The Journal of Physical Chemistry C最新文献

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Controlled Synthesis of MoNi4 Ultrathin Nanosheet Arrays as an Efficient Bifunctional Electrocatalyst for Urea-Assisted Hydrogen Production 受控合成 MoNi4 超薄纳米片阵列作为尿素辅助制氢的高效双功能电催化剂
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-12 DOI: 10.1021/acs.jpcc.4c03904
Guoliang Gao, Guang Yang, Xueqing Gao, Yifan Li, Rong Huang, Yi Cui
{"title":"Controlled Synthesis of MoNi4 Ultrathin Nanosheet Arrays as an Efficient Bifunctional Electrocatalyst for Urea-Assisted Hydrogen Production","authors":"Guoliang Gao, Guang Yang, Xueqing Gao, Yifan Li, Rong Huang, Yi Cui","doi":"10.1021/acs.jpcc.4c03904","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c03904","url":null,"abstract":"The utilization of water electrolysis as a technology for industrial hydrogen production is considered highly appealing. Currently, the sluggish anodic oxygen evolution reaction (OER), which involves a four-electron transfer process, hampers the overall efficiency of water splitting. The coupling of urea electrocatalysis with the hydrogen evolution reaction (HER) holds significant promise in achieving energy-efficient hydrogen production. Here, we present a study showcasing the in situ synthesis of arrays consisting of ultrathin MoNi<sub>4</sub> nanosheets on a Ni foam (NF) substrate (MoNi<sub>4</sub>/NF). The catalyst exhibits high bifunctional activity due to its excellent intrinsic activity, increased exposure of active sites, and favorable morphology and structure of the electrode material. Specifically, overpotentials as low as 146 mV and 1.42 V are sufficient to drive a current density of 100 mA cm<sup>–2</sup> for the HER and urea oxidation reaction (UOR), respectively. Moreover, the utilization of optimized MoNi<sub>4</sub>/NF as a dual-electrode catalyst enables the provision of a current density of 100 mA cm<sup>–2</sup> for hybrid water splitting when operating at a cell voltage of 1.54 V. This study presents a novel concept for the advancement of effective and enduring bifunctional electrocatalysts capable of facilitating both the HER and the UOR.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597481","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
Tuning Excitonic Properties of Monochalcogenides via Design of Janus Structures 通过设计杰纳斯结构调整单质钙钛矿的激子特性
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-12 DOI: 10.1021/acs.jpcc.4c01813
Mateus B. P. Querne, Alexandre C. Dias, Anderson Janotti, Juarez L. F. Da Silva, Matheus P. Lima
{"title":"Tuning Excitonic Properties of Monochalcogenides via Design of Janus Structures","authors":"Mateus B. P. Querne, Alexandre C. Dias, Anderson Janotti, Juarez L. F. Da Silva, Matheus P. Lima","doi":"10.1021/acs.jpcc.4c01813","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c01813","url":null,"abstract":"Two-dimensional (2D) Janus structures offer a unique range of properties as a result of their symmetry breaking, resulting from the distinct chemical composition on each side of the monolayers. Here, we report a theoretical investigation of 2D Janus <i>Q</i>′<i>A</i>′<i>AQ P</i>3<i>m</i>1 monochalcogenides from group IV (<i>A</i> and <i>A</i>′ = Ge and Sn; <i>Q</i>, <i>Q</i>′ = S and Se) and 2D non-Janus <i>QAAQ P</i>3̅<i>m</i>1 counterparts. Our theoretical framework is based on density functional theory calculations combined with maximally localized Wannier functions and tight-binding parametrization to evaluate the excitonic properties. The phonon band structures exhibit exclusively real (nonimaginary) branches for all materials. Particularly, SeGeSnS has greater energetic stability than its non-Janus counterparts, representing an outstanding energetic stability among the investigated materials. However, SGeSnS and SGeSnSe have higher formation energies than the already synthesized MoSSe, making them more challenging to grow than the other investigated structures. The electronic structure analysis demonstrates that materials with Janus structures exhibit band gaps wider than those of their non-Janus counterparts, with the absolute value of the band gap predominantly determined by the core rather than the surface composition. Moreover, exciton binding energies range from 0.20 to 0.37 eV, reducing band gap values in the range of 21% to 32%. Thus, excitonic effects influence the optoelectronic properties more than the point-inversion symmetry breaking inherent in the Janus structures; however, both features are necessary to enhance the interaction between the materials and sunlight. We also found anisotropic behavior of the absorption coefficient, which was attributed to the inherent structural asymmetry of the Janus materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597428","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
Chemical Modulation of Charge Transport Perpendicular to the Molecular Plane 垂直于分子平面的电荷传输化学调制
