Article
Chemistry, Physical
Hirosuke Matsui, Koshin Sato, Naoko Isobe, Gabor Samjeske, Tomoya Uruga, Mizuki Tada
Summary: Researchers used operando Pt L-III-edge X-ray absorption fine structure (XAFS)-computed tomography (CT) imaging to spatially image the poisoning of Pt/C PEFC cathode electrocatalyst with SO2. The results showed that SO2 strongly adsorbed on the active sites on the Pt cathode catalyst surface, rather than on Pt catalyst particles. However, subsequent electrochemical treatment led to the degradation of the Pt electrocatalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Patricia Poths, Anastassia N. Alexandrova
Summary: Improvements in operando spectroscopy have allowed for detailed investigation of the dynamic nature of catalysts under operating conditions. However, the high dynamicity of some catalysts presents a challenge, as they contain various thermally accessible states. Different techniques in catalysis research, such as ensemble-based and localized techniques, can provide insights into the dynamics of catalysts.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
David Ochoa-Resendiz, Antonio Gamboa-Suarez, Ramon Hernandez-Lamoneda
Summary: This article presents a detailed theoretical characterization of the structure and interactions in dichlorine clathrate hydrate cages, including the influence of halogen bonding and rotational motion. Monte Carlo simulations and energy decomposition analysis are used to further understand these effects.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Katsutoshi Sato, Shuhei Zaitsu, Godai Kitayama, Sho Yagi, Yuto Kayada, Yoshihide Nishida, Yuichiro Wada, Katsutoshi Nagaoka
Summary: Hydrogen is a promising clean energy source, but the presence of carbon monoxide in the reformate is a major issue. Ru-based catalysts are commonly used for removal of carbon monoxide in polymer electrolyte fuel cell systems. However, their durability against nitrogen impurities such as ammonia is a concern. This study investigated the deactivation of an Ru-based PROX catalyst by ammonia and the mechanism of suppression of this deactivation by adding Pt.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Review
Multidisciplinary Sciences
Ajin Rajan, Anoop P. Pushkar, Balaji C. Dharmalingam, Jithin John Varghese
Summary: Modern heterogeneous catalysis benefits greatly from computational predictions of catalyst structure and its evolution, first-principles mechanistic investigations, and detailed kinetic modeling. This article presents operando catalyst structure prediction techniques using density functional theory simulations and ab initio thermodynamics calculations, as well as surface structure characterization and hierarchical approaches in kinetic parameter estimation. In addition, a bottom-up hierarchical and closed loop modeling framework is proposed.
Article
Chemistry, Physical
Seda Karaboga
Summary: The study focuses on the preparation and characterization of tungsten(VI) oxide supported rhodium(0) nanoparticles (Rh-0/WO3 NPs) used as catalysts for releasing H-2 from dimethylamine borane (DMAB). Rh-0/WO3 NPs exhibit high catalytic activity, with the sample containing 0.1% wt. Rh showing the highest catalytic activity (TOF = 2816 h(-1)). Additionally, the Rh-0/WO3 NPs show good reusability, retaining 55% of their initial catalytic activity after being reused in the dehydrogenation reaction.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
Lidan Deng, Jiawei Wang, Zaikun Wu, Chenhong Liu, Ling Qing, Xiaowei Liu, Jie Xu, Zijian Zhou, Minghou Xu
Summary: Supported Pt-based bimetallic catalysts were investigated for propane dehydrogenation, and the impact of geometric and electronic properties on the catalytic activity was studied. The activity was found to be closely related to the D-holes of Pt in Pt-M bimetallic catalysts, rather than the lattice parameters of Pt-M alloys.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Materials Science, Multidisciplinary
Alejandro Lopez-Bezanilla
Summary: Design principles are used to create dynamically stable transition metal, lanthanide, and actinide-based low-dimensional borides, predicting complex covalent heterostructures hosting Dirac states. Layered borides can be stacked in a layer-by-layer fashion to explore new physical properties and materials, with multiple Dirac states, highly dispersive electronic bands, and decoupled acoustic-optical phonon branches being studied.
