Interlayer Transport Research Articles

Covalent Organic Frameworks Interfacial Modification of Ceramic Electrolytes for Enhanced Electrochemical Performance

AbstractThe interface instability between inorganic ceramic electrolytes and lithium metal anodes seriously affects the cycling behavior of high‐performance lithium‐metal batteries. Herein, an in situ interfacial modification strategy is proposed to build the precise hybrid organic/inorganic lithium‐ion conducting layer where the Li1.3Al0.3Ti1.7(PO4)3 (LATP) particle surface is anchored by ion‐conducting covalent organic frameworks (COF) with affluent poly(ethylene glycol) (PEG) moieties. This interlayer features ion transport regulation to avoid high interfacial resistance and enhances interfacial stability by building a functional COF‐based shield against electrons. These as‐prepared particles are employed to fabricate flexible quasi‐solid electrolyte membranes interconnected by polytetrafluoroethylene binder based on the dry process. The obtained membranes perform two‐fold increase in ion conductivity at 30 °C of 2.55 × 10−3 S cm−1 and the prolonged lithium deposition up to 1000 h compared to the pristine, which are attributed to synergistic effects in the inorganic/organic phase. Moreover, an integrated cathode/electrolytes design is proposed and exhibits excellent cycling performance with capacity retention of 98.8% after 200 cycles at 1 C. The corresponding pouch cells can light up LED after bending and recovery. This research provides new insights into the great potential of fabricating soft ceramic‐based membranes in a low‐cost and green way for highly‐stable lithium‐metal batteries.

Modulation of Interlayer Nanochannels via the Moderate Heat Treatment of Graphene Oxide Membranes.

In response to the phenomenon of interlayer transport channel swelling caused by the hydration of oxygen-containing functional groups on the GO membrane surface, a moderate heat treatment method was employed to controllably reduce the graphene oxide (GO) membrane and prepare a reduced GO composite nanofiltration membrane (mixed cellulose membrane (MCE)/ethylenediamine (EDA)/reduced GO-X (RGO-X)). The associations of different heat treatment temperatures with the hydrophilicity, interlayer structure, permeability and dye/salt rejection properties of GO membranes were systematically explored. The results indicated that the oxygen-containing groups of the GO membrane were partially eliminated after heat treatment, and the hydrophilicity was weakened. This effectively weakened the hydration between the GO membrane and the water molecules and inhibited the swelling of the oxidized graphene membrane. In the dye desalination test, the MCE/EDA/RGO membrane exhibited an ultra-high rejection rate of over 97% for methylene blue (MB) dye molecules. In addition, heat treatment increased the structural defects of the GO membrane and promoted the fast passage of water molecules via the membrane. In pure water flux testing, the water flux of the membrane remained above 46.58 Lm-2h-1bar-1, while the salt rejection rate was relatively low.

Robust and Efficient Out-of-Plane Exciton Transport in Two-Dimensional Perovskites via Ultrafast Förster Energy Transfer.

Two-dimensional (2D) perovskites, comprising inorganic semiconductor layers separated by organic spacers, hold promise for light harvesting and optoelectronic applications. Exciton transport in these materials is pivotal for device performance, often necessitating deliberate alignment of the inorganic layers with respect to the contacting layers to facilitate exciton transport. While much attention has focused on in-plane exciton transport, little has been paid to out-of-plane interlayer transport, which presumably is sluggish and unfavorable. Herein, by time-resolved photoluminescence, we unveil surprisingly efficient out-of-plane exciton transport in 2D perovskites, with diffusion coefficients (up to ∼0.1 cm2 s-1) and lengths (∼100 nm) merely a few times smaller or comparable to their in-plane counterparts. We unambiguously confirm that the out-of-plane exciton diffusion coefficient corresponds to a subpicosecond interlayer exciton transfer, governed by the Förster resonance energy transfer (FRET) mechanism. Intriguingly, in contrast to temperature-sensitive intralayer band-like transport, the interlayer exciton transport exhibits negligible temperature dependence, implying a lowest-lying bright exciton state in 2D perovskites, irrespective of spacer molecules. The robust and ultrafast interlayer exciton transport alleviates the constraints on crystal orientation that are crucial for the design of 2D perovskite-based light harvesting and optoelectronic devices.

