Pub Date : 2024-10-18DOI: 10.1016/j.chemphys.2024.112486
Ilia Grishin
The present study explores the mechanochemical synthesis of porous silicon oxycarbide composites using commercial activated carbon and hydrated silica as precursors without additional functionalization, aiming to be used as effective adsorbents for carbon dioxide removal from gas streams. By adjusting the hydrated silica/activated carbon mass ratio, a set of materials were prepared with varying surface areas (256–662 m2/g), pore volumes (0.28–0.45 cm3/g), and surface functional groups concentrations (0.824–0.996 mmol/g). The optimal silicon oxycarbide composite (hydrated silica/activated carbon mass ratio of 1.5) demonstrated the CO2 adsorption capacity of 3.41 mmol/g at 25 °C and 1 bar, which can be attributed to the composite’s well-developed porosity and high surface functionality. In addition, the adsorbent exhibited high CO2/N2 selectivity of 15.2 along with stable cycling performance. These findings indicate that mechanochemically synthesized silicon oxycarbide composites have a considerable potential in the field of CO2 capture.
本研究探讨了以商用活性炭和水合二氧化硅为前驱体，在不进行额外功能化的情况下，机械化学合成多孔碳氧硅复合材料的方法，旨在将其用作去除气流中二氧化碳的有效吸附剂。通过调整水合二氧化硅/活性炭的质量比，制备出了一组具有不同表面积（256-662 m2/g）、孔体积（0.28-0.45 cm3/g）和表面官能团浓度（0.824-0.996 mmol/g）的材料。最佳碳氧硅复合材料（水合二氧化硅/活性炭质量比为 1.5）在 25 °C 和 1 bar 条件下的二氧化碳吸附容量为 3.41 mmol/g，这归功于复合材料发达的孔隙率和高表面官能团。此外，该吸附剂还具有 15.2 的 CO2/N2 高选择性和稳定的循环性能。这些研究结果表明，机械化学合成的氧碳化硅复合材料在二氧化碳捕集领域具有相当大的潜力。
{"title":"Adsorption of CO2 on mechanochemically synthesized silicon oxycarbide composites","authors":"Ilia Grishin","doi":"10.1016/j.chemphys.2024.112486","DOIUrl":"10.1016/j.chemphys.2024.112486","url":null,"abstract":"<div><div>The present study explores the mechanochemical synthesis of porous silicon oxycarbide composites using commercial activated carbon and hydrated silica as precursors without additional functionalization, aiming to be used as effective adsorbents for carbon dioxide removal from gas streams. By adjusting the hydrated silica/activated carbon mass ratio, a set of materials were prepared with varying surface areas (256–662 m<sup>2</sup>/g), pore volumes (0.28–0.45 cm<sup>3</sup>/g), and surface functional groups concentrations (0.824–0.996 mmol/g). The optimal silicon oxycarbide composite (hydrated silica/activated carbon mass ratio of 1.5) demonstrated the CO<sub>2</sub> adsorption capacity of 3.41 mmol/g at 25 °C and 1 bar, which can be attributed to the composite’s well-developed porosity and high surface functionality. In addition, the adsorbent exhibited high CO<sub>2</sub>/N<sub>2</sub> selectivity of 15.2 along with stable cycling performance. These findings indicate that mechanochemically synthesized silicon oxycarbide composites have a considerable potential in the field of CO<sub>2</sub> capture.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"588 ","pages":"Article 112486"},"PeriodicalIF":2.0,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529808","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1016/j.chemphys.2024.112489
K. Ma , Z.B. Chen
This manuscript is devoted to explore the atomic structure and electron impact excitation process of atom impurities in quantum dots. To achieve this goal, a method that solves the fully relativistic Dirac equation within the framework of relativistic configuration interaction is proposed. The Gaussian potential is used, which can accurately describe the location of impurities in quantum dots and their local effects on the surrounding electron cloud. The coupled Dirac equation is modified to include a new central potential, providing solutions that include both the continuous and bound state wave functions. The process of electron impact excitation is elucidated using the distorted wave method, all within the framework of relativistic Dirac theory. For illustrative purposes, a detailed investigation of the excitation energies, transition rates, wave functions, and excitation cross sections is carried out for a wide range of confinement strengths of the potential and quantum dot radii, using the helium impurities in spherical quantum dots as an example. Our results reveal that for a given confinement strength of the potential, the bound state wave functions are initially pulled into the inner region by the attractive Gaussian potential well, but eventually reflect the free atom scenario at large quantum dot radii. In contrast, the continuous electron wave functions exhibit monotonic variations as a function of the quantum dot radii. Such behavior of the wave functions gives rise to distinctive phenomena in the variation of excitation energies, transition rates, and excitation cross sections in relation to the potential parameters. Good agreement between the present results and existing data, where available, is obtained. This work holds importance not only for basic research in atomic physics but also for the optical and electronic applications of quantum dots. I.e., in the design and optimization of quantum dot lasers and quantum dot sensors.