PHYSICAL REVIEW MATERIALS
(2021)
Article
Chemistry, Physical
E. M. Mastin, S. E. Dutton, G. A. Blake
Summary: The potential energy surfaces of pure methanol and mixed methanol-water pentamers were investigated using chirped pulse Fourier-transform microwave spectroscopy and ab initio calculations. The study found that the pentamers were bound in a planar ring through hydrogen bonding interactions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
E. M. Mastin, S. E. Dutton, G. A. Blake
Summary: In this study, chirped pulse Fourier-transform microwave spectroscopy aided by ab initio calculations was used to explore the potential energy surfaces of pure methanol and mixed methanol-water pentamers. Rotational constants, anharmonic corrections, dipole moments, and relative energies were calculated for different conformers. The results show that as the methanol content increases, the 23 lowest energy conformers are bound in a planar ring of hydrogen bonding with a steady decrease in the RO-O distance along this ring. Interspersed methanol and water conformers have comparable relative abundances to those with micro-aggregation, but structures with micro-aggregated methanol and water have a higher fitting error. The strong donor-acceptor hydrogen bonding in these clusters leads to well-defined minima on the intermolecular potential energy surface.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Hao Wang, Jiangwen Liao, Jiajun Zhong, Yunpeng Liu, Lei Yao, Lixiong Qian, Yuecheng Lai, Xin Wang, Yikun Li, Jianxin Song, Xueqing Xing, Guang Mo, Zhongjun Chen, Zhonghua Wu
Summary: This paper thoroughly discusses the evolution of the Ni atom coordination structure in the synthesis of Ni single atom catalyst using graphitic carbon nitride as a support. The results reveal a three-stage process in which the coordination configurations change as the temperature increases. The findings are further confirmed by simulations and calculations.
Article
Chemistry, Multidisciplinary
Yuzhen Ge, Xuetao Qin, Aowen Li, Yuchen Deng, Lili Lin, Mengtao Zhang, Qiaolin Yu, Siwei Li, Mi Peng, Yao Xu, Xueyao Zhao, Mingquan Xu, Wu Zhou, Siyu Yao, Ding Ma
Summary: This study reports the synthesis of highly dispersed CoNi bimetallic catalysts on alpha-MoC surface through the strong metal support interaction (SMSI) effect. The as-synthesized CoNi/alpha-MoC catalysts exhibited robust and synergistic performance for hydrogen production from hydrolysis of ammonia borane, with metal-normalized activity surpassing all previously reported noble metal-free catalysts and being four times higher than that of the commercial Pt/C catalyst.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Shunsaku Yasumura, Taisetsu Kato, Yucheng Qian, Takashi Toyao, Zen Maeno, Ken-ichi Shimizu
Summary: The dynamic structural evolution of Rh species in MOR zeolite was studied, revealing oxidation and cluster formation of Rh species under NO and H2 flow. Al sites increased the thermodynamic stability of Rh+ species and prevented over-oxidation reactions. NO capture and selective reduction to NH3 were observed using in situ IR measurements.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Linwei Sai, Xue Wu, Fengyu Li
Summary: A highly symmetric core-shell structure B-96 with good stability at high temperatures has been designed and studied. It exhibits superatomic electronic configuration and spherical aromaticity. The theoretical work not only confirms the energetic advantage of the core-shell structure for large-sized boron clusters, but also provides a strategy for designing large boron clusters with high symmetry core-shell structures.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Muhammad Zeeshan, Qing-Yu Chang, Jun Zhang, Ping Hu, Zhi-Jun Sui, Xing-Gui Zhou, De Chen, Yi-An Zhu
Summary: The catalytic properties of CeO2 catalyst for propane dehydrogenation were studied using density functional theory calculations, revealing a considerable Lewis acid-base interaction on the defective surfaces that enhances bond formation between adsorbates and the catalyst surface, resulting in increased surface reactivity.