Van der Waals heterojunctions comprising double/single-walled carbon nanotubes: Insights into heat flux and thermal rectification

Van der Waals (vdWs) heterojunctions constructed from double/single-walled carbon nanotubes (DSCNTs) demonstrate exceptional thermal rectification (TR) ratios, coupled with a straightforward fabrication process, making them highly suitable for thermal rectifier applications. In this study, we employed a Nonequilibrium Molecular Dynamics method to investigate the heat flux and TR across DSCNTs with varying interlayer spacings. Our findings reveal that at smaller interlayer spacings, high temperatures readily overcome vdWs interactions. Conversely, increasing the interlayer spacing initially impedes this effect, though elevated temperatures can surmount this barrier. Significantly, at specific combinations of temperature and interlayer spacing, the left side in DSCNTs establishes interlayer phonons transport channels, facilitating forward heat flux but impeding the backward. This mechanism results in an exceptionally high TR ratio, reaching up to 757 %. Additionally, altering the chiral configurations of the CNTs in the inner and outer layers, while preserving interlayer spacing, further enhances the TR ratio and reduces the temperature threshold required to achieve peak TR ratio. Our findings contribute valuable insights into the phonon transport mechanisms within one-dimensional vdWs heterojunctions.

Multinetwork constrained planning of hydrogen-power supplying facilities under double-layer coupling mechanisms

The proliferation of hydrogen fuel cell vehicles calls for effective planning of hydrogen supply facilities. This paper focuses on renewable energy-based distributed hydrogen supply networks (DHSNs), with on-site production and vehicle-based transport. To explore the energy synergism effect, we propose multinetwork constrained planning of hydrogen-power supplying facilities. Considering the double-layer coupling mechanism (DCM), multiple DHSN equipment planning is coordinated with the generation planning of the power distributed networks (PDN). Firstly, the DCM is proposed considering structured multi-component equipment, inter-layer hydrogen couplings, and cross-network power couplings. Secondly, to formulate the DCM, we develop a structured deployment model for DHSN equipment to enhance system integrality and non-redundancy. Specially, to release more flexibilities, inter-layer transport is modeled by proposing a spatiotemporal extended vehicle routing problem model incorporating multiple loading stations with trip coordination. Thirdly, a planning method is proposed to coordinate the planning of hydrogen-power supply facilities in coupled networks, incorporating the double-layer coupling constraints, station operation constraints, and PDN constraints. Test systems are employed to verify the effectiveness of the proposed method.

Controlled Preparation of High Quality Bubble-Free and Uniform Conducting Interfaces of Vertical van der Waals Heterostructures of Arrays.

Sharp and clean interfaces of van der Waals (vdW) heterostructures are highly demanded in two-dimensional (2D) materials-based devices. However, current assembly methods usually cause interfacial bubbles and wrinkles, hindering carrier interlayer transport. The preparation of a large-scale vdW heterostructure with a bubble-free interface is still a challenge. Although many efforts have been made to eliminate bubbles, the evolution processes of the interfacial bubbles are rarely studied. Here, the interface bubble formation and evolution of the transferred 2D materials and their vdW heterostructure are systemically studied by the atomic force microscopy (AFM) technique and high-resolution surface current mapping. A thermal annealing procedure is developed to reduce the number of bubbles and to improve the quality of interfaces. In addition, influences of the interface residues and nanosteps on bubble evolution are also discussed. Further, we develop the polystyrene (PS)-mediated polydimethylsiloxane (PDMS) transfer technique to realize the high-quality transfer of heterostructure arrays. Finally, high-resolution surface current mapping results confirm that we can now produce highly uniform electrical conduction interfaces of heterojunctions. This study provides guidance for assembling high quality interfaces and paves the way for production of bubble-free heterostructure-based electronic devices with high performance and good uniformity.

Electronic transport in graphene with out-of-plane disorder

Real-world samples of graphene often exhibit various types of out-of-plane disorder–ripples, wrinkles and folds–introduced at the stage of growth and transfer processes. These complex out-of-plane defects resulting from the interplay between self-adhesion of graphene and its bending rigidity inevitably lead to the scattering of charge carriers thus affecting the electronic transport properties of graphene. We address the ballistic charge-carrier transmission across the models of out-of-plane defects using tight-binding and density functional calculations while fully taking into account lattice relaxation effects. The observed transmission oscillations in commensurate graphene wrinkles are attributed to the interference between intra- and interlayer transport channels, while the incommensurate wrinkles show vanishing backscattering and retain the transport properties of flat graphene. The suppression of backscattering reveals the crucial role of lattice commensuration in the electronic transmission. Our results provide guidelines to controlling the transport properties of graphene in presence of this ubiquitous type of disorder.

