Article
Chemistry, Physical
T. V. Pavlova, V. M. Shevlyuga, B. V. Andryushechkin, K. N. Eltsov
Summary: This study reports the removal of individual halogen atoms from Si(100)-2x1-Cl and -Br surfaces in STM. The charge states of DBs formed on the Si surface can be manipulated, allowing for tuning the reactivity of the Cl- and Br-terminated surfaces.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Isaac J. Gresham, Chiara Neto
Summary: Over the past decade, a new class of slippery, anti-adhesive surfaces known as SCALS has emerged, characterized by low contact angle hysteresis with water and most solvents. The physico-chemical characteristics that enable ultra-low contact angle hysteresis are still unknown, making rational design of these systems impossible. In this review, a quantitative and comparative analysis is conducted to understand the optimal conditions for SCALS, including the type of material, molecular weight, grafting density, and layer thickness. The existing literature on SCALS is reviewed, revealing trends in the reported data and suggesting areas for future experimental study.
ADVANCES IN COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Isaac J. Gresham, Seamus G. Lilley, Andrew R. J. Nelson, Kaloian Koynov, Chiara Neto
Summary: This study quantifies the properties of a range of PDMS SCALS and elucidates their nanostructure responsible for their properties. The study also shows that the properties of SCALS can be predicted by reducing the grafting density, with the lowest water contact angle hysteresis achieved at a grafting density of approximately 2.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Deb Kumar Bhowmick, Adrian Joe Urban, Manfred Bartsch, Bjoern Braunschweig, Helmut Zacharias
Summary: Efficient control of interface chemistry enables better tunability of electronic properties, and a novel near-UV-initiated direct modification method has been demonstrated to form stable organic monolayers on silicon surfaces with high hydrolytic stability.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Esther Frederick, Quinn Campbell, Igor Kolesnichenko, Luis F. Pena, Angelica Benavidez, Evan M. Anderson, David R. Wheeler, Shashank Misra
Summary: This study demonstrates the achievement of ultradoping concentrations of boron using a solvothermal process, but faces challenges such as catalyst cross-reactions and ambiguity in experimental confirmation of direct surface attachment.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Limei Wang, Rui Zhu, Zhitao Shen, Yeheng Song, Limin She, Xuesen Wang, Yu Jia, Zhenyu Zhang, Weifeng Zhang
Summary: In this study, two well-ordered self-assembled covalently linked wavy chains were obtained on Ag(111) surface through the reaction of 1,2-bis(3-bromophenyl)ethane with multiple conformations. The wavy chains exhibited distinct conformational arrangements and coassembled with dissociated bromine atoms.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Esther Frederick, Quinn Campbell, Angelica Benavidez, David R. Wheeler, Shashank Misra
Summary: Traditional approaches for functionalizing silicon with dopants involve grafting the dopant onto silicon substrates through O-Si or C-Si bonds, resulting in indirect attachment. Recent ultrahigh vacuum work has shown that high densities of direct B-Si bonds can enable unprecedented electronic behaviors in silicon, making it a potential next-generation electronic material. Work is currently being done to develop solvothermal approaches for forming direct dopant-Si bonds to further enhance the potential of silicon in the electronic materials field.
Article
Chemistry, Analytical
Miriam Chavez, Laura Fuentes-Rodriguez, Guadalupe Sanchez-Obrero, Rafael Madueno, Jose Manuel Sevilla, Manuel Blazquez, Teresa Pineda
Summary: Bis[2-(2-bromoisobutyryloxy) undecyl] disulphide (DTBU) is an initiator for surface-initiated atom transfer radical polymerization (SI-ATRP) that can functionalize metal surfaces through formation of self-assembled monolayers (SAM). This article characterizes the DTBU initiator monolayers on gold polycrystalline electrodes using electrochemical methods such as cyclic voltammetry, capacity-potential curves, electrochemical impedance spectroscopy, and angle contact measurements. The monolayers' integrity and permeability are determined through capacitance potential measurements and impedance spectra. Furthermore, the effect of SAM as a physical barrier on different redox probes is explored. The study also examines mixed monolayers of DTBU and 6-mercaptopurine for their potential use in electron exchange through monolayers.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2022)
Review
Chemistry, Multidisciplinary
Chinmay Dey, Madhuparna Roy, Somdatta Ghosh Dey
Summary: This article introduces the use of self-assembled monolayers (SAMs) on Au electrodes to mimic the aggregation state of A beta and investigate its interaction with different metals and cytochrome c, as well as the changes in structure and reactivity.
Article
Physics, Applied
V Danesh, H. Nejat Pishkenari, H. Zohoor
Summary: This letter discusses the surface-reconstruction-induced self-twisting behavior of Si <100> nanobelts and nanowires with rectangular cross section, and presents a continuum-based model to explain the phenomenon. It is revealed that these structures can self-assemble into both right- and left-handed helicoids depending on their crystal arrangements, with different torsion angle values for each morphology. Additionally, atomistic simulations using Tersoff's potential support the analytical discussions and are consistent with the continuum model predictions.
