Review
Chemistry, Multidisciplinary
Eugene P. Meshcheryakov, Sergey Reshetnikov, Mariya P. Sandu, Alexey S. Knyazev, Irina A. Kurzina
Summary: The review discusses the main methods of obtaining hydroxides and aluminium oxides from gibbsite, as well as techniques for improving the adsorbent properties of aluminium oxide adsorbents. The study shows that modification can significantly enhance the adsorption activity of the adsorbents.
APPLIED SCIENCES-BASEL
(2021)
Article
Chemistry, Physical
Ningjing Luo, Zhufeng Hou, Guo-Liang Chai
Summary: This study systematically explores the catalytic activity of tungsten monocarbide (WC) by studying the methane dehydrogenation and C-C coupling processes on WC surfaces using density functional theory (DFT) calculations. The results indicate that the W-terminated WC(0001) surface is the most favorable exposed surface with a lower surface energy. Additionally, the Co(111), Ni(111), and W-terminated WC(0001) surfaces exhibit similar catalytic properties in methane dehydrogenation, and the rate-limiting step on the W-terminated WC(0001) surface is the dissociation of CH*. C-C coupling through CH* intermediates on the W-terminated WC(0001) surface favors the formation of C2H2 kinetically.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Applied
Ming-Tsz Chen, Yu-Yang Chen, Ting-Hsun Huang, Hui-Chu Pi, Ching-Han Hu, Chi-Tien Chen
Summary: This study describes a new mutual transformation mode between two aluminum complexes with different ligands, supported by density functional theory (DFT) studies. Their catalytic activities were investigated in the ring opening polymerization of ε-caprolactone and l-lactide, showing potential applications in these processes.
APPLIED ORGANOMETALLIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Felipe Toledo, Eduardo Schott, Mario Saavedra-Torres, Eduardo Delgado, Gina Pecchi, Ximena Zarate
Summary: This research investigated the adsorption of biomass derivatives styrene and styrene oxide on perovskite-like structures KTaO3(001) and LiTaO3(0001) from a theoretical perspective. Density functional theory (DFT) calculations were performed to study the adsorption phenomenon. The results provide insights into the structural features, surface reactivity, and adsorption sites of LiTaO3 and KTaO3 perovskites, which are important in heterogeneous catalytic processes such as styrene oxidation.
Article
Chemistry, Physical
Xia Wang, Wei Gui, Fangli Duan, Xiaojing Mu
Summary: The study shows that adsorbed functional groups can enhance the interaction strength between graphene oxide and iron oxide substrate, with the magnitude of binding energy enhancement depending on the adsorption sites of functional groups. Models with adjacent C atom to the top oxygen atom on the oxide surface exhibit significantly enhanced binding energy, while other models show slightly increased binding energy.
Article
Engineering, Chemical
Yanjing He, Yandong Guo, Fang Yan, Tianhao Yu, Lei Liu, Xiaochun Zhang, Tao Zheng
Summary: In this study, the interaction between ionic liquids (ILs) and graphene oxide (GO) was investigated using density functional theory. It was found that the adsorption of ILs on GO reduced the HOMO-LUMO energy gap, weakened hydrogen bonding interactions, and charge transfer played a key role in the adsorption process. Additionally, the forces at play depended on whether the ILs were on the hydroxyl side of GO or not, with van der Waals interactions being prominent.
CHEMICAL ENGINEERING SCIENCE
(2021)
Article
Engineering, Environmental
Asmita S. Jadhav, Prajakta Ramteke, Sunit K. Singh, Nitin K. Labhasetwar
Summary: The study demonstrated that the Al-Fe mixed oxide has efficient adsorption capabilities for selenium contamination in water, effectively removing selenium ions at different pH ranges without significant decrease in adsorption efficiency. Additionally, the adsorbent can be regenerated with mild alkali and reused multiple times without a notable reduction in adsorption efficiency.
JOURNAL OF WATER PROCESS ENGINEERING
(2022)
Article
Environmental Sciences
S. Muthusaravanan, K. Balasubramani, Rahul Suresh, R. Sankar Ganesh, N. Sivarajasekar, H. Arul, K. Rambabu, G. Bharath, V. E. Sathishkumar, A. P. Murthy, Fawzi Banat
Summary: Graphene oxide nanosheets were successfully prepared and studied as an adsorbent for atrazine removal from simulated wastewater. The adsorption of atrazine onto GO was found to be higher in acidic pH and lower temperature, and Langmuir isotherm was a suitable model for the adsorption process.
