Pub Date : 2025-01-22DOI: 10.1016/j.cplett.2025.141909
Jiajun Sun , Yanglin Chen , Xin Qian , Yu Liang , Yong Jie Kee , Ruiming Fang , Yajuan Xu , Guangwen Xu , Can Xue
A novel 2D/2D foursquare BiOCl/g-C3N4 heterojunction photocatalyst was fabricated using mannitol by a simple method. Square sheets of BiOCl were dispersed on the surfaces of g-C3N4 uniformly. The influence of Bi dosage on the structure and performance of the composite was investigated and the best sample could degrade 93.87 % of RhB after visible-light irradiation for 3 h, which was 7.39 and 3.09 times higher than pure g-C3N4 and pure BiOCl, respectively. The enhanced photocatalytic efficiency can be attributed to the reduced recombination of photogenerated electrons and holes. Superoxide anion radicals and photogenerated holes are the two main active species.
{"title":"Facile synthesis of 2D/2D foursquare BiOCl/g-C3N4 heterojunctions with enhanced photocatalysis performance under visible light irradiation","authors":"Jiajun Sun , Yanglin Chen , Xin Qian , Yu Liang , Yong Jie Kee , Ruiming Fang , Yajuan Xu , Guangwen Xu , Can Xue","doi":"10.1016/j.cplett.2025.141909","DOIUrl":"10.1016/j.cplett.2025.141909","url":null,"abstract":"<div><div>A novel 2D/2D foursquare BiOCl/g-C<sub>3</sub>N<sub>4</sub> heterojunction photocatalyst was fabricated using mannitol by a simple method. Square sheets of BiOCl were dispersed on the surfaces of g-C<sub>3</sub>N<sub>4</sub> uniformly. The influence of Bi dosage on the structure and performance of the composite was investigated and the best sample could degrade 93.87 % of RhB after visible-light irradiation for 3 h, which was 7.39 and 3.09 times higher than pure g-C<sub>3</sub>N<sub>4</sub> and pure BiOCl, respectively. The enhanced photocatalytic efficiency can be attributed to the reduced recombination of photogenerated electrons and holes. Superoxide anion radicals and photogenerated holes are the two main active species.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"863 ","pages":"Article 141909"},"PeriodicalIF":2.8,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143147943","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 : 2025-01-22DOI: 10.1016/j.cplett.2025.141911
Huan Wang, Cen Shi, Liangliang Yin, Yanqin Ji
To remove lutetium from wastewater, superparamagnetic Fe3O4@SiO2–HOPO nanoparticles were successfully synthesized, containing approximately 460 μmol·g−1 of 3,2-HOPO. The material demonstrated high stability in 0.1 mol·L−1 HNO3 and retained 97 % of its adsorption capacity after five cycles. The nanoparticles showed strong selectivity for lutetium, with minimal interference from coexisting ions in different matrices. This selective adsorption was primarily due to monodentate or multidentate chelation of 3,2-HOPO on the particle surface with lutetium. Adsorption equilibrium was achieved within 15 min, with a maximum capacity of 29 mg·g−1, highlighting its potential for large-scale wastewater treatment.
{"title":"Synthesis of highly selective magnetic Fe3O4@SiO2–HOPO nanoparticles for efficient lutetium removal from wastewater","authors":"Huan Wang, Cen Shi, Liangliang Yin, Yanqin Ji","doi":"10.1016/j.cplett.2025.141911","DOIUrl":"10.1016/j.cplett.2025.141911","url":null,"abstract":"<div><div>To remove lutetium from wastewater, superparamagnetic Fe<sub>3</sub>O<sub>4</sub>@SiO<sub>2</sub>–HOPO nanoparticles were successfully synthesized, containing approximately 460 μmol·g<sup>−1</sup> of 3,2-HOPO. The material demonstrated high stability in 0.1 mol·L<sup>−1</sup> HNO<sub>3</sub> and retained 97 % of its adsorption capacity after five cycles. The nanoparticles showed strong selectivity for lutetium, with minimal interference from coexisting ions in different matrices. This selective adsorption was primarily due to monodentate or multidentate chelation of 3,2-HOPO on the particle surface with lutetium. Adsorption equilibrium was achieved within 15 min, with a maximum capacity of 29 mg·g<sup>−1</sup>, highlighting its potential for large-scale wastewater treatment.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"864 ","pages":"Article 141911"},"PeriodicalIF":2.8,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143104732","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 : 2025-01-20DOI: 10.1016/j.cplett.2025.141905
Akihiro Tateno, Hiroki Nagashima, Kiminori Maeda
Spin-correlated radical pairs (RPs) are crucial for understanding how magnetic fields influence reaction yield and spin polarization. Reaction Yield Detected Magnetic Resonance (RYDMR) enables the observation of oscillating magnetic field effects on reaction yield, linking radical pairs to subsequent reactions. This study introduces the use of an arbitrary waveform generator (AWG) in RYDMR experiments, termed AWG-RYDMR, focusing on low-field RYDMR and its impact on spin-mixing efficiency. It is demonstrated that frequency-modulated RF pulses enhance spin mixing compared to single-frequency pulses by accessing a broader range of resonant frequencies, thus paving the way for advanced electron spin and reaction control techniques.
