Enhanced Charge Transport Research Articles

Effective N‐Doping of Non‐Fullerene Acceptor via Sequential Deposition Enables High‐Efficiency Organic Solar Cells

AbstractCharge transport in the active layer, which can be effectively modulated by molecular doping of organic semiconductors, significantly affects the photovoltaic performance of organic solar cells (OSCs). However, it is difficult to control the dopant distribution in the bulk heterojunction (BHJ) films, which hinders efficient doping in OSCs. Herein, an effective n‐doping strategy is developed via sequential deposition (SD) of D18 donor and doped acceptor. The favorable vertical component distribution in SD films helps to optimize carrier transport pathways. The SD method confines the n‐dopant N‐DMBI to the acceptor layer, allowing positive effects of molecular doping. Consequently, the doped SD device exhibits superior charge transport with suppressed charge recombination, lower trap density, and enhanced charge extraction compared to the undoped one, resulting in a high power conversion efficiency of 19.55% for D18/L8‐BO binary OSCs. In addition, the doping does not affect the thermal stability of the devices, with the doped SD device retaining over 90% of its initial efficiency after 1200 h of heating at 80 °C. The universality of the SD doping method is also verified in other non‐fullerene acceptor systems. These results demonstrate the great potential of SD doping strategy for building high‐performance OSCs with enhanced charge transport.

Enhanced charge transport in 2D inorganic molecular crystals constructed with charge‐delocalized molecules

AbstractOutstanding charge transport in molecular crystals is of great importance in modern electronics and optoelectronics. The widely adopted strategies to enhance charge transport, such as restraining intermolecular vibration, are mostly limited to organic molecules, which are nearly inoperative in 2D inorganic molecular crystals currently. In this contribution, charge transport in 2D inorganic molecular crystals is improved by integrating charge‐delocalized Se8 rings as building blocks, where the delocalized electrons on Se8 rings lift the intermolecular orbitals overlap, offering efficient charge transfer channels. Besides, α‐Se flakes composed of charge‐delocalized Se8 rings possess small exciton binding energy. Benefitting from these, α‐Se flake exhibits excellent photodetection performance with an ultrafast response rate (~5 μs) and a high detectivity of 1.08 × 1011 Jones. These findings contribute to a deeper understanding of the charge transport of 2D inorganic molecular crystals composed of electron‐delocalized inorganic molecules and pave the way for their potential application in optoelectronics.

Ionic Liquid‐Induced 1D Perovskite: Exploring 1D Perovskite Structure to 1D/3D Heterojunction‐Based Photovoltaics

AbstractThe synergistic utilization of low‐dimensional perovskites with 3D perovskite architectures represents a pervasive approach for fabrication of high‐performance and enduring perovskite solar cells (PSCs). In this work, four distinct ionic liquids (ILs) with distinct cations, were introduced on the surface of 3D perovskite to induce the formation of 1D perovskite.Starting with the analysis of 1D/3D heterojunction structures, the assessment foucsed on the binding energies in four ILs‐induced 1D/3D heterojunctions, comparing electron cloud density within 1D/3D structures, and calculating the formation energies associated with iodine and lead defects within these four 1D/3D perovskite structures via DFT calculations. Furthermore, the time‐resolved grazing‐incidence wide‐angle X‐ray scattering technique, as employed in this study, offers real‐time insights into the phase‐transition occurring during the process of ILs coating and the formation of 1D/3D heterojunctions. The well‐designed and optimized 1D perovskite layer significantly reduces the residual lead iodide (PbI2), modulates the work function of the perovskite, and passivates defects in the 3D perovskite, thereby reducing non‐radiative recombination and enhancing charge transport. With the assistance of 1D/3D hybrid films, we achieved an exceptional power conversion efficiency (PCE) of 24.75% in the generated PSCs with remarkable stability.

Enhancing Charge Transport Using Boron and Nitrogen Substitutions into Triphenylene-Based Discotic Liquid Crystals.

