Molecular weight (M-n) and conjugation of polymers can profoundly influence the performance of all-polymer solar cells (all-PSCs) via nanostructures of bulk heterojunctions (BHJs). To study the correlation between M-n and the performance of all-PSCs based on an acceptor with a flexible conjugation-break spacer (FCBS), three batches of acceptors, named PYTS, were synthesized with different number-average M-n from 9, 13 to 19 kDa. Blends with a polymer donor PBDB-T, the all-PSCs based on PYTS with M-n of 9 kDa and 19 kDa, exhibit power conversion efficiencies (PCEs) of 5.99% and 9.43%, respectively, primarily due to the increased short-circuit current density (J(sc)) from 13.02 to 18.73 mA cm(-2). To disclose the impact of M-n on device performance, dynamics of mixed PBDB-T:PYTS solutions to solid BHJs is studied by monitoring the drying process with home-made in situ multifunctional spectroscopy, which demonstrates that PYTS with M-n of 19 kDa has a longer drying time than the PYTS with M-n of 9 kDa. Prolonged drying of the BHJs with higher M-n PYTS facilitates more tightly packed structures with higher crystallinity. A systematic investigation on the nanostructures of BHJs, charge generation, transport and recombination is carried out with grazing-incidence wide-angle X-ray scattering (GIWAXS), transient absorption spectroscopy (TAS) and characterization of all-PSCs. The results indicate that increased crystallinity in the BHJs benefits exciton dissociation, electron transport, prolonged carrier lifetimes, and decreased non-geminate recombination rate constants in the corresponding devices. Combining the in situ study of drying and the investigation on films and devices provides us a comprehensive understanding of the interplay between M-n, the drying process, the nanostructures of BHJs and device performance. This work not only emphasizes the essential role of M-n in governing the device performance, but also exhibits recorded film formation through the in situ spectroscopy, enabling us to manipulate the nanostructure of BHJs by optimizing M-n of polymers and processing parameters.

Supercapacitors based on two-dimensional MXene (Ti3C2Tz) have shown extraordinary performance in ultrathin electrodes with low mass loading, but usually there is a significant reduction in high-rate performance as the thickness increases, caused by increasing ion diffusion limitation. Further limitations include restacking of the nanosheets, which makes it challenging to realize the full potential of these electrode materials. Herein, we demonstrate the design of a vertically aligned MXene hydrogel composite, achieved by thermal-assisted self-assembled gelation, for high-rate energy storage. The highly interconnected MXene network in the hydrogel architecture provides very good electron transport properties, and its vertical ion channel structure facilitates rapid ion transport. The resulting hydrogel electrode show excellent performance in both aqueous and organic electrolytes with respect to high capacitance, stability, and high-rate capability for up to 300 mu m thick electrodes, which represents a significant step toward practical applications.

Fiber type devices are promising for applications in wearable and portable electronics. However, scalable fabrication of fiber electrodes with multifunctional performance for use in distinct fields remains challenging. Herein, high performance smart fibers based on Mo1.33C i-MXene nanosheets and poly(3,4-ethylenedioxythiophene):polystyrene sulfonate hybrid paste are fabricated with an easily scalable spinning approach. The hybrid fibers produced by this method can be applied in both high-performance supercapacitors and electrochemical transistors (ECTs). When assembled into a fiber type asymmetric supercapacitor with reduced graphene oxide (rGO) fiber, a capacitance of 105 F g(-1) and an energy density of 37 mW h g(-1) were reached for a potential window of 1.6 V. The hybrid fiber based ECT shows high transconductance and fast response time. This work demonstrates the potential of i-MXene-based fiber electrodes for multifunctional applications, to aid in the development of the next-generation, high-performance wearable electronic devices.