{"title":"Study of the electronic structure and electron impact excitation cross section of helium impurities in spherical quantum dots","authors":"K. Ma , Z.B. Chen","doi":"10.1016/j.chemphys.2024.112489","DOIUrl":"10.1016/j.chemphys.2024.112489","url":null,"abstract":"<div><div>This manuscript is devoted to explore the atomic structure and electron impact excitation process of atom impurities in quantum dots. To achieve this goal, a method that solves the fully relativistic Dirac equation within the framework of relativistic configuration interaction is proposed. The Gaussian potential is used, which can accurately describe the location of impurities in quantum dots and their local effects on the surrounding electron cloud. The coupled Dirac equation is modified to include a new central potential, providing solutions that include both the continuous and bound state wave functions. The process of electron impact excitation is elucidated using the distorted wave method, all within the framework of relativistic Dirac theory. For illustrative purposes, a detailed investigation of the excitation energies, transition rates, wave functions, and excitation cross sections is carried out for a wide range of confinement strengths of the potential and quantum dot radii, using the helium impurities in spherical quantum dots as an example. Our results reveal that for a given confinement strength of the potential, the bound state wave functions are initially pulled into the inner region by the attractive Gaussian potential well, but eventually reflect the free atom scenario at large quantum dot radii. In contrast, the continuous electron wave functions exhibit monotonic variations as a function of the quantum dot radii. Such behavior of the wave functions gives rise to distinctive phenomena in the variation of excitation energies, transition rates, and excitation cross sections in relation to the potential parameters. Good agreement between the present results and existing data, where available, is obtained. This work holds importance not only for basic research in atomic physics but also for the optical and electronic applications of quantum dots. I.e., in the design and optimization of quantum dot lasers and quantum dot sensors.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"588 ","pages":"Article 112489"},"PeriodicalIF":2.0,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529807","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1016/j.chemphys.2024.112477
B. Arunkumar, M. Jothibas
The comparative studies of pure and different doping materials of α-XFe2O3 (X = Co, Mn, Ni and Zn) nanoparticles in Structural, Morphological, Optical, and magnetic behavior were analyzed in this article. The synthesis of α-XFe2O3 nanoparticles through the Sol-gel method for magnetic properties with various doping materials such as Co, Mn, Ni, and Zn. The structural, morphological, optical, and magnetic properties were carefully examined, revealing enhanced characteristics. XRD studies confirmed the successful incorporation of dopants into the crystal structure of α-Fe2O3, while Morphological analysis through SEM images indicated superparamagnetic properties in Co and Zn doped samples, and ferrite behavior in Mn and Ni doped samples. UV Spectra analysis showed optical transitional changes related to magnetic behavior, and the dielectric effect was attributed to the presence of multiple domains within the sample. The study effectively demonstrated the unique magnetic properties of pure and α-XFe2O3 nanoparticles, highlighting the importance of different doping materials in influencing their characteristics.
