Asymmetric Coordination of Bimetallic Fe-Co Single-Atom Pairs toward Enhanced Bifunctional Activity for Rechargeable Zinc-Air Batteries.

The advancement of rechargeable zinc-air batteries (RZABs) faces challenges from the pronounced polarization and sluggish kinetics of oxygen reduction and evolution reactions (ORR and OER). Single-atom catalysts offer an effective solution, yet their insufficient or singular catalytic activity hinders their development. In this work, a dual single-atom catalyst, FeCo-SAs, was fabricated, featuring atomically dispersed N3-Fe-Co-N4 sites on N-doped graphene nanosheets for bifunctional activity. Introducing Co into Fe single-atoms and secondary pyrolysis altered Fe coordination with N, creating an asymmetric environment that promoted charge transfer and increased the density of states near the Fermi level. This catalyst achieved a narrow potential gap of 0.616 V, with a half-wave potential of 0.884 V for ORR (vs the reversible hydrogen electrode) and a low OER overpotential of 270 mV at 10 mA cm-2. Owing to the superior activity of FeCo-SAs, RZABs exhibited a peak power density of 203.36 mW cm-2 and an extended cycle life of over 550 h, exceeding the commercial Pt/C + IrO2 catalyst. Furthermore, flexible RZABs with FeCo-SAs demonstrated the promising future of bimetallic pairs in wearable energy storage devices.

Aqueous synthesis of perovskite precursors for highly efficient perovskite solar cells.

High-purity precursor materials are vital for high-efficiency perovskite solar cells (PSCs) to reduce defect density caused by impurities in perovskite. In this study, we present aqueous synthesized perovskite microcrystals as precursor materials for PSCs. Our approach enables kilogram-scale mass production and synthesizes formamidinium lead iodide (FAPbI3) microcrystals with up to 99.996% purity, with an average value of 99.994 ± 0.0015%, from inexpensive, low-purity raw materials. The reduction in calcium ions, which made up the largest impurity in the aqueous solution, led to the greatest reduction in carrier trap states, and its deliberate introduction was shown to decrease device performance. With these purified precursors, we achieved a power conversion efficiency (PCE) of 25.6% (25.3% certified) in inverted PSCs and retained 94% of the initial PCE after 1000 hours of continuous simulated solar illumination at 50°C.

A multi-layer reduced graphene oxide catalyst encapsulating a high-entropy alloy for rechargeable zinc-air batteries.

A reduced graphene oxide encapsulating Fe6Ni20Co2Mn2Cu1.5@rGO catalyst is prepared using a Joule heating strategy. The graphene-coated layer with high crystallinity enhances the stability of the crystal structure, resulting in superior OER activity. Rechargeable zinc-air batteries with Fe6Ni20Co2Mn2Cu1.5@rGO demonstrate remarkable performance, boasting a high specific capacity of 800 mA h gZn-1, an impressive peak power density of 154.612 mW cm-2, and a cycle life of 300 hours at a current density of 10 mA cm-2.

Functional-Group-Induced Single Quantum Well Dion-Jacobson 2D Perovskite for Efficient and Stable Inverted Perovskite Solar Cells.

In two-dimensional/three-dimensional (2D/3D) perovskite heterostructure, randomly distributed multiple quantum wells (QW) 2D perovskites are frequently generated, which are detrimental to carrier transport and structural stability. Here, the high quality 2D/3D perovskite heterostructure is constructed by fabricating functional-group-induced single QW Dion-Jacobson (DJ) 2D perovskites. The utilization of ─OCH3 in the precursor solution facilitates the formation of colloidal particles with uniform size, resulting in the production of a pure 2D DJ perovskite with an n value of 3. This strategy facilitates the improvement of 3D structural stability and expedites carrier transport. The resultant devices accomplish a power conversion efficiency of 25.26% (certified 25.04%) and 23.56% at a larger area (1 cm2 ) with negligible hysteresis. The devices maintain >96% and >89% of their initial efficiency after continuous maximum power point tracking under simulated AM1.5 illumination for 1300 h and under damp-heat conditions (85 °C and 85% RH) for 1010 h, respectively.

Quenching Detrimental Reactions and Boosting Hole Extraction via Multifunctional NiOx /Perovskite Interface Passivation for Efficient and Stable Inverted Solar Cells.

