Article
Chemistry, Physical
Yongjie Xi, Tingting Wang, Jia Wang, Jinlei Li, Fuwei Li
Summary: This study comprehensively investigates the mechanism of CO2 hydrogenation to ethanol, revealing the crucial role of CO surface coverage in affecting the reaction energy profiles. CO adsorption facilitates the CH-CO coupling and CH hydrogenation, increasing the selectivity towards ethanol.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Jibao Wu
Summary: The coverage-dependent adsorption and stability of functionalized Ge(1 0 0) and (1 1 1) surfaces terminated with different chemical groups were systematically investigated using density functional theory calculations. The results show that Ge-X chemical bond slightly decreases with the increase of surface coverage, and Ge(1 1 1) surface exhibits stronger adsorption stability compared to Ge(1 0 0) surface.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Rene Ebeling, Narendra P. Arasu, Lisa Bensch, Bertram Schulze Lammers, Bernhard Mayer, Thomas J. J. Mueller, Hector Vazquez, Silvia Karthaeuser
Summary: Studies have shown that inserting a flexible bridge can break the conjugation between donor-acceptor molecules on a metal substrate, preserving their reduced donor-acceptor character. This research investigates the adsorption behavior and electronic properties of a donor-bridge-acceptor dyad on a Pt(111) surface.
NANOSCALE ADVANCES
(2021)
Article
Materials Science, Multidisciplinary
Wanxin Lv, Yuzhou Hao, Aojie Li, Xiaoliang Zhong
Summary: The study focuses on the Young's moduli of ultrathin oxygen-adsorbed 2D Pt slabs with a (111) surface using density functional theory methods. It shows that the Young's moduli typically decrease as surface oxygen coverage increases, and thinner slabs generally exhibit higher stiffness. The nonlinear elastic properties of both the core and surface regions of the considered 2D structures contribute to the overall effective elastic properties.
Article
Chemistry, Physical
David Raciti, Thomas P. Moffat
Summary: Electrochemical mass spectrometry (EC-MS) combined with chronoamperometry was used to quantify the coverage of surface hydride phase on Cu(111) in 0.1 mol/L H2SO4. The study tracked the 2 atomic mass unit (amu) signal for H2 production and charge passed to examine anion desorption, hydride formation, and the hydrogen evolution reaction (HER).
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Dmitriy Borodin, Oihana Galparsoro, Igor Rahinov, Jan Fingerhut, Michael Schwarzer, Stefan Horandl, Daniel J. Auerbach, Alexander Kandratsenka, Dirk Schwarzer, Theofanis N. Kitsopoulos, Alec M. Wodtke
Summary: This study presents a detailed kinetics analysis of NH3 thermal desorption rates from p(2 x 2) O/Pt(111). It is found that the adsorption of O-atoms on Pt(111) greatly reduces the desorption rate of NH3. A physical model is proposed to explain the interactions between adsorbed NH3 and O-atoms, and the model is fitted to derive the desorption rate constants. The results indicate a higher stabilization and rotational barrier for NH3 on p(2 x 2) O/Pt(111) compared to Pt(111). The study also highlights the importance of dispersion interactions for accurately predicting the NH3-O adsorbate-adsorbate interactions and NH3 binding energies.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Lukas Hormann, Andreas Jeindl, Oliver T. Hofmann
Summary: Virtually all organic (opto)electronic devices rely on organic/inorganic interfaces with specific properties. A study found that a change in interface structure can introduce a shift in function. Researchers achieved this by using tetrachloropyrazine on Pt(111), which created switchable interface structures with significantly different adsorption geometries. These structures facilitated different work function changes and coherent fractions, making them ideal for reading out the interface state. The possibility of reversible switching between different classes of structures was demonstrated, creating a dynamic interface for potential applications in organic electronics.
Article
Chemistry, Physical
Griffin Ruehl, S. Elizabeth Harman, Liney Arnadottir, Charles T. Campbell
Summary: The study measured the heat of adsorption of acetonitrile on Pt(111) surface as a function of coverage, revealing a difference in adsorption heats at different temperatures and their impact on saturation coverage. The estimated adhesion energy for liquid acetonitrile on Pt(111) was found to be lower than water, benzene, and phenol, but higher than methanol and formic acid. This information can be useful in estimating the effect of acetonitrile as a solvent on the adsorption energies of catalytic reactants compared to gas phase.
