Pub Date : 2023-11-09DOI: 10.1080/00268976.2023.2279694
Even Xu, Jonathan Tennyson
An exhaustive review of the measured rovibrational transitions of the 16O12C32S isotopologue of carbonyl sulphide is undertaken. A comprehensive analysis of data from 100 papers is carried out using a consistent set of harmonic oscillator quantum numbers which are recommended for future studies. A corrected compilation of 14,071 OCS transitions is then subjected to a Measured Active Rotational-Vibrational Energy Levels (MARVEL) analysis, resulting in 5729 empirical energy levels. The uncertainties corresponding to these levels are analysed using different procedures; the newly implemented bootstrap method is used to provide final uncertainties.
{"title":"Empirical rovibrational energy levels for carbonyl sulphide","authors":"Even Xu, Jonathan Tennyson","doi":"10.1080/00268976.2023.2279694","DOIUrl":"https://doi.org/10.1080/00268976.2023.2279694","url":null,"abstract":"An exhaustive review of the measured rovibrational transitions of the 16O12C32S isotopologue of carbonyl sulphide is undertaken. A comprehensive analysis of data from 100 papers is carried out using a consistent set of harmonic oscillator quantum numbers which are recommended for future studies. A corrected compilation of 14,071 OCS transitions is then subjected to a Measured Active Rotational-Vibrational Energy Levels (MARVEL) analysis, resulting in 5729 empirical energy levels. The uncertainties corresponding to these levels are analysed using different procedures; the newly implemented bootstrap method is used to provide final uncertainties.","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":" 40","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135291166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-08DOI: 10.1080/00268976.2023.2277823
Aysha Bente Akbor, Md. Rafikul Islam, Aboud Ahmed Awadh Bahajjaj, K. M. Anis-Ul-Haque, Md Abdul Goni, Md. Anamul Hoque, D. M. Shafiqul Islam
AbstractHerein, the assessment of interactions between a non-ionic surfactant (NIS) triton X-100 (TNX-100) and a globular protein bovine serum albumin (BSA) was explored through the determination of clouding nature in aqueous solution of sodium salts (Na-salts). Sodium chloride (NaCl), sodium acetate (NaOAc), sodium carbonate (Na2CO3), sodium oxalate (Na2Oxal), sodium sulphate (Na2SO4), and sodium phosphate (Na3PO4) have been chosen to assess their impacts on the clouding nature of TNX-100 + BSA mixture. The estimated cloud point (CP) values were noticed to be lowered with the enhancement of [Na-salts]. The lessening of CP values has been explained by the salting out effect of anions. The calculated standard Gibbs free energy change (ΔGco) was positive at all examined conditions which illustrates the nonspontaneity of phase change. The standard enthalpy (ΔHco) and entropy (ΔSco) changes exhibited negative values at low contents of aq. Na-salts and positive values at high aq. Na-salts content. These consequences illustrate the presence of electrostatic interactions at low Na-salts concentration and hydrophobic interactions at high Na-salts concentration. Furthermore, enthalpy-entropy parameters were successfully computed and explained with proper clarification.KEYWORDS: Triton X-100bovine serum albuminclouding naturethermodynamicssodium salts Disclosure statementNo potential conflict of interest was reported by the authors.Additional informationFundingThis work was funded by the Researchers Supporting Project Number (RSPD2023R763) King Saud University, Riyadh, Saudi Arabia.