{"title":"Effect of frequency chirp on RYDMR spectrum in AWG-RYDMR system at low magnetic field","authors":"Akihiro Tateno, Hiroki Nagashima, Kiminori Maeda","doi":"10.1016/j.cplett.2025.141905","DOIUrl":"10.1016/j.cplett.2025.141905","url":null,"abstract":"<div><div>Spin-correlated radical pairs (RPs) are crucial for understanding how magnetic fields influence reaction yield and spin polarization. Reaction Yield Detected Magnetic Resonance (RYDMR) enables the observation of oscillating magnetic field effects on reaction yield, linking radical pairs to subsequent reactions. This study introduces the use of an arbitrary waveform generator (AWG) in RYDMR experiments, termed AWG-RYDMR, focusing on low-field RYDMR and its impact on spin-mixing efficiency. It is demonstrated that frequency-modulated RF pulses enhance spin mixing compared to single-frequency pulses by accessing a broader range of resonant frequencies, thus paving the way for advanced electron spin and reaction control techniques.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"864 ","pages":"Article 141905"},"PeriodicalIF":2.8,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143095068","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 : 2025-01-20DOI: 10.1016/j.cplett.2025.141906
Kang Xu , Zhenhua Li , Xin Li , Ran Jia , Zhiqiang Wang , Xiaodi Huo , Dongyan Cao , Chunling Wang , Lei Xu
Developing novel 2D semiconductors with overall water splitting capacity and high carrier mobility is essential for efficient visible-light-driven photocatalysis. Here, we have designed a novel Janus multicomponent bismuth-layered semiconductor monolayer, Bi8M2O16XY (M = Nb, Ta; X/Y = Cl, Br, I; X ≠ Y). Our findings demonstrate that Bi8M2O16XY exhibits suitable band edge positions and robust stability for overall water splitting. By varying halogen surface coverages, this material achieves a tunable internal electric field (0.06–0.21 eV/Å) and bandgap (2.40–2.89 eV), with carrier mobility reaching ∼103 cm2 V−1 s−1. This study advances the development of innovative multicomponent 2D materials.
{"title":"Janus monolayer Bi8M2O16XY (M = Nb, Ta; X/Y = Cl, Br, I; X ≠ Y) for photocatalytic overall water splitting with high carrier mobility: A first principles study","authors":"Kang Xu , Zhenhua Li , Xin Li , Ran Jia , Zhiqiang Wang , Xiaodi Huo , Dongyan Cao , Chunling Wang , Lei Xu","doi":"10.1016/j.cplett.2025.141906","DOIUrl":"10.1016/j.cplett.2025.141906","url":null,"abstract":"<div><div>Developing novel 2D semiconductors with overall water splitting capacity and high carrier mobility is essential for efficient visible-light-driven photocatalysis. Here, we have designed a novel Janus multicomponent bismuth-layered semiconductor monolayer, Bi<sub>8</sub>M<sub>2</sub>O<sub>16</sub>XY (M = Nb, Ta; X/Y = Cl, Br, I; X ≠ Y). Our findings demonstrate that Bi<sub>8</sub>M<sub>2</sub>O<sub>16</sub>XY exhibits suitable band edge positions and robust stability for overall water splitting. By varying halogen surface coverages, this material achieves a tunable internal electric field (0.06–0.21 eV/Å) and bandgap (2.40–2.89 eV), with carrier mobility reaching ∼10<sup>3</sup> cm<sup>2</sup> V<sup>−1</sup> s<sup>−1</sup>. This study advances the development of innovative multicomponent 2D materials.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"863 ","pages":"Article 141906"},"PeriodicalIF":2.8,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143147942","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 : 2025-01-19DOI: 10.1016/j.cplett.2025.141903
Yekaterina Omelkova, Ella Tkachenko, Victor Kostjukov
We have shown that ultrafast switching of photochromic oxazine (PCOX) can occur via a singlet mechanism. Previously, only a triplet model of PCOX photoconversion was proposed by other authors. According to our TD-DFT/DFT calculations, PCOX undergoes a photoinduced S0 → S3 electron transition. As a result, the electron density between the C2 and O1 atoms decreases and with the participation of thermal motion, the bond between them is broken. In the resulting excited open form of PCOX, an intramolecular stacking excimer is formed. During its relaxation to the ground state, the stacking is preserved, preventing the rotation of the aromatic systems around the alkyl linker connecting them and thus facilitating a very rapid recovery of the C2-O1 bond. Therefore, the photochemical pathway of PCOX can be represented as the following scheme: Closed(S0) → Closed(S3) → Open stacked(S3) → Open stacked(S0) → Closed(S0).