The substitution of p-block heteroatoms into polyaromatic hydrocarbons offers the potential for introducing enhanced molecular properties and advancing material development for electro-optical applications. Using density functional theory, we characterize the substitution of boron and nitrogen atoms into a 2,3,6,7,10,11-hexakis(hexathiol)triphenylene (TTP) core, a precursor for a material with a discotic liquid crystal phase, to determine the strength of exciton dissociation and the influence doping has on the formation of a heterojunction with graphene. The substitution of nitrogen and boron into the TTP motif enables tunability of both electron and hole coupling between hetero- and homodyads. The coupling is found to far exceed that of TTP and varied transport behavior with different combinations of doped cores of nitrogen-TTP and boron-TTP is reported. Heterodyads of nitrogen-TTP with boron-TTP appear to be ambipolar in electron/hole coupling, whereas heterodyads of boron- or nitrogen-TTP with TTP form strong electron coupling dyads and homodyads of nitrogen-TTP and boron-TTP form strong hole coupling. Finally, we describe the heterojunction of nitrogen- or boron-TTP with monolayer graphene and observe Ohmic contacts with large hole transport barriers. The presence of induced dipoles occurs at the interface in all heterojunctions, suggesting the possibility of tuning the junction with external potentials and improving exciton dissociation.

Zn-assisted low-temperature reconstruction of NiCo heterogeneous catalysts for lithium-oxygen batteries

Developing catalysts with high catalytic activity and durability is an effective strategy for improving the electrochemical performance of lithium-oxygen batteries (LOBs). Metal atom doping and heterostructure construction have shown great potential in catalysis and are expected to be widely used in energy storage. In this study, a Zn-doped NiCo2O4/NiO heterostructured complex catalyst is designed and prepared as a cathode catalyst for LOBs. This metal-doped heterostructured complex catalyst, prepared at a lower annealing temperature, retains the most active sites. Additionally, the three-dimensional hollow structure of the catalyst not only facilitates mass transfer but also provides active sites through doping and heterostructure formation. The Zn-doped NiCo2O4/NiO catalyst exhibits excellent catalytic performance, resulting the generation of a silky Li2O2 discharge product film, and the higher adsorption energy for the intermediate product LiO2 also allows the discharge product to be tightly bound to the catalyst. The improved contact between the discharge products and the catalyst's active sites, along with the increased surface area, enhances charge transport and decomposition properties, leading to good reversibility of the LOB. Consequently, the LOB based on Zn-doped NiCo2O4/NiO heterostructure complex catalyst features high discharge capacity (12160 mAh/g at 200 mA g−1) and excellent durability (353 cycles, ∼1765 h). Furthermore, theoretical calculations show that the Zn-doped complex heterostructures have enhanced reaction kinetics of OER and ORR. This straightforward method of producing metal-doped heterostructured complex catalysts that induce uniform Li2O2 deposition valuable insights for enhancing the performance of LOBs.

Enhanced solar light-induced performance of a step-scheme heterojunction nanostructure (C3N4/ZrO2) for mixed dye degradation and methanol oxidation

This study focuses on the high demand for innovative nanostructured materials with boosted photocatalytic performance for the degradation of organic pollutants and oxidation of organic compounds. A nanostructure consisting of graphitic carbon nitride (C3N4) and zirconium oxide (ZrO2) denoted as C3N4/ZrO was synthesized via direct thermal pyrolysis. A comprehensive array of characterization techniques (XRD, FESEM, HRTEM and UV-DRs analysis) was utilized for a detailed analysis of the prepared photocatalysts. The photoactivity of the C3N4/ZrO nanostructure was explored by the photocatalytic degradation of a mixture of dyes (Rh B + CV), and methanol oxidation reaction and compared with those of pristine C3N4 and ZrO2. The photoactivity of C3N4/ZrO for degrading the mixed dye under simulated solar light was 97% higher than those of pristine C3N4 (88%) and ZrO2 (31%). The C3N4/ZrO nanostructure, functioning as a step-scheme heterojunction, demonstrated superior photocatalytic performance due to enhanced charge transport facilitated by robust interfacial contact between C3N4 and ZrO2. This enhanced photodegradation efficiency, reaching 97%, establishes a foundation for the development of heterojunction catalysts with exceptional photocatalytic activities. Furthermore, the methanol oxidation activity of the C3N4/ZrO nanostructure was exceptionally high, yielding a 138.25 mA/cm2 current density at a 2 M methanol. The proposed material has a high application potential for mitigating pollution and energy issues.