摘要本文通过测定钠盐水溶液的混浊性质，探讨了非离子表面活性剂triton X-100 (TNX-100)与球形蛋白牛血清白蛋白(BSA)的相互作用。选择氯化钠(NaCl)、乙酸钠(NaOAc)、碳酸钠(Na2CO3)、草酸钠(Na2Oxal)、硫酸钠(Na2SO4)和磷酸钠(Na3PO4)来评估它们对TNX-100 + BSA混合物云雾性质的影响。估计的浊点(CP)值随着[钠盐]的增强而降低。CP值的降低可以用阴离子的盐析作用来解释。计算得到的标准吉布斯自由能变化(ΔGco)在所有检测条件下均为正，说明相变的非自发性。标准焓(ΔHco)和熵(ΔSco)的变化在aq. na盐含量低时呈负值，在aq. na盐含量高时呈正值。这些结果说明在低钠盐浓度下存在静电相互作用，在高钠盐浓度下存在疏水相互作用。此外，还成功地计算了焓熵参数，并对其进行了适当的解释。关键词:Triton x -100牛血清白蛋白混浊性热力学钠盐披露声明作者未报告潜在利益冲突。本工作由研究人员支持项目号(RSPD2023R763)资助，沙特阿拉伯利雅得沙特国王大学。
{"title":"Phase partitioning nature, interaction forces and thermodynamic parameters of triton X-100 and bovine serum albumin mixture: impacts of the composition of Na-salt","authors":"Aysha Bente Akbor, Md. Rafikul Islam, Aboud Ahmed Awadh Bahajjaj, K. M. Anis-Ul-Haque, Md Abdul Goni, Md. Anamul Hoque, D. M. Shafiqul Islam","doi":"10.1080/00268976.2023.2277823","DOIUrl":"https://doi.org/10.1080/00268976.2023.2277823","url":null,"abstract":"AbstractHerein, the assessment of interactions between a non-ionic surfactant (NIS) triton X-100 (TNX-100) and a globular protein bovine serum albumin (BSA) was explored through the determination of clouding nature in aqueous solution of sodium salts (Na-salts). Sodium chloride (NaCl), sodium acetate (NaOAc), sodium carbonate (Na2CO3), sodium oxalate (Na2Oxal), sodium sulphate (Na2SO4), and sodium phosphate (Na3PO4) have been chosen to assess their impacts on the clouding nature of TNX-100 + BSA mixture. The estimated cloud point (CP) values were noticed to be lowered with the enhancement of [Na-salts]. The lessening of CP values has been explained by the salting out effect of anions. The calculated standard Gibbs free energy change (ΔGco) was positive at all examined conditions which illustrates the nonspontaneity of phase change. The standard enthalpy (ΔHco) and entropy (ΔSco) changes exhibited negative values at low contents of aq. Na-salts and positive values at high aq. Na-salts content. These consequences illustrate the presence of electrostatic interactions at low Na-salts concentration and hydrophobic interactions at high Na-salts concentration. Furthermore, enthalpy-entropy parameters were successfully computed and explained with proper clarification.KEYWORDS: Triton X-100bovine serum albuminclouding naturethermodynamicssodium salts Disclosure statementNo potential conflict of interest was reported by the authors.Additional informationFundingThis work was funded by the Researchers Supporting Project Number (RSPD2023R763) King Saud University, Riyadh, Saudi Arabia.","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"6 9","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135390925","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-08DOI: 10.1080/00268976.2023.2276904
Stephan Mohr, Rémi Pétuya, Ioannis N. Tsimpanogiannis
AbstractWe present a detailed overview of the calculation of the enthalpy of dissociation of structure II pure propane or mixed methane + propane hydrates, focussing primarily on methods that are based on either the Clausius-Clapeyron equation or the direct calculation of the enthalpies of all the components that are involved in the hydrate dissociation reaction. Molecular dynamics simulations are used extensively in order to calculate the enthalpies and molar volumes of water, methane, propane, and the sII mixed hydrate (with variant degree of occupancy) at pressure and temperature conditions along the three-phase (Hydrate–Liquid water–Vapor or Hydrate–Liquid water–Liquid hydrocarbon) equilibrium line.KEYWORDS: Methane +propane hydratesmolecular dynamics simulationsenthalpy of dissociationClausius-Clapeyron AcknowledgmentsWe acknowledge PRACE for awarding us access to JUWELS at GCS@FZJ, Germany.Disclosure statementNo potential conflict of interest was reported by the author(s).