Key issues and solutions affecting efficiency and stability of perovskite/heterojunction tandem solar cells

Efficient and stable perovskite/heterojunction tandem solar cells (PTSC) are a direction of joint exploration in both academia and industry. Achieving efficient solar energy utilization by assembling structural layers with different bandgaps in an optical sequence is the original design strategy for PTSC. Through the reasonable distribution of the absorption spectra of each layer, the photoelectric conversion efficiency (PCE) of PTSC can theoretically be increased to more than 40%. At present, the efficiency advantage of small-area PTSC is well-established, but there are still many challenges in the commercialization of solar cell efficiency and stability. Therefore, in this work, the two-terminal (2T) and four-terminal (4T) stacking methods are regarded as the main structural routes, and the optimal design of the key structural layers of PTSC, bandgap adjustment, additive regulation, optimization of interlayer transport, and optimization of the module interconnection and encapsulation methods are focused on. Based on the existing research results, the key problems and solutions affecting the efficiency and stability of PTSC are summarized and outlooked, aiming to provide directional solutions to the key problems in the structural design of PTSC. In addition, from the application perspective, it is proposed that before the stability problem of the perovskite is fundamentally solved, the 4T PTSC is more likely to achieve product iteration and industrial efficiency improvement, with the expectation of taking the lead in commercialization. This work emphasizes the popularization and practical application of commercialization, with a perspective that is more in line with the market trend and close to the industrial demand, and is expected to provide an important reference for the commercialization of PTSC in the academic circles.

Gradient tungsten-doped Bi3TiNbO9 ferroelectric photocatalysts with additional built-in electric field for efficient overall water splitting

Bi3TiNbO9, a layered ferroelectric photocatalyst, exhibits great potential for overall water splitting through efficient intralayer separation of photogenerated carriers motivated by a depolarization field along the in-plane a-axis. However, the poor interlayer transport of carriers along the out-of-plane c-axis, caused by the significant potential barrier between layers, leads to a high probability of carrier recombination and consequently results in low photocatalytic activity. Here, we have developed an efficient photocatalyst consisting of Bi3TiNbO9 nanosheets with a gradient tungsten (W) doping along the c-axis. This results in the generation of an additional electric field along the c-axis and simultaneously enhances the magnitude of depolarization field within the layers along the a-axis due to strengthened structural distortion. The combination of the built-in field along the c-axis and polarization along the a-axis can effectively facilitate the anisotropic migration of photogenerated electrons and holes to the basal {001} surface and lateral {110} surface of the nanosheets, respectively, enabling desirable spatial separation of carriers. Hence, the W-doped Bi3TiNbO9 ferroelectric photocatalyst with Rh/Cr2O3 cocatalyst achieves an efficient and durable overall water splitting feature, thereby providing an effective pathway for designing excellent layered ferroelectric photocatalysts.

Transport channel engineering between MXene interlayers for Zn‐ion hybrid microsupercapacitor with enhanced energy output and cycle stability

AbstractTwo‐dimensional (2D) transition metal carbonitrides/nitrides (MXene) materials have proven to be promising alternatives as novel capacitor‐type electrodes for aqueous Zn‐ion hybrid microsupercapacitors (ZHMSCs). However, during self‐assembly processes, serious restacking between 2D MXene nanosheets induced by strong van der Waals forces makes ion transport channels narrow within the compact MXene film electrodes, which would result in poor energy output of ZHMSCs. Herein, interlayer transport channel engineering is designed by intercalating bacterial cellulose (BC) between MXene interlayers to develop MXene/BC electrodes with fast ion transport channels in contrast to pure MXene electrodes. Benefiting from fast anion intercalation/deintercalation on MXene/BC capacitor‐type cathode and reversible Zn stripping/plating on Zn foil anode, the fabricated ZHMSCs exhibit wide working potential windows (1.36 V), high areal capacitance (404 mF cm−2), and landmark areal energy density (94 µWh cm−2 at 1 mA cm−2). The areal capacitance and energy density of the developed ZHMSCs are much higher than those of the ZHMSCs based on pure MXene capacitor‐type cathode (239 mF cm−2/57 µWh cm−2 at 1 mA cm−2). Besides, the developed ZHMSCs can perform more than 10,000 cycles, showing outstanding capacity retention. In general, our work provides a novel strategy to break through the performance bottlenecks afflicting MXene‐based ZHMSCs.

Probing the Formation of Dark Interlayer Excitons via Ultrafast Photocurrent.