Electrostatic Potential Design of Solid Additives for Enhanced Molecular Order of Polymer Donor in Efficient Organic Solar Cells.

Polymeric semiconducting materials struggle to achieve fast charge mobility due to low structural order. In this work, five 1H-indene-1,3(2H)dione-benzene structured halogenated solid additives namely INB-5F, INB-3F, INB-1F, INB-1Cl, and INB-1Br with gradually varied electrostatic potential are designed and utilized to regulate the structural order of polymer donor PM6. Molecular dynamics simulations demonstrate that although the dione unit of these additives tends to adsorb on the backbone of PM6, the reduced electrostatic potential of the halogen-substituted benzene can shift the benzene interacting site from alkyl side chains to the conjugated backbone of PM6, not only leading to enhanced π-π stacking in out-of-plane but also arising new π-π stacking in in-plane together with the appearance of multiple backbone stacking in out-of-plane, consequent to the co-existence of face-on and edge-on molecular orientations. This molecular packing transformation further translates to enhanced charge transport and suppressed carrier recombination in their photovoltaics, with a maximum power conversion efficiency of 19.4% received in PM6/L8-BO layer-by-layer deposited organic solar cells.

Surface doping effect on the optoelectronic performance of 2D organic crystals based on cyano-substituted perylene diimides

Compared to organic thin films, organic single crystals offer significant potential in organic phototransistors (OPTs) due to their enhanced charge transport, large surface area, and defect-free nature. However, the development of n-type semiconductors has lagged behind p-type semiconductors. To enhance semiconductor device performance, a doping process can be employed, which typically involves the introduction of charged impurities into the crystalline semiconducting material. Its aim is to reduce the Ohmic losses, increase carrier density, improve transport capabilities, and facilitate effective carrier injection, ultimately enhancing the electrical properties of the material. Traditional doping processes, however, often pose a risk of damaging the structure of single crystals. In this study, we have synthesized novel cyano-substituted chiral perylene diimides, which self-assemble into two-dimensional single crystals that can be used for n-type semiconductor devices. We have employed a surface doping strategy using diethylamine vapor without disrupting the crystal structure. The fabricated devices exhibit significantly higher charge transport properties after doping, achieving a maximum electron mobility of 0.14 cm² V−¹ s−¹, representing an improvement of over threefold. Furthermore, the optoelectronic performance of the doped devices has significantly improved, with the external quantum efficiency increased by over 9 times and the significantly improved response time. These results suggest that our surface doping technology is a promising way for enhancing the performance of 2D organic single-crystal OPTs.

Inherent D-A Architecture in Indoloquinoxalines with an Array of Substituents for Non-Volatile Memory Device Applications.

Donor-acceptor (D-A)-based architecture has been the key to increase storage capability efficiency through the enhanced charge transportation in the fabricated device. We have designed and synthesized a series of functionalized indoloquinoxalines (IQ) for non-volatile organic memory devices. The investigation on UV-visible spectra reveals the absorption maxima of the compounds around 420 nm, attributed to the intramolecular charge transfer between indole and quinoxaline moiety. The irreversible anodic peak in the 1.0 to 1.5 V range indicates the indole moiety's oxidation ability. Besides, the cathodic peak in the range of -0.5 to -1.0 V, contributed to the stability of the reduced quinoxaline unit. All the compounds exhibited uniformly covered thin film in SEM analysis, potentially facilitating the seamless charge carrier migration between adjacent molecules. The methoxyphenyl substituted compound exhibited the binary write-once read-many (WORM) memory behavior with the lowest threshold voltage of -0.81 V. The molecular simulations displayed the efficient intramolecular charge transfer, providing the fabricated device's distinctive conductive states. Except for the tert-butylphenyl compound, which showed volatile dynamic random-access memory (DRAM) behavior, all the other compounds exhibited non-volatile WORM memory behavior, suggesting IQs potential as an intrinsic D-A molecule in organic memory devices on further structural refinement.