{"title":"Enthalpy of dissociation of the mixed methane + propane sII hydrate along the three-phase equilibrium line","authors":"Stephan Mohr, Rémi Pétuya, Ioannis N. Tsimpanogiannis","doi":"10.1080/00268976.2023.2276904","DOIUrl":"https://doi.org/10.1080/00268976.2023.2276904","url":null,"abstract":"AbstractWe present a detailed overview of the calculation of the enthalpy of dissociation of structure II pure propane or mixed methane + propane hydrates, focussing primarily on methods that are based on either the Clausius-Clapeyron equation or the direct calculation of the enthalpies of all the components that are involved in the hydrate dissociation reaction. Molecular dynamics simulations are used extensively in order to calculate the enthalpies and molar volumes of water, methane, propane, and the sII mixed hydrate (with variant degree of occupancy) at pressure and temperature conditions along the three-phase (Hydrate–Liquid water–Vapor or Hydrate–Liquid water–Liquid hydrocarbon) equilibrium line.KEYWORDS: Methane +propane hydratesmolecular dynamics simulationsenthalpy of dissociationClausius-Clapeyron AcknowledgmentsWe acknowledge PRACE for awarding us access to JUWELS at GCS@FZJ, Germany.Disclosure statementNo potential conflict of interest was reported by the author(s).","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"9 4","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135390139","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-08DOI: 10.1080/00268976.2023.2279261
Sümeyya Serin, Öznur Doğan Ulu
AbstractHerein, the molecular structures of amide ↔ imide tautomers of articaine (ART) were computationally investigated at the DFT/B3LYP/6–311++G (d,p) methodology. Experimental FT-IR and UV-Vis characterisation results of ART were compared with the theoretical results of amide (ART-A) and imide (ART-I) forms. Thermodynamic parameters computed for each phase revealed that the amide tautomer of ART was preferred with energy values in the range of 11.9–13.8 kcal/mol. The modification in surface properties as a function of prototropic tautomerism in the ART molecule was studied by electrostatic surface properties (ESP) analysis. Frontier molecular orbital (FMO), natural bond orbital (NBO), and nonlinear optical (NLO) analyses were performed. It is revealed that energy gap values of the ART-I (4.670–4.738 eV) for each phase are slightly higher than those of the corresponding phases in the ART-A (4.515–4.586 eV). Therefore, it can be concluded that the imide form exhibits lower chemical reactivity compared to the amide form. Regarding NLO characteristics, dipole moment (μtot), mean polarisability (αtot), and mean first-order hyperpolarisability (βtot) values of tautomers have been reported. It was determined that the βtot values computed for ART-A (0.653 × 10−30 esu) and ART-I (0.710 × 10−30 esu) were approximately twice the value of the standard urea.KEYWORDS: Prototropic tautomerismArticaineReactivityDFTNBO analysis AcknowledgementThe numerical calculations reported in this paper were fully performed at TUBITAK ULAKBIM, High Performance and Grid Computing Center (TRUBA resources).Disclosure statementNo potential conflict of interest was reported by the author(s).Data availability statementThe datasets generated during and/or analysed the current study are available from the corresponding author on reasonable request.
