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Graphdiyne: A promising nonlinear optical material modulated by tetrahedral alkali-metal nitrides
摘要： A new series of the functionalized graphdiyne (GDY) material was designed by adsorbing the tetrahedral Li3NM molecules on the largely delocalized π-conjugated GDY surface, namely Li3NM@GDY (M = Li, Na, K), and its structure, chemical stability, electronic property, and the first hyperpolarizability were investigated by using the density functional theory computations. Our results reveal that the Li3NM molecules can interact with three triangular holes on the GDY surface, in which the van der Waals interactions play a crucial role in enhancing the structural stability. Meanwhile, the total NPA charges on the Li3NM molecules are gradually increased from Li to K, and the Li3NM molecules can transfer an electron to GDY, forming intramolecular electron donor and acceptor pairs. All of studied complexes exhibit the giant static first hyperpolarizabilities (βtot), up to ~2.88 × 105 a.u. for Li3NK@GDY, which can be explained by two-level expression from the TDDFT calculations. This study will inevitably stimulate further synthesis of the novel graphdiyne-based nonlinear optical materials.
关键词： Graphdiyne,Electronic structure,TDDFT,Charge transfer,Nonlinear optical property
更新于2025-09-23 15:23:52
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Graphdiyne: Bridging SnO <sub/>2</sub> and Perovskite in Planar Solar Cells
摘要： The collocation between charge transport layer and photoactive layer is extremely critical in solar energy conversion devices. More recently, it is especially prominent for promising planar perovskite solar cell based on SnO2 electron transfer layer (ETL) due to its unmatched photogenerated electron and hole extraction rates. Thereby, graphdiyne (GDY) with multi-roles has been incorporated to maximize the collocation between SnO2 and perovskite regarding perspectives of electron extraction rate optimization as well as the interface engineering for perovskite growth inducement and interfacial defect passivation, enabling such interfacial function towards both perovskite crystallization process and subsequent photovoltaic service duration. The GDY doped SnO2 layer finally results 4-times improved electron mobility and more facilitated band alignment. Simultaneously, the enhanced hydrophobicity effectively inhibits heterogeneous perovskite nucleation, contributing to high quality film with diminished grain boundaries and lower defect density. The systematical density functional theory study has further indicated that freshly formed C-O σ bond resulted electrical property enhancement and the passivated Pb-I antisite defects are both originated from GDY introduction. The 21.11% power conversion efficiency with negligible hysteresis indicate such scenario may trigger unlimited reverie of promising GDY materials and provide more insights on elaborately interfacial design in perovskite solar cells.
关键词： graphdiyne,SnO2,solar cells,perovskite,interface engineering
更新于2025-09-23 15:21:01
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Graphdiyne: Bridging SnO <sub/>2</sub> and Perovskite in Planar Solar Cells
摘要： The collocation between charge transport layer and photoactive layer is extremely critical in solar energy conversion devices. More recently, it is especially prominent for promising planar perovskite solar cell based on SnO2 electron transfer layer (ETL) due to its unmatched photogenerated electron and hole extraction rates. Thereby, graphdiyne (GDY) with multi-roles has been incorporated to maximize the collocation between SnO2 and perovskite regarding perspectives of electron extraction rate optimization as well as the interface engineering for perovskite growth inducement and interfacial defect passivation, enabling such interfacial function towards both perovskite crystallization process and subsequent photovoltaic service duration. The GDY doped SnO2 layer finally results 4-times improved electron mobility and more facilitated band alignment. Simultaneously, the enhanced hydrophobicity effectively inhibits heterogeneous perovskite nucleation, contributing to high quality film with diminished grain boundaries and lower defect density. The systematical density functional theory study has further indicated that freshly formed C-O σ bond resulted electrical property enhancement and the passivated Pb-I antisite defects are both originated from GDY introduction. The 21.11% power conversion efficiency with negligible hysteresis indicate such scenario may trigger unlimited reverie of promising GDY materials and provide more insights on elaborately interfacial design in perovskite solar cells.
