Sacrificial photocatalytic hydrogen evolution has advanced rapidly, yet meaningful benchmarking remains hindered by inconsistent metrics and the incomplete reporting of key experimental parameters. In this Perspective, we outline a minimal "reporting set"-intended to be practical for authors, reviewers, and editors-that improves transparency and enables cross-study comparison. We further show that the widely used mass-normalized hydrogen evolution rate (HER) can be strongly affected by the experimental conditions. As a simple step toward improved comparability, we advocate incorporating the irradiation surface area into rate reporting and introduce an area-mass normalized metric (HERA,M), which markedly improves cross-study consistency. In addition, we explored solar-to-chemical conversion SCC(H2) as a complementary metric tailored for sacrificial hydrogen evolution and a diagnostic tool "HER x SCC" to identify trade-offs associated with photocatalyst concentrations. Finally, we propose a two-axis benchmarking concept (HERA,M and SCC(H2)) to visualize performance and report quality simultaneously.
Controlling active-layer morphology without processing additives remains a core challenge for high-efficiency organic solar cells (OSCs), particularly for molecular-weight-sensitive polymer donors. Here, we report an additive-free morphology control strategy based on molecular-weight-mediated aggregation kinetics using the benchmark donor polymer D18. We show that both low- and high-molecular-weight D18 exhibit aggregation behavior mismatched to the nonfullerene acceptor L8-BO, causing to suboptimal film formation. By blending D18 with different molecular weights, the donor aggregation time window is broadened and moderated, enabling kinetically synchronized film formation without additive assistance. As a result, additive-free D18-mix:L8-BO devices deliver a high power conversion efficiency of 20.0% with balanced charge transport and suppressed recombination, while maintaining efficiencies above 19% over a wide blending range. Moreover, this intrinsic kinetic regulation strategy is compatible with advanced device architectures and scalable fabrication: ternary D18-mix:L8-BO:AITC devices achieve an enhanced efficiency of 20.5%, and large-area modules (17.14 cm2) retain an efficiency of 17.2%. This work establishes molecular weight as an intrinsic kinetic handle for additive-free morphology control, offering a robust and scalable materials strategy for high-performance OSCs.
Nitroxide radical-conjugated polymer additives (nr-PAs) have been employed as newly emerged additives to mitigate the non-radiative energy loss (Elossnon_ rad), thus to boost the performance and stability of the non-fullerene acceptors-based organic solar cells (NFAs-OSCs). Herein, the small molecular nitroxide radical compounds (SMTEMPO) of racemic 4-glycidyloxy-substituted 2,2,6,6-tetramethylpiperidine-1-oxyl (GTEMPO), the stereoisomers of (R)-GTEMPO and (S)-GTEMPO, are employed as the additives for NFAs-OSCs. Upon addition of 1.0 wt% (relative to the weight of polymer donor) of the SM-TEMPO radical additives, the power conversion efficiencies (PCEs) of the devices improved as follows: PM6:Y6: from 15.73% (pristine) to 16.46% (GTEMPO), 17.20% ((R)GTEMPO), and 16.91% ((S)-GTEMPO). D18-Cl:L8-BO: from 17.53% (pristine) to 18.66% (GTEMPO), 19.42% ((R)-GTEMPO), and 19.38% ((S)-GTEMPO). On the contrary, the addition of the unglycidylated 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) radical additive always results in a slight decrease in the PCEs of the PM6:Y6based NFAs-OSCs. Moreover, the reasons behind the performance enhancement, as well as the specific correlation between the improved performances of NFAs-OSCs and the difference in aggregation behaviours between the SM-TEMPO and TEMPO radical additives, are investigated and discussed through a set of physical investigations of representative PM6:Y6-based blends and devices. This work not only demonstrates that SMTEMPO radical additives, which tend to aggregate in the active layer, can serve as effective additives to improve the performance and stability of the NFAs-OSCs as their nr-PAs counterparts, but also points towards simpler avenues for the development of the nitroxide radical-based additives to achieve high-performance NFAsOSCs with enhanced stability.
