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Metal-organic frameworks (MOFs) are promising electrochemical materials that possess large specific surface areas, high porosities, good adjustability, and high activities. However, many conventional MOFs exhibit poor conductivity, which hinders their application in electrochemistry. In recent years, conductive MOFs (cMOFs) have attracted a considerable attention. As an important transition metal hydroxide, Ni(OH)

Incorporating non-aqueous hole-transporting materials (HTMs) to replace the widely used PEDOT:PSS is favorable for improving the stability of tin-lead perovskite solar cells (Sn-Pb PSCs). Herein, hexaazatrinaphthylene (HATNA) is found to be a promising HTM building block for Sn-Pb PSCs. By introducing triphenylamine (TPA) and methoxy-triphenylamine into the HATNA core, molecular energy levels and surface wettability can be well regulated, and a high hole mobility and thermal stability can be maintained. Moreover, a homogeneous Sn-Pb perovskite film with low Sn

Lithium-sulfur (Li-S) batteries are recognized as one of the most promising next-generation energy storage devices, but their practical application is greatly limited by several obstacles, such as the highly insulating nature and sluggish redox kinetics of sulfur and the dissolution of lithium polysulfides. Herein, three-dimensional carbon nanosheet frameworks anchored with Ni@Ni3N heterostructure nanoparticles (denoted Ni@Ni3N/CNS) are designed and fabricated by a chemical blowing and thermal nitridation strategy. It is demonstrated that the Ni@Ni3N heterostructure can effectively accelerate polysulfide conversion and promote the chemical trapping of polysulfides. Meanwhile, the carbon nanosheet frameworks of Ni@Ni3N/CNS establish a highly conductive network for fast electron transportation. The cells with Ni@Ni3N heterostructures as the catalyst in the cathode show excellent electrochemical performance, revealing stable cycling over 600 cycles with a low-capacity fading rate of 0.04% per cycle at 0.5 C and high-rate capability (594 mAh g-1 at 3 C). Furthermore, Ni@Ni3N/CNS can also work well in room-temperature sodium-sulfur (RT-Na/S) batteries, delivering a high specific capacity (454 mAh g-1 after 400 cycles at 0.5 C). This work provides a rational way to prepare the metal-metal nitride heterostructures to enhance the performance both of Li-S and RT-Na/S batteries.

Inverted perovskite solar cells (IPSCs) attract growing interest because of their simple configuration, reliable stability, and compatibility with tandem applications. However, the power conversion efficiency (PCE) of IPSCs still lags behind their regular counterparts, mainly due to the more serious nonradiative loss. Here, we design three donor-π-acceptor (D-π-A) dipoles with various dipole moments to introduce extra electric fields at the interface of perovskites and electron transport materials via the binding between the carboxylate end group and under-coordinated divalent Pb. The chemical binding reduces the recombination centers, while the superposition of the built-in electric field facilitates the electron collection and the hole blocking. As a result, the nonradiative loss is diminished as the dipole moments of D-π-A dipoles increase, which contributes to a PCE of 21.4% with enhancement in both the open-circuit voltage and fill factor. The stability for an unencapsulated device is also improved due to the hydrophobic property of D-π-A dipoles.

Commercial or clinical tissue adhesives are currently limited due to their weak bonding strength on wet biological tissue surface, low biological compatibility, and slow adhesion formation. Although catechol-modified hyaluronic acid (HA) adhesives are developed, they suffer from limitations: insufficient adhesiveness and overfast degradation, attributed to low substitution of catechol groups. In this study, we demonstrate a simple and efficient strategy to prepare mussel-inspired HA hydrogel adhesives with improved degree of substitution of catechol groups. Because of the significantly increased grafting ratio of catechol groups, dopamine-conjugated dialdehyde-HA (DAHA) hydrogels exhibit excellent tissue adhesion performance (i.e., adhesive strength of 90.0 ± 6.7 kPa), which are significantly higher than those found in dopamine-conjugated HA hydrogels (∼10 kPa), photo-cross-linkable HA hydrogels (∼13 kPa), or commercially available fibrin glues (2-40 kPa). At the same time, their maximum adhesion energy is 384.6 ± 26.0 J m-2, which also is 40-400-fold, 2-40-fold, and ∼8-fold higher than those of the mussel-based adhesive, cyanoacrylate, and fibrin glues, respectively. Moreover, the hydrogels can gel rapidly within 60 s and have a tunable degradation suitable for tissue regeneration. Together with their cytocompatibility and good cell adhesion, they are promising materials as new biological adhesives.