本文分析了纯α-XFe2O3（X = Co、Mn、Ni 和 Zn）纳米粒子和不同掺杂材料在结构、形态、光学和磁学行为方面的比较研究。通过溶胶-凝胶法合成了α-XFe2O3纳米粒子，并掺杂了不同的磁性材料，如Co、Mn、Ni和Zn。对这些纳米粒子的结构、形态、光学和磁学特性进行了仔细研究，结果表明它们具有更强的特性。XRD 研究证实掺杂剂成功地掺入了 α-Fe2O3 的晶体结构中，而通过 SEM 图像进行的形态分析表明，掺杂 Co 和 Zn 的样品具有超顺磁性，而掺杂 Mn 和 Ni 的样品则具有铁氧体特性。紫外光谱分析显示了与磁性行为相关的光学过渡变化，而介电效应则归因于样品中存在多个畴。该研究有效地证明了纯纳米颗粒和 α-XFe2O3 纳米颗粒的独特磁特性，突出了不同掺杂材料对其特性影响的重要性。
{"title":"Exploring different dopant materials in conjunction with iron oxide and analyzing their characterization and magnetic properties","authors":"B. Arunkumar, M. Jothibas","doi":"10.1016/j.chemphys.2024.112477","DOIUrl":"10.1016/j.chemphys.2024.112477","url":null,"abstract":"<div><div>The comparative studies of pure and different doping materials of α-XFe<sub>2</sub>O<sub>3</sub> (X = Co, Mn, Ni and Zn) nanoparticles in Structural, Morphological, Optical, and magnetic behavior were analyzed in this article. The synthesis of α-XFe<sub>2</sub>O<sub>3</sub> nanoparticles through the Sol-gel method for magnetic properties with various doping materials such as Co, Mn, Ni, and Zn. The structural, morphological, optical, and magnetic properties were carefully examined, revealing enhanced characteristics. XRD studies confirmed the successful incorporation of dopants into the crystal structure of α-Fe<sub>2</sub>O<sub>3</sub>, while Morphological analysis through SEM images indicated superparamagnetic properties in Co and Zn doped samples, and ferrite behavior in Mn and Ni doped samples. UV Spectra analysis showed optical transitional changes related to magnetic behavior, and the dielectric effect was attributed to the presence of multiple domains within the sample. The study effectively demonstrated the unique magnetic properties of pure and α-XFe<sub>2</sub>O<sub>3</sub> nanoparticles, highlighting the importance of different doping materials in influencing their characteristics.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"588 ","pages":"Article 112477"},"PeriodicalIF":2.0,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142446160","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-15DOI: 10.1016/j.chemphys.2024.112480
A.V. Nikitin , A.E. Protasevich , M. Rey , Vl.G. Tyuterev
Potential energy surfaces (PES) of methane which are constructed using ten symmetrised combinations of four bond length and six interbond angles are referred to as (10S) PESs. At high energy ranges, it was found that (10S) PESs permitted improving by factor of five the fit quality of ab initio electronic energies of methane versus standard nine symmetric coordinates (9S) PES representations both in internal, orthogonal or normal-mode coordinates. We extend predictions of vibrational band origins to spectral range above 10,000 cm−1 to help future analyses of experimental spectra. The accuracy at high energies is increased without notable deterioration at low-E levels (rms deviation of 0.26 cm−1). Based on a comparison between various variants of (10S) PESs we expect that new theoretical band origins should have the accuracy not worse than 1–3 cm−1 up to 13,400 cm−1.
利用四个键长和六个键间角的十个对称组合构建的甲烷势能面（PES）被称为（10S）PES。研究发现，在高能量范围内，(10S) PES 与标准九对称坐标 (9S) PES 相比，在内部、正交或常模坐标下，甲烷的 ab initio 电子能量拟合质量提高了五倍。我们将振动频带起源的预测扩展到 10,000 cm-1 以上的光谱范围，以帮助未来的实验光谱分析。高能量下的准确性得到了提高，而低能量下的准确性却没有明显下降（均方根偏差为 0.26 cm-1）。根据 (10S) PES 各种变体之间的比较，我们预计新的理论谱带起源在 13,400 cm-1 以下的精确度应不低于 1-3 cm-1。
{"title":"Extending the functional form of the methane PES in redundant coordinates for highly excited vibrational energy levels calculation","authors":"A.V. Nikitin , A.E. Protasevich , M. Rey , Vl.G. Tyuterev","doi":"10.1016/j.chemphys.2024.112480","DOIUrl":"10.1016/j.chemphys.2024.112480","url":null,"abstract":"<div><div>Potential energy surfaces (PES) of methane<!--> <!-->which are constructed using ten symmetrised combinations of four bond length and six interbond angles are referred to as (10S) PESs. At high energy ranges, it was found that (10S) PESs permitted improving by factor of five the fit quality of <em>ab initio</em> electronic energies of methane versus standard nine symmetric coordinates (9S) PES representations both in internal, orthogonal or normal-mode coordinates. We extend predictions of vibrational band origins to spectral range above 10,000 cm<sup>−1</sup> to help future analyses of experimental spectra. The accuracy at high energies is increased without notable deterioration at low-E levels (<em>rms</em> deviation of 0.26 cm<sup>−1</sup>). Based on a comparison between various variants of (10S) PESs we expect that new theoretical band origins should have the accuracy not worse than 1–3 cm<sup>−1</sup> up to 13,400 cm<sup>−1</sup>.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"589 ","pages":"Article 112480"},"PeriodicalIF":2.0,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560899","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-15DOI: 10.1016/j.chemphys.2024.112481
Jiantao Yin , Yipeng Chen , Yanhui Liu , Damao Xun , Wenjun Zong , Huanhuan Qiu , Rongri Tan