Optically dark excitons determine a wide range of properties of photoexcited semiconductors yet are hard to access via conventional time-resolved spectroscopies. Here, we develop a time-resolved ultrafast photocurrent technique (trPC) to probe the formation dynamics of optically dark excitons. The nonlinear nature of the trPC makes it particularly sensitive to the formation of excitons occurring at the femtosecond time scale after the excitation. As a proof of principle, we extract the interlayer exciton formation time of 0.4 ps at 160 μJ/cm2 fluence in a MoS2/MoSe2 heterostructure and show that this time decreases with fluence. In addition, our approach provides access to the dynamics of carriers and their interlayer transport. Overall, our work establishes trPC as a technique to study dark excitons in various systems that are hard to probe by other approaches.

(Digital Presentation) Kinetic Control of Angstrom-Scale Porosity in 2D Lattices for Direct Scalable Synthesis of Atomically Thin Proton Exchange Membranes

Angstrom-scale pores introduced into atomically thin 2D materials offer transformative advances for proton exchange membranes in several energy applications. Here, we show that facile kinetic control of scalable chemical vapor deposition (CVD) can allow for direct formation of angstrom-scale proton-selective pores in monolayer graphene with significant hindrance to even small, hydrated ions (K+ diameter ∼6.6 Å) and gas molecules (H2 kinetic diameter ∼2.9 Å). We demonstrate centimeter-scale Nafion|Graphene|Nafion membranes with proton conductance ∼3.3–3.8 S cm–2 (graphene ∼12.7–24.6 S cm–2) and H+/K+ selectivity ∼6.2–44.2 with liquid electrolytes. The same membranes show proton conductance ∼4.6–4.8 S cm–2 (graphene ∼39.9–57.5 S cm–2) and extremely low H2 crossover ∼1.7 × 10–1 – 2.2 × 10–1 mA cm–2 (∼0.4 V, ∼25 °C) with H2 gas feed. We rationalize our findings via a resistance-based transport model and introduce a stacking approach that leverages combinatorial effects of interdefect distance and interlayer transport to allow for Nafion|Graphene|Graphene|Nafion membranes with H+/K+ selectivity ∼86.1 (at 1 M) and record low H2 crossover current density ∼2.5 × 10–2 mA cm–2, up to ∼90% lower than state-of-the-art ionomer Nafion membranes ∼2.7 × 10–1 mA cm–2 under identical conditions, while still maintaining proton conductance ∼4.2 S cm–2 (graphene stack ∼20.8 S cm–2) comparable to that for Nafion of ∼5.2 S cm–2. Our experimental insights enable functional atomically thin high flux proton exchange membranes with minimal crossover.

Nitrogen-doped graphene quantum dots embedding CuCo-LDH hierarchical hollow structure for boosted charge storage capability in supercapacitor

The nanostructure optimization of layered double hydroxide (LDH) can effectively alleviate fragile agglomerated problems. Herein, nitrogen-doped graphene quantum dots (NGQDs) embedded in CuCo-LDH hierarchical hollow structure is synthesized by hydrothermal and impregnation methods. The electrochemical results show that the ordered multi-component structure could effectively inhibit the aggregation and layer stacking. At the same time, the hierarchical structure establishes new electron and ion transfer channels, greatly reducing the resistance of interlayer transport and accelerating the diffusion rate of electrolyte ions. Besides, NGQDs have both good electrical conductivity and abundant active sites, which can further improve the electron transmission rate and effectively strengthen the energy storage capacity of the material. Therefore, the large specific capacity of 1009 F g−1 can be displayed at 1 A g−1. The energy density of the assembled carbon cloth (CC)@CuCo-LDH/NGQDs//activated carbon (AC) device can reach 58.6 Wh kg−1 at 850 W kg−1. Above test results indicate that CC@CuCo-LDH/NGQDs//AC devices exhibit stable multi-component hierarchical structure and excellent electrical conductivity, which provides an effective strategy for enhancing the electrochemical characteristics of asymmetric supercapacitors.

