Chemphyschem最新文献

Accessing Transient Isomers in the Photoreaction of Metastable-State Photoacid. 亚稳态光酸光反应中瞬时异构体的获取。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-14 DOI: 10.1002/cphc.202500184

Yingzhong Ma, Uvinduni I Premadasa, May Waters, Nitesh Kumar, Benjamin Doughty, Melyse Laud, Yi Liao, Vyacheslav S Bryantsev

{"title":"Accessing Transient Isomers in the Photoreaction of Metastable-State Photoacid.","authors":"Yingzhong Ma, Uvinduni I Premadasa, May Waters, Nitesh Kumar, Benjamin Doughty, Melyse Laud, Yi Liao, Vyacheslav S Bryantsev","doi":"10.1002/cphc.202500184","DOIUrl":"https://doi.org/10.1002/cphc.202500184","url":null,"abstract":"The photoreaction of a metastable-state photoacid (mPAH) generally involves multiple isomers with various connected pathways of photoinduced structural changes during a single reaction cycle. However, only a limited number of isomers have been identified experimentally so far owing to the inherent complexity in combination with the presence of various competing electronic and vibrational processes, as well as the constantly varying interactions between mPAH isomers and solvent molecules. Here, we report an optical spectroscopic study on a benzimidazole-based mPAH, a novel photoacid using benzimidazole as the structural moiety with the active proton. Through measurements of linear absorption and steady-state fluorescence in neat solvents and binary mixtures, we discovered a pronounced effect of neat water and its binary mixture with glycerol on the photoreaction of this benzimidazole-mPAH, manifested by the remarkably distinct spectral responses to irradiation from that observed for an organic solution under an identical condition. Measurements of time- and frequency-resolved fluorescence emission further enable us to access transient isomers and the associated spectral characteristics process from other competing electronic excited-state relaxation processes. Spectral deconvolution analysis and time-dependent density functional theory (TDDFT) calculations were applied to separate distinct spectral components and access their potential origin.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500184"},"PeriodicalIF":2.3,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144076296","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

Exploring the Influence of Carbonaceous Material on the Photocatalytic Performance of Composites Containing Bi-BiOBr and P25 TiO2 for NOx Remediation. 探讨碳质材料对含Bi-BiOBr和P25 TiO2复合材料光催化性能的影响

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-14 DOI: 10.1002/cphc.202500237

Paransa Alimard, Stanley Cazaly, Ioanna Itskou, Hanieh Akbari, Srinivas Gadipelli, Nazila Kamaly, Flurin Eisner, Andreas Kafizas

{"title":"Exploring the Influence of Carbonaceous Material on the Photocatalytic Performance of Composites Containing Bi-BiOBr and P25 TiO2 for NOx Remediation.","authors":"Paransa Alimard, Stanley Cazaly, Ioanna Itskou, Hanieh Akbari, Srinivas Gadipelli, Nazila Kamaly, Flurin Eisner, Andreas Kafizas","doi":"10.1002/cphc.202500237","DOIUrl":"https://doi.org/10.1002/cphc.202500237","url":null,"abstract":"Bi-BiOBr-P25 TiO2 composite exhibits high and synergistic improvements in the photocatalytic activity for nitrogen oxide (NOx) removal. Herein, we explored the influence of adding carbonaceous material to this composite, namely graphene (G), graphene oxide (GO), carbon nanotubes (CNT) and buckminsterfullerene (F); all at 1 wt.%. All samples were synthesised using a one-pot solvothermal method. The structural and morphological properties, composition, and photocatalytic performance of the composites and their parent materials were examined using scanning electron microscopy (SEM), carbon-hydrogen-nitrogen (CHN) elemental analysis, high-resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), Raman spectroscopy, attenuated total reflectance Fourier transform infra-red (ATR-FTIR) spectroscopy, ultraviolet-visible (UV-vis) spectroscopy, X-ray photoelectron spectroscopy (XPS), N2 sorption at 77 K, photoluminescence (PL) spectroscopy, diffuse reflectance transient absorption spectroscopy (DR-TAS) and photocatalytic testing against NOx gas in accordance with ISO protocol (22197-1:2016). Among the studied carbonaceous composites, the composite including GO showed the highest performance towards NOx remediation. For reactions in NO gas, it showed a combined higher NOx removal rate (21.9%) than its parent materials P25 (8.7%), Bi-BiOBr (6.5%) and GO (0%). For reactions in NO2 gas, it showed a higher NOx removal rate (~15%) than its parent materials P25 (~10%), Bi-BiOBr (~5%) and GO (0%).","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500237"},"PeriodicalIF":2.3,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144076297","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 Investigation of a High-Chern-Number Quantum Anomalous Hall Insulator Mn2Bi2O6 and its BN-Coupled Multilayer Heterostructures. 高陈氏数量子反常霍尔绝缘子Mn2Bi2O6及其bn耦合多层异质结构的第一性原理研究。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-14 DOI: 10.1002/cphc.202500161