Self-assembled monolayers (SAMs) are widely used as hole-transport layers (HTLs) in organic solar cells (OSCs), yet conventional single-component SAMs often form quasi-monolayers with incomplete coverage and interfacial defects that become increasingly detrimental upon device scaling. Here, we develop a co-assembled multilayered SAM (coSAMu) strategy that combines two SAM molecules, 2PACz and 2Cl-4PACz, with distinct dipoles and steric configurations through blend casting and sequential casting. Photoelectron spectroscopy, X-ray analysis, and molecular simulations support a layered structure in which a chemisorbed, 2PACz-rich bottom layer primarily sets the indium tin oxide (ITO) work function, while a 2Cl-4PACz-rich upper layer fills interfacial voids, improves molecular packing, and passivates defects. Consistent with this picture, coSAMu promotes a more favorable vertical composition near the ITO surface and suppresses trap-assisted recombination, enabling more efficient charge extraction and collection. Consequently, a representative D18:L8-BO OSC incorporating the sequential-cast coSAMu HTL achieves a power conversion efficiency of 20.1
The development of multifunctional, flexible, and sustainable wearable electronics is critical for the advancement of next-generation smart systems. In this paper, a dual-functional, self-powered device capable of both piezoelectric energy harvesting and high-sensitivity strain sensing is reported. This device was fabricated using sulfated cellulose nanocrystals (SCNCs) derived from waste tissue. These SCNCs were integrated with carbon nanotubes (CNTs) and polyvinyl alcohol (PVA) and supported on biodegradable mulberry paper (MP). It was found that sulfation enhanced the surface charge density, crystallinity, and dipole alignment of the CNCs, thereby significantly improving the piezoelectric performance confirmed with theoretical simulation such as DFT, COMSOL Multiphysics simulation, piezobased dielectric studies and characterization experiments. Based on the experimental demonstration, the optimized composite device exhibited an open-circuit voltage of 6–8 V and short-circuit current of 120–150 nA under mechanical deformation. Furthermore, it demonstrated a rapid response (0.5–2 s) and high sensitivity of more than 80
Self-assembled monolayers (SAMs) are widely used as hole-transport layers (HTLs) in organic solar cells (OSCs), yet conventional single-component SAMs often form quasi-monolayers with incomplete coverage and interfacial defects that become increasingly detrimental upon device scaling. Here, we develop a co-assembled multilayered SAM (coSAMu) strategy that combines two SAM molecules, 2PACz and 2Cl-4PACz, with distinct dipoles and steric configurations through blend casting and sequential casting. Photoelectron spectroscopy, X-ray analysis, and molecular simulations support a layered structure in which a chemisorbed, 2PACz-rich bottom layer primarily sets the indium tin oxide (ITO) work function, while a 2Cl-4PACz-rich upper layer fills interfacial voids, improves molecular packing, and passivates defects. Consistent with this picture, coSAMu promotes a more favorable vertical composition near the ITO surface and suppresses trap-assisted recombination, enabling more efficient charge extraction and collection. Consequently, a representative D18:L8-BO OSC incorporating the sequential-cast coSAMu HTL achieves a power conversion efficiency of 20.1% (0.042 cm2), outperforming pristine 2PACz. Importantly, when scaled to a 17.14 cm2 mini-module (six serially connected subcells), coSAMu delivers 17.0% efficiency versus 12.2% for the 2PACz control. This work demonstrates controlled multilayer co-assembly as an effective strategy for scalable OSC interface engineering that is broadly applicable to multiple donor-acceptor systems.
The development of high-performance, non-halogenated organic solar cells (OSCs) is essential for sustainable commercialization. However, the high boiling points of halogen-free solvents often trigger excessive pre-aggregation of non-fullerene acceptors (NFAs) and unfavorable phase separation, severely limiting device performance. Herein, a side-chain steric engineering strategy is employed to develop a weakly crystalline NFA, TPD-Y, featuring a thieno[3,4-c]pyrrole-4,6-dione unit. The reduced crystallinity of TPD-Y effectively suppresses aggregation-caused quenching (ACQ), yielding a high photoluminescence quantum yield (PLQY) of 8.19% and significantly minimized non-radiative voltage loss. Furthermore, TPD-Y acts as a potent crystallization-kinetics modulator in multi-component blends with the benchmark acceptor BTP-eC9. It forms an alloy phase that simultaneously promotes nucleation and inhibits excessive grain growth in non-halogenated solvents, accelerating film formation while refining oversized domains. This kinetic modulation yields an optimized nanoscale morphology with enlarged interfacial areas, synergistically enhancing exciton dissociation and charge collection. Consequently, quaternary OSCs processed from a non-halogenated o-xylene/carbon disulfide mixture achieve a remarkable fill factor of nearly 82% and a record power conversion efficiency exceeding 21%. This work provides a robust molecular design to overcome the efficiency bottleneck of chlorinated-solvent-free OSCs, marking a significant step toward the industrialization of high-performance, low-toxicity photovoltaics.