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-12 DOI: 10.1021/acs.jpcc.4c02372
Parisa Yasini, Stuart Shepard, Manuel Smeu, Eric Borguet
{"title":"Chemical Modulation of Charge Transport Perpendicular to the Molecular Plane","authors":"Parisa Yasini, Stuart Shepard, Manuel Smeu, Eric Borguet","doi":"10.1021/acs.jpcc.4c02372","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c02372","url":null,"abstract":"The electronic structure of molecules can have a considerable effect on charge transport through molecular junctions. However, this is known only where molecular anchoring groups define the transport direction to be along the molecular plane. It is not clear how different chemical substituents can affect conductance perpendicular to the molecular plane. In this study, the conductance measurement perpendicular to the plane of mesitylene substituted with electron-withdrawing groups (e.g., NO<sub>2</sub>, Br) and electron-donating groups (e.g., CH<sub>3</sub>) showed that the conductance increases by introducing electron-withdrawing groups and decreases as electron-donating groups are added to the mesitylene molecule. These results are supported by density functional theory and nonequilibrium Green’s function calculations. We demonstrated that the changes in the conductance perpendicular to the molecular plane correlate well with the Hammett constant of the corresponding functional groups, indicating the importance of the nature and strength of chemical substituents on the degree of conductance modulations, at least for mesitylene derivatives. The generalization of the Hammett parameters to the perpendicular charge transport through single molecules could serve as a predictive framework, motivating the design and fabrication of molecular devices with desired functionalities.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597480","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
Single Atomic Catalyst of Hydrogen Evolution Supported by Semimetallic γ-GeSe 半金属 γ-GeSe 支持的单原子氢气进化催化剂
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-12 DOI: 10.1021/acs.jpcc.4c02261
Dan Liang, Hejin Yan, Yongqing Cai
{"title":"Single Atomic Catalyst of Hydrogen Evolution Supported by Semimetallic γ-GeSe","authors":"Dan Liang, Hejin Yan, Yongqing Cai","doi":"10.1021/acs.jpcc.4c02261","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c02261","url":null,"abstract":"Motivated by the recent synthesis of a new polymorph of germanium selenide (γ-GeSe) with a honeycomb lattice and an astonishingly high conductivity (even higher than graphite), here we conduct a study on the hydrogen evolution reaction (HER) electrocatalytic performance and electronic properties of γ-GeSe with respect to the thickness effect from monolayer (1L) to trilayer (3L), along with the defect effect. The band structure of γ-GeSe exhibits a camel’s back-like structure near the Γ point, existing for all the layers and in the presence of dilute Se vacancy and surface adsorbate like the Pt atom, and a narrow bandgap ranging from 0.544 eV for 1L to 0.252 eV for 3L. We find that pristine γ-GeSe is electrocatalytically inert for all the layers with an endothermic uptake of hydrogen, as indicated by the calculated Gibbs free energy (Δ<i>G</i><sub>H</sub>). However, upon introduction of Se vacancies and surface Pt adsorbates, the HER performance is enhanced, with the HER activity of 1L γ-GeSe surpassing those of bilayer (2L) and 3L γ-GeSe. Moreover, an increase in defect concentration and thickness leads to a decrease in bandgap, developing semimetallic characteristics. With the absence of a transition element and solely s and p orbitals, semimetallic γ-GeSe is unique and holds great promise as a support for fabricating a single atomic catalyst for HER, and our work offers valuable insights into the rational design of 2D electrocatalysts.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597427","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
Path ahead: Tackling the Challenge of Computationally Estimating Lithium Diffusion in Cathode Materials 前进之路:应对计算估算阴极材料中锂扩散的挑战
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-11 DOI: 10.1021/acs.jpcc.4c00960
Laura Bonometti, Loredana E. Daga, Riccardo Rocca, Naiara L. Marana, Silvia Casassa, Maddalena D’Amore, Kari Laasonen, Martin Petit, Fabrizio Silveri, Mauro F. Sgroi, Anna M. Ferrari, Lorenzo Maschio
