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Novel Janus Co3GeXTe (X= S, Se) monolayers with high structural stability: First-principles predictions
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-26 DOI: 10.1016/j.chemphys.2025.112660
Nguyen T. Hiep , Vo Q. Nha , Le D. Hieu , Bui D. Hoi , Nguyen P.Q. Anh , Huynh V. Phuc , Cuong Q. Nguyen , Nguyen N. Hieu
{"title":"Novel Janus Co3GeXTe (X= S, Se) monolayers with high structural stability: First-principles predictions","authors":"Nguyen T. Hiep , Vo Q. Nha , Le D. Hieu , Bui D. Hoi , Nguyen P.Q. Anh , Huynh V. Phuc , Cuong Q. Nguyen , Nguyen N. Hieu","doi":"10.1016/j.chemphys.2025.112660","DOIUrl":"10.1016/j.chemphys.2025.112660","url":null,"abstract":"<div><div>This study attempts to construct two-dimensional (2D) Janus Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>Ge<span><math><mi>X</mi></math></span>Te (<span><math><mrow><mi>X</mi><mo>=</mo></mrow></math></span> S and Se) monolayers from the original Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>GeTe<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> based on first-principles predictions for new magnetic materials. The optimized Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>GeTe<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>GeSTe, and Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>GeSeTe configurations show hexagonal structures with honeycomb lattices from Co and Te atoms. Then their stabilities are investigated to evaluate the feasibility of synthesizing the Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>Ge<span><math><mi>X</mi></math></span>Te materials by experiments. From the phonon dispersion spectra, all three monolayers expose eighteen positive phonon modes without any imaginary frequency. This implies that the Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>Ge<span><math><mi>X</mi></math></span>Te structures are dynamically stable. Only small total energy fluctuations and no structure fracture/reconstruction are observed after the <em>ab initio</em> molecular dynamics tests, revealing the high thermal stability of the Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>Ge<span><math><mi>X</mi></math></span>Te systems. Besides, the Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>Ge<span><math><mi>X</mi></math></span>Te monolayers have high negative <span><math><msub><mrow><mi>E</mi></mrow><mrow><mi>coh</mi></mrow></msub></math></span> of about <span><math><mrow><mo>−</mo><mn>5</mn></mrow></math></span> eV/atom and the <span><math><msub><mrow><mi>C</mi></mrow><mrow><mn>11</mn></mrow></msub></math></span>, <span><math><msub><mrow><mi>C</mi></mrow><mrow><mn>12</mn></mrow></msub></math></span>, and <span><math><msub><mrow><mi>C</mi></mrow><mrow><mn>66</mn></mrow></msub></math></span> elastic constants obey the condition of Born and Huang for mechanical stability. According to the Poisson’s ratio and Young’s modulus polar diagrams, the isotropic elastic properties are found in all three Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>GeTe<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>GeSTe, and Co<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>GeSeTe monolayers. The obtained evidence indicates the good stabilities of t","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112660"},"PeriodicalIF":2.0,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143519907","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}
引用次数: 0
Adsorption of CO, F2, and NO2 on stanene nanoribbons: Optoelectronic properties and sensing applications
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-22 DOI: 10.1016/j.chemphys.2025.112668
Nguyen Thanh Tung , Tran Cong Phong , Hoang Van Ngoc
{"title":"Adsorption of CO, F2, and NO2 on stanene nanoribbons: Optoelectronic properties and sensing applications","authors":"Nguyen Thanh Tung ,&nbsp;Tran Cong Phong ,&nbsp;Hoang Van Ngoc","doi":"10.1016/j.chemphys.2025.112668","DOIUrl":"10.1016/j.chemphys.2025.112668","url":null,"abstract":"<div><div>The structural and optoelectronic properties of pristine stanene nanoribbons and their modifications upon adsorption of CO, F<sub>2</sub>, and NO<sub>2</sub> gas molecules were systematically investigated using density functional theory. Pristine SnNRs were identified as semiconductors with an intrinsic band gap of approximately 0.308 eV. Notably, the adsorption