Jiaming Hu, Jingshen Yan, Kaixuan Chen, Shu-Shen Lyu

{"title":"First-Principles Investigation of a High-Chern-Number Quantum Anomalous Hall Insulator Mn2Bi2O6 and its BN-Coupled Multilayer Heterostructures.","authors":"Jiaming Hu, Jingshen Yan, Kaixuan Chen, Shu-Shen Lyu","doi":"10.1002/cphc.202500161","DOIUrl":"https://doi.org/10.1002/cphc.202500161","url":null,"abstract":"In modern condensed matter physics, the quantum anomalous Hall effect (QAHE), an important manifestation of topological quantum states, has attracted much attention due to its ability to exhibit the quantum Hall effect without the need for an external magnetic field. In this study, we report the discovery of a new high-Chern-number quantum anomalous Hall insulator, Mn2Bi2O6. Utilizing first-principles calculations, we systematically investigate its electronic and topological properties. The results reveal that monolayer Mn2Bi2O6 possesses a remarkable energy gap of 110 meV and a Chern number of 3, corresponding to three intrinsic conductive edge channels. The material exhibits both strong robustness and stability upon applied strain. Moreover, by stacking double layers with a BN insulating layer, a heterostructure system with a larger bandgap (117.4 meV) and an increased Chern number of 6 can be realized. When substituting the upper layer's oxygen atoms with tellurium atoms, it forms a Janus structure, accompanied with a transition of Chern number from 3 to 1. This work not only introduces new candidates for expanding the class of QAHE materials, but also establishes a new platform for applications in low-power electronic devices and topological quantum computing.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500161"},"PeriodicalIF":2.3,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143983808","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

Temperature Tunable Optical Properties of Tetraheptylaluminum(III) Porphyrin Toward Molecular Thermometer. 面向分子温度计的四庚基铝（III）卟啉的温度可调光学性质。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-14 DOI: 10.1002/cphc.202500087

Stefan Charon, Niloofar Zarrabi, Jatan K Sharma, Paul A Karr, Francis D'Souza, Prashanth K Poddutoori

引用次数: 0

Understanding the active site structures and achieving catalytic activity tuning of atomically dispersed FeN4 sites for oxygen reduction reaction. 了解氧还原反应中原子分散的FeN4位点的活性位点结构并实现催化活性调整。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-12 DOI: 10.1002/cphc.202401158