{"title":"Ultrafast switching of photochromic oxazine: A theoretical explanation","authors":"Yekaterina Omelkova, Ella Tkachenko, Victor Kostjukov","doi":"10.1016/j.cplett.2025.141903","DOIUrl":"10.1016/j.cplett.2025.141903","url":null,"abstract":"<div><div>We have shown that ultrafast switching of photochromic oxazine (PCOX) can occur via a singlet mechanism. Previously, only a triplet model of PCOX photoconversion was proposed by other authors. According to our TD-DFT/DFT calculations, PCOX undergoes a photoinduced S<sub>0</sub> → S<sub>3</sub> electron transition. As a result, the electron density between the C2 and O1 atoms decreases and with the participation of thermal motion, the bond between them is broken. In the resulting excited open form of PCOX, an intramolecular stacking excimer is formed. During its relaxation to the ground state, the stacking is preserved, preventing the rotation of the aromatic systems around the alkyl linker connecting them and thus facilitating a very rapid recovery of the C2-O1 bond. Therefore, the photochemical pathway of PCOX can be represented as the following scheme: Closed(S<sub>0</sub>) → Closed(S<sub>3</sub>) → Open stacked(S<sub>3</sub>) → Open stacked(S<sub>0</sub>) → Closed(S<sub>0</sub>).</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"863 ","pages":"Article 141903"},"PeriodicalIF":2.8,"publicationDate":"2025-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143147936","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 : 2025-01-18DOI: 10.1016/j.cplett.2025.141874
Emmanouil Semidalas , A. Daniel Boese , Jan M.L. Martin
For noncovalent interactions, it is generally assumed that CCSD(T) approaches the exact solution within the basis set. For most of the S66 benchmark, we present CCSDT and CCSDT(Q) corrections with a DZP basis set. For hydrogen bonds, pure London, and mixed-influence complexes, CCSD(T) benefits from error cancellation between (repulsive) higher-order triples, , and (attractive) connected quadruples, (Q). For -stacking complexes, this cancellation starts breaking down and CCSD(T) overbinds; CCSD(T) corrects the problem at the expense of London complexes. Simple two- or three-parameter models predict CCSDT(Q)–CCSD(T) differences to 0.01 kcal molRMS, requiring no calculations with steeper scaling than .
{"title":"Post-CCSD(T) corrections in the S66 noncovalent interactions benchmark","authors":"Emmanouil Semidalas , A. Daniel Boese , Jan M.L. Martin","doi":"10.1016/j.cplett.2025.141874","DOIUrl":"10.1016/j.cplett.2025.141874","url":null,"abstract":"<div><div>For noncovalent interactions, it is generally assumed that CCSD(T) approaches the exact solution within the basis set. For most of the S66 benchmark, we present CCSDT and CCSDT(Q) corrections with a DZP basis set. For hydrogen bonds, pure London, and mixed-influence complexes, CCSD(T) benefits from error cancellation between (repulsive) higher-order triples, <span><math><mrow><msub><mrow><mi>T</mi></mrow><mrow><mn>3</mn></mrow></msub><mo>−</mo><mrow><mo>(</mo><mi>T</mi><mo>)</mo></mrow></mrow></math></span>, and (attractive) connected quadruples, (Q). For <span><math><mi>π</mi></math></span>-stacking complexes, this cancellation starts breaking down and CCSD(T) overbinds; CCSD(T)<span><math><msub><mrow></mrow><mrow><mi>Λ</mi></mrow></msub></math></span> corrects the problem at the expense of London complexes. Simple two- or three-parameter models predict CCSDT(Q)–CCSD(T) differences to 0.01 kcal<!--> <!-->mol<span><math><msup><mrow></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msup></math></span>RMS, requiring no calculations with steeper scaling than <span><math><mrow><mi>O</mi><mrow><mo>(</mo><msup><mrow><mi>N</mi></mrow><mrow><mn>7</mn></mrow></msup><mo>)</mo></mrow></mrow></math></span>.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"863 ","pages":"Article 141874"},"PeriodicalIF":2.8,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143148305","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}
Pub Date : 2025-01-18DOI: 10.1016/j.cplett.2025.141895
Ke Zhang, Tianfeng Chen
In this work, Co3O4 materials with different morphologies were synthesized based on cobalt sources containing different anions by hydrothermal method, and the effects of anions on their microscopic morphology and gas sensing properties were explored. The test results showed that the Co3O4 material synthesized with CoCl2 as the precursor had the best comprehensive gas sensing performance, with a high specific surface area of 93.47 m2/g, and a response value of 23.14 to 100 ppm ethanol at 200 °C. Exploring the effect of anions on the properties of Co3O4 materials has a certain guiding effect on the subsequent synthesis of gas-sensitive materials.