Nickel oxide (NiOx ) is one of the most promising hole transport materials for inverted perovskite solar cells (PSCs). However, its application is severely restrained due to unfavorable interfacial reactions and insufficient charge carrier extraction. Herein, a multifunctional modification at the NiOx /perovskite interface is developed via introducing fluorinated ammonium salt ligand to synthetically solve the obstacles. Specifically, the interface modification can chemically convert detrimental Ni≥3+ to lower oxidation state, resulting in the elimination of interfacial redox reactions. Meanwhile, interfacial dipole is incorporated simultaneously to tune the work function of NiOx and optimize energy level alignment, which effectively promotes the charge carrier extraction. Therefore, the modified NiOx -based inverted PSCs achieve a remarkable power conversion efficiency (PCE) of 22.93%. Moreover, the unencapsulated devices obtain a significantly enhanced long-term stability, maintaining over 85% and 80% of the initial PCEs after storage in ambient air with a high relative humidity of 50-60% for 1000 h and continuous operation at maximum power point under one-sun illumination for 700 h, respectively.

Homogenizing out-of-plane cation composition in perovskite solar cells.

Perovskite solar cells with the formula FA1-xCsxPbI3, where FA is formamidinium, provide an attractive option for integrating high efficiency, durable stability and compatibility with scaled-up fabrication. Despite the incorporation of Cs cations, which could potentially enable a perfect perovskite lattice1,2, the compositional inhomogeneity caused by A-site cation segregation is likely to be detrimental to the photovoltaic performance of the solar cells3,4. Here we visualized the out-of-plane compositional inhomogeneity along the vertical direction across perovskite films and identified the underlying reasons for the inhomogeneity and its potential impact for devices. We devised a strategy using 1-(phenylsulfonyl)pyrrole to homogenize the distribution of cation composition in perovskite films. The resultant p-i-n devices yielded a certified steady-state photon-to-electron conversion efficiency of 25.2% and durable stability.

Depression screening using hybrid neural network.

Depression is a common cause of increased suicides worldwide, and studies have shown that the number of patients suffering from major depressive disorder (MDD) increased several-fold during the COVID-19 pandemic, highlighting the importance of disease detection and depression management, while increasing the need for effective diagnostic tools. In recent years, machine learning and deep learning methods based on electroencephalography (EEG) have achieved significant results in the field of automatic depression detection. However, most current studies have focused on a small number of EEG signal channels, and experimental data require special processing by professionals. In this study, 128 channels of EEG signals were simply filtered and 24-fold leave-one-out cross-validation experiments were performed using 2DCNN-LSTM classifier, support vector machine, K-nearest neighbor and decision tree. The current results show that the proposed 2DCNN-LSTM model has an average classification accuracy of 95.1% with an AUC of 0.98 for depression detection of 6-second participant EEG signals, and the model is much better than 72.05%, 79.7% and 79.49% for support vector machine, K nearest neighbor and decision tree. In addition, we found that the model achieved a 100% probability of correctly classifying the EEG signals of 300-second participants.

Rechargeable Zinc-Air Batteries with an Ultralarge Discharge Capacity per Cycle and an Ultralong Cycle Life.

A conventional two-electrode rechargeable zinc-air battery (RZAB) has two major problems: 1) opposing requirements for the oxygen reduction (ORR) and oxygen evolution (OER) reactions from the catalyst at the air cathode; and 2) zinc-dendrite formation, hydrogen generation, and zinc corrosion at the zinc anode. To tackle these problems, a three-electrode RZAB (T-RZAB) including a hydrophobic discharge cathode, a hydrophilic charge cathode, and a zinc-free anode is developed. The decoupled cathodes enable fast ORR and OER kinetics, and avoid oxidization of the ORR catalyst. The zinc-free anode using tin-coated copper foam that induces the growth of (002)Zn planes, suppresses hydrogen evolution, and prevents Zn corrosion. As a result, the T-RZABs have a high discharge capacity per cycle of 800 mAh cm-2 , a low voltage gap between the discharge/charge platforms of 0.66 V, and an ultralong cycle life of 5220 h at a current density of 10 mA cm-2 . A large T-RZAB with a discharge capacity of 10 Ah per cycle with no obvious degradation after cycling for 1000 h is developed. Finally, a T-RZAB pack that has an energy density of 151.8 Wh kg-1 and a low cost of 46.7 US dollars kWh-1  is assembled.

Efficient and stable organic solar cells enabled by multicomponent photoactive layer based on one-pot polymerization.