Balancing high performance, morphological controllability, and compatibility with non-halogenated solvent processing remains a critical bottleneck for scalable and sustainable organic solar cells (OSCs). Herein, we address this challenge via rational terpolymer design: integrating a siloxane-functionalized electron-deficient pyrazine unit (DTCPz-SiO) into the benchmark D18 backbone, with the optimized terpolymer DN1 containing 5 mol% DTCPz-SiO. DTCPz-SiO imparts two key synergies: (i) enhanced conformational rigidity and intramolecular noncovalent interactions (N···S, N···H), which improve backbone planarity, strengthen π-π stacking, and accelerate crystallization; (ii) synergistic regulation of donor-acceptor miscibility and compatibility with non-halogenated solvents. These effects collectively enable a well-optimized bulk-heterojunction morphology with enhanced molecular ordering and charge dynamics. Consequently, DN1-based binary devices deliver a significantly improved power conversion efficiency (PCE) of 20.1% compared to 18.7% for the parent polymer, together with a broadened processing window. Notably, high efficiencies of ∼19.5% are retained under common non-halogenated processing conditions. Furthermore, DN1-based ternary OSCs enhance PCE to outstanding values of 20.9% and 20.0% under chlorinated and non-halogenated processing conditions, respectively, among the highest efficiencies reported for single-junction OSCs. Overall, this work establishes siloxane-functionalized terpolymers as an effective molecular design strategy for regulating multi-scale morphology and processing tolerance, providing new insights for the development of scalable OSC systems.
The molecular orientation is crucial for the efficiency of organic solar cells. A face-on orientation, in which the pi-pi stacking direction is oriented perpendicular to the substrate, is typically preferred because it enhances vertical charge transport to the electrodes and can additionally modify the position of energy levels. In this study, near-edge x-ray absorption fine structure (NEXAFS) spectroscopy was employed to investigate the molecular orientation of the acceptor polymers PYT and PF5-Y5 and the donor polymer PBDB-T in spin-coated blend films with different donor: acceptor ratios. From the comparison of NEXAFS spectra acquired in partial electron yield (PEY), total electron yield (TEY), and fluorescence yield (FY) modes, depth-dependent information about the orientation of the components in the films can be extracted. We found that the absorption resonances in the PEY carbon K-edge spectra of all the blend films resembled the spectral signatures of PBDB-T, indicating that the surface of these blend films is PBDB-T-rich, even at a 1:10 donor-to-acceptor ratio. To identify the acceptor component in the carbon spectra, deeper subsurface probing was required using TEY and FY modes, alongside analysis of the angular dependence of these spectra. Nitrogen K-edge NEXAFS spectra were employed to selectively probe the acceptor orientation in the blend films, revealing that generally the polymer acceptors retain their face-on orientation observed in neat acceptor films. However, in one blend, a decrease in the dichroic ratio suggests that the donor polymer influences the molecular orientation of the acceptor at the film's surface. This work demonstrates a novel strategy to probe molecular orientation in all-polymer blend films. The approach exploits dichroism at selective absorption edges to access detailed information on the molecular orientation of one component within the blend film.
The larger non-radiative energy loss (Delta Vnon-radoc) of the non-fullerene-based organic solar cells (NFAs-OSCs) has been demonstrated to be the main barrier to further boosting the efficiency of NFAs-OSCs. In response, extensive studies have been implemented, focusing on the optimization of the photoactive layer morphology, molecular engineering of donors and acceptors, and the development of multi-component NFAs-OSCs etc., thereby achieving a series of devices with markedly enhanced performance. As an emerging strategy, the utilization of nitroxide radical-conjugated polymer additives is also worthy of attention due to their ability to simultaneously enhance the performance and stability of NFAs-OSCs. In this study, the racemic and isotactic nitroxide radical polymonothiocarbonates (PTC-NOs, with the specific names of Rac-PTC-NO, (R)-PTC-NO and (S)-PTC-NO) are employed as solid additives to mitigate the Delta Vnon-radoc of the NFAs-OSCs. Upon the addition of 0.5 wt% of Rac-PTC-NO, (R)-PTC-NO and (S)-PTC-NO, the PCEs of the PM6:Y6-based NFAs-OSCs are respectively improved from 15.73% to 16.59%, 17.30% and 17.40%. Besides, the reasons behind the improvement in the performance of the NFAs-OSCs from the representative photovoltaic material pair of PM6:Y6, such as the increase of the exciton dissociation probability, suppression of charge carrier recombination and mitigation of the non-radiative energy loss of the devices upon the addition of the PTC-NOs additives, are supported by and discussed through a set of comparative investigations. This work not only broadens the scope but also provides new insights for designing and developing efficient nitroxide radical-based polymeric additives to mitigate the non-radiative energy loss, thus further boosting the performance of NFAs-OSCs.