The detection of indoor hazardous gases poses significant complexity and challenges. Based on first-principles theoretical calculations, Y-adsorbed MoS (Y-MoS) monolayer is selected to investigate its adsorption, magnetism and sensitivity to NH, HCHO and CH gas molecules. The presence of Y atom profoundly alters the electronic and magnetic properties of MoS while enhancing its gas adsorption capability. The adsorption capacity of Y-MoS monolayer for these indoor hazardous gases follows the order: HCHO CH NH. Notably, at temperatures around 500 K, the Y-MoS monolayer exhibits potential as a sensor material for NH based on an analysis of recovery performance in the adsorption system. Although the Y-MoS monolayer is not suitable for gas sensing applications with regards to HCHO and CH, it can be effectively employed as a gas cleansing substance. These findings provide valuable insights into detecting indoor hazardous gases and contribute to our understanding of the gas sensing mechanisms exhibited by MoS materials.
{"title":"Adsorption of NH 3, HCHO and C6H6 onto Y-modified MoS2 monolayer : A DFT study","authors":"Jiantao Yin , Yipeng Chen , Yanhui Liu , Damao Xun , Wenjun Zong , Huanhuan Qiu , Rongri Tan","doi":"10.1016/j.chemphys.2024.112481","DOIUrl":"10.1016/j.chemphys.2024.112481","url":null,"abstract":"<div><div>The detection of indoor hazardous gases poses significant complexity and challenges. Based on first-principles theoretical calculations, Y-adsorbed MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> (Y-MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>) monolayer is selected to investigate its adsorption, magnetism and sensitivity to NH<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>, HCHO and C<span><math><msub><mrow></mrow><mrow><mn>6</mn></mrow></msub></math></span>H<span><math><msub><mrow></mrow><mrow><mn>6</mn></mrow></msub></math></span> gas molecules. The presence of Y atom profoundly alters the electronic and magnetic properties of MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> while enhancing its gas adsorption capability. The adsorption capacity of Y-MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> monolayer for these indoor hazardous gases follows the order: HCHO <span><math><mo>></mo></math></span> C<span><math><msub><mrow></mrow><mrow><mn>6</mn></mrow></msub></math></span>H<span><math><msub><mrow></mrow><mrow><mn>6</mn></mrow></msub></math></span> <span><math><mo>></mo></math></span> NH<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>. Notably, at temperatures around 500 K, the Y-MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> monolayer exhibits potential as a sensor material for NH<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span> based on an analysis of recovery performance in the adsorption system. Although the Y-MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> monolayer is not suitable for gas sensing applications with regards to HCHO and C<span><math><msub><mrow></mrow><mrow><mn>6</mn></mrow></msub></math></span>H<span><math><msub><mrow></mrow><mrow><mn>6</mn></mrow></msub></math></span>, it can be effectively employed as a gas cleansing substance. These findings provide valuable insights into detecting indoor hazardous gases and contribute to our understanding of the gas sensing mechanisms exhibited by MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> materials.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"588 ","pages":"Article 112481"},"PeriodicalIF":2.0,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-15DOI: 10.1016/j.chemphys.2024.112483
Plinio Cantero-López , Julio Sánchez , Manuel S. Páez Meza , C.A. García-Negrete , Daniel Bustos , Osvaldo Yáñez
Host- guest complexes are commonly found in several disciplines such as biochemistry, cosmetics, food, pharmaceuticals, and the environment. Studying the relationships between host and guest is essential in this context to understand their physicochemical behavior. This study aimed to examine the intermolecular interactions of cyclic alcohols within β-cyclodextrin (β-CD). The experimental spectroscopic results demonstrated the formation of the studied complexes. In this work, two orientations were used: orientation A (hydroxyl group toward the primary hydroxyl of β-CD) and orientation B (hydroxyl group toward the secondary hydroxyl of β-CD). The results indicate that regardless of the orientation used, the profile energy is thermodynamically favorable. However, there are differences in terms of greater or less stability in terms of the thermodynamic parameters studied. Physicochemical properties demonstrate that the host–guest complex forms spontaneously, and exothermic mode. The interaction between cyclic alcohols and β-CD in orientation A promotes a more pronounced deformation of the secondary edge of β-CD. Moreover, the arrangement of molecules demonstrates that intramolecular hydrogen bonds are less stable between the glycosidic units of β-CD. This arrangement may help or hinder the development of intermolecular hydrogen bonds.