CHINESE JOURNAL OF CHEMISTRY
(2021)
Article
Biochemical Research Methods
Cameron Giberson, Rajesh K. Singh, Jaehun Chun, Adam P. Huntley, Jason Zhong, Yehia M. Ibrahim, Gregory K. Schenter, Joon-Yong Lee, Sandilya V. B. Garimella
Summary: In this article, a novel ion trajectory simulation platform called SimELIT is introduced for studying ion dynamics in mass spectrometry systems. SimELIT is a modular program with a user-friendly graphical user interface, and it provides extensions of multiple physics and two numerical solvers for ion trajectory simulations. The accuracy and reliability of SimELIT are verified by comparing the results with other simulation software and theoretical estimates.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2022)
Article
Chemistry, Multidisciplinary
Shichao Ding, Jordan Alysia Barr, Zhaoyuan Lyu, Fangyu Zhang, Maoyu Wang, Peter Tieu, Xin Li, Mark H. Engelhard, Zhenxing Feng, Scott P. Beckman, Xiaoqing Pan, Jin-Cheng Li, Dan Du, Yuehe Lin
Summary: The introduction of phosphorus into Fe-N-C single-atom catalysts enhances the peroxidase-like activity, showing excellent selectivity and stability. A 1D carbon nanowire catalyst with enriched Fe-N-4 active sites and phosphorus doping is designed and synthesized, and it is employed in an enzyme cascade platform for highly sensitive colorimetric detection of the neurotransmitter acetylcholine.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Zhun Dong, Ahmad Mukhtar, Thomas Ludwig, Sneha A. Akhade, ShinYoung Kang, Brandon Wood, Katarzyna Grubel, Mark Engelhard, Tom Autrey, Hongfei Lin
Summary: This study investigates the kinetics of surface-functionalized Pd on carbon catalysts for formate dehydrogenation and the impact of O-functional groups. The study shows that O-functional groups play critical roles in dispersing Pd nanoparticles and decreasing the activation energy, while C-O groups hinder the formation of metallic Pd.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Kevin Carter-Fenk, Britta A. Johnson, John M. Herbert, Gregory K. Schenter, Christopher J. Mundy
Summary: A new simulation method is used to directly study the generation of hydrated electrons from the charge-transfer-to-solvent state. The simulations reveal a two-step process involving ionization and solute reorganization leading to the equilibrated ground state of the solvated electron. This methodology has implications for photochemical electron transfer processes in solution, with potential application in photocatalysis and energy transfer.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Biochemistry & Molecular Biology
Ewa C. E. Ronnebro, Mark Engelhard, Danny Edwards, Katarzyna Grubel, Anthony Guzman, Randall Storms
Summary: The coating of metal specimens affects the hydrogen gettering performance. This study evaluated the role of post-plating heat treatments on gettering rates, surface composition, and texture. It was found that the pre-heat treatment in air before activation is necessary to avoid slower gettering rates.
Article
Chemistry, Multidisciplinary
Hao Jia, Ju-Myung Kim, Peiyuan Gao, Yaobin Xu, Mark H. Engelhard, Bethany E. Matthews, Chongmin Wang, Wu Xu
Summary: This study systematically investigates and compares localized high-concentration electrolytes (LHCEs) based on five different solvents in lithium-ion batteries (LIBs). The unique solvation structure of LHCEs facilitates the formation of solid electrolyte interphase (SEI) on graphite anode, enabling previously incompatible solvents to achieve reversible lithiation/delithiation. The study also reveals that the long-term cyclability of LIBs can be improved by introducing additives into LHCEs, which results in effective SEIs and cathode electrolyte interphases (CEIs).
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Trent R. Graham, Maxime Pouvreau, Rafal Gorniak, Hsiu-Wen Wang, Emily T. Nienhuis, Quin R. S. Miller, Jian Liu, Micah P. Prange, Gregory K. Schenter, Carolyn I. Pearce, Kevin M. Rosso, Aurora E. Clark
Summary: The thermal transformation of crystalline sodium aluminum salt hydrate was studied in this research. It was found that the change in aluminum coordination during melting occurs within a highly disordered quasi-two-dimensional phase at the solid-solution interface. This study provides insights into the mechanisms controlling aluminum phase transformations in highly alkaline solutions.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Konstantin Khivantsev, Nicholas R. Jaegers, Hristiyan A. Aleksandrov, Inhak Song, Xavier Isidro Pereira-Hernandez, Mark H. Engelhard, Jinshu Tian, Linxiao Chen, Debora Motta Meira, Libor Kovarik, Georgi N. Vayssilov, Yong Wang, Janos Szanyi
Summary: Atom trapping leads to catalysts with atomically dispersed Ru1O5 sites on (100) facets of ceria, showing excellent activity in catalytic NO oxidation and high NOx storage properties. The Ru1O5 sites exhibit higher stability during calcination and the Ru1/CeO2 catalyst is stable during continuous cycling and in the presence of moisture. In addition, the catalyst shows excellent reactivity for NO reduction by CO at low temperatures. This study highlights the applicability of novel ceria-based single-atom catalysts in NO and CO abatement.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Guangxia Feng, Hao Jia, Yaping Shi, Xu Yang, Yanliang Liang, Mark H. Engelhard, Ye Zhang, Chaojie Yang, Kang Xu, Yan Yao, Wu Xu, Xiaonan Shan
Summary: Reflection interference microscopy enables real-time imaging of the formation and evolution of the solid-electrolyte interphase in batteries, providing valuable insights into its structure and dynamics. The imaging reveals the stratified structure of the interphase, with an inner inorganic layer, an interfacial electrified double layer, and an outer organic-rich layer that is reversible with cycling. The thicknesses of the interphase subcomponents show an inverse correlation, indicating the influence of the inner layer on the formation of the outer layer and lithium nucleation.