{"title":"Vibrational (FT-IR), electronic (UV-Vis), thermodynamic, and NBO analyses of amide ↔ imide forms of articaine: a computational perspective on prototropic tautomerism","authors":"Sümeyya Serin, Öznur Doğan Ulu","doi":"10.1080/00268976.2023.2279261","DOIUrl":"https://doi.org/10.1080/00268976.2023.2279261","url":null,"abstract":"AbstractHerein, the molecular structures of amide ↔ imide tautomers of articaine (ART) were computationally investigated at the DFT/B3LYP/6–311++G (d,p) methodology. Experimental FT-IR and UV-Vis characterisation results of ART were compared with the theoretical results of amide (ART-A) and imide (ART-I) forms. Thermodynamic parameters computed for each phase revealed that the amide tautomer of ART was preferred with energy values in the range of 11.9–13.8 kcal/mol. The modification in surface properties as a function of prototropic tautomerism in the ART molecule was studied by electrostatic surface properties (ESP) analysis. Frontier molecular orbital (FMO), natural bond orbital (NBO), and nonlinear optical (NLO) analyses were performed. It is revealed that energy gap values of the ART-I (4.670–4.738 eV) for each phase are slightly higher than those of the corresponding phases in the ART-A (4.515–4.586 eV). Therefore, it can be concluded that the imide form exhibits lower chemical reactivity compared to the amide form. Regarding NLO characteristics, dipole moment (μtot), mean polarisability (αtot), and mean first-order hyperpolarisability (βtot) values of tautomers have been reported. It was determined that the βtot values computed for ART-A (0.653 × 10−30 esu) and ART-I (0.710 × 10−30 esu) were approximately twice the value of the standard urea.KEYWORDS: Prototropic tautomerismArticaineReactivityDFTNBO analysis AcknowledgementThe numerical calculations reported in this paper were fully performed at TUBITAK ULAKBIM, High Performance and Grid Computing Center (TRUBA resources).Disclosure statementNo potential conflict of interest was reported by the author(s).Data availability statementThe datasets generated during and/or analysed the current study are available from the corresponding author on reasonable request.","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"95 3","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135341890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
AbstractWater in the shale obstructs the enrichment and transportation of shale gas, so it is crucial to identify the occurrence mechanism of water in shale. In this work, molecular dynamics (MD) simulation had been performed to explore the occurrence state, dynamic characteristics, and nuclear magnetic resonance (NMR) relaxation properties of confined water in shale inorganic nanopores (quartz). The results show that the number of adsorbed layers, diffusion coefficients (D) and rotational correlation time (τc) of water in quartz pores are strongly influenced by pore width (H). Layer analysis of water held in confinement indicates that the D value increases and the τc value decreases as the water approaches the centre of the pore. Furthermore, varying occurrence states lead to different NMR relaxation mechanisms. With the increase of H, the transverse relaxation time of adsorbed water is basically stable at 10−1 s. Finally, an exponential formula for evaluating pore size distribution is established. The total thickness of the water layer with the ratio of the intramolecular relaxation rate to the total relaxation rate less than 40% is defined as the thickness of the adsorbed water film.KEYWORDS: Quartz nanopores; confined water; occurrence state; nuclear magnetic resonance AcknowledgementThis research was financially supported by the Natural Science Foundation of Shandong Province (ZR2022MA052), the Independent Innovation Research Program of China University of Petroleum (East China) (22CX03004A), and the National Natural Science Foundation of China (42174142).Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingThis work was supported by National Natural Science Foundation of China: [Grant Number 42174142]; Natural Science Foundation of Shandong Province: [Grant Number ZR2022MA052]; the Independent Innovation Research Program of China University of Petroleum (East China): [Grant Number 22CX03004A].