ABSTRACT Fabric‐based wearable electronics are gaining increasing attention owing to their flexibility, breathability, biocompatibility, and seamless integration into clothing. However, most existing studies rely primarily on metallic or carbon‐based conductive materials. In contrast, the integration of semiconducting metal oxides in wearable textiles remains limited, despite their advantages in achieving tunable electrical and thermal responses. In this study, we developed a sandwich‐structured coating on cotton fabric, where a semiconductive layer of WO3‐doped ZnO nanorods was embedded between two conductive layers of MXene and carbon nanotubes (CNTs). This hierarchical and heterogeneous coating architecture enabled synergistic interactions that significantly enhance multifunctional performance. The engineered fabric exhibited reliable strain sensing with a short response and recovery time (∼200 ms), excellent mechanical durability over 2000 stretch/release cycles, and the ability to monitor human motion. Furthermore, the fabric demonstrated efficient Joule heating, reaching ∼110°C within ∼15 s, and high electromagnetic interference (EMI) shielding effectiveness (∼34.4 dB), which increased to ∼78 dB by raising fabric thickness, meeting commercial EMI standards. Notably, these functionalities were achieved without compromising flexibility, light weight, and breathability. Thus, this study presents a new paradigm for designing multifunctional textile electronics by integrating semiconductive and conductive nanomaterials, overcoming the limitations of conventional conductive‐only approaches.
At present, the synthetic difficulty of white light-emitting polymers needs to be reduced, and their operational stability still requires further enhancement. In this work, a series of cardo polyimides (PI) containing green thermally activated delayed fluorescence (TADF) units on the main chain and red TADF units on the side chain, respectively, designated as PITFN-x (x = 0, 0.5, 1, 3, 5, 10, or 100), were synthesized via a facile method. Ultimately, the white light emission was achieved by adjusting the molar ratio of green/red TADF units in PIs. All PIs demonstrated outstanding thermal stability (Td > 448 °C, Tg > 343 °C) and excellent solubility in common solvents such as trichloromethane (TCM) and dichloromethane (DCM). Meanwhile, they maintained the photophysical characteristics of the corresponding small-molecule emitters. The non-doped OLED device using PITFN-10 as the emitting layer (EML) achieved a maximum external quantum efficiency (EQEmax) of 0.86% and a maximum brightness (Lmax) of 1185.9 cd/m2. Moreover, the doped device using the 10 wt.% PITFN-10 in CBP as the EML exhibited white light with CIE coordinates of (0.35, 0.34), an EQEmax of 1.94% and a Lmax of 1236.4 cd/m2. This research offers a new design approach for developing white light-emitting materials with both facile synthesis and good thermal stability.
ABSTRACT Solution‐processed tunable broadband photodetectors are fabricated by using acidochromic polymers in photodiode and phototransistor geometries with SnO2/polymer p‐n heterojunctions. This organic‐inorganic heterojunction works as a rectifying junction and bilayer channel of the photodiodes and phototransistors, respectively. In both devices, the lower bandgap acidochromic polymers (PIDT‐BAB, PIDT‐BIB, and PIDT‐BVB) work as the photoactive layer, whereas n‐type SnO2 works as the electron transport layer, and the devices show high spectrally selective blue and green sensitivity. The responsivity, detectivity, and response time of these photodiodes are in the range of 20–40 mA/W, 4–7.5 × 109 Jones, and ∼7–10 s, respectively. The phototransistors are fabricated by using high‐κ Li‐Al2O3 gate dielectric, which enables them to reach their operating voltage within 2 V. Furthermore, the thin‐film transistors (TFTs) show a large variation of threshold voltage with light intensity, with good linearity of variation with illumination power. The responsivity, detectivity, and response time of these phototransistors are in the same range as those of the photodiodes. Additionally, the spectral response of the photodiodes is tuned from the visible to the NIR region by using vapor‐phase trifluoroacetic acid (TFA) due to their acidochromic effect in a reversible way, indicating their possible application as an optoelectrical switch.