of F<sub>2</sub> and NO<sub>2</sub> induced a semiconductor-to-metal transition, whereas CO-adsorbed SnNRs retained semiconducting behavior with a band gap of 0.288 eV. Magnetic analysis revealed a transition from a nonmagnetic ground state in pristine SnNRs to a magnetic state upon gas adsorption, with magnetic moments of 2.624 μ<sub>B</sub>, and 1.099 μ<sub>B</sub> for F<sub>2</sub> and NO<sub>2</sub>, respectively. The underlying adsorption mechanisms were elucidated through detailed investigations of multi-orbital hybridization, charge density redistribution, and optical properties, including the dielectric function, absorption coefficient, and joint density of states. These findings underscore the potential of SnNRs for nanoscale optoelectronic applications and as gas sensors for CO, F<sub>2</sub>, and NO<sub>2</sub>.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112668"},"PeriodicalIF":2.0,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473897","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}
引用次数: 0
Vibrational spectra and ab initio investigations of CH3Br-water complexes isolated in neon matrix
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-22 DOI: 10.1016/j.chemphys.2025.112667
P. Soulard, B. Tremblay
{"title":"Vibrational spectra and ab initio investigations of CH3Br-water complexes isolated in neon matrix","authors":"P. Soulard,&nbsp;B. Tremblay","doi":"10.1016/j.chemphys.2025.112667","DOIUrl":"10.1016/j.chemphys.2025.112667","url":null,"abstract":"<div><div>The infrared spectra of the CH<sub>3</sub>Br-H<sub>2</sub>O and CH<sub>3</sub>Br-(H<sub>2</sub>O)<sub>2</sub> complexes have been obtain for the first time in solid neon at 3 K from 100 to 5500 cm<sup>−1</sup> using Fourier transform infrared spectroscopy. We have identified several vibrational transitions for these complexes and also for the CH<sub>3</sub>Br homodimer. The structure of the complexes has been investigated with calculations at the second-order Møller-Plesset (MP2) level. The observed bands are compared with the calculated vibrational spectra at the harmonic level. The CH<sub>3</sub>Br-water heterodimer complex forms a cyclic structure as well as for all CH<sub>3</sub>X-water complexes (X = F, Cl, Br and I). Comparisons of calculated and experimental data for the CH<sub>3</sub>X-water complexes series are also presented.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112667"},"PeriodicalIF":2.0,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510079","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}
引用次数: 0
First-principles insight into SnS2/graphene heterostructure as potential anode materials for rechargeable lithium/sodium ion batteries
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-20 DOI: 10.1016/j.chemphys.2025.112664
Lijuan Zhang , Tianhang Zhang , Cong Wang , Wei Jin , Yin Li , Hao Wang , Changchun Ding , Zongyi Wang
{"title":"First-principles insight into SnS2/graphene heterostructure as potential anode materials for rechargeable lithium/sodium ion batteries","authors":"Lijuan Zhang ,&nbsp;Tianhang Zhang ,&nbsp;Cong Wang ,&nbsp;Wei Jin ,&nbsp;Yin Li ,&nbsp;Hao Wang ,&nbsp;Changchun Ding ,&nbsp;Zongyi Wang","doi":"10.1016/j.chemphys.2025.112664","DOIUrl":"10.1016/j.chemphys.2025.112664","url":null,"abstract":"<div><div>The investigation of anode materials possessing stable capacity, outstanding electrical conductivity, and rapid ion transport is crucial for the advancement of lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs). Previous research has demonstrated that graphene-based heterostructures display outstanding electrical conductivity, high mechanical rigidity, and specific capacity when utilized as anodes. In this work, we systematically investigated the use of SnS<sub>2</sub>/graphene (SnS<sub>2</sub>/G) heterostructure as anode materials for LIBs and SIBs through first-principles calculations. The resultsindicate that, in comparison with the monolayer SnS<sub>2</sub>, the SnS<sub>2</sub>/G heterojunction demonstrates metallic characteristics and enhanced electrical conductivity. It also exhibits excellent Li and Na adsorption capacity, low ion migration barriers, and low open circuit voltage. The Na storage capacity of the SnS<sub>2</sub>/G heterojunction is 481.78 mAh/g, surpassing that of other common anodes. Moreover, the structure of Na embedding process remains stable, rendering it suitable for application as a high-performance anode material for SIBs.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112664"},"PeriodicalIF":2.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510080","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}