Zinc oxide (ZnO) is one of the most extensively used electron-transporting layers (ETLs) in organic solar cells. However, owing to numerous surface defects and mismatched energy bands with the photoactive layer, light-soaking process is usually required to achieve a high device performance for the ZnO-based cells. Herein, we reported the synthesis of N,S-doped carbon quantum dots (N,S-CQDs) by a simple hydrothermal treatment using ascorbic acid and ammonium persulfate as reagents. As characterized by high-resolution transmission electron microscopy and X-ray diffraction, the synthesized CQDs were found to be 2-7 nm in dimensions, having a graphite-structured core and amorphous carbon on the shell. Fourier transform infrared and X-ray photoelectron spectroscopy analyses confirmed that these CQDs are highly nitrogen- and sulfur-doped, which leads to efficient (with a quantum yield of 33%) downconversion and excitation-dependent photoluminescence character. Application of these N,S-CQDs as surface modifier for ZnO layer in inverted organic solar cells was investigated. Results indicate that the cells with N,S-CQDs-decorated ZnO ETL showed higher power conversion efficiency without S-shaped kink in the current density-voltage curves. The performance improvement and the elimination of light-soaking effect for ZnO:N,S-CQDs cells are attributed to the ZnO surface defect passivation by N,S-CQDs, as confirmed by fluorescence spectroscopy and scanning Kelvin probe microscopy. The cells with N,S-CQDs-modified ZnO ETL showed a high power conversion efficiency of 9.31%, which is higher than the reference ZnO cells. The current work provides a feasible way to achieve shell element-doped CQDs for specific application in organic electronic devices.

Ultrafine SnS2 nanocrystals–reduced graphene oxide nanoribbon paper (SnS2–RGONRP) has been created by a well-designed process including in situ reduction, evaporation-induced self-assembly, and sulfuration. The as-formed SnS2 nanocrystals possess an average diameter of 2.3 nm and disperse on the surface of RGONRs uniformly. The strong capillary force formed during evaporation leads to a compact assembly of RGONRs to give a flexible paper structure with a high density of 0.94 g cm–3. The as-prepared SnS2–RGONRP composite could be directly used as free-standing electrode for sodium ion batteries. Due to the synergistic effects between the ultrafine SnS2 nanocrystals and the conductive, tightly connected RGONR networks, the composite paper electrode exhibits excellent electrochemical performance. A high volumetric capacity of 508–244 mAh cm–3 was obtained at current densities in the range of 0.1–10 A g–1. Discharge capacities of 334 and 255 mAh cm–3 were still kept, even after 1500 cycles tested at current d...

We have demonstrated in this article that both power conversion efficiency (PCE) and performance stability of inverted planar heterojunction perovskite solar cells can be improved by using a ZnO:PFN nanocomposite (PFN: poly[(9,9-bis(3'-(N,N-dimethylamion)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctyl)-fluorene]) as the cathode buffer layer (CBL). This nanocomposite could form a compact and defect-less CBL film on the perovskite/PC61BM surface (PC61BM: phenyl-C61-butyric acid methyl ester). In addition, the high conductivity of the nanocomposite layer makes it works well at a layer thickness of 150 nm. Both advantages of the composite layer are helpful in reducing interface charge recombination and improving device performance. The power conversion efficiency (PCE) of the best ZnO:PFN CBL based device was measured to be 12.76%, which is higher than that of device without CBL (9.00%), or device with ZnO (7.93%) or PFN (11.30%) as the cathode buffer layer. In addition, the long-term stability is improved by using ZnO:PFN composite cathode buffer layer when compare to that of the reference cells. Almost no degradation of open circuit voltage (VOC) and fill factor (FF) was found for the device having ZnO:PFN, suggesting that ZnO:PFN is able to stabilize the interface property and consequently improve the solar cell performance stability.

Indoline-based D-A-π-A organic sensitizers are promising candidates for highly efficient and long-term stable dye-sensitized solar cells (DSSCs). In order to further broaden the spectral response of the known indoline dye WS-2, we rationally engineer the molecular structure through enhancing the electron donor and extending the π-bridge, resulting in two novel indoline-based D-A-π-A organic sensitizers WS-92 and WS-95. By replacing the 4-methylphenyl group on the indoline donor of WS-2 with a more electron-rich carbazole unit, the intramolecular charge transfer (ICT) absorption band of dye WS-92 is slightly red-shifted from 550 nm (WS-2) to 554 nm (WS-92). In comparison, the incorporation of a larger π-bridge of cyclopentadithiophene (CPDT) unit in dye WS-95 not only greatly bathochromatically tunes the absorption band to 574 nm but also largely enhances the molar extinction coefficients (ε), thus dramatically improving the light-harvesting capability. Under the standard global AM 1.5 solar light condition, the photovoltaic performances of both organic dyes have been evaluated in DSSCs on the basis of the iodide/triiodide electrolyte without any coadsorbent or cosensitizer. The DSSCs based on WS-95 display better device performance with power conversion efficiency (η) of 7.69%. The additional coadsorbent in the dye bath of WS-95 does not improve the photovoltaic performance, indicative of its negligible dye aggregation, which can be rationalized by the grafted dioctyl chains on the CPDT unit. The cosensitization of WS-95 with a short absorption wavelength dye S2 enhances the IPCE and improves the η to 9.18%. Our results indicate that extending the π-spacer is more rational than enhancing the electron donor in terms of broadening the spectral response of indoline-based D-A-π-A organic sensitizers.