Semitransparent organic solar cells (ST-OSCs) are promising candidates for applications in building-integrated photovoltaics (BIPV) as windows and facades. The challenge to achieve highly efficient ST-OSCs is the trade-off between power conversion efficiency (PCE) and average visible transmittance (AVT). Herein, solution-processed ST-OSCs are demonstrated on the basis a polymer donor, PM6, and a small molecule acceptor, Y6; lowering the visible-absorbing PM6 contents in blends could increase AVT and maintain PCE. Additionally, conductive polymer PEDOT:PSS is used as the top electrode due to its high transparency, good conductivity, and solution processability. Efficient ST-OSCs with 20 wt % PM6 achieve high PCE of 7.46% and AVT of 36.4%. The light utilization efficiency (LUE) of 2.72% is among the best reported values for solution-processed ST-OSCs. This work provides a straightforward approach for solution-processed ST-OSCs by combining a low fraction of visible-wavelength-selective polymer donors with near-infrared nonfullerene acceptors to achieve high PCE and AVT simultaneously.

Two-dimensional (2D) transition metal carbides and carbonitrides, called MXenes, with metallic conductivity and hydrophilic surfaces, show great promise as electrode materials for supercapacitors. A major drawback of 2D nanomaterials is the re-stacking of the nanosheets, which prevents full utilization of surface area and blocks the access of the electrolyte. In this study, a free-standing nanocomposite paper electrode is realized by combining Mo1.33C MXene and positively charged biopolymer lignin (the second most abundant biopolymer in nature, L-DEA). The self-assembled layered architecture with alternating polymer and MXene flakes increases the interlayer space to promote ion transport, and with combining charge storage capability of the lignin derivative and MXene in an interpenetrating MXene/L-DEA nanocomposite, which offers an impressive capacitance of 503.7 F g(-1). Moreover, we demonstrate flexible solid-state asymmetric supercapacitors (ASCs) using Mo1.33C@L-DEA as the negative electrode and electrochemically exfoliated graphene with ruthenium oxide (EG@RuOx) as the positive electrode. This asymmetric device operates at a voltage window of 1.35 V, which is about two times wider than that of a symmetric Mo1.33C@L-DEA based supercapacitor. Finally, the ASCs can deliver an energy density of 51.9 Wh kg(-1) at a power density of 338.5 W kg(-1), with 86 % capacitance retention after 10000 charge-discharge cycles.

Low-cost, non-toxic, abundant organic thermoelectric materials are currently under investigation for use as potential alternatives for the production of electricity from waste heat. While organic conductors reach electrical conductivities as high as their inorganic counterparts, they suffer from an overall low thermoelectric figure of merit (ZT) due to their small Seebeck coefficient. Moreover, the lack of efficient n-type organic materials still represents a major challenge when trying to fabricate efficient organic thermoelectric modules. Here, a novel strategy is proposed both to increase the Seebeck coefficient and achieve the highest thermoelectric efficiency for n-type organic thermoelectrics to date. An organic mixed ion-electron n-type conductor based on highly crystalline and reduced perylene bisimide is developed. Quasi-frozen ionic carriers yield a large ionic Seebeck coefficient of -3021 mu V K-1, while the electronic carriers dominate the electrical conductivity which is as high as 0.18 S cm(-1)at 60% relative humidity. The overall power factor is remarkably high (165 mu W m(-1)K(-2)), with aZT= 0.23 at room temperature. The resulting single leg thermoelectric generators display a high quasi-constant power output. This work paves the way for the design and development of efficient organic thermoelectrics by the rational control of the mobility of the electronic and ionic carriers.

Here, we report the usage of two-dimensional MXene, Mo1.33C-assisted poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) as an efficient hole transport layer (HTL) to construct high-efficiency polymer solar cells. The composite HTLs are prepared by mixing Mo1.33C and PEDOT:PSS aqueous solution. The conventional devices based on Mo1.33C:PEDOT:PSS exhibit an average power conversion efficiency (PCE) of 9.2%, which shows a 13% enhancement compared to the reference devices. According to the results from hole mobilities, charge extraction probabilities, steady-state photoluminescence, and atomic force microscopy, the enhanced PCE can be ascribed to the improved charge transport and extraction properties of the HTL, along with the morphological improvement of the active layer on top. This work clearly demonstrates the feasibility to combine advantages of Mo1.33C MXene and PEDOT:PSS as the promising HTL in organic photovoltaics.