{"title":"Nature of host–guest interaction of cyclic alcohols in β-Cyclodextrin: A molecular view of its structural features","authors":"Plinio Cantero-López , Julio Sánchez , Manuel S. Páez Meza , C.A. García-Negrete , Daniel Bustos , Osvaldo Yáñez","doi":"10.1016/j.chemphys.2024.112483","DOIUrl":"10.1016/j.chemphys.2024.112483","url":null,"abstract":"<div><div>Host- guest complexes are commonly found in several disciplines such as biochemistry, cosmetics, food, pharmaceuticals, and the environment. Studying the relationships between host and guest is essential in this context to understand their physicochemical behavior. This study aimed to examine the intermolecular interactions of cyclic alcohols within β-cyclodextrin (β-CD). The experimental spectroscopic results demonstrated the formation of the studied complexes. In this work, two orientations were used: orientation A (hydroxyl group toward the primary hydroxyl of β-CD) and orientation B (hydroxyl group toward the secondary hydroxyl of β-CD). The results indicate that regardless of the orientation used, the profile energy is thermodynamically favorable. However, there are differences in terms of greater or less stability in terms of the thermodynamic parameters studied. Physicochemical properties demonstrate that the host–guest complex forms spontaneously, and exothermic mode. The interaction between cyclic alcohols and β-CD in orientation A promotes a more pronounced deformation of the secondary edge of β-CD. Moreover, the arrangement of molecules<!--> <!-->demonstrates that intramolecular hydrogen bonds are less stable between the glycosidic units of β-CD. This arrangement may help or hinder the development of intermolecular hydrogen bonds.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"588 ","pages":"Article 112483"},"PeriodicalIF":2.0,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142442067","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-14DOI: 10.1016/j.chemphys.2024.112492
Nayana Sut , Priyanga Manjuri Bhuyan , Swapnali Hazarika , Brajendra K. Sharma , Jaemin Kim , Parikshit Gogoi
MIL-53(Fe), a metal–organic framework (MOF), is capable of degrading harmful organic contaminants, but it has relatively low Fenton catalytic efficiency. To enhance the degradation performance of MIL-53(Fe), we synthesized MIL-53(Fe)-MKL by incorporating modified kraft lignin (MKL) into pristine MIL-53(Fe). The as-prepared composite demonstrated Fenton activity, degrading 97 % of methylene blue (MB) within 50 min. Compared to pristine MIL-53(Fe) (which achieved 62.4 % MB degradation), the MIL-53(Fe)-MKL composite showed a 34.6 % improvement in MB degradation under identical reaction conditions. The incorporated MKL promotes Fe2+ regeneration from Fe3+ in the Fenton process, activating H2O2 to produce OH radicals, which were identified through scavenging experiments and chemical dosimetry with ESR analysis. The MIL-53(Fe)-MKL composite was reused for at least five cycles without a significant decrease in catalytic efficiency. This reported catalyst takes advantage of both MKL and MIL-53(Fe) to enhance catalytic activity, providing a basis for developing innovative catalysts for organic pollutant degradation.
