic Chemistry, Fritz-Haber Institute of the Max Planck Society, Berlin, Germany.
Future carbon management strategies require storage in elemental form, achievable through a sequence of CO hydrogenation reactions. Hydrogen is recycled from molecular intermediates by dehydrogenation, and side product acetylene selectively hydrogenated to ethylene. Existing Pd alloy catalysts for gas purification underperform in concentrated feeds, necessitating novel concepts.
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