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2021)
Article
Nanoscience & Nanotechnology
Liping Wang, Zheng Hou, Dicky Pranantyo, En-Tang Kang, Mary Chan-Park
Summary: A novel pretreatment chemistry was developed to create a high-density 3-D RSNO network coating on biomedical device surfaces, effectively inhibiting biofilm formation with good biocompatibility and antibacterial activity. The high-density RSNO coating showed nearly 99% reduction of P. aeruginosa and MRSA in vivo, demonstrating potential for application in various biomedical devices.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Polymer Science
Jianliang Jiang, Junxue Zhai, Yiqun Zhang, Yakai Feng
Summary: A biomimetic design for high mechanical and flame-retardant chloroprene rubber (CR) by introducing sacrificial bond (disulfide) crosslinked networks and two new types of vulcanization reactions.
Article
Chemistry, Multidisciplinary
Yi-Chin Lai, Yu-Chieh Chiu, Kai-Wen Chuang, Balaji Ramachandran, I-Feng Wu, Ying-Chih Liao
Summary: In this study, a water transfer method was developed to fabricate thin-film patterns on 3D curvilinear surfaces. By suspending crystalline silver nanoplates in ethanol with a surfactant and spreading the suspension over the water surface, a self-assembled thin film was generated. The thin film could be effectively transferred to object surfaces with nanometer thickness and exhibited superior conductivity without thermal sintering.
Article
Nanoscience & Nanotechnology
Pooria Tajalli, Jennifer M. Hernandez Rivera, Mina Omidiyan, Hung-Vu Tran, T. Randall Lee
Summary: Two different positional isomers of carbonate-terminated alkanethiol molecules were synthesized and used to create self-assembled monolayers (SAMs) on gold as mimics of commercially available polycarbonate surfaces. The characterization of the adsorbate molecules and SAMs was done using various spectroscopic techniques. The wettabilities of both SAMs were found to be similar to that of poly(ethylene carbonate) samples, indicating that the carbonate-terminated SAMs can be used to study the interfacial properties of polycarbonates without interference from surface reconstruction.
ACS APPLIED NANO MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Aman Bhardwaj, Lalit M. Pandey
Summary: Hospital-acquired infections (HAIs) are a serious medical threat affecting the efficacy of existing medical infrastructure, with antibiotics contributing to multi-drug resistant bacteria and biofilm formation. Silver nanoparticles (AgNPs) based antimicrobial surfaces show potential in preventing bacterial adhesion and biofilm formation, offering a promising solution to address the issue of HAIs.
Article
Chemistry, Physical
Isaiah Barth, James Akinola, Jonathan Lee, Oliver Y. Gutierrez, Udishnu Sanyal, Nirala Singh, Bryan R. Goldsmith
Summary: Phenol is an important model compound for understanding the hydrogenation of biomass to biofuels, and the active facets of Pt and Rh catalysts for this reaction have been identified. The study reveals that the activity trends of Pt and Rh nanoparticles in the hydrogenation of phenol are size-dependent, with higher turnover frequencies observed on certain terraces. The increase in experimental turnover frequencies with larger Pt and Rh nanoparticle diameters is attributed to a larger fraction of terraces on the larger particles.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Biotechnology & Applied Microbiology
Eric Musa, Francis Doherty, Bryan R. Goldsmith
Summary: Identifying the structure of heterogeneous catalysts is crucial for understanding catalytic reactions and structure-property relationships. Machine learning is now being used to accelerate the search of catalyst structures, enabling modeling of larger and more complex catalyst structures and aiding catalyst design.
CURRENT OPINION IN CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Physical
Jacques A. Esterhuizen, Bryan R. Goldsmith, Suljo Linic
Summary: Most applications of machine learning in heterogeneous catalysis use black-box models, which are not easily interpretable. Interpretable machine learning methods offer an alternative by merging the predictive capacity of black-box models with the interpretability of physics-based models. This Perspective discusses the potential, challenges, and opportunities of interpretable machine learning in catalysis research.
Editorial Material
Materials Science, Multidisciplinary
Ghanshyam Pilania, Bryan R. Goldsmith, Mina Yoon, Avinash M. Dongare
JOURNAL OF MATERIALS SCIENCE
(2022)
Article
Chemistry, Physical
Samuel D. Young, Bianca M. Ceballos, Amitava Banerjee, Rangachary Mukundan, Ghanshyam Pilania, Bryan R. Goldsmith
Summary: This article discusses the potential of metal oxynitrides as a new material category for e-NRR and compares them with metal nitrides and metal oxides. The article focuses on the challenges faced by metal oxynitrides in e-NRR and provides an outlook for future research.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Harsh Agarwal, Jacob Florian, Daniel Pert, Bryan R. Goldsmith, Nirala Singh
Summary: Transition-metal ions regularly undergo charge transfer reactions by directly interacting with electrodes. The average energy of the d electrons of a transition-metal electrode (d-band center) can rationalize the kinetic trends of inner-sphere charge transfer reactions. This descriptor aids in the design of electrochemical systems with improved kinetics.