关键词： SnO2,Solar Cells,Graphdiyne,Perovskite,Interface Engineering
更新于2025-09-23 15:21:01
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Graphdiynea??Based Flexible Photodetectors with High Responsivity and Detectivity
摘要： Graphdiyne (GDY), a newly emerging 2D carbon allotrope, has been widely explored in various fields owing to its outstanding electronic properties such as the intrinsic bandgap and high carrier mobility. Herein, GDY-based photoelectrochemical-type photodetection is realized by spin-coating ultrathin GDY nanosheets onto flexible poly(ethylene terephthalate) (PET) substrates. The GDY-based photodetectors (PDs) demonstrate excellent photo-responsive behaviors with high photocurrent (Pph, 5.98 μA cm-2), photoresponsivity (Rph, 1086.96 μA W-1), detectivity (7.31 × 1010 Jones), and excellent long-term stability (more than 1 month). More importantly, the PDs maintain an excellent Pph after 1000 cycles of bending (4.45 μA cm-2) and twisting (3.85 μA cm-2), thanks to the great flexibility of the GDY structure that is compatible with the flexible PET substrate. Density functional theory (DFT) calculations are adopted to explore the electronic characteristics of GDY, which provides evidence for the performance enhancement of GDY in alkaline electrolyte. In this way, the GDY-based flexible PDs can enrich the fundamental study of GDY and pave the way for the exploration of GDY heterojunction-based photodetection.
关键词： photoelectrochemical,photodetection,graphdiyne,flexible devices,long-term stability
更新于2025-09-23 15:19:57
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Superhydrophilic Graphdiyne Accelerates Interfacial Mass/Electron Transportation to Boost Electrocatalytic and Photoelectrocatalytic Water Oxidation Activity
摘要： Graphdiyne (GDY), with a highly π-conjugated structure of sp2- and sp-hybridized carbon, has triggered a huge interest in water splitting. However, all of the systems perform with no consideration of the surface wettability of GDY. Herein, for the first time, the fabrication of superhydrophilic GDY electrode via air-plasma for oxygen evolution is described. As a representative catalyst, ultrathin CoAl-LDH (CO3 2?) nanosheets have been successfully assembled onto the superhydrophilic GDY electrostatically. The resulting superhydrophilic CoAl-LDH/GDY electrode exhibites superior activity with an overpotential of ≈258 mV to reach 10 mA cm?2. The turnover frequency (TOF) is calculated to be ≈0.60 s?1 at η = 300 mV, which is the best record in both CoAl-based and GDY-based layered double hydroxides (LDH) electrocatalysts for oxygen evolution. Density functional theory (DFT) calculations reveal that superhydrophilic GDY has stronger interactions with catalysts and attracts H2O molecules around catalysts, thus facilitating interfacial mass/electron transportation. Further, the fabrication is capable of improving the photoelectrochemical oxygen evolution activity remarkably. The results show the great potential of superhydrophilic GDY to boost water oxidation activity by promoting interfacial mass/electron transportation.
关键词： superhydrophilic graphdiyne,water oxidation,electrocatalysis,photoelectrocatalysis
更新于2025-09-19 17:15:36
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Graphdiyne Derivative as Multifunctional Solid Additive in Binary Organic Solar Cells with 17.3% Efficiency and High Reproductivity
摘要： Morphology tuning of the blend film in organic solar cells (OSCs) is a key approach to improve device efficiencies. Among various strategies, solid additive is proposed as a simple and new way to enable morphology tuning. However, there exist few solid additives reported to meet such expectations. Herein, chlorine-functionalized graphdiyne (GCl) is successfully applied as a multifunctional solid additive to fine-tune the morphology and improve device efficiency as well as reproductivity for the first time. Compared with 15.6% efficiency for control devices, a record high efficiency of 17.3% with the certified one of 17.1% is obtained along with the simultaneous increase of short-circuit current (Jsc) and fill factor (FF), displaying the state-of-the-art binary organic solar cells at present. The redshift of the film absorption, enhanced crystallinity, prominent phase separation, improved mobility, and decreased charge recombination synergistically account for the increase of Jsc and FF after introducing GCl into the blend film. Moreover, the addition of GCl dramatically reduces batch-to-batch variations benefiting mass production owing to the nonvolatile property of GCl. All these results confirm the efficacy of GCl to enhance device performance, demonstrating a promising application of GCl as a multifunctional solid additive in the field of OSCs.