{"title":"Path ahead: Tackling the Challenge of Computationally Estimating Lithium Diffusion in Cathode Materials","authors":"Laura Bonometti, Loredana E. Daga, Riccardo Rocca, Naiara L. Marana, Silvia Casassa, Maddalena D’Amore, Kari Laasonen, Martin Petit, Fabrizio Silveri, Mauro F. Sgroi, Anna M. Ferrari, Lorenzo Maschio","doi":"10.1021/acs.jpcc.4c00960","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c00960","url":null,"abstract":"In the roadmap toward designing new and improved materials for Lithium ion batteries, the ability to estimate the diffusion coefficient of Li atoms in electrodes, and eventually solid-state electrolytes, is key. Nevertheless, as of today, accurate prediction through computational tools remains challenging. Its experimental measurement does not appear to be much easier. In this work, we devise a computational protocol for the determination of the Li-migration energy barrier and diffusion coefficient, focusing on a common cathode material such as LiNiO<sub>2</sub>, which represents a prototype of the widely adopted NMC (LiNi<sub>1–<i>x</i>–<i>y</i></sub>Mn<sub><i>x</i></sub>Co<sub><i>y</i></sub>O<sub>2</sub>) class of materials. Different methodologies are exploited, combining ab initio metadynamics, path sampling, and density functional theory. Furthermore, we propose a novel, fast, and simple 1D approximation for the estimation of the effective frequency. The outlined computational protocol aims to be generally applicable to Lithium diffusion in other materials and components for batteries, including anodes and solid electrolytes.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597478","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
Key Role of Electronic and Structural Properties in Regulating Intersystem Crossing: An In-Depth Investigation on Naphthalene-Diimide Triads for Thermally Activated Delayed Fluorescence Applications 电子和结构特性在调节系统间交叉中的关键作用:用于热激活延迟荧光的萘二亚胺三元组的深入研究
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-11 DOI: 10.1021/acs.jpcc.4c02033
Federico Coppola, Mushraf Hussain, Jianzhang Zhao, Ahmed M. El-Zohry, Mariachiara Pastore
{"title":"Key Role of Electronic and Structural Properties in Regulating Intersystem Crossing: An In-Depth Investigation on Naphthalene-Diimide Triads for Thermally Activated Delayed Fluorescence Applications","authors":"Federico Coppola, Mushraf Hussain, Jianzhang Zhao, Ahmed M. El-Zohry, Mariachiara Pastore","doi":"10.1021/acs.jpcc.4c02033","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c02033","url":null,"abstract":"We report an extensive theoretical investigation of the photophysical properties of new carbazole core-substituted naphthalene-diimide dyes to elucidate the effects of different donor–acceptor arrangements on the direct and reverse intersystem crossing rates. These dyes were recently experimentally characterized using steady-state and time-resolved spectroscopy ( <cite><i>J. Phys. Chem.\u0000B</i></cite> <span>2021</span>, 125, 10813). We analyzed the molecular structures of ground states, singlet and triplet excited states, excitation energies, orbital characteristics, and spin–orbit couplings using density functional theory (DFT)/time-dependent DFT calculations to determine the rates of the electronic spin-flip processes. Our findings reveal how different donor–acceptor configurations, by modulating ground and excited state conformational dynamics, may significantly influence the energetic landscape of singlet and triplet electronic states, their nature, and thus the extent of spin–orbit couplings, finally impacting the intersystem crossing rate constants and the reverse ones for thermally activated delayed fluorescence applications.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597479","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
Partial Water Intrusion and Extrusion in Hydrophobic Nanopores for Thermomechanical Energy Dissipation 疏水性纳米孔中的部分水渗入和挤出以实现热机械能量耗散
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-11 DOI: 10.1021/acs.jpcc.4c02900
Gonçalo Paulo, Luis Bartolomé, Oleksandr Bondarchuk, Simone Meloni, Yaroslav Grosu, Alberto Giacomello
{"title":"Partial Water Intrusion and Extrusion in Hydrophobic Nanopores for Thermomechanical Energy Dissipation","authors":"Gonçalo Paulo, Luis Bartolomé, Oleksandr Bondarchuk, Simone Meloni, Yaroslav Grosu, Alberto Giacomello","doi":"10.1021/acs.jpcc.4c02900","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c02900","url":null,"abstract":"Forced wetting (intrusion) and spontaneous dewetting (extrusion) of hydrophobic/lyophobic nanoporous materials by water/nonwetting liquid are of great importance for a broad span of technological and natural systems such as shock-absorbers, molecular springs, separation, chromatography, ion channels, nanofluidics, and many more. In most of these cases, the process of intrusion-extrusion is not complete due to the stochastic nature of external stimuli under realistic operational conditions. However, understanding of these partial processes is limited, as most of the works are focused on an idealized complete intrusion-extrusion cycle. In this work, we show an experimental system operating under partial intrusion/extrusion conditions and present a simple model that captures its main features. We rationalize these operational conditions in terms of the pore entrance and cavity size distributions of the material, which control the range of intrusion/extrusion pressures.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597482","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