{"title":"Occurrence state and nuclear magnetic resonance relaxation characteristics of confined water in quartz nanopores","authors":"Qing Sun, Yansong Gu, Zhiyang Xie, Leyang Yu, Xinmin Ge, Wenjing Fang, Bing Liu","doi":"10.1080/00268976.2023.2274964","DOIUrl":"https://doi.org/10.1080/00268976.2023.2274964","url":null,"abstract":"AbstractWater in the shale obstructs the enrichment and transportation of shale gas, so it is crucial to identify the occurrence mechanism of water in shale. In this work, molecular dynamics (MD) simulation had been performed to explore the occurrence state, dynamic characteristics, and nuclear magnetic resonance (NMR) relaxation properties of confined water in shale inorganic nanopores (quartz). The results show that the number of adsorbed layers, diffusion coefficients (D) and rotational correlation time (τc) of water in quartz pores are strongly influenced by pore width (H). Layer analysis of water held in confinement indicates that the D value increases and the τc value decreases as the water approaches the centre of the pore. Furthermore, varying occurrence states lead to different NMR relaxation mechanisms. With the increase of H, the transverse relaxation time of adsorbed water is basically stable at 10−1 s. Finally, an exponential formula for evaluating pore size distribution is established. The total thickness of the water layer with the ratio of the intramolecular relaxation rate to the total relaxation rate less than 40% is defined as the thickness of the adsorbed water film.KEYWORDS: Quartz nanopores; confined water; occurrence state; nuclear magnetic resonance AcknowledgementThis research was financially supported by the Natural Science Foundation of Shandong Province (ZR2022MA052), the Independent Innovation Research Program of China University of Petroleum (East China) (22CX03004A), and the National Natural Science Foundation of China (42174142).Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingThis work was supported by National Natural Science Foundation of China: [Grant Number 42174142]; Natural Science Foundation of Shandong Province: [Grant Number ZR2022MA052]; the Independent Innovation Research Program of China University of Petroleum (East China): [Grant Number 22CX03004A].","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"17 7","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135684525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-03DOI: 10.1080/00268976.2023.2276905
M. C. Shanmukha, K. J. Gowtham, A. Usha, K. Julietraja
AbstractGraph theory plays a crucial role in various applications of mathematics and applied sciences. One specialised branch of graph theory is mathematical chemistry, which focuses on mathematical modelling and analysing chemical compounds and their properties. In this context, graphs are used to represent the structural and topological features of molecules, enabling chemists to gain insights into chemical reactions and make predictions about molecular properties. Recently, new versions of Sombor indices have been introduced using a geometric approach. This article specifically focuses on entropy-based variations of these Sombor indices, which includes SO, SOred, SOavg, mSO, SO3 and SO4, in the context of graphene sheet. Graphene has gained significant attention in the scientific and technological communities due to its exceptional properties. It finds widespread applications in diverse fields such as nanotechnology, electronics, energy storage, sensors, materials science and optoelectronics. Given the promising applications of graphene, it becomes essential to theoretically analyse its structure. Molecular descriptors play a crucial role, as they are strongly linked to various characteristics of chemical compounds. To better understand the Sombor indices, this article graphically represents their entropy measures.Keywords: Chemical graph theorytopological indicesSombor indicesentropy descriptorsgraphene sheet Disclosure statementNo potential conflict of interest was reported by the author(s).
{"title":"Expected values of Sombor indices and their entropy measures for graphene","authors":"M. C. Shanmukha, K. J. Gowtham, A. Usha, K. Julietraja","doi":"10.1080/00268976.2023.2276905","DOIUrl":"https://doi.org/10.1080/00268976.2023.2276905","url":null,"abstract":"AbstractGraph theory plays a crucial role in various applications of mathematics and applied sciences. One specialised branch of graph theory is mathematical chemistry, which focuses on mathematical modelling and analysing chemical compounds and their properties. In this context, graphs are used to represent the structural and topological features of molecules, enabling chemists to gain insights into chemical reactions and make predictions about molecular properties. Recently, new versions of Sombor indices have been introduced using a geometric approach. This article specifically focuses on entropy-based variations of these Sombor indices, which includes SO, SOred, SOavg, mSO, SO3 and SO4, in the context of graphene sheet. Graphene has gained significant attention in the scientific and technological communities due to its exceptional properties. It finds widespread applications in diverse fields such as nanotechnology, electronics, energy storage, sensors, materials science and optoelectronics. Given the promising applications of graphene, it becomes essential to theoretically analyse its structure. Molecular descriptors play a crucial role, as they are strongly linked to various characteristics of chemical compounds. To better understand the Sombor indices, this article graphically represents their entropy measures.Keywords: Chemical graph theorytopological indicesSombor indicesentropy descriptorsgraphene sheet Disclosure statementNo potential conflict of interest was reported by the author(s).","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"13 10","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135818482","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-02DOI: 10.1080/00268976.2023.2274503