ENVIRONMENTAL RESEARCH
(2021)
Article
Chemistry, Physical
Michael Fischer
Summary: This study used electronic structure calculations to investigate the adsorption of carbamazepine (CBZ) in eleven all-silica zeolites. It was found that zeolites with one-dimensional channels formed by twelve-membered rings exhibited the highest affinity towards CBZ. The fit of CBZ into the zeolite pores, maximizing dispersion interactions, was identified as the dominant factor determining the interaction strength. The calculations also contributed to the understanding of the atomic-level interaction between functional organic molecules and all-silica zeolites.
Article
Chemistry, Physical
Hui Zhang, Qi-Chao Liu, Chun-Qi Zhou, Zi-Hao Yue, Zhen-Kun Tang
Summary: Novel 2D functionalized hexagonal boron phosphides breaking mirror symmetry are demonstrated as potential high efficiency water splitting photocatalysts. These catalysts exhibit moderate band gap, spatial separation of photoexcited carriers, and strong light absorption.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Bowen Zhu, Kexuan Wang, Haili Gao, Qinhua Wang, Xiaofeng Pan, Mizi Fan
Summary: The interaction between organic molecules and MXene surface depends on the type of functional groups, while the strength of the interaction is determined by the type of surface functional groups and the number of hydrogen bonds. MXene saturated with -OH or -F groups can form strong chemical and hydrogen bonds with organic molecules, leading to strong adsorption energy and charge transfer, while MXene saturated with -F or -O groups mainly exhibits physical interactions, with low adsorption energy and minimal charge transfer.
Article
Chemistry, Physical
K. N. D. Bandara, K. M. D. C. Jayathilaka, J. K. D. S. Jayanetti, D. P. Dissanayake
Summary: It has been found that Cu2O (100) is a better sensing surface for hydrocarbons compared to Cu2O (111). Density functional theory calculations were used to obtain adsorption energies and activation energies for C-H bond dissociation on oxygen terminated cuprous oxide surfaces. Results showed that Cu2O (111) has a higher affinity towards H2O and CO2. Additionally, it was observed that the activation energy for H3C-H bond dissociation on Cu2O (100) is significantly lower than that on Cu2O (111), making it a better sensing surface for hydrocarbons.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Orest Pizio, Stefan Sokolowski
Summary: The wetting phase diagrams for model systems consisting of water and chemically modified graphite surfaces with grafted chain molecules were explored using the density functional approach. The topology of the phase diagram was found to depend on the amount and length of grafted chains.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Physical
Akanksha Ashok Sangolkar, Rubi Agrawal, Ravinder Pawar
Summary: This study investigates the dissociative adsorption of H2S on the Li(110) surface using density functional theory calculations. The results show that the dissociation of H2S on Li surface occurs stepwise, with completely dissociated moieties H/H/S being the most stable form. Orbital and electrostatic contributions play a vital role in stabilizing the dissociated moieties during the process.
Article
Chemistry, Multidisciplinary
Jakob Heller, Tobias F. Pascher, Christian van der Linde, Milan Oncak, Martin K. Beyer
Summary: Hydrated aluminium cations were investigated as a photochemical model system with up to ten water molecules using UV action spectroscopy. The intense photodissociation starts at 4.5 eV for two to eight water molecules, and quantum chemical calculations show that solvation shifts the excitations into the photon energy range. During photochemical relaxation, internal conversion occurs, leading to hydrogen formation and further reactions on different energy surfaces.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Philip M. Kester, Jerry T. Crum, Sichi Li, William F. Schneider, Rajamani Gounder
Summary: The arrangement of framework Al heteroatoms in zeolite lattices influences the energetics of proton siting and the distribution of protons among crystallographically-distinct oxygen atoms and void environments. Experimental results show that different arrangements of framework Al in zeolites lead to changes in vibrational frequencies and molar absorptivities of protons, affecting the equilibrium proton populations and OH IR spectra.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Patrick M. Barboun, Luke L. Daemen, Craig Waitt, Zili Wu, William F. Schneider, Jason C. Hicks
Summary: The study reports INS observations of alumina-supported Ni particles after treatment with N-2 and H-2 plasmas, revealing the presence of NHx species and hydrides, generated through plasma-facilitated surface reactions. Experimental assignments of surface intermediates through INS spectra support the direct implication of plasma stimulation of dinitrogen in generation of surface-bound reactions. The results suggest that these reactions can be driven thermally or with H(2) plasma.
