Self-consistent convolutional density functional approximations: Application to adsorption at metal surfaces
Chemphyschem. 2024 Feb 29:e202300688. doi: 10.1002/cphc.202300688. Online ahead of print.ABSTRACTThe exchange-correlation (XC) functional in density functional theory is used to approximate multi-electron interactions. A plethora of different functionals are available, but nearly all are based on the hierarchy of inputs commonly referred to as "Jacob's ladder." This paper introduces an approach to construct XC functionals with inputs from convolutions of arbitrary kernels with the electron density, providing a route to move beyond Jacob's ladder. We derive the variational derivative of these functionals, showing consistenc...
Source: Chemphyschem - February 29, 2024 Category: Chemistry Authors: Sushree Jagriti Sahoo Qimen Xu Xiangyun Lei Daniel Staros Gopal R Iyer Brenda Rubenstein Phanish Suryanarayana Andrew Medford Source Type: research
In Situ Fabrication of SnO < sub > 2 < /sub > Nanowalls for Robust Acetylene Sensing at Low Temperature
This study examines the direct fabrication of ultrathin SnO2 nanowalls on Ag-Pd substrates using a simple solvothermal method that doesn't demand the use of any additional motivators or templates. The thickness and shape of the nanowalls can be controlled by varying the cetyl trimethyl ammonium bromide (CTAB) concentration in the solvent. As observed, the gas sensor (SnO2 -3) fabricated by 2.4 g CTAB exhibits superior gas-sensing features. This is primarily due to the hollow structure constructed by the arrangement of nanowalls, which delivers not only enough gas diffusion pathways but also enough reaction sites during the...
Source: Chemphyschem - February 28, 2024 Category: Chemistry Authors: Chuantao Zhang Lingmin Yu Xingyu He Chao Shi Senlin Li Fan Zhao Xinhui Fan Source Type: research
Evaluation of the effect of polyethylenimine on boron adsorption by soil minerals
This study investigates the interaction between boron ions and soil minerals (gibbsite, kaolinite, and montmorillonite) in the presence of polyethylenimine (PEI). The minerals underwent characterization based on specific surface area, particle size distribution, zeta potential, and the presence of functional groups. The influence of PEI addition on the stability of the soil mineral suspension was evaluated by turbidimetry. Mineral-boron and mineral-boron-PEI interactions were explored under varying conditions, including pH, initial boron concentration, and mineral quantity, with all adsorption experiments conducted over 24...
Source: Chemphyschem - February 28, 2024 Category: Chemistry Authors: Justyna Ulatowska Katarzyna Szewczuk-Karpisz Izabela Polowczyk Source Type: research
Online-Monitoring of the Enantiomeric Ratio in Microfluidic Chip Reactors Using Chiral Selector Ion Vibrational Spectroscopy
Chemphyschem. 2024 Feb 28:e202300975. doi: 10.1002/cphc.202300975. Online ahead of print.ABSTRACTA novel experimental approach for the rapid online monitoring of the enantiomeric ratio of chiral analytes in solution is presented. The charged analyte is transferred to the gas phase by electrospray. Diastereomeric complexes are formed with a volatile chiral selector in a buffer-gas-filled ion guide held at room temperature, mass-selected, and subsequently spectrally differentiated by cryogenic ion trap vibrational spectroscopy. Based on the spectra of the pure complexes in a small diastereomer-specific spectral range, the co...
Source: Chemphyschem - February 28, 2024 Category: Chemistry Authors: Sonja Schmahl Francine Horn Jiaye Jin Hannes Westphal Detlev Belder Knut R Asmis Source Type: research
In Situ Fabrication of SnO < sub > 2 < /sub > Nanowalls for Robust Acetylene Sensing at Low Temperature
This study examines the direct fabrication of ultrathin SnO2 nanowalls on Ag-Pd substrates using a simple solvothermal method that doesn't demand the use of any additional motivators or templates. The thickness and shape of the nanowalls can be controlled by varying the cetyl trimethyl ammonium bromide (CTAB) concentration in the solvent. As observed, the gas sensor (SnO2 -3) fabricated by 2.4 g CTAB exhibits superior gas-sensing features. This is primarily due to the hollow structure constructed by the arrangement of nanowalls, which delivers not only enough gas diffusion pathways but also enough reaction sites during the...