关键词： graphdiyne derivative,binary organic solar cells,high fill factor,high efficiency,solid additives
更新于2025-09-19 17:13:59
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Graphdiyne for Ultrashort Pulse Generation in an Erbium-Doped Hybrid Mode-Locked Fiber Laser
摘要： An erbium-doped hybrid passively mode-locked ?ber laser based on few-layer graphdiyne (GDY) saturable absorber (SA) has been investigated for the ?rst time. Hybrid mode-locked ?ber laser is composed of non-linear polarization rotation (NPR) technology and GDY-SA. The central wavelength, pulse width and repetition rate of the output pulse are 1530.7 nm, 690.2 fs and 14.7 MHz, respectively. Compared with the passively mode-locked pulse laser with GDY-SA or NPR technology alone, the output pulse width of hybrid passively mode-locked ?ber laser is reduced more than 50 fs. It is demonstrated that the performance of GDY can be potentially applied in ultrafast laser.
关键词： saturable absorber,?ber laser,ultrafast photonics,mode-locked,graphdiyne
更新于2025-09-11 14:15:04
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High-Yield Formation of Graphdiyne Macrocycles Through On-Surface Assembling and Coupling Reaction
摘要： Rationally designed halogenated hydrocarbons are widely used building blocks to fabricate covalent-bonded carbon nanostructures on surface through a reaction pathway involving generation and dissociation of organometallic intermediates and irreversible covalent bond formation. Here we provide a comprehensive picture of the on-surface-assisted homocoupling reaction of 1,3-bis(2-bromoethynyl)benzene on Au(111), aiming for the synthesis of graphdiyne nanostructures. Submolecular resolution scanning tunneling microscopy and noncontact atomic force microscopy observations identify the organometallic intermediates and their self-assemblies formed in the dehalogenation process. The demetallization of the organometallic intermediates at elevated temperatures produces butadiyne moieties that spontaneously formed two different covalent structures, i.e. graphdiyne zigzag chains and macrocycles, whose ratio was found to depend on the initial coverage of organometallic intermediates. At the optimal condition, the stepwise demetallization and cyclization led to a high yield production of graphdiyne macrocycles up to 95 %. Statistical analysis and theoretical calculations suggested that the favored formation of macrocycles was resulted from the complex interplay between thermodynamic and kinetic processes involving the organometallic bonded intermediates and the covalently bonded butadiyne moieties.
关键词： on-surface reaction,graphdiyne macrocycle,organometallic intermediate,scanning tunneling microscopy,noncontact atomic force microscopy,thermodynamic and kinetic control
更新于2025-09-10 09:29:36
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High-Yield and Damage-free Exfoliation of Layered Graphdiyne in Aqueous Phase
摘要： The two-dimensional carbon material graphdiyne (GDY) holds great promise as a semiconductor and porous material, however, exfoliation of bulk GDY into single- or few-layered GDY in the aqueous phase remains a challenge. We report an efficient method for the damage-free exfoliation of bulk GDY into single- or few-layered GDY with high yield in an aqueous solution of inorganic salts (e.g., Li2SiF6). This was confirmed by spherical-aberration-corrected scanning transmission electron microscopy, scanning/transmission electron microscopy, atomic force microscopy, Fourier transform infrared/Raman spectroscopy, X-ray photoelectron spectroscopy. The method gives high exfoliation efficiency (75 wt %) without creating additional structural defects or oxides in the exfoliated GDY. Theoretical calculations suggest that non-covalent adsorption of the anion, diffusion of the cation, and subsequent repulsive forces between adjacent flakes are the main driving force for the efficient exfoliation.
关键词： non-covalent adsorption,carbon materials,graphdiyne,surface chemistry,liquid-phase exfoliation
更新于2025-09-09 09:28:46