{"title":"Preparation of Co3O4 nanostructure morphology by anion-pairing hydrothermal and the effect of gas sensitivity","authors":"Ke Zhang, Tianfeng Chen","doi":"10.1016/j.cplett.2025.141895","DOIUrl":"10.1016/j.cplett.2025.141895","url":null,"abstract":"<div><div>In this work, Co<sub>3</sub>O<sub>4</sub> materials with different morphologies were synthesized based on cobalt sources containing different anions by hydrothermal method, and the effects of anions on their microscopic morphology and gas sensing properties were explored. The test results showed that the Co<sub>3</sub>O<sub>4</sub> material synthesized with CoCl<sub>2</sub> as the precursor had the best comprehensive gas sensing performance, with a high specific surface area of 93.47 m<sup>2</sup>/g, and a response value of 23.14 to 100 ppm ethanol at 200 °C. Exploring the effect of anions on the properties of Co<sub>3</sub>O<sub>4</sub> materials has a certain guiding effect on the subsequent synthesis of gas-sensitive materials.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"863 ","pages":"Article 141895"},"PeriodicalIF":2.8,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143147940","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 : 2025-01-18DOI: 10.1016/j.cplett.2025.141898
Jing Chen, Zhanyu Wu, Mingzi Xu, Yijun Liu, Luanfang Duan, Pan Xu, Lei Wu
In this paper, the adsorption process of dissolved gases in four oils on Nb, Ta, V-modified ZnO nanosheets was simulated using a density functional theory approach, and the related adsorption and sensing mechanisms were revealed by the calculations of energy band structure, density of states, and differential charge density. The results show that the Nb, Ta, V modification can significantly enhance the gas-sensitive response of ZnO nanosheets, especially for the capture of CO, CH4 and C2H2, which is mainly attributed to the contribution of the d-orbital electron layer of the doped metal particles. The adsorption capacity of Nb,Ta-modified ZnO nanosheets for dissolved gases in transformer oils is in the order of C2H2 > CO > CH4 > H2, and the work function of Ta and V-ZnO adsorption system decreases significantly, which also proves that the modification of the metal Ta and V atoms improves the carrier density and carrier mobility of the ZnO system. This study provides a theoretical basis for the development of high-performance gas sensors for the detection of dissolved gases in transformer oil.