ACS ENERGY LETTERS
(2021)
Article
Chemistry, Physical
Parisa Nematollahi, Hanyu Ma, William F. Schneider, Erik C. Neyts
Summary: This study investigates the mechanisms and kinetics of formic acid decomposition and formation over single Ru atoms anchored on pyridinic nitrogen in a planar graphene flake and curved carbon nanotubes. The results show that curvature control has the potential to enhance catalytic performance.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Craig Waitt, Audrey R. Miles, William F. Schneider
Summary: This study compared the performance of standard models with numerical solutions in describing adsorption free energies, finding that numerical solutions are more effective in evaluating free energies and translational potential energy surfaces.
JOURNAL OF PHYSICAL CHEMISTRY C
(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
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, Physical
Xiaoyu Wang, Yujia Wang, Ahmad Moini, Rajamani Gounder, Edward J. Maginn, William F. Schneider
Summary: This study investigates the influence of organic structure directing agents (OSDAs) on the structure of zeolites and finds a relationship between OSDA orientation, Al3+ siting, and lattice energy. Density functional theory calculations are used to parameterize a fixed-charge classical model, revealing that interaction energies are sensitive to the proximity of Al3+ ions.
CHEMISTRY OF MATERIALS
(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
Chemistry, Multidisciplinary
Patrick M. Barboun, Hope O. Otor, Hanyu Ma, Anshuman Goswami, William F. Schneider, Jason C. Hicks
Summary: This article investigates the adsorption of nitrogen on metal catalysts activated by nonthermal plasma. The experimental results confirm the conversion of plasma-activated nitrogen into ammonia through surface catalyzed pathways. The study also shows the relationship between the hydrogenation ability of the catalyst and the desorption temperature of NH3.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
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
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)
Article
Chemistry, Physical
Erhao Gao, Wenjing Feng, Qi Jin, Li Han, Yi He
Summary: The influence of K-doping on the reactive oxygen species and elementary reactions of HCHO catalytic oxidation was investigated using density functional theory (DFT). The introduction of K-doping changed the electronic structures of Ce and O, facilitating the adsorption and activation of HCHO and O2 molecules, enhancing lattice oxygen mobility, and reducing the energy barrier for HCHO oxidation. K-doping also promoted the formation of hydroxyl groups, facilitating HCHO adsorption and oxidation.
Article
Chemistry, Physical
Hao Fu, Zhangliang Xu
Summary: In this study, the adsorption mechanisms and detection performance of formaldehyde, ammonia, and sulfur dioxide on undoped and metal-doped ZnO surfaces were investigated using density functional theory. The results showed that formaldehyde and ammonia were physically adsorbed on the undoped ZnO surface, while sulfur dioxide was weakly chemisorbed. The adsorption energy was enhanced when ZnO was doped with metals. These findings provide theoretical guidance for the application of ZnO substrate materials in gas sensitivity research.
Article
Chemistry, Physical
Atsushi Nomura, Tohru Kurosawa, Migaku Oda, Satoshi Demura, Shogo Kuwahara, Sora Kobayashi, Hideaki Sakata
Summary: The study investigates the tunneling spectra of 1T-TiSe2 in the CDW state and the dip structure below the Fermi level, aiming to determine whether this dip is a CDW gap. The answer to this question is crucial for understanding the driving mechanism of CDW.
Article
Chemistry, Physical
A. S. Petrov, D. I. Rogilo, A. I. Vergules, V. G. Mansurov, D. V. Sheglov, A. V. Latyshev
Summary: This study investigates Si mass transport and morphological transformations on the Si(111) surface during (root 3 x root 3)-Sn reconstruction formation and Si homoepitaxy. The research shows that the formation of different Sn phases at different temperatures affects the Si island nucleation and monatomic step shift, which in turn impact the morphology of the Sn/Si(111) interface. Electromigration-induced drift of disordered Sn domains leads to enhanced noncompensated Si mass transport and surface roughening.
Article
Chemistry, Physical
D. V. Gruznev, L. V. Bondarenko, A. Y. Tupchaya, A. A. Yakovlev, A. N. Mihalyuk, A. V. Zotov, A. A. Saranin
Summary: Deposition of thallium (Tl) onto the Au/Si(111)5 x 2 reconstruction followed by annealing results in the formation of a surface structure with 4 x 2 periodicity. The immiscibility of Au and Tl leads to the migration of Tl atoms over the Si chains. Thallium donates electrons to the surface, converting the metallic surface into an insulating state and altering the inter-chain distance within the array of Au atomic wires.