An ultrathin Fe-based film was prepared by electrodeposition from an Fe(II) solution through a fast and simple cyclic voltammetry method. The extremely low Fe loading of 12.3 nmol cm(-2) on indium tin oxide electrodes is crucial for high atom efficiency and transparence of the resulted film. This Fe-based film was shown to be a very efficient electrocatalyst for oxygen evolution from neutral aqueous solution with remarkable activity and stability. In a 34 h controlled potential electrolysis at 1.45 V (vs NHE) and pH 7.0, impressive turnover number of 5.2 × 10(4) and turnover frequency of 1528 h(-1) were obtained. To the best of our knowledge, these values represent one of the highest among electrodeposited catalyst films for water oxidation under comparable conditions. The morphology and the composition of the catalyst film was determined by scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray, and X-ray photoelectron spectroscopy, which all confirmed the deposition of Fe-based materials with Fe(III) oxidation state on the electrode. This study is significant because of the use of iron, the fast and simple cyclic voltammetry electrodeposition, the extremely low catalyst loading and thus the transparency of the catalyst film, the remarkable activity and stability, and the oxygen evolution in neutral aqueous media.

The dye-sensitized solar cell (DSSC) is one of the most promising photovoltaic technologies with potential of low cost, light weight, and good flexibility. The practical application of DSSCs requires further improvement in power conversion efficiency and long-term stability. Recently, significant progress has been witnessed in DSSC research owing to the novel concept of the D-A-π-A motif for the molecular engineering of organic photosensitizers. New organic and porphyrin dyes based on the D-A-π-A motif can not only enhance photovoltaic performance, but also improve durability in DSSC applications. This Spotlight on Applications highlights recent advances in the D-A-π-A-based photosensitizers, specifically focusing on the mechanism of efficiency and stability enhancements. Also, we find insight into the additional acceptor as well as the trade-off of long wavelength response. The basic principles are involved in molecular engineering of efficient D-A-π-A sensitizers, providing a clear road map showing how to modulate the energy bands, rationally extending the response wavelength, and optimizing photovoltaic efficiency step by step.

In the efficient cosensitization, the pure organic sensitizers with high molecular extinction coefficients and long wavelength response are highly preferable since the dye loading amount for each dye in cosensitization is decreased with respect to single dye sensitization. A D-A-π-A featured quinoxaline organic sensitizer IQ21 is specifically designed. The high conjugation building block of 4H-cyclopenta[2,1-b:3,4-b']dithiophene (CPDT) is introduced as the π bridge, instead of the traditional thiophene unit, especially in realizing high molecular extinction coefficients (up to 66 600 M(-1) cm(-1)) and extending the light response wavelength. With respect to the reference dye IQ4, the slightly lower efficiency of IQ21 (9.03%) arises from the decrease of VOC, which offsets the gain in JSC. While cosensitized with a smaller D-π-A dye S2, the efficiency in IQ21 is further improved to 10.41% (JSC = 19.8 mA cm(-2), VOC = 731 mV, FF = 0.72). The large improvement in efficiency is attributed to the well-matched molecular structures and loading amounts of both dyes in the cosensitization system. We also demonstrated that coabsorbent dye S2 can distinctly compensate the inherent drawbacks of IQ21, not only enhancing the response intensity of IPCE, making up the absorption defects around low wavelength region of IPCE, but also repressing the charge recombination rate to some extent.

The option of using conjugated π-linkers is critical for rational molecular design toward an energy-level strategy for organic sensitizers. To further optimize photovoltaic performance, methyl- and octyl-substituted 4H-cyclopenta[2,1-b:3,4-b']dithiophene (CPDT) are introduced into D-A-π-A featured sensitizers. Along with CPDT, instead of thiophene as conjugated bridge, WS-39 and WS-43 exhibit an extended spectral response due to the excellent conjugation and coplanarity of CPDT. Specifically, we focused on the critical effect of length of the alkyl group linked to the bridging carbon atoms of CPDT on the photovoltaic performances. Octyl-substituted WS-39 shows a broader IPCE onset with an enhanced photovoltage relative to the analogue WS-5. In contrast, WS-43, with methyl substituted on the CPDT moiety, presents a relatively low quantum conversion efficiency within the whole spectral response region, along with low photocurrent density. WS-43 displays a distinctly low IPCE platform, predominately arising from the short electron diffusion length with significant electron loss during the electron transport. The relative movement of the conduction band edge (E(CB)) and charge transfer resistance as well as lifetime of injected electrons are studied in detail. Under standard AM 1.5 conditions, WS-39-based solar cells show a promising photovoltaic efficiency of 9.07% (J(SC) = 16.61 mA cm(-2), V(OC) = 770 mV, FF = 0.71). The octyl chains attached on CPDT can provide dual protection and exhibit a high propensity to prevent binding of the iodide-triiodide redox couple, producing an efficient shielding effect to retard the charge recombination and resulting in improvement of V(OC). Our research paves the way to explore more efficient sensitizers through ingenious molecular engineering.