Article
Chemistry, Physical
August E. G. Mikkelsen, Henrik H. Kristoffersen, Jakob Schiotz, Tejs Vegge, Heine A. Hansen, Karsten W. Jacobsen
Summary: In this study, molecular dynamics simulations with an ensemble of neural network potentials were used to investigate the structure and energetics of liquid water and hydroxyl species on Pt(111) surfaces. The results revealed a gradual increase in differential adsorption energy at high hydroxyl coverages, which was explained by the reduction in hydrogen bonds between the water molecules and hydroxyls.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Alexandra C. Davila Lopez, Thorben Eggert, Karsten Reuter, Nicolas G. Hoermann
Summary: This work systematically studies the relationship between static and dynamic water models at the water-Pt(111) interface, revealing that static structures tend to overemphasize the in-plane hydrogen bonding network and may introduce systematic biases. The analysis suggests that averaging over consistently created structural ensembles could reduce these biases.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Nanoscience & Nanotechnology
Milena Zorko, Pedro Farinazzo Bergamo Dias Martins, Justin G. Connell, Pietro Papa Lopes, Nenad M. Markovic, Vojislav R. Stamenkovic, Dusan Strmcnik
Summary: The development of efficient, stable, and selective oxygen reduction reaction (ORR) electrocatalysts is crucial for the commercialization of alkaline, phosphoric acid, and polymer electrolyte membrane fuel cells. By adsorbing melamine onto the Pt(111) surface, researchers were able to significantly increase the ORR activity while selectively inhibiting the adsorption of toxic substances, leading to enhanced chemical stability.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Keita Okuda, Musa Alaydrus, Nagahiro Hoshi, Ikutaro Hamada, Masashi Nakamura
Summary: This study investigated the structures of H2O, OHad, and Li using infrared spectroscopy and density functional theory calculations. By optimizing the coverage of OHad and Li, a quasi-Electrical Double Layer (EDL) model composed of OHad species interacting with hydrated Li+ on Pt(111) was successfully modeled under ultrahigh vacuum conditions. Modeling the EDL, including the outer Helmholtz plane, is beneficial for identifying the microscopic details of the EDL under electrochemical conditions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Maatje J. E. de Willigen, Mitsunori Kurahashi, Ludo B. F. Juurlink
Summary: The interaction between oxygen and platinum surfaces is a valuable model for understanding reaction mechanisms. In this study, we investigated the influence of surface structure on the dynamics of this interaction and found that the sticking probability of oxygen molecules varies significantly depending on their orientation. Vicinal surfaces exhibited higher reactivity than Pt(111) and showed a more complex angular dependence with little alignment dependence. Our findings suggest that at low incident energies, the highest sticking probabilities occur when the molecules are incident perpendicular to step facets, indicating a weak alignment dependence and a predominance of scattering into a physisorbed state preceding chemisorbed states.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Egidius W. F. Smeets, Geert-Jan Kroes
Summary: Accurately modeling heterogeneous catalysis requires precise descriptions of rate-controlling elementary reactions on metal surfaces, which can be achieved through a specific reaction parameter approach to density functional theory. Combining meta-generalized gradient approximation density functionals with nonlocal correlation leads to improved accuracy in describing gas-surface systems, although at the expense of slightly less accurate metal descriptions compared to standard DFs. The results indicate that the combination of MS mGGA DFs with nonlocal correlation provides a better description of gas-surface reactions involving late transition metals.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Jie Wei, Zheng-da He, Wei Chen, Yan-Xia Chen, Elizabeth Santos, Wolfgang Schmickler
Summary: The activity of Pt(111) electrodes for the hydrogen evolution reaction in 0.5M H2SO4 solution increases with continuous potential cycling. Changes in cyclic voltammograms after the hydrogen evolution reaction show a decrease in current waves for hydrogen and sulfate adsorption, possibly due to absorption of a small amount of hydrogen in the subsurface layer.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Engineering, Environmental
Justin Easa, Chang Yan, William F. Schneider, Casey P. O'Brien
Summary: This study compares the inhibiting effects of CO and C3H6 on H-2 permeation across Pd77Ag23 and Pd membranes, showing that alloying Pd with Ag can enhance its sensitivity to poisoning. CO primarily inhibits H-2 permeation by adsorbing on available sites, while C3H6 affects electronic structure to hinder H-2 dissociation on both Pd and Pd77Ag23 surfaces.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Anshuman Goswami, Hanyu Ma, William F. Schneider
Summary: This article investigates the influence of lateral adsorbate interactions on reaction rates, rate orders, apparent activation energies, and Sabatier plots using lattice-based kinetic Monte Carlo simulations. The results demonstrate that lateral interactions can decrease adsorbate coverage and have complex effects on absolute rates, Sabatier plots, and reaction kinetics.
