Organic photovoltaics (OPVs) offer a promising solution for indoor energy harvesting. However, fundamental investigations to understand and optimize industrial processes such as roll-to-roll lamination for upscaling remain limited. This study investigates a critical failure mode in the upscaling of OPVs. One major challenge for thick semitransparent laminated OPV devices is current-voltage (J-V) asymmetry, where performance under cathode-side illumination exceeds that under anode-side illumination. X-ray reflectivity, neutron reflectivity, and drift-diffusion simulations reveal that a vertically stratified polymer-rich region within the bulk of photoactive layers is the main cause of asymmetric J-V characteristics. Based on this fundamental understanding, a model is proposed to explain the mechanism, wherein electron extraction is hindered by the polymer-rich region during anode illumination. By exploring upscaling-compatible blends, cathode/anode-balanced, high-performing, and air-stable semitransparent laminated OPVs are developed for indoor applications using commercially available PV-X-plus material. These findings provide valuable guidance for designing OPVs with balanced performance, facilitating roll-to-roll adoption and commercialization.

UV protection of polymer solar cells is significant to extend the duration of life and to improve their efficiency. Diatom shells doped with Eu3+/Tb3+ complexes (ETDSs) can be used as an efficient absorber and down-conversion agent for these purposes. In this work, the goal is effective UV protection and photovoltaic efficiency enhancement of polymer solar cells using DSs doped with Eu3+/Tb3+ complexes. These Eu3+/Tb3+ complexes in DSs are anchored at porous walls through a grafted coupling agent. As a strong UV absorber and efficiency enhancer, ETDSs were compounded into the cellulose acetate (CA) matrix to get an ETDS@CA flexible luminescent film. This luminescent film with high UV absorption in the range of 200-400 nm down converts UV photons into photons in visible, at 612 nm. We spin-coat the mixture solution of ETDS and CA onto the back surface of the transparent ITO/glass electrode to set up the ETDS@CA protected polymer solar cell. In this way, both UV protection and polymer solar cell efficiency enhancement are achieved. The experimental data indicated that ETDS@CA coated polymer solar cells can maintain 80% of the initial efficiency after UV-radiation for 1000 h, compared with 40% of unprotected polymer solar cells. Correspondingly, the efficiency of polymer solar cells has been enhanced by 4%. This method can be developed into a new and highly efficient way to UV protect polymer solar cells, as the original structure of polymer solar cells is not modified, with only an additional UV protection layer on the other side of the substrate.

Green and scalable materials are essential to fulfill the need of electrification for transitioning into a fossil-fuels free society, and sustainability is a requirement for all new technologies. Rechargeable batteries are one of the most important elements for electrification, enabling the transition to mobile electronics, electrical vehicles and grid storage. We here report synthesis and characterization of polyelectrolyte complexes of alginate and chitosan, both biopolymers deriving from the sea, for transport of zinc ions in hydrogel electrolytes. We have used vibrational spectroscopy, thermal measurements and microscopy, as well as transport measurements with ohmic or blocking contacts. The transference number for zinc ions is close to 1, the conductivity is approximate to 10 mS/cm, with stability at Zn interfaces seen through 7000 cycles in symmetric zinc//zinc cell. A zinc ion aqueous electrolyte was prepared from blends of chitosan and alginate, by using a simple and scalable route. These green zinc ion electrolytes exhibit a stability window up to 2 V, a zinc ion transference number close to 1, and electrochemical cyclability over 7000 cycles at interfaces to zinc. This biologically derived polyelectrolyte complex offers many possibilities for optimizing transport and stability at electrode interfaces.image

The integration of organic photovoltaic (OPV) modules on greenhouses is an encouraging practice to offset the energy demands of crop growth and provide extra functionality to dedicated farmland. Nevertheless, such OPV devices must meet certain optical and stability requirements to turn net zero energy greenhouse systems a reality. Here a donor:acceptor polymer blend is optimized for its use in laminated devices while matching the optical needs of crops. Optical modeling is performed and a greenhouse figure-of-merit is introduced to benchmark the trade-off between photovoltaic performance and transparency for both chloroplasts and humans. Balanced donor:acceptor ratios result in better-performing and more thermally stable devices than acceptor-enriched counterparts. The optimized polymer blend and state-of-the-art polymer:small-molecule blends are next transferred to 25 cm(2) laminated modules processed entirely from solution and in ambient conditions. The modules are mounted on a greenhouse as standalone or 4-terminal tandem configurations and their outdoor stability is tracked for months. The study reveals degradation modes undetectable under laboratory conditions such as module delamination, which accounts for 10-20% loss in active area. Among the active layers tested, polymer:fullerene blends are the most stable and position as robust light harvesters in future building-integrated OPV systems.

A green, though black, sustainable and low-cost carbon material-charcoal produced from wood-is developed for electricity storage. Charcoal electrodes are fabricated by ball-milling charcoal and adding protein nanofibril binders. The charcoal electrode presents a capacitance of 360 F g(-1) and a conductivity of 0.2 S m(-1). A pair of redox peaks is observed in the cyclic voltammetry and assigned to originate from quinone groups. Compared with other wooden electrodes, these charcoal electrodes display better cycling stability with 88% capacity retention after 1000 cycles. Their discharge capacity is 2.5 times that of lignosulfonate/graphite hybrid electrodes.