{"title":"Enhanced dye degradation using MIL-53(Fe)-Modified kraft lignin as a heterogeneous Fenton catalyst","authors":"Nayana Sut , Priyanga Manjuri Bhuyan , Swapnali Hazarika , Brajendra K. Sharma , Jaemin Kim , Parikshit Gogoi","doi":"10.1016/j.chemphys.2024.112492","DOIUrl":"10.1016/j.chemphys.2024.112492","url":null,"abstract":"<div><div>MIL-53(Fe), a metal–organic framework (MOF), is capable of degrading harmful organic contaminants, but it has relatively low Fenton catalytic efficiency. To enhance the degradation performance of MIL-53(Fe), we synthesized MIL-53(Fe)-MKL by incorporating modified kraft lignin (MKL) into pristine MIL-53(Fe). The as-prepared composite demonstrated Fenton activity, degrading 97 % of methylene blue (MB) within 50 min. Compared to pristine MIL-53(Fe) (which achieved 62.4 % MB degradation), the MIL-53(Fe)-MKL composite showed a 34.6 % improvement in MB degradation under identical reaction conditions. The incorporated MKL promotes Fe<sup>2+</sup> regeneration from Fe<sup>3+</sup> in the Fenton process, activating H<sub>2</sub>O<sub>2</sub> to produce <img>OH radicals, which were identified through scavenging experiments and chemical dosimetry with ESR analysis. The MIL-53(Fe)-MKL composite was reused for at least five cycles without a significant decrease in catalytic efficiency. This reported catalyst takes advantage of both MKL and MIL-53(Fe) to enhance catalytic activity, providing a basis for developing innovative catalysts for organic pollutant degradation.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"588 ","pages":"Article 112492"},"PeriodicalIF":2.0,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142442064","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This paper discusses the adsorption of metal single-atoms (SAs) on graphitic C3N4 (gCN) multilayered surface models based on density functional theory (DFT) calculations. We systematically searched stable adsorption sites on gCN and showed that the cavity site is preferred for metal SAs. We also discussed the usefulness of several descriptors, such as the distance between the SA and gCN, charge donation (electron transfer), and atomic radius, for evaluating the SA adsorption energy, based on the linear regression method. In addition, the most stable adsorption energy for fifth- and sixth-row metals can be predicted using only the “group” descriptor of the periodic table. The group descriptor is closely related to the atomic radius, and hence the stability of fifth- and sixth-row metals is determined from the fit between the SA radius and the gCN cavity size. The study findings facilitate the development of various metal-dopant techniques for gCN-based applications.
本文基于密度泛函理论（DFT）计算，讨论了金属单原子（SA）在石墨化 C3N4（gCN）多层表面模型上的吸附。我们系统地搜索了 gCN 上的稳定吸附位点，结果表明空腔位点是金属 SA 的首选吸附位点。我们还基于线性回归方法，讨论了 SA 与 gCN 之间的距离、电荷捐赠（电子转移）和原子半径等几个描述因子对评估 SA 吸附能的作用。此外，仅使用元素周期表中的 "基团 "描述符就能预测第五排和第六排金属最稳定的吸附能。基团描述符与原子半径密切相关，因此第五排和第六排金属的稳定性是通过 SA 半径与 gCN 空腔尺寸之间的拟合来确定的。研究结果有助于开发各种基于 gCN 应用的金属掺杂技术。
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Pub Date : 2024-10-12DOI: 10.1016/j.chemphys.2024.112482
Mahmoud A.S. Sakr , Hazem Abdelsalam , Omar H. Abd-Elkader , Ghada M. Abdelrazek , Nahed H. Teleb , Qinfang Zhang
This research explores the structural, electronic, optical, and hydrogen storage properties of borophene nanoribbons (BNRs) with armchair (ANR-B-H) and zigzag (ZNR B-H) edges. Computational simulations optimized these structures, revealing that 7ZNR-B-H has a superior binding energy. Chemical modifications, such as fluorine passivation and functionalization, influenced bond parameters and quantum properties. Bilayer BNRs showed increased stability and enhanced electrical conductivity. Our study demonstrated promising hydrogen storage capabilities, with passivated and functionalized BNRs achieving suitable adsorption energies and a significant gravimetric storage capacity of 20.32 wt%, exceeding DOE standards. NH2 functionalization notably improved adsorption energy, enhancing potential for efficient hydrogen storage. Changes in absorption spectra post-H2 adsorption further highlight BNRs’ potential for hydrogen storage applications. These findings provide valuable insights into BNRs, paving the way for their use in electronic devices and hydrogen storage systems.