Optimization of preparation conditions by response surface methodology for synthesis of titanium dioxide/reduced graphene oxide composite in dye-sensitized solar cells

This study aimed to address the need for alternative materials in the anode layer to enhance the performance of dye-sensitized solar cells (DSSCs). The synthesis of titanium dioxide/reduced graphene oxide (TiO2/rGO) was carried out using the response surface methodology by face central composite design (RSM/FCC). This method allowed us to systematically evaluate the influence of two key factors, namely the weight percentage of precursor graphene oxide (GO wt%) and the L-ascorbic acid ratio, | on the power conversion efficiency (PCE) of DSSCs. Our research is significant because it explores the synthesis of TiO2/rGO as a novel material for the anode layer in DSSCs. This material holds promise for improving device performance due to its unique properties, such as enhanced charge transport and light harvesting capabilities. Additionally, TiO2/rGO can serve multiple functions within the DSSCs device, acting not only as a charge transport layer but also potentially as a light scattering layer to increase photon absorption. The statistical analysis revealed that the GO wt% had a more significant influence on PCE compared to the L-ascorbic acid ratio. Furthermore, our simulation results demonstrated high validity and accuracy, with a correlation coefficient (R2) of 0.9988 and a residual standard error of less than 5 %. The optimized DSSCs-based TiO2/rGO anode achieved a remarkable PCE of 7.12 %, representing a 29 % improvement compared to the pure TiO2-based DSSCs anode. In summary, our study highlights the importance of synthesizing TiO2/rGO as a novel material for the anode layer in DSSCs and demonstrates its potential for significantly enhancing device performance. This study emphasizes these key points more prominently in the abstract to better convey the novelty and significance of our findings.

Interfacial Engineering of Selenium‐Based Photodiodes for Extremely Low‐Noise Photodetection and Single‐Pixel Imaging

AbstractSelenium as one of the most historical semiconductors has been used for photovoltaics and photodetection, thanks to its excellent optoelectronic properties, superior stability, facile and low‐cost fabrication. However, commercialized Se‐based devices are mainly based on its amorphous state, which significantly limits the charge transport and requires relatively large bias voltage. The charge carrier dynamics of high‐performance crystalline Se thin films are barely reported, and related photodiodes have not been realized mainly limited by the large dark current and slow response speed. Here, poly‐crystalline Se thin films via vacuum evaporation, in situ thermal annealing, and engineered the interfaces with various metal electrodes are fabricated, which resulted in enhanced charge transport properties and reduced device leakage. The optimized Se photodiodes exhibited excellent performance metrics, including extremely low dark current density, decent specific detectivity, and superior stability. Furthermore, the optimized Se photodetectors are also introduced for single‐pixel imaging, which demonstrates excellent sensitivity and great potential for real applications.

Vacuum‐free lamination via controlled polymer adhesion for selective photogeneration and photodetection

AbstractThis study attempts to develop a reproducible thin‐film formation technique called vacuum‐free (VF) lamination, which transfers thin films using elastomeric polymer‐based laminating mediators. Precisely, by controlling the interface characteristics of the mediator based on the work of adhesion, VF lamination is successfully performed for various thicknesses (from 20 to 240 nm) of a conjugated photoactive material composed of poly[(2,6‐(4,8‐bis(5‐(2‐ethylhexyl‐3‐fluoro)thiophen‐2‐yl)‐benzo[1,2‐b:4,5‐bʹ]dithiophene))‐alt‐(5,5‐(1ʹ,3ʹ‐di‐2‐thienyl‐5ʹ,7ʹ‐bis(2‐ethylhexyl)benzo[1ʹ,2ʹ‐c:4ʹ,5ʹ‐cʹ]dithiophene‐4,8‐dione)] (a polymer donor) and 2,2ʹ‐((2Z,2ʹZ)‐((12,13‐bis(2‐butyloctyl)‐3,9‐diundecyl‐12,13‐dihydro‐[1,2,5]thiadiazolo[3,4‐e]thieno[2ʹʹ,3ʹʹ:4ʹ,5ʹ]thieno[2ʹ,3ʹ:4,5]pyrrolo[3,2‐g]thieno[2ʹ,3ʹ:4,5]thieno[3,2‐b]indole‐2,10‐diyl)bis(methanylylidene))bis(5,6‐difluoro‐3‐oxo‐2,3‐dihydro‐1H‐indene‐2,1‐diylidene))dimalononitrile (a nonfullerene acceptor). Interestingly, the organic photovoltaic and photodetecting applications, prepared by the VF lamination process, showed superior performance compared to those of devices prepared by conventional spin‐coating. This is due to the overturned surface morphology, which led to enhanced charge transport ability and blocking of the externally injected charge. Thus, the reproducible VF lamination process, exploiting an adhesion‐based elastomeric polymer mediator, is a promising thin‐film formation technique for developing efficient next‐generation organic optoelectronic materials consistent with the solution process.