{"title":"Gas-sensitive performance study of Nb, Ta and V-modified ZnO for dissolved gases in transformer oil","authors":"Jing Chen, Zhanyu Wu, Mingzi Xu, Yijun Liu, Luanfang Duan, Pan Xu, Lei Wu","doi":"10.1016/j.cplett.2025.141898","DOIUrl":"10.1016/j.cplett.2025.141898","url":null,"abstract":"<div><div>In this paper, the adsorption process of dissolved gases in four oils on Nb, Ta, V-modified ZnO nanosheets was simulated using a density functional theory approach, and the related adsorption and sensing mechanisms were revealed by the calculations of energy band structure, density of states, and differential charge density. The results show that the Nb, Ta, V modification can significantly enhance the gas-sensitive response of ZnO nanosheets, especially for the capture of CO, CH<sub>4</sub> and C<sub>2</sub>H<sub>2</sub>, which is mainly attributed to the contribution of the d-orbital electron layer of the doped metal particles. The adsorption capacity of Nb,Ta-modified ZnO nanosheets for dissolved gases in transformer oils is in the order of C<sub>2</sub>H<sub>2</sub> > CO > CH<sub>4</sub> > H<sub>2</sub>, and the work function of Ta and V-ZnO adsorption system decreases significantly, which also proves that the modification of the metal Ta and V atoms improves the carrier density and carrier mobility of the ZnO system. This study provides a theoretical basis for the development of high-performance gas sensors for the detection of dissolved gases in transformer oil.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"863 ","pages":"Article 141898"},"PeriodicalIF":2.8,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143147948","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 : 2025-01-17DOI: 10.1016/j.cplett.2025.141901
Baoming Hou , Yuheng Li , Meiqi Liu , Yuyu Pan , Bing Yang
TADF emitters have great potential for OLEDs applications. In this paper, the TADF emission mechanisms of 3 experimental and 2 designed molecules with “axial and equatorial carbazolyl extension” configurations are theoretically investigated based on the TVCF method and multiscale calculations. It was concluded that increasing the molecules’ conjugation length by utilizing carbazolylbenzene can effectively maintain a smaller ΔEST while increasing the SOC, which improves the kRISC. Importantly, in the aggregated state, the vibrations of the molecules are suppressed, which reduces the kIC. Our work rationally confirms the experimental results and 2 molecules have been designed that predict better optoelectronic properties.
{"title":"Theoretical study and molecular design of luminescent properties of TADF emitters with “axial and equatorial carbazolyl extension” structures","authors":"Baoming Hou , Yuheng Li , Meiqi Liu , Yuyu Pan , Bing Yang","doi":"10.1016/j.cplett.2025.141901","DOIUrl":"10.1016/j.cplett.2025.141901","url":null,"abstract":"<div><div>TADF emitters have great potential for OLEDs applications. In this paper, the TADF emission mechanisms of 3 experimental and 2 designed molecules with “axial and equatorial carbazolyl extension” configurations are theoretically investigated based on the TVCF method and multiscale calculations. It was concluded that increasing the molecules’ conjugation length by utilizing carbazolylbenzene can effectively maintain a smaller ΔE<sub>ST</sub> while increasing the SOC, which improves the k<sub>RISC</sub>. Importantly, in the aggregated state, the vibrations of the molecules are suppressed, which reduces the k<sub>IC</sub>. Our work rationally confirms the experimental results and 2 molecules have been designed that predict better optoelectronic properties.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"863 ","pages":"Article 141901"},"PeriodicalIF":2.8,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143148304","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 : 2025-01-17DOI: 10.1016/j.cplett.2025.141902
Miguel Fernández , Reinaldo Marín , Morella Sánchez , Fernando Ruette
MgSO4 has been of great interest for its antioxidant properties. Its ion pairs were capable of transforming the OH radical (OH−) by a spin-electron transfer from SO42− to OH besides the formation of a Mg2+…OH− bond. Molecular and natural orbital of conformations are explored to analyze the SOMO-HOMO inversion (SHI) behavior related to the spin-electron transfer mechanism. An orbital scheme for the spin-electron transfer and SHI is proposed. Natural orbitals showed the formation of a partial O-O bond in the sulfate that stabilized the SO4− radical. The antioxidant capacity of MgSO4 is explained by spin-electron delocalization of unpaired electron.
{"title":"Relevance of SOMO-HOMO inversion in the antioxidant activity of MgSO4-OH radical complex: A theoretical insight","authors":"Miguel Fernández , Reinaldo Marín , Morella Sánchez , Fernando Ruette","doi":"10.1016/j.cplett.2025.141902","DOIUrl":"10.1016/j.cplett.2025.141902","url":null,"abstract":"<div><div>MgSO<sub>4</sub> has been of great interest for its antioxidant properties. Its ion pairs were capable of transforming the <sup><img></sup>OH radical (OH<sup>−</sup>) by a spin-electron transfer from SO<sub>4</sub><sup>2−</sup> to <sup><img></sup>OH besides the formation of a Mg<sup>2+</sup>…OH<sup>−</sup> bond. Molecular and natural orbital of conformations are explored to analyze the SOMO-HOMO inversion (SHI) behavior related to the spin-electron transfer mechanism. An orbital scheme for the spin-electron transfer and SHI is proposed. Natural orbitals showed the formation of a partial O-O bond in the sulfate that stabilized the SO<sub>4</sub><sup><img>−</sup> radical. The antioxidant capacity of MgSO<sub>4</sub> is explained by spin-electron delocalization of unpaired electron.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"863 ","pages":"Article 141902"},"PeriodicalIF":2.8,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143149167","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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