Jiayi Xu, Prajay Patel, Chang Yan, Cong Liu

{"title":"Understanding the active site structures and achieving catalytic activity tuning of atomically dispersed FeN4 sites for oxygen reduction reaction.","authors":"Jiayi Xu, Prajay Patel, Chang Yan, Cong Liu","doi":"10.1002/cphc.202401158","DOIUrl":"https://doi.org/10.1002/cphc.202401158","url":null,"abstract":"Atomically dispersed Fe-N-C catalysts with high oxygen reduction reaction (ORR) activity have attracted great attention since the last decade. Due to its comparable ORR activity and low material cost, it is a promising platinum-group metal (PGM) free catalyst that can replace the commercialized Pt/C materials; furthermore, it can facilitate the efficiency of the fuel cell technologies and mitigate our dependence on fossil fuels. Great advancements have been made to experimentally optimize the synthesis approach of the Fe-N-C catalysts, enhance the ORR activity, and improve the catalyst stability. Similarly, recent theoretical studies also provide enriched understanding of the active site structures, properties, and reaction mechanisms. In this review, discussions are made upon utilizing combined experimental and computational spectroscopy to reveal the active site structures, employing mechanistic studies to investigate reaction thermodynamics and kinetics, as well as developing scaling relationships to assist the design and development of future PGM free catalyst materials. Furthermore, recent advances in studying Fe-N-C catalysts utilizing electrified surface and explicit solvation models are discussed. Not only can these aspects improve the accuracy of theoretical simulation and predictions but also deepen the understanding of the catalyst properties and reaction mechanisms under the effect of surface charges and solvent molecules.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202401158"},"PeriodicalIF":2.3,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143980606","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

Realizing improved sodium-ion storage for anthracite-derived hard carbon anode by activation-surface modification strategy. 通过活化-表面改性策略实现无烟煤硬炭阳极钠离子存储性能的改善。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-12 DOI: 10.1002/cphc.202500054

Huibo Qiao, Ning Dang, Chenxi He, Jin Zhang, Zhiheng Zhao, Baoshu Chen, Tianbao Zhao, Junhong Tao, Wanqi Ying

{"title":"Realizing improved sodium-ion storage for anthracite-derived hard carbon anode by activation-surface modification strategy.","authors":"Huibo Qiao, Ning Dang, Chenxi He, Jin Zhang, Zhiheng Zhao, Baoshu Chen, Tianbao Zhao, Junhong Tao, Wanqi Ying","doi":"10.1002/cphc.202500054","DOIUrl":"https://doi.org/10.1002/cphc.202500054","url":null,"abstract":"Anthracite offers several advantages, including a high carbon content, a well-developed aromatic structure, and low cost, making it a cost-effective precursor for hard carbon anodes in sodium-ion batteries. However, its higher impurity levels and fewer surface defects limit its broader applications. In this study, we proposed an activation and surface modification strategy to address its shortcomings, specifically low sodium storage-ion capacity and low initial coulombic efficiency (ICE). ZnCl2 was used as an activator to introduce numerous pores into the structure of hard carbon, thereby increasing the sodium-ion storage sites. Furthermore, soft carbon pitch was applied to refine the oversized pore structure in hard carbon, improving its initial coulombic efficiency. As a result, the modified hard carbon achieved a reversible capacity of 240 mAh g⁻¹ and an initial coulombic efficiency of 82.52% at a discharge rate of 0.1C. The PCAC-1200 also demonstrated good cycle stability with 76.2% retention after 100 cycles. Besides, it still has a capacity of 101.2 mAh g⁻¹ at a high magnification of 5C. We believe that this anthracite hard carbon anode prepared by activation-surface modification strategy shows good application prospects in the field of sodium-ion energy storage.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500054"},"PeriodicalIF":2.3,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143981181","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

UNDERSTANDING THE IRMPD SPECTRA OF HYDROGEN-TAGGED PROTONATED BETAINE: VIBRATIONAL CONFINEMENT COUNTERACTS THE HYDROGEN BONDING INDUCED O-H STRETCHING FREQUENCY DOWNSHIFT. 氢标记质子甜菜碱的irmpd光谱：振动约束抵消氢键诱导的o-h拉伸频率降频。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-12 DOI: 10.1002/cphc.202401089