引用次数: 0
Synthesis and properties of carbon quantum dots: Antioxidant, antibacterial and pH response monitoring applications
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-20 DOI: 10.1016/j.chemphys.2025.112658
Jingyi Peng , Chengjun Hu , Xiaohan Zhou , Dingyu Wu , Xun Sun , Anqi Tang , Xing-Yu Long , Xiaoqiang Li , Jie Peng , Junlong Tian
{"title":"Synthesis and properties of carbon quantum dots: Antioxidant, antibacterial and pH response monitoring applications","authors":"Jingyi Peng ,&nbsp;Chengjun Hu ,&nbsp;Xiaohan Zhou ,&nbsp;Dingyu Wu ,&nbsp;Xun Sun ,&nbsp;Anqi Tang ,&nbsp;Xing-Yu Long ,&nbsp;Xiaoqiang Li ,&nbsp;Jie Peng ,&nbsp;Junlong Tian","doi":"10.1016/j.chemphys.2025.112658","DOIUrl":"10.1016/j.chemphys.2025.112658","url":null,"abstract":"<div><div>The pH value of a wound during the healing process significantly impacts the speed and quality of healing. Real-time monitoring of the wound's healing status is crucial for doctors to assess infection and healing conditions and provide appropriate treatment plans. The carbon nanoparticles prepared in this study exhibit good fluorescence properties and pH-responsive characteristics, showing a good linear correlation in the pH range of 5.0 to 9.5. They also possess strong antioxidant and antibacterial properties, making them a promising nanomaterial for real-time pH monitoring and the promotion of wound healing.</div><div>By increasing the contents of sulfur (S) and nitrogen (N) elements, and adding amino and carboxyl group modifications on the surface of carbon nanoparticles, the antioxidant, antibacterial and fluorescence properties of carbon nanoparticles were improved. The antioxidant activity of carbon quantum dots was verified by DPPH method, and the antibacterial mechanism of carbon quantum dots was further investigated by surface charge measurement and in vivo study of mouse infected wound model. The results demonstrate that the carbon quantum dots exhibit excellent antibacterial performance, providing a new approach for the development of wound care materials capable of real-time pH monitoring.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112658"},"PeriodicalIF":2.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473896","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}
引用次数: 0
Unveiling the propensity of magnetism in Li intercalated RuO2, using first principles
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-20 DOI: 10.1016/j.chemphys.2025.112657
J.J. Pulikkotil
{"title":"Unveiling the propensity of magnetism in Li intercalated RuO2, using first principles","authors":"J.J. Pulikkotil","doi":"10.1016/j.chemphys.2025.112657","DOIUrl":"10.1016/j.chemphys.2025.112657","url":null,"abstract":"<div><div>RuO<sub>2</sub>, traditionally considered a Pauli paramagnet, exhibits more complex magnetic behavior when influenced by factors like Li intercalation and Ru vacancies, suggesting the importance of strong Coulomb correlations. To understand this, we utilized first-principles calculations to examine the effects of Li intercalation on the structural, electronic, and magnetic properties of RuO<sub>2</sub>. Our results show that Li intercalation weakens Ru-O bonds, alters Ru-Ru interactions at the Fermi energy, and potentially enhances Coulomb correlations. Notably, we predict an antiferromagnetic ground state in Li-intercalated RuO<sub>2</sub> due to half-filled Ru <span><math><msub><mrow><mi>t</mi></mrow><mrow><mn>2</mn><mi>g</mi></mrow></msub></math></span> orbitals. This aligns with improved catalytic activity after Li intercalation. Further experimental investigation, including magnetic characterization, is essential to confirm our theoretical predictions and explore the potential of alkali/alkaline earth metal intercalation in RuO<sub>2</sub>.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112657"},"PeriodicalIF":2.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463307","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}
引用次数: 0
A perspective on Fermi levels and insights into the surface characteristics of S- and Fe-doped InP substrates