Generally, single-molecule white-emitting polymers (SMWEPs) are synthesized by the direct polymerization of functional monomers. Herein, we designed conjugated polymers PCFTN-X (X = 0.5, 1, 3, 5, or 10) by grafting red/green TADF units onto the backbone via alkyl linkers. This structural design balances the charge transport of the conjugated backbone with the independent photophysical properties of the TADF units on the side chains. PCFTN-X was synthesized via Suzuki polymerization and post-Click reaction, ensuring good reproducibility and tunable red/green ratios. The nondoped device based on PCFTN-3 achieved stable white emission with CIE coordinates of (0.34, 0.38), a low turn-on voltage (V on) of 3.4 V, a maximum external quantum efficiency (EQEmax) of 10.23%, and a maximum luminance (L max) of 3264 cd m-2. This design and synthesis strategy can be extended to other optoelectronic polymers.
Photomultiplication-type organic photodetectors (PM-OPDs) have attracted significant attention for their high gain and simplified device architecture. However, their practical application is severely constrained by the high dark current density inherent to charge injection-type multiplication mechanisms, which compromises specific detectivity (D*), as well as the poor environmental stability associated with conventional acidic and hygroscopic interlayers. Herein, we demonstrate that replacing the conventional PEDOT:PSS hole-transport layer with a self-assembled monolayer of 1F-2PACz not only dramatically suppresses dark current but also significantly enhances device robustness. In PM-OPDs with a P3HT:PC71BM (100:1, w/w) active layer, the 1F-2PACz-modified devices effectively suppress electron back-injection owing to the high work function and electron-blocking lowest unoccupied molecular orbital level of 1F-2PACz, exhibiting a dark current one order of magnitude lower than PEDOT:PSS-based counterparts, resulting in a high specific detectivity exceeding 1013 Jones. Mechanistic investigations reveal that 1F-2PACz facilitates faster hole extraction and mitigates interfacial trap-mediated recombination. Crucially, the hydrophobic nature of the fluorinated carbazole moiety endows the devices with superior water resistance and long-term stability; the device maintains stable performance after direct water immersion for 30 min and continuous storage for 60 days. This work demonstrates that self-assembling hole-transport molecules provide a robust strategy for simultaneously achieving high gain, low noise, and excellent stability in PM-OPDs.
Minimizing nonradiative energy loss (ΔEnr) is a critical imperative for bridging the efficiency gap in organic solar cells (OSCs). Herein, we demonstrate a thiophene-terminal engineering strategy to develop a twisted small-molecule acceptor, named as AQx-2T. By substituting conventional terminal groups with electron-donating thiophene moieties, the intramolecular charge-transfer character is effectively moderated, leading to upshifted frontier molecular orbitals and a high open-circuit voltage (VOC) exceeding 1.0 V in D18:AQx-2T binary devices. Crucially, the rotational freedom of the thiophene linkages induces a more twisted molecular conformation, which successfully mitigates excessive aggregation and reduces crystallinity. Consequently, AQx-2T achieves an ultralow ΔEnr of 0.182 eV. When introduced as a guest acceptor into the highly crystalline D18:L8-BO host matrix, AQx-2T promotes acceptor co-assembly, moderates molecular ordering, suppresses large-scale phase separation, and refines the bulk-heterojunction morphology. Benefiting from improved exciton dissociation, balanced charge transport, and minimized recombination, the optimized ternary D18:L8-BO:AQx-2T device achieves an outstanding power conversion efficiency of 20.79%, accompanied by a reduced ΔEnr from 0.216 eV to 0.197 eV. This work demonstrates that balancing molecular planarity and electronic structures via terminal engineering provides a powerful paradigm for overcoming the voltage deficit in high-performance OSCs.
The growing demand for flexible and wearable energy storage systems calls for sustainable and mechanically robust substrates that overcome the limitations of conventional rigid and nonbiocompatible materials. Here, we present a binder-free and flexible supercapacitor fabricated on mulberry paper, integrating electrostatically engineered carbon nanotubes (CNTs) and covalently cross-linked poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS). CNTs modified with a cationic surfactant, cetyltrimethylammonium bromide (CTAB), uniformly adhere to the hydroxyl-rich fibers via electrostatic interactions, enhancing interfacial stability and minimizing resistance. PEDOT:PSS is cross-linked using divinyl sulfone (DVS), simultaneously improving electrical conductivity and aqueous stability. The resulting device exhibits an areal capacitance of 30.4 mF cm(-2) at 50 mV s(-1) and maintains 95.9% of its capacitance over 80,000 cycles at 4.0 mA cm(-2). This study provides a scalable and low-cost platform for high-performance, durable, and flexible energy storage, highlighting a novel interfacial engineering strategy for natural fiber substrates.