JOURNAL OF CATALYSIS
(2022)
Correction
Physics, Applied
Hanyu Ma, William F. Schneider
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2022)
Article
Multidisciplinary Sciences
Hanyu Ma, Rakesh K. Sharma, Stefan Welzel, Mauritius C. M. van de Sanden, Mihalis N. Tsampas, William F. Schneider
Summary: This study investigates the synergy between heterogeneous catalysts and non-thermal plasma. Through experimental evidence and reactor model construction, it is revealed that neither catalyst nor plasma alone is productive, but their combination can generate nitrogen oxides. The study provides clear evidence for the synergy between heterogeneous catalysts and non-thermal plasma, and highlights the importance of their combined use.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Jie Zhang, Chen Cai, George Kim, Yusu Wang, Wei Chen
Summary: In this study, a large HEA dataset was generated using the EMTO-CPA method, and a ML model with the Deep Sets architecture was trained to achieve better predictive performance and generalizability. Association rule mining was also applied to describe the compositional dependence of HEA elastic properties and demonstrate the potential for data-driven alloy design.
NPJ COMPUTATIONAL MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
Xianli Wang, Forough Jahanbazi, Jialiang Wei, Carlo U. Segre, Wei Chen, Yuanbing Mao
Summary: In this study, the unexpected near-infrared emission of trivalent bismuth doped pyrochlore material was observed, and a dual-mode luminescence thermometry was demonstrated. The thermometry is based on the lifetime and luminescence intensity ratio of the near-infrared emission, providing high temperature sensitivity over a wide range.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Engineering, Chemical
Jeonghyun Ko, Hanyu Ma, William F. Schneider
Summary: In this study, complete ethane dehydrogenation (EDH) reaction networks over Ni and Ni2P surfaces were investigated using DFT calculations. The results showed that the intermediates were more weakly bound to Ni2P and had higher activation energies compared to Ni. Microkinetic modeling revealed that ethylene formation rates and selectivities were higher over Ni2P across a wide temperature range, while Ni was more susceptible to coke generation.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Chemistry, Multidisciplinary
Songhyun Lee, Claire T. Nimlos, Elijah R. Kipp, Yujia Wang, Xuyao Gao, William F. Schneider, Marcella Lusardi, Vivek Vattipalli, Subramanian Prasad, Ahmad Moini, Rajamani Gounder
Summary: The arrangement and structure of Al heteroatoms in zeolite frameworks play a crucial role in catalytic reactions and redox processes. In this study, the evolution of Al framework structure in chabazite zeolites under hydrothermal treatment was investigated. The presence of organic and inorganic structure directing agents (SDAs) was found to influence the formation of Al sites in the zeolite framework. The results showed that the presence of N,N,N-trimethyl-1-adamantylam-monium (TMAda(+)) resulted in the formation of isolated Al sites, while the coexistence of Na+ and TMAda(+) led to the formation of paired Al sites. Ab initio molecular dynamics (AIMD) simulations confirmed the thermodynamic driving force for the formation of different Al arrangements in the presence of different SDAs.