While photovoltaic blends based on non-fullerene acceptors are touted for their thermal stability, this type of acceptor tends to crystallize, which can result in a gradual decrease in photovoltaic performance and affects the reproducibility of the devices. Two halogenated indacenodithienothiophene-based acceptors that readily co-crystallize upon mixing are studied, which indicates that the use of an acceptor mixture alone does not guarantee the formation of a disordered mixture. The addition of the donor polymer to the acceptor mixture readily suppresses the crystallization, which results in a fine-grained ternary blend with nanometer-sized domains that do not coarsen due to a highT(g)approximate to 200 degrees C. As a result, annealing at temperatures of up to 170 degrees C does not markedly affect the photovoltaic performance of ternary devices, in contrast to binary devices that suffer from acceptor crystallization in the active layer. The results indicate that the ternary approach enables the use of high-temperature processing protocols, which are needed for upscaling and high-throughput fabrication of organic solar cells. Further, ternary devices display a stable photovoltaic performance at 130 degrees C for at least 205 h, which indicates that the use of acceptor mixtures allows to fabricate devices with excellent thermal stability.

A pronounced enhancement of the power conversion efficiency (PCE) by 38% is achieved in one-step doctor-blade printing organic solar cells (OSCs) via a simple solvent vapor annealing (SVA) step. The organic blend composed of a donor polymer, a nonfullerene acceptor, and an interfacial layer (IL) molecular component is found to phase-separate vertically when exposed to a solvent vapor-saturated atmosphere. Remarkably, the spontaneous formation of a fine, self-organized IL between the bulk heterojunction (BHJ) layer and the indium tin oxide (ITO) electrode facilitated by SVA yields solar cells with a significantly higher PCE (11.14%) than in control devices (8.05%) without SVA and in devices (10.06%) made with the more complex two-step doctor-blade printing method. The stratified nature of the ITO/IL/BHJ/cathode is corroborated by a range of complementary characterization techniques including surface energy, cross-sectional scanning electron microscopy, grazing incidence wide angle X-ray scattering, and X-ray photoelectron spectroscopy. This study demonstrates that a spontaneously formed IL with SVA treatment combines simplicity and precision with high device performance, thus making it attractive for large-area manufacturing of next-generation OSCs.

A free-standing high-output power density polymeric thermoelectric (TE) device is realized based on a highly conductive (approximate to 2500 S cm(-1)) structure-ordered poly(3,4-ethylenedioxythiophene):polystyrene sulfonate film (denoted as FS-PEDOT:PSS) with a Seebeck coefficient of 20.6 mu V K-1, an in-plane thermal conductivity of 0.64 W m(-1) K-1, and a peak power factor of 107 mu W K-2 m(-1) at room temperature. Under a small temperature gradient of 29 K, the TE device demonstrates a maximum output power density of 99 +/- 18.7 mu W cm(-2), which is the highest value achieved in pristine PEDOT:PSS based TE devices. In addition, a fivefold output power is demonstrated by series connecting five devices into a flexible thermoelectric module. The simplicity of assembling the films into flexible thermoelectric modules, the low out-of-plane thermal conductivity of 0.27 W m(-1) K-1, and free-standing feature indicates the potential to integrate the FS-PEDOT:PSS TE modules with textiles to power wearable electronics by harvesting human bodys heat. In addition to the high power factor, the high thermal stability of the FS-PEDOT:PSS films up to 250 degrees C is confirmed by in situ temperature-dependent X-ray diffraction and grazing incident wide angle X-ray scattering, which makes the FS-PEDOT:PSS films promising candidates for thermoelectric applications.