Controlling the sensitizer morphology on a nanocrystalline TiO2 surface is beneficial to facilitating electron injection and suppressing charge recombination. Given that the grafted alkyl chain on a π-bridge thiophene segment for preventing π aggregation can deteriorate its intrinsic photostability, we incorporate a promising building block of 2,3-diphenylquinoxaline as the additional acceptor to construct a novel D-A-π-A-featured dye IQ4, which exhibits several characteristics: (i) efficiently decreasing the molecular HOMO-LUMO energy gap by extending its absorption bands; (ii) showing a moderate electron-withdrawing capability for an ideal balance in both promising photocurrent and photovoltage; (iii) endowing an ideal morphology control with strong capability of restraining the intermolecular aggregation and facilitating the formation of a compact sensitizer layer via two twisted phenyl groups grafted onto the quinoxaline unit. The coadsorbent-free dye-sensitized solar cell (DSSC) based on dye IQ4 exhibits very promising conversion efficiency as high as 9.24 ± 0.05%, with a short-circuit current density (Jsc) of 17.55 mA cm(-2), an open-circuit voltage (Voc) of 0.74 V, and a fill factor (FF) of 0.71 under AM 1.5 illumination (100 mW cm(-2)). IQ4-based DSSC devices with an ionic liquid electrolyte can keep constant performance during a 1000 h aging test under 1 sun at 60 °C. Because of spatial restriction, the two phenyl groups grafted onto the additional electron-withdrawing quinoxaline are demonstrated as efficient building blocks, not only improving its photostability and thermal stability but also allowing it to be a successful antiaggregation functional unit. As a consequence, the incorporated 2,3-diphenylquinoxaline unit can realize a facile structural modification for constructing organic coadsorbent-free D-A-π-A-featured sensitizers, thus paving a way to replace the common, stability-deleterious grafted alkyl chain on the thienyl bridge.

Two organic D-A-π-A sensitizers LS-2 and WS-5 containing N-octyl substituted phthalimide and benzotriazole as auxiliary electron withdrawing units with similar dimension and structure architecture were systematically studied, focusing on photophysical and electrochemical as well as photovoltaic properties in nanocrystalline TiO(2)-based dye-sensitized solar cells (DSSCs). Interestingly, with similar five-member benzo-heterocycles, the two auxiliary acceptors of phthalimide and benzotriazole play exactly different roles in absorption and intramolecular charge transfer: (i) in contrast with WS-5 delocalized throughout the entire chromophore, the HOMO orbital of LS-2 is mainly located at the donor part due to the twist conformation with the existence of two carbonyl groups in phthalimide; (ii) the dihedral angles of "D-A" plane and "A-π" plane in LS-2 further suggest that the incorporation of phthalimide moiety results in curvature of electron delocalization over the whole molecule, in agreement with its blue-shifted, relatively narrow absorption spectra and low photocurrent density; (iii) in contrast with the beneficial charge transfer of benzotriazole in WS-5, the phthalimide unit in LS-2 plays an oppositely negative contribution to the charge transfer, that is, blocking intramolecular electron transfer (ICT) from donor to acceptor to some extent; and (iv) in electrochemical impedance spectroscopy, the incorporated benzotriazole unit enhances electron lifetime by 18.6-fold, the phthalimide only increases electron lifetime by 5.0-fold. Without coadsorption of chenodeoxylic acid (CDCA), the DSSCs based on WS-5 exhibited a promising maximum conversion efficiency (η) of 8.38% with significant enhancement in all photovoltaic parameters (J(SC) = 15.79 mA cm(-2), V(OC) = 791 mV, ff = 0.67). In contrast, with the very similar D-A-π-A feature changing the additional acceptor from benzotriazole to phthalimide unit, the photovoltaic efficiency based on LS-2 was only 5.11%, decreased by 39%, with less efficient photovoltaic parameters (J(SC) = 10.06 mA cm(-2), V(OC) = 748 mV, ff = 0.68). Therefore, our results demonstrate that it is essential to choose proper subsidiary withdrawing unit in D-A-π-A sensitizer configuration for DSSCs.