Haoyan Zhang, Lin Cheng, Kai Li, Ying Wang, Zhijian Wu
AbstractElectrochemical CO2 reduction reaction (CO2RR) provides a feasible technology for alleviating global warming, energy crisis and sustainable energy production. In this work, CO2RR reaction mechanism on TM-THTA (TM = Fe, Co, Ni, Ru, Rh, Pd, THTA is composed by two types of building blocks of 2,3,6,7,10,11-triphenylenehexathiol and 2,3,6,7,10,11-triphenylenehexamine) has been studied by using density functional method. Our study showed that the studied catalysts are stable both thermodynamically and electrochemically. Rh-THTA is a good CO2 reduction catalyst in producing CH4. Pd-THTA is a potential CO2 reduction catalyst in producing HCOOH. Solvent effect plays important role in reaction mechanism. The strong hydrogen evolution reaction in Rh-THTA and Pd-THTA can be refrained by adjusting the pH values of electrolyte. We hope this study could provide a useful way to develop 2D-MOF-based CO2RR electrocatalysts.KEYWORDS: CO2 reduction; two-dimensional metal-organic frameworks; density functional study; reaction mechanism Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingThis work is supported by The National Natural Science Foundation of China (21963009 and 22373097), The Program for Innovative Research Program of Science and Technology at Universities of Inner Mongolia Autonomous Region Team in Universities of Inner Mongolia Autonomous Region (NMGIRT2214), The Local Scientific and Technological Development Plan guided by the Central Government (2021ZY0025), The Grassland Talents Engineering of Inner Mongolia and The Light of West China Program by Chinese Academy of Sciences. The computational time is supported by the computing centre of Changchun Institute of Applied Chemistry.
{"title":"CO <sub>2</sub> Electrochemical reduction on the two dimensional transition metal coordinated by 2,3,6,7,10,11-triphenylenehexathiol and 2,3,6,7,10,11-triphenylenehexamine, a computational survey","authors":"Haoyan Zhang, Lin Cheng, Kai Li, Ying Wang, Zhijian Wu","doi":"10.1080/00268976.2023.2274503","DOIUrl":"https://doi.org/10.1080/00268976.2023.2274503","url":null,"abstract":"AbstractElectrochemical CO2 reduction reaction (CO2RR) provides a feasible technology for alleviating global warming, energy crisis and sustainable energy production. In this work, CO2RR reaction mechanism on TM-THTA (TM = Fe, Co, Ni, Ru, Rh, Pd, THTA is composed by two types of building blocks of 2,3,6,7,10,11-triphenylenehexathiol and 2,3,6,7,10,11-triphenylenehexamine) has been studied by using density functional method. Our study showed that the studied catalysts are stable both thermodynamically and electrochemically. Rh-THTA is a good CO2 reduction catalyst in producing CH4. Pd-THTA is a potential CO2 reduction catalyst in producing HCOOH. Solvent effect plays important role in reaction mechanism. The strong hydrogen evolution reaction in Rh-THTA and Pd-THTA can be refrained by adjusting the pH values of electrolyte. We hope this study could provide a useful way to develop 2D-MOF-based CO2RR electrocatalysts.KEYWORDS: CO2 reduction; two-dimensional metal-organic frameworks; density functional study; reaction mechanism Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingThis work is supported by The National Natural Science Foundation of China (21963009 and 22373097), The Program for Innovative Research Program of Science and Technology at Universities of Inner Mongolia Autonomous Region Team in Universities of Inner Mongolia Autonomous Region (NMGIRT2214), The Local Scientific and Technological Development Plan guided by the Central Government (2021ZY0025), The Grassland Talents Engineering of Inner Mongolia and The Light of West China Program by Chinese Academy of Sciences. The computational time is supported by the computing centre of Changchun Institute of Applied Chemistry.","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"9 24","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135973525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-02DOI: 10.1080/00268976.2023.2276912
Jonathan Tennyson
The carbon trimer, C3 also known as propadienediylidene, is a quasi-linear molecule with an unusual electronic structure and a very flat bending potential in its ground electronic state. C3 is an important species in astrophysics and carbon plasmas. Observed transition wavenumbers within and between the X~1Σg+ and A~1Πu states of C3 are extracted from 21 papers and then subjected to a Measured Active Rotational-Vibrational Energy Levels (MARVEL) analysis: a corrected list of 4940 transitions are inverted to yield 1887 empirical energy levels. Uncertainties for these levels are determined using a newly implemented bootstrap method. These levels will provide input for developing a full spectroscopic model for C3 which can used to generate a line list for the X~1Σg+ and A~1Πu states.