Enhancing charge transport and photoluminescence characteristics via transition metals doping in ITO thin films

Abstract This study presents the synthesis and characterization of pristine and transition metal (Co, Fe, and Zr)-doped indium tin oxide (ITO) thin films fabricated via RF magnetron sputtering. The effect of transition metal doping on ITO thin films properties was comprehensively examined using numerous spectroscopic and microscopic methods such as XRD, FTIR, and SEM coupled with EDX, UV–visible and PL spectroscopy, and four-probe and J–V measurements. The cubic crystal structure of the materials was confirmed through XRD spectroscopy, while FTIR results validated the existence of chemical bonds, signified by sharp peaks at 608 cm−1 and 667 cm−1 in the fingerprint region. SEM imaging revealed a granular-like agglomerated structure, with EDX confirming the elemental composition of the samples. The incorporation of Co, Fe, and Zr ions into ITO is aimed at improving photoconductivity and the optical bandgap, with the ultimate objective of enhancing performance in photovoltaic applications. Our findings showed a significant decrease in optical transmission in the visible spectrum. The bandgap also experienced a minor decrease from 3.67 eV to 3.53 eV. Analysis of the photoluminescence spectra exhibited the majority of emission peaks in the UV region, ascribed to electronic transitions occurring via band-to-band and band-to-impurity interactions within the ITO. Electrical measurements indicated lower resistance, higher current flow, and increased carrier concentration in transition metals–doped ITO compared to the undoped ITO, with Zr-doped ITO exhibiting the highest conductivity and optimal charge flow among all dopants. These promising findings in terms of optical, structural, and electrical attributes signal the potential of these materials for photovoltaic system applications.

Multiarmed Aromatic Ammonium Salts Boost the Efficiency and Stability of Inverted Organic Solar Cells.

Inverted organic solar cells (OSCs) have attracted much attention because of their outstanding stability, with zinc oxide (ZnO) being commonly used as the electron transport layer (ETL). However, both surface defects and the photocatalytic effect of ZnO could lead to serious photodegradation of acceptor materials. This, in turn, hampers the improvement of the efficiency and stability in OSCs. Herein, we developed a multiarmed aromatic ammonium salt, namely, benzene-1,3,5-triyltrimethanaminium bromide (PhTMABr), for modifying ZnO. This compound possesses mild weak acidity aimed at removing the residual amines present within ZnO film. In addition, the PhTMABr could also passivate surface defects of ZnO through multiple hydrogen-bonding interactions between its terminal amino groups and the oxygen anion of ZnO, leading to a better interface contact, which effectively enhances charge transport. As a result, an efficiency of 18.75% was achieved based on the modified ETL compared to the bare ZnO (PCE = 17.34%). The devices utilizing the modified ZnO retained 87% and 90% of their initial PCE after thermal stress aging at 65 °C for 1500 h and continuous 1-sun illumination with maximum power point (MPP) tracking for 1780 h, respectively. Importantly, the extrapolated T80 lifetime with MPP tracking exceeds 10 000 h. The new class of materials employed in this work to modify the ZnO ETL should pave the way for enhancing the efficiency and stability of OSCs, potentially advancing their commercialization process.