Optimization of a new system for organic solar cells is a multiparametric analysis problem that requires substantial efforts in terms of time and resources. The strong microstructure-dependent performance of polymer:polymer cells makes them particularly difficult to optimize, or to translate previous knowledge from spin coating into more scalable techniques. In this work, the photovoltaic performance of blade-coated devices was studied based on the promising polymer:polymer system PBDB-T and PF5-Y5 as donor and acceptor, respectively. Using the recently developed high-throughput methodology, the system was optimized for multiple variables, including solvent system, active layer composition, ratio, and thickness, among others, by fabricating more than 500 devices with less than 24 mg of each component. As a result, the power conversion efficiency of the blade-coated devices varied from 0.08 to 6.43 % in the best device. The performed statistical analysis of the large experimental data obtained showed that solvent selection had the major impact on the final device performance due to its influence on the active layer microstructure. As a conclusion, the use of the plot of the device efficiency in the Hansen space was proposed as a powerful tool to guide solvent selection in organic photovoltaics.

The desired attributes of organic photovoltaics (OPV) as a low cost and sustainable energy harvesting technology demand the use of non-halogenated solvent processing for the photoactive layer (PAL) materials, preferably of low synthetic complexity (SC) and without compromising the power conversion efficiency (PCE). Despite their record PCEs, most donor-acceptor conjugated copolymers in combination with non-fullerene acceptors are still far from upscaling due to their high cost and SC. Here we present a non-halogenated and low SC ink formulation for the PAL of organic solar cells, comprising PTQ10 and PC61BM as donor and acceptor materials, respectively, showing a record PCE of 7.5% in blade coated devices under 1 sun, and 19.9% under indoor LED conditions. We further study the compatibility of the PAL with 5 different electron transport layers (ETLs) in inverted architecture. We identify that commercial ZnO-based formulations together with a methanol-based polyethyleneimine-Zn (PEI-Zn) chelated ETL ink are the most suitable interlayers for outdoor conditions, providing fill factors as high as 74% and excellent thickness tolerance (up to 150 nm for the ETL, and >200 nm for the PAL). In indoor environments, SnO2 shows superior performance as it does not require UV photoactivation. Semi-transparent devices manufactured entirely in air via lamination show indoor PCEs exceeding 10% while retaining more than 80% of the initial performance after 400 and 350 hours of thermal and light stress, respectively. As a result, PTQ10:PC61BM combined with either PEI-Zn or SnO2 is currently positioned as a promising system for industrialisation of low cost, multipurpose OPV modules.

The mass implementation of renewable energies is limited by the absence of efficient and affordable technology to store electrical energy. Thus, the development of new materials is needed to improve the performance of actual devices such as batteries or supercapacitors. Herein, the facile consecutive chemically oxidative polymerization of poly(1-amino-5-chloroanthraquinone) (PACA) and poly(3,4-ethylenedioxythiophene (PEDOT) resulting in a water dispersible material PACA-PEDOT is shown. The water-based slurry made of PACA-PEDOT nanoparticles can be processed as film coated in ambient atmosphere, a critical feature for scaling up the electrode manufacturing. The novel redox polymer electrode is a nanocomposite that withstands rapid charging (16 A g−1) and delivers high power (5000 W kg−1). At lower current density its storage capacity is high (198 mAh g−1) and displays improved cycling stability (60% after 5000 cycles). Its great electrochemical performance results from the combination of the redox reversibility of the quinone groups in PACA that allows a high amount of charge storage via Faradaic reactions and the high electronic conductivity of PEDOT to access to the redox-active sites. These promising results demonstrate the potential of PACA-PEDOT to make easily organic electrodes from a water-coating process, without toxic metals, and operating in non-flammable aqueous electrolyte for large scale pseudocapacitors. 

Charge separation dynamics after the absorption of a photon is a fundamental process relevant both for photosynthetic reaction centers and artificial solar conversion devices. It has been proposed that quantum coherence plays a role in the formation of charge carriers in organic photovoltaics, but experimental proofs have been lacking. Here we report experimental evidence of coherence in the charge separation process in organic donor/acceptor heterojunctions, in the form of low frequency oscillatory signature in the kinetics of the transient absorption and nonlinear two-dimensional photocurrent spectroscopy. The coherence plays a decisive role in the initial ~200 femtoseconds as we observe distinct experimental signatures of coherent photocurrent generation. This coherent process breaks the energy barrier limitation for charge formation, thus competing with excitation energy transfer. The physics may inspire the design of new photovoltaic materials with high device performance, which explore the quantum effects in the next-generation optoelectronic applications.

Organic solar cells (OSCs) have been dominated by donor: acceptor blends based on fullerene acceptors for over two decades. This situation has changed recently, with non-fullerene (NF) OSCs developing very quickly. The power conversion efficiencies of NF OSCs have now reached a value of over 13%, which is higher than the best fullerene-based OSCs. NF acceptors show great tunability in absorption spectra and electron energy levels, providing a wide range of new opportunities. The coexistence of low voltage losses and high current generation indicates that new regimes of device physics and photophysics are reached in these systems. This Review highlights these opportunities made possible by NF acceptors, and also discuss the challenges facing the development of NF OSCs for practical applications.