NATURE NANOTECHNOLOGY
(2023)
Article
Chemistry, Physical
Vanessa Lebarbier Dagle, Gregory Collinge, Mohammed Rahmana, Austin Winkelman, Wenda Hu, Jian Zhi Hu, Libor Kovarik, Mark Engelhard, Jennifer Jocz, Yong Wang, Mal-Soon Lee, Vassiliki-Alexandra Glezakou, Debmalya Ray, Roger Rousseau, Robert Dagle
Summary: This study reports on a Cu/ZrO2/SBA-16 catalyst with remarkable olefins selectivity and enhanced stability compared to the Ag/ZrO2/SBA-16 catalyst. Replacing Ag with Cu shifts the reaction pathway of crotonaldehyde hydrogenation, leading to the formation of butyraldehyde. Experimental and computational tools were used to verify the performance and stability advantage of the Cu/ZrO2/SBA-16 catalyst.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Multidisciplinary Sciences
Jianghao Zhang, Wenda Hu, Binbin Qian, Houqian Li, Berlin Sudduth, Mark Engelhard, Lian Zhang, Jianzhi Hu, Junming Sun, Changbin Zhang, Hong He, Yong Wang
Summary: In this study, the authors demonstrate that coordinating Pd with alkenyl-type ligands creates an electron-rich environment for selective hydrogenation. The method of forming homogeneous-like Pd catalyst structure with noble metals is crucial for inhibiting side reactions in hydrotreating processes.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Robert F. Hansen, Evan Z. Dalton, Rebecca B. Abney, Mark H. Engelhard, Gerardo Castillo Valdes, Sarah D. Burton, Rosalie K. Chu, Daniel P. Veghte, Swarup China, Yaroslav Losovyj, John B. Cliff, Jonathan D. Raff
Summary: Organicnitrate ester compounds (RONO2) act as sinks for nitrogen oxides (NO x & EQUIV;NO + NO2) and play a crucial role in the formation of ozone and organic aerosols in the lower atmosphere. This study investigates the production of RONO2 in organic aerosols through aqueous phase reactions involving nitronium (NO2 (+)) and humic and fulvic acids. The results provide evidence that NO2 (+) targets the lipid fraction of organic matter and forms stable RONO2 compounds through reactions with terminal alcohols (ROH) and alkenes.
ACS EARTH AND SPACE CHEMISTRY
(2023)
Article
Materials Science, Multidisciplinary
Martin Weiser, Matthew J. Olszta, Mark H. Engelhard, Zihua Zhu, Daniel K. Schreiber
Summary: The transport paths of oxygen during intergranular oxidation in binary Ni-Cr were studied using electron microscopy, atom probe tomography (APT), secondary ion mass spectroscopy, and oxygen tracer exchange experiments. The selective oxidation of Cr was isolated by performing oxidation with a CO/CO2 gas mixture. The results reveal nanometer-scale details of passivation and penetrative intergranular oxidation processes, as well as preferred transport paths at the oxide/alloy interface.
NPJ MATERIALS DEGRADATION
(2023)
Article
Biophysics
Michael J. Taylor, Hoshin Kim, William Kew, Amity Andersen, Arunima Bhattacharjee, Mark H. Engelhard, Christopher R. Anderton
Summary: In beam-based ionization methods, the substrate plays a crucial role in the desorption mechanism of molecules from surfaces. Atomistic simulations combined with density functional theory calculations were used to study the desorption of a sphingolipid from a model surface. The results provide insights into the effects of biointerfacial lipid ordering on SIMS imaging.
Article
Chemistry, Multidisciplinary
Xia Cao, Yaobin Xu, Lianfeng Zou, Jie Bao, Yunxiang Chen, Bethany E. Matthews, Jiangtao Hu, Xinzi He, Mark H. Engelhard, Chaojiang Niu, Bruce W. Arey, Chunsheng Wang, Jie Xiao, Jun Liu, Chongmin Wang, Wu Xu, Ji-Guang Zhang
Summary: The calendar life of Lithium Metal Batteries (LMBs) can be significantly improved by forming a stable Solid Electrolyte Interphase (SEI) layer on the surface of Li metal anodes. The stability and reusability of this SEI during repeated lithium stripping/deposition processes have been studied using in situ electron microscopy. LMBs stored under fully charged or fully discharged conditions exhibit longer calendar life.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