Charge generation layer with Yb assistant interlayer for tandem organic light-emitting diodes

Tandem organic light-emitting diode (OLED) devices require an efficient charge generation layer (CGL) between two stacked OLED units. In this study, a CGL with an Yb assistant interlayer was fabricated and investigated. The optical transmittance and charge generation performances of the CGLs were analyzed with respect to the Yb thickness. The best result was obtained at a Yb thickness of 3 nm, at which both the electrical and optical properties exhibited optimal performances. The optical transmittance was greater than 90 %; this was superior to the performances using Ag and Al interlayers. The insertion of a 3-nm Yb layer reduced the threshold voltage from 18 to 6 V. Capacitance measurements revealed that the insertion of the Yb layer enhanced charge generation in the CGLs, reducing the threshold voltage and enhancing charge transport. The tandem OLED device fabricated using Bphen:Liq/Yb/MoO3/TAPC as a CGL exhibited a 1.92 × enhancement in the current efficiency, which is nearly twice the ideal value, compared to a single-unit device. Thus, Yb is a promising candidate for use as an assistant interlayer in CGLs for high-performance tandem OLED devices.

Hydrogen-Bonded Cocrystals Encapsulating CsPbBr3 Perovskite Nanocrystals with Enhancement of Charge Transport for Photocatalytic Reduction of Uranium.

At present, poor stability and carrier transfer efficiency are the main problems that limit the development of perovskite-based photoelectric technologies. In this work, hydrogen-bonded cocrystal-coated perovskite composite (PeNCs@NHS-M) is easily obtained by inducing rapid crystallization of melamine (M) and N-hydroxysuccinimide (NHS) with PeNCs as the nuclei. The outer NHS-M cocrystal passivates the undercoordinated lead atoms by forming covalent bonds, thereby greatly reducing the trap density while maintaining good structure stability for perovskite nanocrystals. Moreover, benefiting from the interfacial covalent band linkage and long-range ordered structures of cocrystals, the charge transfer efficiency is effectively enhanced and PeNCs@NHS-M displays superior photoelectric performance. Based on the excellent photoelectric performance and abundant active sites of PeNCs@NHS-M, photocatalytic reduction of uranium is realized. PeNCs@NHS-M exhibits U(VI) reduction removal capability of up to 810.1mg g-1 in the presence of light. The strategy of cocrystals trapping perovskite nanocrystals provides a simple synthesis method for composites and opens up a new idea for simultaneously improving the stability and photovoltaic performance of perovskite.

Facile Ligand Exchange of Ionic Ligand-Capped Amphiphilic Ag2S Nanocrystals for High Conductive Thin Films.

A surface ligand modification of colloidal nanocrystals (NCs) is one of the crucial issues for their practical applications because of the highly insulating nature of native long-chain ligands. Herein, we present straightforward methods for phase transfer and ligand exchange of amphiphilic Ag2S NCs and the fabrication of highly conductive films. S-terminated Ag2S (S-Ag2S) NCs are capped with ionic octylammonium (OctAH+) ligands to compensate for surface anionic charge, S2-, of the NC core. An injection of polar solvent, formamide (FA), into S-Ag2S NCs dispersed in toluene leads to an additional envelopment of the charged S-Ag2S NC core by FA due to electrostatic stabilization, which allows its amphiphilic nature and results in a rapid and effective phase transfer without any ligand addition. Because the solvation by FA involves a dissociation equilibrium of the ionic OctAH+ ligands, controlling a concentration of OctAH+ enables this phase transfer to show reversibility. This underlying chemistry allows S-Ag2S NCs in FA to exhibit a complete ligand exchange to Na+ ligands. The S-Ag2S NCs with Na+ ligands show a close interparticle distance and compatibility for uniformly deposited thin films by a simple spin-coating method. In photoelectrochemical measurements with stacked Ag2S NCs on ITO electrodes, a 3-fold enhanced current response was observed for the ligand passivation of Na+ compared to OctAH+, indicating a significantly enhanced charge transport in the Ag2S NC film by a drastically reduced interparticle distance due to the Na+ ligands.