{"title":"Unlocking the potential of borophene nanoribbons for efficient hydrogen storage","authors":"Mahmoud A.S. Sakr , Hazem Abdelsalam , Omar H. Abd-Elkader , Ghada M. Abdelrazek , Nahed H. Teleb , Qinfang Zhang","doi":"10.1016/j.chemphys.2024.112482","DOIUrl":"10.1016/j.chemphys.2024.112482","url":null,"abstract":"<div><div>This research explores the structural, electronic, optical, and hydrogen storage properties of borophene nanoribbons (BNRs) with armchair (ANR-B-H) and zigzag (ZNR B-H) edges. Computational simulations optimized these structures, revealing that 7ZNR-B-H has a superior binding energy. Chemical modifications, such as fluorine passivation and functionalization, influenced bond parameters and quantum properties. Bilayer BNRs showed increased stability and enhanced electrical conductivity. Our study demonstrated promising hydrogen storage capabilities, with passivated and functionalized BNRs achieving suitable adsorption energies and a significant gravimetric storage capacity of 20.32 wt%, exceeding DOE standards. NH<sub>2</sub> functionalization notably improved adsorption energy, enhancing potential for efficient hydrogen storage. Changes in absorption spectra post-H<sub>2</sub> adsorption further highlight BNRs’ potential for hydrogen storage applications. These findings provide valuable insights into BNRs, paving the way for their use in electronic devices and hydrogen storage systems.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"588 ","pages":"Article 112482"},"PeriodicalIF":2.0,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529806","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-12DOI: 10.1016/j.chemphys.2024.112484
Zhigang Cao , Huifang Wu , Yukai An
Through first-principles calculation, the performance of B2C2 monolayer as the Li-S batteries cathode anchoring material is systematically investigated. The B2C2 monolayer exhibits excellent thermodynamic, kinetic and mechanical stability, which are helpful to resist the volume change caused by the reaction during charging and discharging process. Importantly, the adsorption energy of S8 clusters and LiPSs in the B2C2 monolayer is remarkably higher than that in the cathode electrolyte, which greatly inhibits the generation of shuttle effect. The calculations of the catalytic performance of B2C2 monolayer further suggest that the system possesses a lower the Gibbs free energy (ΔG) barrier of 0.71 eV and a fast kinetic conversion process with low diffusion barrier of 0.257 eV along hexatomic ring B2C4, implying a fast charge and discharge rate and excellent cycle performance. The B2C2 monolayer with high energy conversion efficiency and catalytic activity can be expected as an emerging sustainable clean energy source.
{"title":"Anchoring ability and catalytic activity of B2C2 monolayer as the lithium-sulfur batteries cathode materials: A first principle calculation","authors":"Zhigang Cao , Huifang Wu , Yukai An","doi":"10.1016/j.chemphys.2024.112484","DOIUrl":"10.1016/j.chemphys.2024.112484","url":null,"abstract":"<div><div>Through first-principles calculation, the performance of B<sub>2</sub>C<sub>2</sub> monolayer as the Li-S batteries cathode anchoring material is systematically investigated. The B<sub>2</sub>C<sub>2</sub> monolayer exhibits excellent thermodynamic, kinetic and mechanical stability, which are helpful to resist the volume change caused by the reaction during charging and discharging process. Importantly, the adsorption energy of S<sub>8</sub> clusters and LiPSs in the B<sub>2</sub>C<sub>2</sub> monolayer is remarkably higher than that in the cathode electrolyte, which greatly inhibits the generation of shuttle effect. The calculations of the catalytic performance of B<sub>2</sub>C<sub>2</sub> monolayer further suggest that the system possesses a lower the Gibbs free energy (ΔG) barrier of 0.71 eV and a fast kinetic conversion process with low diffusion barrier of 0.257 eV along hexatomic ring B<sub>2</sub>C<sub>4</sub>, implying a fast charge and discharge rate and excellent cycle performance. The B<sub>2</sub>C<sub>2</sub> monolayer with high energy conversion efficiency and catalytic activity can be expected as an emerging sustainable clean energy source.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"588 ","pages":"Article 112484"},"PeriodicalIF":2.0,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142442100","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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