Article
Chemistry, Physical
Simone Giusepponi, Francesco Buonocore, Barbara Ferrucci, Massimo Celino
Summary: Using ab-initio calculations, the interaction between lead adatom and both clean and doped iron (100) surfaces was investigated. It was found that the lead adatom prefers to adsorb in the hollow site, which is more stable compared to the top and bridge sites, and in this position, it is energetically favorable over the iron adatom. Moreover, lead adsorbed in the hollow site of the iron (100) surface doped with chromium was found to create a more stable system compared to nickel-doped surfaces with an iron adatom in the same position. The study also explored inter-layer distances, bonding mechanisms, magnetic behaviors, and charge density differences. The results provide insights into the role of doping in the interaction between lead adatom and iron surface, and have implications for the analysis of corrosion processes caused by liquid lead.
Article
Chemistry, Physical
Shuo Zhang, Jin-Ho Choi
Summary: The recent synthesis of two-dimensional layered WSi2N4 has attracted attention due to its potential applications. This study investigates the catalytic performance of WSi2N4 monolayers with nitrogen vacancies in the hydrogen evolution reaction using first-principles calculations. The results show that the defective WSi2N4 monolayers exhibit remarkably high catalytic activity comparable to platinum catalysts. Electronic structure calculations also reveal the emergence of spin-polarized states due to the introduction of nitrogen vacancies.
Article
Chemistry, Physical
Xiaoyan Yu, Xin Cao, Wei Kang, Shanhua Chen, Ao Jiang, Yuhao Luo, Wenwei Deng
Summary: First-principles calculations were used to investigate the electronic properties of a TiO2 heterostructure modified with Bi2Te3 co-catalyst. The study revealed that the Bi2Te3/TiO2 interface introduced optimal band offsets, effectively suppressing electron-hole recombination and enhancing the utilization efficiency of photo-generated carriers. Additionally, the Bi2Te3 co-catalyst introduced extra catalytic active sites, further boosting the photo-catalytic hydrogen evolution efficiency.
Article
Chemistry, Physical
Filippo Longo, Emanuel Billeter, Selim Kazaz, Alessia Cesarini, Marin Nikolic, Aarati Chacko, Patrik Schmutz, Zbynek Novotny, Andreas Borgschulte
Summary: Alkaline water electrolysis is a simple and efficient method for renewable hydrogen production, utilizing cheap and abundant transition metals. The catalytic properties of Ni materials are enhanced by the formation of oxidized compounds on the surface. The high electrocatalytic activity of Ni (oxy)-hydroxides is directly related to water intercalation in the passivation layer, supporting the hypothesis of a water mediated OH- diffusion mechanism. The self-organization of the surface structure during passivation layer formation enables high electrode performance.
Article
Chemistry, Physical
Mohan Kumar Kuntumalla, Miriam Fischer, Alon Hoffman
Summary: By investigating the bonding, retention, and thermal stability of nitrogen in H-Diamond (100), it was found that nitrogen can partially recover its bonding with carbon atoms after high-temperature annealing, indicating a high thermal stability of nitrogen in diamond.
Article
Chemistry, Physical
Dong Yue, Liangying Wen, Rong Chen, Jianxin Wang, Zhongqing Yang
Summary: The adsorption behavior of Cl2 molecules on the TiC surface and the formation and transfer of reaction products were studied using first-principles ab initio calculations. The results show that the Cl atoms bonded to the surface Ti atoms are more stable, and the TiCl3 intermediate is easier to form than the TiCl2 intermediate.
Article
Chemistry, Physical
Yatao Wang, Peng Zhang, Hongjuan Li, Qiuju Xu, Shujun Liu, Xiaopeng Liu, Xuehua Guo, Yitao Li, Jinzhang Liu, Sen Dong, Zhi Wei Seh, Qianfan Zhang
Summary: In this study, the adsorption performance of two types of metal-organic frameworks (MOFs) for thiophene and benzene was experimentally investigated. The results showed that IZE-1 exhibited high selectivity and superior adsorption capacity for thiophene, especially at low concentrations. First-principles calculations and molecular dynamics simulations provided insights into the mechanism of thiophene adsorption and the high selectivity observed. This research demonstrates the potential of MOFs for thiophene adsorption, particularly at high concentrations.
