Interpretable Machine Learning Models for Practical Antimonate Electrocatalyst Performance
Chemphyschem. 2024 Mar 28:e202400010. doi: 10.1002/cphc.202400010. Online ahead of print.ABSTRACTComputationally predicting the performance of catalysts under reaction conditions is a challenging task due to the complexity of catalytic surfaces and their evolution in situ, different reaction paths, and the presence of solid-liquid interfaces in the case of electrochemistry. We demonstrate here how relatively simple machine learning models can be found that enable prediction of experimentally observed onset potentials. Inputs to our model are comprised of data from the oxygen reduction reaction on non-precious transition-me...
Source: Chemphyschem - March 28, 2024 Category: Chemistry Authors: Shyam Deo Melissa Kreider Gaurav Kamat McKenzie Hubert Jos é Zamora Zeledón Lingze Wei Jesse Matthews Nathaniel Keyes Ishaan Singh Thomas Jaramillo Frank Abild-Pedersen Michaela Burke Stevens Kirsten Winther Johannes Voss Source Type: research
A Density Functional Theory Analysis of Electrochemical Oxidation of Methane to Alcohol over High-entropy Oxide (CoCrFeMnNi)3O4 Catalysts
In this study, we utilize density functional theory to explore the potential of the (CoCrFeMnNi)3O4 (CCFMN) high entropy oxide (HEO) for electrochemical oxidation of methane to methanol and ethanol, alongside their competition with CO2 production. Our primary focus in this study is on thermodynamics, enabling a prompt analysis of the catalyst's potential, with the calculation of electrochemical barriers falling beyond our scope. Among all potential active sites within the CCFMN HEO, we identify Co as the most active site for methane activation when using carbonate ions as oxidants. This results in methanol production with ...
Source: Chemphyschem - March 28, 2024 Category: Chemistry Authors: M R Ashwin Kishore Sungwoo Lee Jong Suk Yoo Source Type: research
Evolution of Excited-State Behaviors of Gold Complexes, Nanoclusters and Nanoparticles
Chemphyschem. 2024 Mar 28:e202300687. doi: 10.1002/cphc.202300687. Online ahead of print.ABSTRACTMetal nanomaterials have been extensively investigated owing to their unique properties in contrast to bulk counterparts. Gold nanoparticles (e.g., 3-100 nm) show quasi-continuous energy bands, while gold nanoclusters (<3 nm) and complexes exhibit discrete energy levels and display entirely different photophysical properties than regular nanoparticles. This review summarizes the electronic dynamics of these three types of gold materials studied by ultrafast spectroscopy. Briefly, for gold nanoparticles, their electronic rela...
Source: Chemphyschem - March 28, 2024 Category: Chemistry Authors: Linlin Zeng Meng Zhou Rongchao Jin Source Type: research
Interpretable Machine Learning Models for Practical Antimonate Electrocatalyst Performance
Chemphyschem. 2024 Mar 28:e202400010. doi: 10.1002/cphc.202400010. Online ahead of print.ABSTRACTComputationally predicting the performance of catalysts under reaction conditions is a challenging task due to the complexity of catalytic surfaces and their evolution in situ, different reaction paths, and the presence of solid-liquid interfaces in the case of electrochemistry. We demonstrate here how relatively simple machine learning models can be found that enable prediction of experimentally observed onset potentials. Inputs to our model are comprised of data from the oxygen reduction reaction on non-precious transition-me...
Source: Chemphyschem - March 28, 2024 Category: Chemistry Authors: Shyam Deo Melissa Kreider Gaurav Kamat McKenzie Hubert Jos é Zamora Zeledón Lingze Wei Jesse Matthews Nathaniel Keyes Ishaan Singh Thomas Jaramillo Frank Abild-Pedersen Michaela Burke Stevens Kirsten Winther Johannes Voss Source Type: research
Possibilities and Limitations of Kinetic Studies in pls. insert line break here On-Surface Synthesis by pls. insert 2nd linebreak here Real Time X-ray Photoelectron Spectroscopy
Chemphyschem. 2024 Mar 25:e202400156. doi: 10.1002/cphc.202400156. Online ahead of print.ABSTRACTThe kinetics of coupling reactions on surfaces can be quantitatively studied in real time by X-ray Photoelectron Spectroscopy (XPS). From fitting experimental data, kinetic reaction parameters such as the rate constant's pre-exponential and activation energy can be deduced and compared to quantum chemical simulations. To elucidate the possibilities and limitations of this approach, we propose studies in which experimental data are first simulated and subsequently fitted. Knowing the exact kinetic parameters used in the simulati...