Source: Chemphyschem - February 28, 2024 Category: Chemistry Authors: Chuantao Zhang Lingmin Yu Xingyu He Chao Shi Senlin Li Fan Zhao Xinhui Fan Source Type: research
Evaluation of the effect of polyethylenimine on boron adsorption by soil minerals
This study investigates the interaction between boron ions and soil minerals (gibbsite, kaolinite, and montmorillonite) in the presence of polyethylenimine (PEI). The minerals underwent characterization based on specific surface area, particle size distribution, zeta potential, and the presence of functional groups. The influence of PEI addition on the stability of the soil mineral suspension was evaluated by turbidimetry. Mineral-boron and mineral-boron-PEI interactions were explored under varying conditions, including pH, initial boron concentration, and mineral quantity, with all adsorption experiments conducted over 24...
Source: Chemphyschem - February 28, 2024 Category: Chemistry Authors: Justyna Ulatowska Katarzyna Szewczuk-Karpisz Izabela Polowczyk Source Type: research
Online-Monitoring of the Enantiomeric Ratio in Microfluidic Chip Reactors Using Chiral Selector Ion Vibrational Spectroscopy
Chemphyschem. 2024 Feb 28:e202300975. doi: 10.1002/cphc.202300975. Online ahead of print.ABSTRACTA novel experimental approach for the rapid online monitoring of the enantiomeric ratio of chiral analytes in solution is presented. The charged analyte is transferred to the gas phase by electrospray. Diastereomeric complexes are formed with a volatile chiral selector in a buffer-gas-filled ion guide held at room temperature, mass-selected, and subsequently spectrally differentiated by cryogenic ion trap vibrational spectroscopy. Based on the spectra of the pure complexes in a small diastereomer-specific spectral range, the co...
Source: Chemphyschem - February 28, 2024 Category: Chemistry Authors: Sonja Schmahl Francine Horn Jiaye Jin Hannes Westphal Detlev Belder Knut R Asmis Source Type: research
Theoretical investigation of the adsorbate and potential-induced stability of Cu facets during electrochemical CO2 and CO reduction
Chemphyschem. 2024 Feb 26:e202300959. doi: 10.1002/cphc.202300959. Online ahead of print.ABSTRACTThe activity and product selectivity of electrocatalysts for reactions like the carbon dioxide reduction reaction (CO2RR) are intimately dependent on the catalyst's structure and composition. While engineering catalytic surfaces can improve performance, discovering the key sets of rational design principles remains challenging due to limitations in modeling catalyst stability under operating conditions. Herein, we perform first-principles density functional calculations adopting implicit solvation methods with potential control...
Source: Chemphyschem - February 27, 2024 Category: Chemistry Authors: Henry Yu Nitish Govindarajan Stephen E Weitzner Rui Serra-Maia Sneha A Akhade Joel B Varley Source Type: research
The importance of Spin-Polarized Charge Reorganization in the Catalytic Activity of D-Glucose Oxidase
Chemphyschem. 2024 Feb 27:e202400033. doi: 10.1002/cphc.202400033. Online ahead of print.ABSTRACTThe reaction of D-glucose oxidase (GOx) with D- and L-glucose was investigated using confocal fluorescence microscopy and Hall voltage, after the enzyme was adsorbed as a monolayer. By adsorbing the enzyme on a ferromagnetic substrate, we verified that the reaction is spin dependent. This conclusion was supported by monitoring the reaction when the enzyme is adsorbed on a Hall device that does not contain any magnetic elements. The spin dependence is consistent with the chiral-induced spin selectivity (CISS) effect; it can be e...
Source: Chemphyschem - February 27, 2024 Category: Chemistry Authors: Naupada Preeyanka Qirong Zhu Tapan-Kumar Das Ron Naaman Source Type: research
Autocombustion Route Derived Zinc Ferrite Nanoparticles as Chemiresistive Sensor for Detection of Alcohol Vapors
Chemphyschem. 2024 Feb 27:e202300730. doi: 10.1002/cphc.202300730. Online ahead of print.ABSTRACTProlonged exposure to alcohol vapors can have detrimental effects on human health, potentially leading to eye irritation, dizziness, and in some cases, damage to the nervous system. The present article aims to provide a comprehensive understanding on the synthesis and characterization of zinc ferrite (ZnFe2O4) nanoparticles, as well as their interactions with a range of alcohol vapors, including methanol, ethanol, n-propanol, and isopropanol. These alcohols differ in their molecular weight, boiling points, diffusivity, and othe...