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-20 DOI: 10.1016/j.chemphys.2025.112617
Lijie Liu , Siming Chen , Yuanda Wu , Junming An , Chenhui Li , Zhifeng Wang , Zigang Wang
{"title":"A perspective on Fermi levels and insights into the surface characteristics of S- and Fe-doped InP substrates","authors":"Lijie Liu ,&nbsp;Siming Chen ,&nbsp;Yuanda Wu ,&nbsp;Junming An ,&nbsp;Chenhui Li ,&nbsp;Zhifeng Wang ,&nbsp;Zigang Wang","doi":"10.1016/j.chemphys.2025.112617","DOIUrl":"10.1016/j.chemphys.2025.112617","url":null,"abstract":"<div><div>As a pivotal substrate material in III-V compound semiconductors, indium phosphide (InP) plays a critical role in the development of optoelectronic and high-frequency devices. Although extensive research has been conducted on the Fermi levels of single crystals in bulk materials, studies have also explored how Fermi-level modifications induced by various dopants affect the surface characteristics and adsorption capacities of InP substrates. This study presents a comparative analysis of the significant disparities in surface attributes, including metal ions, absorbed particles, and oxide layer thickness, between sulfur-doped InP and iron-doped InP. Theoretical simulations based on first-principles density functional theory under the plane-wave pseudopotential method reveal that sulfur acts as a shallow donor when substituting phosphorus and as a deep donor in the sulfur gap, whereas iron serves as a deep donor when replacing indium. These substitutions engender variations in the Fermi energy levels, thereby altering the work functions of the substrate surfaces. Consequently, these changes manifest in the surface properties of the substrates, influencing factors such as the metal ion composition, particle dimensions, and oxide thickness.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112617"},"PeriodicalIF":2.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143478814","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}
引用次数: 0
High thermal insulation and optical conductivity of the 2D phase of MgX2 (X=Cl, Br, and I): A DFT and AIMD study
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-19 DOI: 10.1016/j.chemphys.2025.112656
Nzar Rauf Abdullah , Botan Jawdat Abdullah , Vidar Gudmundsson
{"title":"High thermal insulation and optical conductivity of the 2D phase of MgX2 (X=Cl, Br, and I): A DFT and AIMD study","authors":"Nzar Rauf Abdullah ,&nbsp;Botan Jawdat Abdullah ,&nbsp;Vidar Gudmundsson","doi":"10.1016/j.chemphys.2025.112656","DOIUrl":"10.1016/j.chemphys.2025.112656","url":null,"abstract":"<div><div>This work investigates the electronic structure, dynamics, thermal, and optical properties of 2D MgX<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> (where X=Cl, Br, and I) using density functional theory, DFT, and ab initio molecular dynamics, AIMD, simulations. The 2D structures exhibit natural planar buckling, with larger buckling observed in MgI<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> compared to MgBr<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> and MgCl<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, correlating with bond length and lattice constant trends. The band gap in MgX<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> is primarily influenced by planar buckling in addition to differences in electronegativity. Among them, MgCl<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> shows the largest direct band gap, while MgI<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> has the smallest indirect band gap. MgBr<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> lies in between, demonstrating a direct band gap. The stability analysis indicates that all three considered MgX<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> are energetically, dynamically and thermally stable. Thermal properties indicate that MgI<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> has the highest heat capacity, attributed to degenerate acoustic phonon modes. In contrast, MgCl<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> exhibits superior thermal conductivity due to high phonon group velocity. Optical studies show that MgI<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> absorbs in the Mid-UV region, while MgCl<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> and MgBr<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> absorb in the Deep-UV. A higher plasmon frequency is found for lower buckled structures compared to the more buckled ones, with potential applications in optoelectronics and plasmonics. This comprehensive study highlights the significant role of structural distortions, such as planar buckling, in determining the electronic, dynamic, thermal, and optical behavior of MgX<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112656"},"PeriodicalIF":2.0,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143453555","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}