Light-induced coherent interlayer transport in stripe-ordered La1.6−xNd0.4SrxCuO4

We have investigated the photoexcited transient responses of stripe-ordered phase in a cuprate superconductor, ${\rm La}_{1.6-x}{\rm Nd}_{0.4}{\rm Sr}_{x}{\rm CuO}_{4}~(x = 0.12)$ using optical-pump terahertz (THz)-probe spectroscopy. Upon the near-infrared photoexcitation with the electric field polarized along the $c$-axis, a clear plasma edge appears in the THz reflection spectrum along the $c$-axis with its position nearly coinciding with the Josephson plasma resonance of similarly doped ${\rm La}_{2-x}{\rm Sr}_{x}{\rm CuO}_{4}~(x = 0.125)$ in the low-temperature superconducting phase. The appearance of light-induced plasma edge sustains up to the onset temperature of the charge-stripe order, indicating the inherent interplay between the light-induced phase and the charge-stripe order. The optical conductivity spectrum of the light-induced state is mostly reproduced by the Drude model with a scattering rate as small as a few meV, and its imaginary part does not exhibit $1/{\omega}$-divergence behavior in any temporal region after the photoexcitation. We discuss the possible origin of the observed coherent interlayer transport behavior as manifested by the narrow Drude response in the THz reflectivity along the $c$-axis.

UV-cured polyvinyl alcohol-MXene mixed matrix membranes for enhancing pervaporation performance in dehydration of ethanol

In this study, Ti3C2Tx MXene nanosheets were synthesized and loaded into UV-curable acrylate polyvinyl alcohol (APVA) to fabricate a novel APVA-MXene mixed matrix membrane (MMM) for ethanol dehydration by pervaporation (PV) process. UV-curable APVA was synthesized by substituting the hydroxyl groups of PVA with the methacryloyl groups of glycidyl methacrylate (GMA). A rapid and energy-efficient method for fabricating the active layer was achieved by UV-crosslinking of APVA over a 2-min period. The morphology, crystal structure, chemical composition, and thermo-mechanical properties of the membranes were investigated by FESEM, XRD, FTIR, TGA, and static mechanical stretching. Incorporating MXene nanosheets into the APVA matrix resulted in an increase in permeation flux and separation factor for APVA-MXene MMMs due to its laminated structure with interlayer transport channels of two dimensions, excellent compatibility with the polymer matrix, and high surface hydrophilicity. When the MXene loading reached 3 wt%, the optimal separation performance was achieved with a permeation flux of 942 g/(m2.h) (increased by 106% compared to pristine APVA membranes) and a separation factor of 294 (increased by 79% compared to pristine APVA membranes).

Transversal nanochannel-enabled MXene laminated membranes for superior oil-water separation: A fluid mosaic cytomembrane inspired approach

Transition metal carbide and nitride materials (MXenes) have been greatly appreciated for their facilely exfoliated and hydrophilic two-dimensional (2D) layered structure to fabricate laminated membranes for oil separation. However, the denser slits and longer interlayer transport of traditional MXene membranes usually result in the poor permeability and antifouling performance. Herein, a novel approach was developed by synthesizing ultra-thin MXene and ferroferric oxide doped molybdenum disulfide (FM) and subsequently embedding FM into MXene laminates. This method yielded additional transversal nanochannels that enable lateral transport in a manner akin to that of a mosaic transport protein. Additionally, the incorporation of FM resulted in the creation of extremely irregular surfaces that form extensive membrane structures, reminiscent of tightly packed phospholipid bilayers. The incorporation of flower-like FM composites with MXene laminates endowed the resultant membrane with improved interface hydrophilicity, intensive surface roughness and enhanced permeability. These effects synergistically contributed to an exceptionally high pure water flux of the resultant membrane (3.12 × 104 L m−2 h−1), surpassing that of the control membrane (6.15 × 103 L m−2 h−1) without FM by over 5-fold. Furthermore, the optimum membrane exhibited enhanced permeance to oil mixtures (3.75 × 103 L m−2 h−1) and emulsions (4.25 × 102 L m−2 h−1), with separation of over 99% remaining. Impressively, the permeability of severely fouled membranes could be restored by 99% under visible light, highlighting the admirable photocatalytic self-cleaning ability enabled by MXene and FM. The underlying mechanisms that account for the superior antifouling performance and self-cleaning ability of the laminated membrane were also elucidated by the extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory. The facile fabrication strategy employing transversal transport laminates provides a remarkable approach for water purification and other fluidic separation applications.