High-performance lithium storage in Li2SnO3-graphite composite enabled by Ag3Sn nanoparticles and oxygen vacancies

With high capacity (653 mAh g−1) and low voltage (0.6 V), Li2SnO3 is considered as a prospective anode material for Li-ion batteries (LIBs). Nevertheless, its practical uses are restricted by inferior electrochemical kinetics and fast capacity decay. Herein, a novel ternary composite of Ag3Sn alloy-lithium stannate-graphite (denoted as Ag3Sn-Li2SnO3-x-G) is designed and fabricated by ball milling and vacuum annealing. In this ternary composite, oxygen vacancy-containing Li2SnO3 and Ag3Sn alloy nanoparticles are homogeneously dispersed in the exfoliated graphite nanosheets. The introduction of Ag3Sn nanoparticles and oxygen vacancies into Li2SnO3-graphite can significantly enhance charge transport kinetics and structure stability of composite during the lithiation and delithiation processes. Benefiting from these merits, the Ag3Sn-Li2SnO3-x-G composite presents excellent cycling stability (782.4 mAh g−1 at 0.2 A g−1 after 200 cycles) and impressive rate capability (251.5 mAh g−1 at 2 A g−1). Broadly, this design strategy can provide an effective and reliable route for constructing advanced metal oxide-based anode materials for high-energy LIBs.

Crystalline/Amorphous‐Ru/VOx Phase Engineering Expedites The Alkaline Hydrogen Evolution Kinetics

AbstractActive and durable catalysts for hydrogen evolution reaction (HER) are of great significance for developing renewable hydrogen energy. Herein, crystalline/amorphous‐Ru/VOx (c/a‐Ru/VOx) heterogeneous catalysts are conceived, in which the amorphous VOx exposes more active sites and enhances charge transport compared with the counterpart with a crystal phase structure, strengthening the electronic interaction between metal‐support. As expected, c/a‐Ru/VOx‐500 with heat treatment at 500 °C exhibits excellent HER performance under alkaline conditions, with an overpotential of only 33 mV at 10 mA cm−2 and small Tafel slope (27 mV dec−1), superior to commercial platinum/carbon (Pt/C) catalysts. Particularly, its mass activity (0.335 A mgRu−1) is 1.5 times greater than that of Pt/C (0.224 A mgPt−1) at an overpotential of 50 mV. Also, it shows good industrial application prospects through tests under high temperature, high alkalinity, and large current conditions. Theoretical calculations unveil that there exists a charge redistribution at c/a‐Ru/VOx heterointerfaces, which makes the surface of Ru takes on an electron‐deficient state, resulting in optimization of adsorption and desorption for different reaction intermediates. This optimized behavior effectively reduces the thermodynamic energy barrier, allowing the catalyst with greatly enhanced HER performance. The exploration provides a promising strategy for designing efficient and durable catalysts for HER.

Enhanced charge transport and broadband photoresponse of MoS2 photodetectors with sparsely distributed Ag@SiO2 core–shell nanostructures

Integrating metal nanostructures with two-dimensional (2D) material photodetectors has been demonstrated that can greatly improve device performance owning to various extraordinary optoelectronic phenomena. For example, metal nanostructures are served as ideal plasmonic materials to maximize local electromagnetic fields leading to light absorption of 2D materials. In this work, other than the widely reported plasmonic effects, we discover the contribution of metal nanostructures in charge transport engineering in 2D material photodetectors, which is important but always ignored in previous studies by others. Notable improvements of carrier mobility and carrier concentration attributing to the integration of sparsely distributed Ag@SiO2 core–shell nanoparticles on the MoS2 detector were experimentally established, originating from reduced carrier scattering and interfacial gating. Consequently, a 1.5-fold broadband (400–1100 nm) uniform photocurrent enhancement was observed, which was entirely derived from the improved charge transport. These findings open up a new research perspective for the precise identification and objective evaluation of different effects of metal nanostructures on optoelectronic devices.