引用次数: 0
DFT studies on the catalytic hydrogenation of carbon dioxide on Ni (111) in a liquid-phase environment
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-17 DOI: 10.1016/j.chemphys.2025.112662
Weiqi Li , Enguang Ji , Chaoquan Hu , Xuebing Xu , Junfeng Hui , Tao Yang
{"title":"DFT studies on the catalytic hydrogenation of carbon dioxide on Ni (111) in a liquid-phase environment","authors":"Weiqi Li ,&nbsp;Enguang Ji ,&nbsp;Chaoquan Hu ,&nbsp;Xuebing Xu ,&nbsp;Junfeng Hui ,&nbsp;Tao Yang","doi":"10.1016/j.chemphys.2025.112662","DOIUrl":"10.1016/j.chemphys.2025.112662","url":null,"abstract":"<div><div>CO<sub>2</sub> catalytic hydrogenation attracts interest in converting CO<sub>2</sub> into useful chemicals and mitigating the greenhouse effect. In this study, CO<sub>2</sub> hydrogenation in a liquid-phase environment on the Ni (111) surface was investigated using density functional theory calculations. Based on the analysis of hydrogenation in the gas phase, the water H migration model was introduced to examine the kinetic processes in the liquid phase. The results reveal that water plays a key role in this reaction. During the hydrogenation of CO<sub>2</sub>* to COOH* or HCOO*, the adsorbed H atom is first transferred to the water molecule, which subsequently donates another H atom to COOH* or HCOO*. During this process, water directly participates in the reaction as a medium, enabling H* to hydrogenate the adsorbed reactant over a limited distance. According to the proposed mechanism, the HCOO pathway is the optimal route for the reaction, exhibiting an energy barrier of 1.08 eV.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112662"},"PeriodicalIF":2.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463308","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}
引用次数: 0
Selective adsorption, structure and dynamics of CO2 – CH4 mixture in Mg-MOF-74 and the influence of intercrystalline disorder
IF 2 3区 化学
Chemical Physics Pub Date : 2025-02-14 DOI: 10.1016/j.chemphys.2025.112661
I. Dhiman , David R. Cole , Siddharth Gautam
{"title":"Selective adsorption, structure and dynamics of CO2 – CH4 mixture in Mg-MOF-74 and the influence of intercrystalline disorder","authors":"I. Dhiman ,&nbsp;David R. Cole ,&nbsp;Siddharth Gautam","doi":"10.1016/j.chemphys.2025.112661","DOIUrl":"10.1016/j.chemphys.2025.112661","url":null,"abstract":"<div><div>Mg-MOF-74 is a highly efficient adsorbent for CO<sub>2</sub>. We use molecular simulations to study the effects of disorder in Mg-MOF-74 on the selective adsorption, structure, and dynamics of a CO<sub>2</sub>-CH<sub>4</sub> mixture. Positional disorder is introduced in the adsorbent by separating individual Mg-MOF-74 crystallites via inserting intercrystalline space between them. Rotating a crystallite with respect to others by different extents provides the orientational disorder (OD). Disorder is observed to enhance the adsorption selectivity of CO<sub>2</sub> over CH<sub>4</sub>. The additional adsorption sites available by exposing crystallite surfaces may provide added selectivity for CO<sub>2</sub>. Disorder is found to affect both the translational as well as rotational motion of CO<sub>2</sub> in Mg-MOF-74. This behavior follows a systematic pattern dictated by the interplay of the pore geometry of Mg-MOF-74 and Mg<sup>2+</sup> − CO<sub>2</sub> interactions. Our results provide a guide on how to tailor Mg-MOF-74 adsorption behavior with desired properties by purposeful introduction of disorder.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"594 ","pages":"Article 112661"},"PeriodicalIF":2.0,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143444451","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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