Rationally designed Dion-Jacobson Tin-halide perovskites with improved phase stability and Inter-layer charge transport by intercalating alkyl cation-ligands

Currently, the development of CsSnI3 perovskite is still greatly hindered by their intrinsic deficiencies, such as their easy phase transformation. To address this issue, we theoretically constructed Dion-Jacobson (DJ) perovskites intercalated by divalent 1,5-pentamethylenediamine (PeDA2+) exhibit significantly enhanced phase stability. However, the carrier mobility is always depressed owing to the charge localization and severe lattice distortion in the presence of spacers among wafers. Thus, the alkyl ligand cations (e.g., ethylenediamine (EDA), 1,3-propanediamine (PDA), 1,4-butanediamine (BDA)) with varying lengths as organic intercalators are examined for optimizing charge transfer. Compared with the other configures, the (PDA)Cs2Sn3I10 exhibits the most significantly improved stability due to the enhanced chemical bonding and faintest structural distortions, as evidenced by computed the formation enthalpy. Formation energy and transition level of tin-vacancy defect further confirm the improved stability and depressed defect-trapping states. Meanwhile, 2D-(PDA)Cs2Sn3I10 exhibit obviously increased electrical conductivity and reduced carrier effective masses, which might benefit the photoelectric conversion of solar cells.

Signature of quantum interference effect in inter-layer Coulomb drag in graphene-based electronic double-layer systems

The distinguishing feature of a quantum system is interference arising from the wave mechanical nature of particles which is clearly central to macroscopic electronic properties. Here, we report the signature of quantum interference effect in inter-layer transport process. Via systematic magneto-drag experiments on graphene-based electronic double-layer systems, we observe low-field correction to the Coulomb-scattering-dominated inter-layer drag resistance in a wide range of temperature and carrier density, with its characteristics sensitive to the band topology of graphene layers. These observations can be attributed to a new type of quantum interference between drag processes, with the interference pathway comprising different carrier diffusion paths in the two constituent conductors. The emergence of such effect relies on the formation of superimposing planar diffusion paths, among which the impurity potentials from intermediate insulating spacer play an essential role. Our findings establish an ideal platform where the interplay between quantum interference and many-body interaction is essential.

Adjusting Crystal Orientation to Promote Sodium‐Ion Transport in V5S8@Graphene Anode Materials for High‐Performance Sodium‐Ion Batteries

Sodium-ion batteries (SIBs) have inspired the potential for widespread use in energy storage owing to the advantages of abundant resources and low cost. Benefiting from the layered structure, 2D-layered materials enable fast interlayer transport of sodium ions and thus are considered promising candidates as anodes for SIBs. Herein, a strategy of adjusting crystal orientation is proposed via a solvothermal method to improve sodium-ion transport at the edge of the interlayers in 2D-layered materials. By introducing surfactants and templates, the 2D-layered V5 S8 nanosheets are controlled to align the interlayer diffusion channels vertically to the surface, which promotes the fast transport of Na+ at the edge of the interlayers as revealed by experimental methods and ab initio calculations. Benefiting from the aligned crystal orientation and rGO coating, the vertical-V5 S8 @rGO hybrid delivers a high initial discharge capacity of 350.6 mAh g-1 at a high current density of 15 A g-1 . This work provides a strategy for the structural design of 2D-layered anode materials by adjusting crystal orientation, which demonstrates the promise for applications in fast-charging alkaline-ion batteries.

Scalable Non-Halogenated Co-solvent System for Large-Area, Four-Layer Slot-Die-Coated Organic Photovoltaics

Sustainable processing solvents, photoactive materials, and scalable manufacturing will play a key role in commercializing printed organic photovoltaics (OPVs). The record-breaking pioneering OPV reports have done an outstanding job in accelerating the discovery of champion photoactive materials and device engineering practices; however, these works predominantly involve health-hazardous halogenated processing solvents/additives and non-scalable thin-film coating methods. Herein, large-area slot-die-manufactured OPV cells from eco-friendly halogen-free solvents and synthetically scalable materials are showcased. All the four layers; electron transport layer (SnO2), cathode interlayer (PDIN-H), bulk-heterojunction (BHJ, PTQ-10:BTP-4F-12), and hole transport layer [poly(3,4-ethylenedioxythiophene):polystyrene sulfonate) (PEDOT:PSS] are slot-die-coated in air. A non-halogenated co-solvent mixture of toluene and 2-methyl tetrahydrofuran is presented as an optimal processing solvent to realize the high-quality thin films of PTQ10:BTP-4F-12. The unencapsulated champion solar cells characterized in ambient conditions (RH = 30%, T = 22 °C) exhibit power conversion efficiencies (PCEs) of 12.1 and 17.8% under 1 Sun (100 mW/cm2) and indoor light-emitting diode lighting (580 μW/cm2) conditions, respectively. Additionally, PEDOT:PSS is successfully slot-die-coated atop BHJ by mitigating wettability challenges with the aid of surface treatment. The all four-layer slot-die-coated OPVs exhibit a PCE of 9.55%.