Ljupcho Pejov, Blagoj Achevski

{"title":"UNDERSTANDING THE IRMPD SPECTRA OF HYDROGEN-TAGGED PROTONATED BETAINE: VIBRATIONAL CONFINEMENT COUNTERACTS THE HYDROGEN BONDING INDUCED O-H STRETCHING FREQUENCY DOWNSHIFT.","authors":"Ljupcho Pejov, Blagoj Achevski","doi":"10.1002/cphc.202401089","DOIUrl":"https://doi.org/10.1002/cphc.202401089","url":null,"abstract":"Finite - temperature vibrational spectra of protonated betaine and its noncovalently bonded clusters with molecular hydrogen were modeled using Lagrangian dynamics with the atom-centered density matrix propagation scheme (ADMP). The focus was put on the O-H stretching mode, which serves as a primary indicator of the type and strength of the noncovalent intermolecular interactions. The computed anharmonic O-H stretching vibrational frequency shifts in the case of protonated betaine upon tagging with H2 at the OH group site at 40 K is in quantitative agreement with the experimental IRMPD data. The shifts computed from simulations at 4 K contain only the harmonic contributions. We have found out that this is a consequence of vibrational confinement of the O-H oscillator caused by the H2 tagger, which remains close to the vibrating atoms throughout the simulation and counteracts the frequency red shift induced by the weak hydrogen bonding interaction. Confinement relaxation at 40 K enables the OH oscillator to span a wider range of the vibrational potential curve, sampling significantly the more anharmonic parts thereof. Application of the two-trace two-dimensional correlation analysis of the computed vibrational density of states spectra enables a clear distinction between bands of different origin to be made.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202401089"},"PeriodicalIF":2.3,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143967032","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

Planar patterning design and energy storage performance comparison of laser-induced graphene flexible supercapacitors. 激光诱导石墨烯柔性超级电容器的平面图像化设计及储能性能比较。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-12 DOI: 10.1002/cphc.202500145

Qi Xiong, Jiaheng Xu, Huiting Li, Jianghai Li, Lin Li, Jinyu Wu, Xianqing Liang, Wenzheng Zhou, Guangxu Li, Zhiqiang Lan, Haifu Huang

{"title":"Planar patterning design and energy storage performance comparison of laser-induced graphene flexible supercapacitors.","authors":"Qi Xiong, Jiaheng Xu, Huiting Li, Jianghai Li, Lin Li, Jinyu Wu, Xianqing Liang, Wenzheng Zhou, Guangxu Li, Zhiqiang Lan, Haifu Huang","doi":"10.1002/cphc.202500145","DOIUrl":"https://doi.org/10.1002/cphc.202500145","url":null,"abstract":"Laser-induced graphene (LIG) has attracted considerable attention for its efficient production, controllable process, versatile precursors, and patterning capabilities. However, LIG supercapacitors (LIG SCs) devices exhibit low operating voltages and varying performance. based on patterning. Moreover, laser power significantly affects device performance. Herein, the energy storage performance of LIG SCs devices in a variety of patterns and at different laser powers is investigated. The LIG SCs device based on the interdigital pattern shows best performance compared with the spiral pattern, mirror circular pattern and concentric circular pattern LIG device. This superior performance can be attributed to the extended ion transport pathways and limited kinetic properties in interdigital pattern. When the laser power is 2.75 W, the area-specific capacitance of the interdigital LIG SCs is up to 10.78 mF cm⁻2 at 0.2 mA cm⁻2, wide operating voltage (1.8 V) and a maximum energy density of 4.85 μWh cm⁻2. Additionally, it maintained 84.1% of its capacitance after 8,000 charge-discharge cycles and achieved an area-specific capacitance of 8.33 mF cm⁻2 when bent at an angle of 60°, suggesting outstanding cycle stability and excellent flexibility of LIG SCs. This work also provides insights for developing patterned flexible supercapacitors.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500145"},"PeriodicalIF":2.3,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143983117","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

Elucidating the structures of substituted adamantyl esters and ethers using rotational spectroscopy and computations. 用旋转光谱和计算方法阐明取代金刚烷酯和取代金刚烷醚的结构。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-12 DOI: 10.1002/cphc.202500035

Nataša Burić, Donatella Loru, Jasna Alić, Marina Šekutor, Melanie Schnell, Pablo Pinacho

引用次数: 0

Investigating the electrochemical reduction of CO2 to oxalate in aprotic solvents with Pb. 研究了含铅非质子溶剂中CO2电化学还原为草酸盐的过程。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-05-11 DOI: 10.1002/cphc.202500136

Jinfeng Jia, Jiayi Chen, Ioannis Katsounaros, Emiel de Smit, Saifudin M Abubakar, Shuo Chen, Lei Wang, Yanwei Lum

引用次数: 0