Article
Physics, Fluids & Plasmas
Francis Doherty, Bryan R. Goldsmith
Summary: Through density functional theory (DFT) modeling, we investigate the effect of plasma-induced surface charging on CO2 activation by atomically dispersed single atom (SA) catalysts on reducible and irreducible metal oxide supports. We find that the accumulated surface charge on the SA increases the CO2 adsorption strength and decreases the CO2 dissociation barrier. This study demonstrates the importance of considering surface charging in strong electric fields for molecule adsorption and bond-breaking on catalytic surfaces.
PLASMA SOURCES SCIENCE & TECHNOLOGY
(2023)
Article
Multidisciplinary Sciences
Sanat Vibhas Modak, Wanggang Shen, Siddhant Singh, Dylan Herrera, Fairooz Oudeif, Bryan R. R. Goldsmith, Xun Huan, David G. G. Kwabi
Summary: Organic redox-active molecules are attractive as redox-flow battery (RFB) reactants due to their low cost and tunable properties, but material degradation and capacity fade hinder their commercial deployment. In this work, the authors use spectroscopy and statistical inference techniques to elucidate the decay mechanism and establish a quantitative connection between molecular decay and capacity fade in organic redox-flow batteries. The study highlights the potential of using statistical inference to understand the causes of capacity fade and further develop these batteries.
NATURE COMMUNICATIONS
(2023)
Article
Computer Science, Artificial Intelligence
Cameron J. Gruich, Varun Madhavan, Yixin Wang, Bryan R. Goldsmith
Summary: This study investigates the application of three uncertainty quantification (UQ) methods in the field of heterogeneous catalysis. By using a crystal graph convolutional neural network to predict adsorption energies on alloys, the effectiveness of the UQ methods, namely k-fold ensembling, Monte Carlo dropout, and evidential regression, is evaluated. The results demonstrate that evidential regression is a powerful and trustworthy approach for obtaining tunable UQ estimates in heterogeneous catalysis applications using neural networks.
MACHINE LEARNING-SCIENCE AND TECHNOLOGY
(2023)
Article
Chemistry, Physical
Samuel D. D. Young, Jiadong Chen, Wenhao Sun, Bryan R. R. Goldsmith, Ghanshyam Pilania
Summary: Perovskiteoxynitrides (PONs) are promising materials for catalysis and photovoltaics, but their full potential has yet to be explored. This study predicts the stability of PON materials using density functional theory modeling and also determines the suitable range of electrochemical operating conditions. However, not all compounds with zero energy above the thermodynamic convex hull can be easily synthesized.
CHEMISTRY OF MATERIALS
(2023)
Review
Chemistry, Physical
Ankit Mathanker, Wendy Yu, Nirala Singh, Bryan R. Goldsmith
Summary: There is increasing interest in the influence of ions on electrocatalytic reactions. Spectator ions have not been fully explored in their impact on electrocatalytic rates of hydrogenation and oxidation of larger organic molecules. This article discusses various ways in which spectator ions can affect the electrocatalytic reactions of organic molecules and emphasizes the importance of further research in this area to develop more efficient electrocatalytic systems.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Nirala Singh, Cailin A. Buchanan, Dylan Herrera, Mahalingam Balasubramanian, Bryan R. Goldsmith
Summary: In this study, the structures and charge transfer (CT) mechanism of Ce3+ and Ce4+ ions in sulfuric acid were determined through experimental and computational methods. It was found that Ce3+ is coordinated by nine water molecules, while Ce4+ forms complexes with water and bisulfate ions. The kinetics of the Ce3+/Ce4+ redox couple were found to be independent of the electrode, indicating outer-sphere electron-transfer behavior. A two-step mechanism was proposed, in which Ce4+ exchanges bisulfate ions with water in a chemical step, followed by a rate-determining electron transfer step.
Article
Chemistry, Physical
Jacques A. Esterhuizen, Bryan R. Goldsmith, Suljo Linic
Summary: Unsupervised machine learning with principal component analysis offers a straightforward pathway for developing accurate and interpretable electronic-structure descriptors of material properties. These descriptors can predict chemical properties and reveal connections between geometric structure and catalytic properties.
Article
Chemistry, Multidisciplinary
Jacob Florian, Harsh Agarwal, Nirala Singh, Bryan R. Goldsmith
Summary: Research shows that the reaction kinetics of metal redox couples on electrode surfaces are enhanced in the presence of halides. Calculated desorption barriers of metal-anion complexes correlate with experimental kinetic measurements, guiding the design of electrolytes and electrocatalysts with faster kinetics for relevant redox reactions in energy and environmental applications.
Article
Chemistry, Multidisciplinary
Harsh Agarwal, Jacob Florian, Bryan R. Goldsmith, Nirala Singh
Summary: This study investigates the kinetics of V2+/V3+ reaction in vanadium redox flow batteries, and explores the structures of V2+ and V3+ in different electrolytes. The results suggest that the polarizability of anions affects the kinetics of V2+/V3+ reaction in the batteries.
CELL REPORTS PHYSICAL SCIENCE
(2021)