Structural Phase Transition in BiVO4 Nanosheets under High Pressure 高压下生物氧化物纳米片的结构相变
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-11 DOI: 10.1021/acs.jpcc.4c03113
Benyuan Cheng, Hongbo Lou, Zhidan Zeng, Yi Liu, Qiaoshi Zeng
{"title":"Structural Phase Transition in BiVO4 Nanosheets under High Pressure","authors":"Benyuan Cheng, Hongbo Lou, Zhidan Zeng, Yi Liu, Qiaoshi Zeng","doi":"10.1021/acs.jpcc.4c03113","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c03113","url":null,"abstract":"Bismuth vanadate (BiVO<sub>4</sub>) is a well-known photoanode in photocatalytic engineering. The structural stability and tunability of BiVO<sub>4</sub> are of great interest and importance but have not been well-explored, especially under pressure. Here, we studied the structure evolution of fergusonite-type BiVO<sub>4</sub> nanosheets using <i>in situ</i> synchrotron X-ray diffraction, Raman spectroscopy, ultraviolet–visible absorption spectroscopy, and optical microscopy analysis up to ∼41.7 GPa; despite the previously reported fergusonite to scheelite transition (∼5 GPa in this research) and scheelite to a monoclinic structure transition (∼15 GPa in this research), a potential second-order phase transition at ∼10 GPa in the scheelite phase and an amorphization at ∼16.7 GPa in a high-pressure monoclinic phase have been observed for the first time in this work. These results suggest that BiVO<sub>4</sub> nanosheets exhibit a more complex phase transition routine than their bulk or other nanocounterparts under pressure, which could promote our fundamental understanding and guide the application of orthovanadates.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597484","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
Virtual Special Issue on Machine Learning in Physical Chemistry Volume 2 物理化学中的机器学习》虚拟特刊第 2 卷
IF 3.3 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-11 DOI: 10.1021/acs.jpcc.4c03824
Andrew L. Ferguson*,  and , Jim Pfaendtner*, 
{"title":"Virtual Special Issue on Machine Learning in Physical Chemistry Volume 2","authors":"Andrew L. Ferguson*,&nbsp; and ,&nbsp;Jim Pfaendtner*,&nbsp;","doi":"10.1021/acs.jpcc.4c03824","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c03824","url":null,"abstract":"","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141592651","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
Role of C–F Bonding on the Optical Properties of Fluorinated Graphene Oxide C-F 键对氟化氧化石墨烯光学特性的作用
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2024-07-10 DOI: 10.1021/acs.jpcc.4c03031
Moupriya Mukherjee, Sakshi Bhagat, Muhammed Arshad Thottappali, Parveen Garg, Asif Ikbal Nurani, Biswarup Satpati, Shamima Hussain, Samanwita Pal, Uday Deshpande, Soumyaditya Sutradhar, Jiří Pfleger, Goutam Pramanik
{"title":"Role of C–F Bonding on the Optical Properties of Fluorinated Graphene Oxide","authors":"Moupriya Mukherjee, Sakshi Bhagat, Muhammed Arshad Thottappali, Parveen Garg, Asif Ikbal Nurani, Biswarup Satpati, Shamima Hussain, Samanwita Pal, Uday Deshpande, Soumyaditya Sutradhar, Jiří Pfleger, Goutam Pramanik","doi":"10.1021/acs.jpcc.4c03031","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c03031","url":null,"abstract":"Graphene oxide (GO) exhibits very poor photoluminescence (PL) characteristics because of the nonradiative recombination of electron–hole pairs. One of the crucial approaches for the enhancement of the optical features of GO is functionalization. In this study, we present a novel catalyst-free, rapid, one-step, aqueous-phase synthetic approach using SELECTFLUOR under mild conditions that provide access to highly photoluminescent fluorinated graphene oxide (FGO) emitting in the visible region. Time-resolved fluorescence spectroscopy and femtosecond transient absorption spectroscopy revealed that the enhanced PL is due to the increased π* → π transition and weaker electron–phonon interactions in FGO. Most importantly, the structure and composition analyses using <sup>19</sup>F NMR and X-ray photoelectron spectroscopy suggest that the C–F bond on the basal plane neighboring to the aromatic rings is the key factor behind the enhancement of the fluorescence of FGO. Identification of the underlying C–F bonding features behind the emergence of strong orange fluorescence will contribute immensely to the fundamental understanding of the structure and optical property relationship of FGO. Moreover, strong orange fluorescence remains stable in a solid thin film of FGO, which offers a unique solution-processable route toward the integration of FGO in solid-state optoelectronic devices.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597485","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
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