{"title":"Empirical rovibronic energy levels of C <sub>3</sub>","authors":"Jonathan Tennyson","doi":"10.1080/00268976.2023.2276912","DOIUrl":"https://doi.org/10.1080/00268976.2023.2276912","url":null,"abstract":"The carbon trimer, C3 also known as propadienediylidene, is a quasi-linear molecule with an unusual electronic structure and a very flat bending potential in its ground electronic state. C3 is an important species in astrophysics and carbon plasmas. Observed transition wavenumbers within and between the X~1Σg+ and A~1Πu states of C3 are extracted from 21 papers and then subjected to a Measured Active Rotational-Vibrational Energy Levels (MARVEL) analysis: a corrected list of 4940 transitions are inverted to yield 1887 empirical energy levels. Uncertainties for these levels are determined using a newly implemented bootstrap method. These levels will provide input for developing a full spectroscopic model for C3 which can used to generate a line list for the X~1Σg+ and A~1Πu states.","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"95 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135934670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-02DOI: 10.1080/00268976.2023.2276903
A. de J. Ríos-Roldán, J. A. Munguía-Valadez, E. J. Sambriski, J. A. Moreno-Razo
AbstractA coarser model for the Gay-Berne mesogen is developed using the interaction potential from the Approximate Non-Conformal (ANC) theory. The ANC potential contains both repulsive and attractive contributions. We modify intermolecular attractions by conditioning them with a Hess-Su orientation-dependent term. This imparts an anisotropic contribution to the energy of the system. The softness parameter s of the ANC potential is probed to qualitatively identify a threshold capable of sustaining a nematic phase. We construct phase diagrams for each value of s from molecular dynamics simulations and characterise bulk samples to outline phase regions. We find that a softness parameter s∼0.6 or higher supports the emergence of a nematic phase. The stability of the nematic region is enhanced as s→1, corresponding to the conventional Lennard-Jones interaction. The stability of the nematic phase for nearly-spherical mesogens with increasing s leads to a gradual loss in spherical symmetry despite no imposed shape anisotropy. Thus, the energy anisotropy becomes more pronounced and is capable of prompting the emergence of the nematic phase in this model.Keywords: Phase diagramsnematicmesogenanisotropyliquid crystals AcknowledgmentsJAMR gratefully acknowledges the support provided through grants UNAM-DGAPA-PAPIIT IN114721, LANCAD-UNAM-DGTIC-276, and LANCAD-UNAM-DGTIC-247, in addition to the generous computing time provided by the Laboratorio de Supercómputo y Visualización en Paralelo at UAMI (LSVP-UAMI).Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingJMV and AJRR are thankful for the financial support received through a CONACYT graduate fellowship (No. 947695 and 1234731).