CRYSTAL GROWTH & DESIGN
(2022)
Article
Chemistry, Applied
Jerry T. Crum, Justin R. Crum, Cameron Taylor, William F. Schneider
Summary: This paper analyzes the rings and T-sites in a large number of zeolite frameworks using Zeolite Simulation Environment. It compares different ring definitions and proposes an alternative definition for T-sites. Previously unrecognized rings are discovered and this tool serves as an effective platform for characterizing zeolite and T-site structures for modeling and machine learning.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Multidisciplinary Sciences
Gaoxin Lin, Zhuang Zhang, Qiangjian Ju, Tong Wu, Carlo U. U. Segre, Wei Chen, Hongru Peng, Hui Zhang, Qiunan Liu, Zhi Liu, Yifan Zhang, Shuyi Kong, Yuanlv Mao, Wei Zhao, Kazu Suenaga, Fuqiang Huang, Jiacheng Wang
Summary: In this study, we demonstrate a bottom-up evolution route to prepare ultrafine Rh nanoparticles with large lattice spacings and grain boundaries by electrochemically reducing Cs3Rh2I9 halide-perovskite clusters on N-doped carbon. These Rh nanoparticles derived from Cs3Rh2I9 clusters exhibit significantly enhanced mass and area activity toward hydrogen evolution reaction in both alkaline and chloralkali electrolyte, surpassing liquid-reduced Rh nanoparticles and bulk Cs3Rh2I9-derived Rh via top-down electro-reduction transformation. Theoretical calculations reveal that water activation could be promoted on Cs3Rh2I9 clusters-derived Rh nanoparticles enriched with multiply sites, thereby facilitating alkaline hydrogen evolution.
NATURE COMMUNICATIONS
(2023)
Article
Materials Science, Multidisciplinary
Yanfang Liu, Jie Ren, Shuai Guan, Chenyang Li, Yin Zhang, Saideep Muskeri, Zhiyuan Liu, Dunji Yu, Yan Chen, Ke An, Yang Cao, Wei Liu, Yuntian Zhu, Wei Chen, Sundeep Mukherjee, Ting Zhu, Wen Chen
Summary: CoCrFeMnNi high-entropy alloys (HEAs) are additively manufactured using L-DED and L-PBF processes. Comparative studies reveal substantial differences in microstructures, crystallographic texture, and deformation mechanisms between L-DED and L-PBF samples. The L-DED samples exhibit a mixed crystallographic texture, larger solidification cell sizes, and enhanced plastic deformation capabilities, leading to higher ductility compared to the L-PBF samples. This work provides fundamental insights into the deformation mechanisms of additively manufactured HEAs and emphasizes the critical impact of processing conditions on solidification microstructure and material design by additive manufacturing.
Article
Chemistry, Physical
Siddarth H. Krishna, Anshuman Goswami, Yujia Wang, Casey B. Jones, David P. Dean, Jeffrey T. Miller, William F. Schneider, Rajamani Gounder
Summary: In this study, Cu-CHA zeolites with different aluminum densities (0.2-1.7 Al/CHA) were investigated using statistical simulations, steady-state kinetics, and operando X-ray absorption spectroscopy. The results show that increasing the aluminum density leads to an increase in the fraction of Cu-I ions that are SCR active and the Cu-I oxidation rate constants, providing insights into how anionic Al centers in zeolite frameworks regulate the mobility of ionically tethered Cu cations and their dynamic reactivity during low-temperature NOx SCR.
Article
Materials Science, Multidisciplinary
Jie Ren, Margaret Wu, Chenyang Li, Shuai Guan, Jiaqi Dong, Jean-Baptiste Forien, Tianyi Li, Katherine S. Shanks, Dunji Yu, Yan Chen, Ke An, Kelvin Y. Xie, Wei Chen, Thomas Voisin, Wen Chen
Summary: We develop a dual-phase nanolamellar structure in a high-entropy alloy using laser powder-bed fusion additive manufacturing. This structure exhibits a combination of ultrahigh yield strength and large tensile ductility. The deformation mechanisms involve effective blockage of dislocation motion, stacking fault-mediated deformation, and martensitic transformation. The cooperative deformation of the dual phases, assisted by the semi-coherent lamellar interfaces, gives rise to the large ductility.
Article
Materials Science, Multidisciplinary
Wei Chen, Lin Li, Qiang Zhu, Houlong Zhuang
Summary: Complex concentrated alloys (CCAs) have attracted significant attention for their wide range of applications and novel properties. Chemical short-range ordering (CSRO) in CCAs plays a crucial role in understanding their properties and phase stability. This article reviews recent experimental efforts in identifying and characterizing CSRO in CCAs, and discusses theoretical and computational techniques, such as density functional theory (DFT) and molecular dynamics (MD), used to investigate CSRO effects.
Article
Chemistry, Physical
Jeonghyun Ko, William F. Schneider
Summary: By computational study of metal phosphides in catalytic reactions, it was found that binding energies at metal sites correlate with bulk metals, with phosphide sites competing for adsorbates and favorably affecting dehydrogenation.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)