Source: Chemphyschem - March 26, 2024 Category: Chemistry Authors: Markus Lackinger Source Type: research
Pressure Induces Six-fold Coordination for the Lighter Pnictides Phosphorus and Arsenic Triiodide
In this study, we employ an evolutionary algorithm in conjunction with first-principles density functional theory (DFT) calculations to comprehensively investigate the structural transitions, electronic properties, and chemical bonding behaviors of XI3 compounds, where X denotes phosphorus (P) and arsenic (As), across a range of elevated pressures. Our computational analyses reveal a distinctive phenomenon occurring under compression, wherein the initially trigonal structures of PI3 (P 63) and AsI3 (R-3) undergo an intriguing transformation, leading to the emergence of six-coordinated monoclinic phases (C2/m) at 6 GPa and ...
Source: Chemphyschem - March 26, 2024 Category: Chemistry Authors: Pranab Gain Soumya Mondal Ayan Datta Source Type: research
Coarsening of quasi two-dimensional emulsions formed by islands in free-standing smectic films
Chemphyschem. 2024 Mar 26:e202400166. doi: 10.1002/cphc.202400166. Online ahead of print.ABSTRACTWe study the coarsening behavior of assemblies of islands on smectic A freely suspended films in ISS microgravity experiments. The islands can be regarded as liquid inclusions in a two-dimensional fluid in analogy to liquid droplets of the discontinuous phase of an emulsion. The coarsening is effectuated by two processes, predominantly by island coalescence, but to some extend also by Ostwald ripening, whereby large islands grow at the expense of surrounding smaller ones. A peculiarity of this system is that the continuous and ...
Source: Chemphyschem - March 26, 2024 Category: Chemistry Authors: Christoph Klopp Torsten Trittel Ralf Stannarius Source Type: research
New Perspectives on Delocalization Pathways in Aromatic Molecular Chameleons
This study comprehensively analyzes the magnetically induced current density of polycyclic compounds labeled as "aromatic chameleons" since they can arrange their π-electrons to exhibit aromaticity in both the ground and the lowest triplet state. These compounds comprise benzenoid moieties fused to a central skeleton with 4n π-electrons and traditional magnetic descriptors are biased due to the superposition of local magnetic responses. In the S0 state, our analysis reveals that the molecular constituent fragments preserve their (anti)aromatic features in agreement with two types of resonant structures: one associated wi...
Source: Chemphyschem - March 26, 2024 Category: Chemistry Authors: Luis Leyva-Parra Irene Casademont-Reig Ricardo Pino-Rios Lina Ruiz Mercedes Alonso William Tiznado Source Type: research
Possibilities and Limitations of Kinetic Studies in pls. insert line break here On-Surface Synthesis by pls. insert 2nd linebreak here Real Time X-ray Photoelectron Spectroscopy
Chemphyschem. 2024 Mar 25:e202400156. doi: 10.1002/cphc.202400156. Online ahead of print.ABSTRACTThe kinetics of coupling reactions on surfaces can be quantitatively studied in real time by X-ray Photoelectron Spectroscopy (XPS). From fitting experimental data, kinetic reaction parameters such as the rate constant's pre-exponential and activation energy can be deduced and compared to quantum chemical simulations. To elucidate the possibilities and limitations of this approach, we propose studies in which experimental data are first simulated and subsequently fitted. Knowing the exact kinetic parameters used in the simulati...
Source: Chemphyschem - March 26, 2024 Category: Chemistry Authors: Markus Lackinger Source Type: research
Pressure Induces Six-fold Coordination for the Lighter Pnictides Phosphorus and Arsenic Triiodide
In this study, we employ an evolutionary algorithm in conjunction with first-principles density functional theory (DFT) calculations to comprehensively investigate the structural transitions, electronic properties, and chemical bonding behaviors of XI3 compounds, where X denotes phosphorus (P) and arsenic (As), across a range of elevated pressures. Our computational analyses reveal a distinctive phenomenon occurring under compression, wherein the initially trigonal structures of PI3 (P 63) and AsI3 (R-3) undergo an intriguing transformation, leading to the emergence of six-coordinated monoclinic phases (C2/m) at 6 GPa and ...