Source: Chemphyschem - February 27, 2024 Category: Chemistry Authors: Bhooma Bhagat Santosh K Gupta Dipankar Mandal Rajib Badyopadhyay Kalisadhan Mukherjee Source Type: research
Theoretical investigation of the adsorbate and potential-induced stability of Cu facets during electrochemical CO2 and CO reduction
Chemphyschem. 2024 Feb 26:e202300959. doi: 10.1002/cphc.202300959. Online ahead of print.ABSTRACTThe activity and product selectivity of electrocatalysts for reactions like the carbon dioxide reduction reaction (CO2RR) are intimately dependent on the catalyst's structure and composition. While engineering catalytic surfaces can improve performance, discovering the key sets of rational design principles remains challenging due to limitations in modeling catalyst stability under operating conditions. Herein, we perform first-principles density functional calculations adopting implicit solvation methods with potential control...
Source: Chemphyschem - February 27, 2024 Category: Chemistry Authors: Henry Yu Nitish Govindarajan Stephen E Weitzner Rui Serra-Maia Sneha A Akhade Joel B Varley Source Type: research
The importance of Spin-Polarized Charge Reorganization in the Catalytic Activity of D-Glucose Oxidase
Chemphyschem. 2024 Feb 27:e202400033. doi: 10.1002/cphc.202400033. Online ahead of print.ABSTRACTThe reaction of D-glucose oxidase (GOx) with D- and L-glucose was investigated using confocal fluorescence microscopy and Hall voltage, after the enzyme was adsorbed as a monolayer. By adsorbing the enzyme on a ferromagnetic substrate, we verified that the reaction is spin dependent. This conclusion was supported by monitoring the reaction when the enzyme is adsorbed on a Hall device that does not contain any magnetic elements. The spin dependence is consistent with the chiral-induced spin selectivity (CISS) effect; it can be e...
Source: Chemphyschem - February 27, 2024 Category: Chemistry Authors: Naupada Preeyanka Qirong Zhu Tapan-Kumar Das Ron Naaman Source Type: research
Autocombustion Route Derived Zinc Ferrite Nanoparticles as Chemiresistive Sensor for Detection of Alcohol Vapors
Chemphyschem. 2024 Feb 27:e202300730. doi: 10.1002/cphc.202300730. Online ahead of print.ABSTRACTProlonged exposure to alcohol vapors can have detrimental effects on human health, potentially leading to eye irritation, dizziness, and in some cases, damage to the nervous system. The present article aims to provide a comprehensive understanding on the synthesis and characterization of zinc ferrite (ZnFe2O4) nanoparticles, as well as their interactions with a range of alcohol vapors, including methanol, ethanol, n-propanol, and isopropanol. These alcohols differ in their molecular weight, boiling points, diffusivity, and othe...
Source: Chemphyschem - February 27, 2024 Category: Chemistry Authors: Bhooma Bhagat Santosh K Gupta Dipankar Mandal Rajib Badyopadhyay Kalisadhan Mukherjee Source Type: research
The Interplay of Spacer Chirality and Parity in Mesogenic Dimers
In this study, we synthesized a novel series of LC dimers with a chiral center as part of their flexible spacer. The dimers were prepared in racemic and enantiomerically pure forms. Their spacer length and parity were varied to investigate the effect of spacer chirality and parity on mesomorphic behavior and on chiral induction in the nematic phase of achiral mesogens. Our results show that the even-membered chiral dimers only have chiral nematic phases. In contrast, the odd-membered dimers display rich mesomorphism, including the intriguing blue phase (BP) and chiral form of the twist-bend nematic phase (N*TB). The observ...
Source: Chemphyschem - February 26, 2024 Category: Chemistry Authors: Antonija O žegović Anamarija Kne žević Jurica Novak Suzana Šegota Patrick Davidson Andreja Lesac Source Type: research
Identifying Exchangeable Protons in a 1D NMR Spectrum by Spatially Selective Exchange-Editing
Chemphyschem. 2024 Feb 26:e202300713. doi: 10.1002/cphc.202300713. Online ahead of print.ABSTRACTSignals undergoing chemical or conformational exchange in one-dimensional NMR spectra are often identified by deuterium exchange. In order to obtain quantitative information about the dynamic processes involved, one frequently used method is EXchange SpectroscopY (EXSY). To detect all exchange processes, the EXSY experiment requires the acquisition of time-consuming two-dimensional spectra. Here we report a faster alternative, an experiment which uses spatial encoding to extract similar information in a 1D exchange-edited exper...
Source: Chemphyschem - February 26, 2024 Category: Chemistry Authors: Markus Rotzinger Nathalie Schuster Klaus Zangger Source Type: research