摘要利用近似非共形(ANC)理论中的相互作用势，建立了一个较为粗糙的Gay-Berne介圈模型。非国大的潜力既有令人反感的贡献，也有吸引人的贡献。我们修改分子间的吸引力，通过调节他们与Hess-Su取向相关的项。这使得系统的能量具有各向异性。探讨了ANC电位的柔软参数s，以定性地确定能够维持向列相的阈值。我们从分子动力学模拟中为每个s值构建相图，并对大块样品进行表征以勾勒相区域。我们发现柔软度参数s ~ 0.6或更高支持向列相的出现。向列区域的稳定性随着s→1而增强，与传统的Lennard-Jones相互作用相对应。随着s的增加，向列相的稳定性导致球面对称性的逐渐丧失，尽管没有施加形状各向异性。因此，能量各向异性变得更加明显，并且能够促使该模型中向列相的出现。jamr感谢通过赠款UNAM-DGAPA-PAPIIT IN114721, LANCAD-UNAM-DGTIC-276和LANCAD-UNAM-DGTIC-247提供的支持，以及UAMI (LSVP-UAMI)平行实验室Supercómputo y Visualización提供的慷慨计算时间。披露声明作者未报告潜在的利益冲突。jmv和AJRR感谢通过CONACYT研究生奖学金(No. 947695和1234731)获得的财政支持。
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Pub Date : 2023-11-01DOI: 10.1080/00268976.2023.2276906
Uriel Villanueva-Alcalá, José R. Nicolás-Carlock, Denis Boyer
AbstractModels of fractal growth commonly consider particles diffusing in a medium and that stick irreversibly to the forming aggregate when making contact for the first time. As shown by the well-known diffusion limited aggregation (DLA) model and its generalisations, the fractal dimension is sensitive to the nature of the stochastic motion of the particles. Here, we study the structures formed by finite-lived Brownian particles, i.e. particles constrained to find the aggregate within a prescribed time, and which are removed otherwise. This motion can be modelled by diffusion with stochastic resetting, a class of processes which has been widely studied in recent years. In the short lifetime limit, a very small fraction of the particles manage to reach the aggregate. Hence, growth is controlled by atypical Brownian trajectories, that move nearly in straight line according to a large deviation principle. In d dimensions, the resulting fractal dimension of the aggregate decreases from the DLA value and tends to 1, instead of increasing to d as expected from ballistic aggregation. In the zero lifetime limit one recovers the non-trivial model of ‘aggregation by the tips’ proposed long ago by R. Jullien [J. Phys. A: Math. Gen. 19, 2129 (1986)].KEYWORDS: Brownian motionresetting processesdiffusion limited aggregationlarge deviationsgeometrical optics Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingWe thank Carlos E. López Natarén for technical computer support. We acknowledge support from Consejo Nacional de Ciencia y Tecnología (Ciencia de Frontera 2019 (CONACYT)) [grant number 263958].
分形生长模型通常考虑颗粒在介质中扩散，并且在第一次接触时不可逆地粘在形成的聚集体上。众所周知的扩散有限聚集(DLA)模型及其推广表明，分形维数对粒子随机运动的性质很敏感。在这里，我们研究了由有限寿命布朗粒子形成的结构，即在规定时间内找到聚集体的粒子，否则就会被移除。这种运动可以用带有随机重置的扩散来模拟，这是近年来被广泛研究的一类过程。在较短的寿命极限内，只有极小部分的颗粒能够到达聚集体。因此，增长是由非典型布朗轨迹控制的，这种轨迹根据大偏差原理几乎是直线运动的。在d维中，聚合体的分形维数从DLA值开始下降，并趋于1，而不是像弹道聚集所期望的那样增加到d。在零寿命极限下，人们恢复了R. Jullien很久以前提出的“尖端聚合”的非平凡模型[J]。理论物理。答:数学。创19,2129(1986)]。关键词:布朗运动重置过程扩散有限聚集大偏差几何光学披露声明作者未报告潜在的利益冲突。我们感谢Carlos E. López natar文职人员提供的计算机技术支持。我们感谢国家科学委员会通过Tecnología(科学前沿2019 (CONACYT))[批准号263958]的支持。
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