Source: Chemphyschem - March 26, 2024 Category: Chemistry Authors: Pranab Gain Soumya Mondal Ayan Datta Source Type: research
Coarsening of quasi two-dimensional emulsions formed by islands in free-standing smectic films
Chemphyschem. 2024 Mar 26:e202400166. doi: 10.1002/cphc.202400166. Online ahead of print.ABSTRACTWe study the coarsening behavior of assemblies of islands on smectic A freely suspended films in ISS microgravity experiments. The islands can be regarded as liquid inclusions in a two-dimensional fluid in analogy to liquid droplets of the discontinuous phase of an emulsion. The coarsening is effectuated by two processes, predominantly by island coalescence, but to some extend also by Ostwald ripening, whereby large islands grow at the expense of surrounding smaller ones. A peculiarity of this system is that the continuous and ...
Source: Chemphyschem - March 26, 2024 Category: Chemistry Authors: Christoph Klopp Torsten Trittel Ralf Stannarius Source Type: research
New Perspectives on Delocalization Pathways in Aromatic Molecular Chameleons
This study comprehensively analyzes the magnetically induced current density of polycyclic compounds labeled as "aromatic chameleons" since they can arrange their π-electrons to exhibit aromaticity in both the ground and the lowest triplet state. These compounds comprise benzenoid moieties fused to a central skeleton with 4n π-electrons and traditional magnetic descriptors are biased due to the superposition of local magnetic responses. In the S0 state, our analysis reveals that the molecular constituent fragments preserve their (anti)aromatic features in agreement with two types of resonant structures: one associated wi...
Source: Chemphyschem - March 26, 2024 Category: Chemistry Authors: Luis Leyva-Parra Irene Casademont-Reig Ricardo Pino-Rios Lina Ruiz Mercedes Alonso William Tiznado Source Type: research
Doping effects on ethane/ethylene dehydrogenation catalyzed by Pt2X nanoclusters
Chemphyschem. 2024 Mar 25:e202400095. doi: 10.1002/cphc.202400095. Online ahead of print.ABSTRACTThe catalytic dehydrogenation of light alkanes is key to transform low-cost hydrocarbons to high value-added chemicals. Although Pt is extremely efficient at catalyzing this reaction, it suffers from coke formation that deactivates the catalyst. Dopants such as Sn are widely used to increase the stability and lifetime of Pt. In this work, the dehydrogenation reaction of ethane catalyzed by Pt3 and Pt2X (X = Si, Ge, Sn, P and Al) nanocatalysts has been studied computationaly by means of density functional calculations. Our resul...
Source: Chemphyschem - March 25, 2024 Category: Chemistry Authors: Andoni Ugartemendia Jos é M Mercero Elisa Jimenez-Izal Abel de Cozar Source Type: research
XPS Analysis of FexNiyPS3 vdW Materials Used in the Hydrogen Evolution Processes
Chemphyschem. 2024 Mar 25:e202400039. doi: 10.1002/cphc.202400039. Online ahead of print.ABSTRACTIn response to the global demand for sustainable energy solutions, the quest for stable and cost-effective hydrogen production has garnered significant attention in recent decades. Here, the emergence of layered metal phosphorus trichalcogenides (MPX3, M: transition metal, X: chalcogen) materials with customizable composition and electronic structure holds great promise for such purposes. In the present study, we successfully synthesized large-scale and high-quality Fex$NyPS3. Subsequent systematic investigations were conducted...
Source: Chemphyschem - March 25, 2024 Category: Chemistry Authors: Yefei Guo Guopu Cai Junhao Zhou Jiali Yang Elena Voloshina Yuriy Dedkov Source Type: research
Global Potential Energy Surfaces by Compressed-State Multistate Pair-Density Functional Theory for Hyperthermal Collisions in the O2 + O2 System
Chemphyschem. 2024 Mar 25:e202400078. doi: 10.1002/cphc.202400078. Online ahead of print.ABSTRACTInteractions between oxygen molecules play an important role in atmospheric chemistry and hypersonic flow chemistry in atmospheric entries. Recently, high-quality ab initio potential energy surface (PES) of the quintet O4 was reported by Paukku et al. [J. Chem. Phys. 147, 034301 (2017)]. 10543 configurations were sampled and calculated at the level of MS-CASPT2/maug-cc-pVTZ with scaled external correlation. The PES was fitted to a many-body (MB) form with the many-body part described by the permutationally invariant polynomial ...
Source: Chemphyschem - March 25, 2024 Category: Chemistry Authors: Jie Jiang Jiawei Yang Qizhen Hong Quanhua Sun Jun Li Source Type: research