Degradation of the kinetically trapped bulk heterojunction film morphology in organic solar cells (OSCs) remains a grand challenge for their practical application. Herein, we demonstrate highly thermally stable OSCs using multicomponent photoactive layer synthesized via a facile one-pot polymerization, which show the advantages of low synthetic cost and simplified device fabrication. The OSCs based on multicomponent photoactive layer deliver a high power conversion efficiency of 11.8% and exhibit excellent device stability for over 1000 h (>80% of their initial efficiency retention), realizing a balance between device efficiency and operational lifetime for OSCs. In-depth opto-electrical and morphological properties characterizations revealed that the dominant PM6-b-L15 block polymers with backbone entanglement and the small fraction of PM6 and L15 polymers synergistically contribute to the frozen fine-tuned film morphology and maintain well-balanced charge transport under long-time operation. These findings pave the way towards the development of low-cost and long-term stable OSCs.

Dual Optimization of Bulk and Interface via the Synergistic Effect of Ligand Anchoring and Hole Transport Dopant Enables 23.28% Efficiency Inverted Perovskite Solar Cells.

The crystalline morphology of perovskite film plays a key role in determining the stability and performance of perovskite solar cells (PSCs). In addition, the work function and conductivity of hole transport layer (HTL) have a great influence on the effciency of PSCs. Here, we develop a synergistic doping strategy to fabricate high-performance inverted PSCs, doping a functional nanographene (C78-AHM) into the poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine (PTAA) HTL, thus forming an HTL with higher conductivity, lower roughness, and frontier energy levels matching the perovskite absorber work function. On this basis, thiosemicarbazide (TSC) was doped into the precursor solution of perovskite as the grain and interface modifier to further improve the crystalline morphology of perovskite film. Compared with the current single passivation method, this codoping strategy can simultaneously reduce the surface and bulk defects of perovskite film and reduce the interface energy barrier. Eventually, high-quality TSC-doped perovskite films based on C78-AHM-doped PTAA HTL are obtained with over 2 µm sized grains, pinhole-free, and improved crystallinity. As a result, this synergistic doping strategy increases the efficiency of the device from 20.27% to 23.28%. Furthermore, the environmental and thermal stabilities of the devices are significantly improved. Therefore, this work provides a simple way for the preparation of other efficient optoelectronic devices.

Tuning Perovskite Surface Polarity via Dipole Moment Engineering for Efficient Hole-Transport-Layer-Free Sn-Pb Mixed-Perovskite Solar Cells.

Post-treatment has been recognized as one of the effective methods for passivating the underlying defects in perovskite solar cells (PSCs), but little attention has been paid to how to pick suitable passivation agents with diverse isomers for efficient PSCs, particularly for the tin-lead (Sn-Pb) mixed PSCs. Here, we introduce the dependence of the power conversion efficiency (PCE) on a dipole moment for surface passivator screening, in which we chose three trifluoromethyl-phenylethylamine hydroiodide (CF3-PEAI) isomers as surface-treatment materials for hole-transport-layer-free (HTL-free) Sn-Pb mixed PSCs. The different positions of the -CF3 group for the CF3-PEAI isomer result in different dipole moments, which influences the interaction between CF3-PEAI and lead iodide. The para position CF3 with the highest dipole moment exhibits a higher PCE than the ortho-position with a lower dipole moment, which is attributed to the large dipole moment on the surface that could tune the surface polarity from p-type to n-type, facilitating electron charge transport in the HTL-free Sn-Pb mixed PSCs. An ultrathin 2D layer is formed on the perovskite surface to passivate the surface defects, which is responsible for the enhancement of the PCE and stability of the PSCs. As a result, the open-circuit voltage (VOC) of the device is improved from 0.775 to 0.824 V, yielding a champion PCE of 20.17%, which is one of the highest PCEs among the reported HTL-free Sn-Pb mixed PSCs. The device also shows improved stability with remaining 75% of its initial PCEs after storage in N2 for 700 h.

Flexible Zinc-Air Batteries with Ampere-Hour Capacities and Wide-Temperature Adaptabilities.

Flexible Zn-air batteries (FZABs) have significant potentials as efficient energy storage devices for wearable electronics because of their safeties and high energy-to-cost ratios. However, their application is limited by their short cycle lives, low discharge capacities per cycle, and high charge/discharge polarizations. Accordingly, herein, a poly(sodium acrylate)-polyvinyl alcohol (PANa-PVA)-ionic liquid (IL) hydrogel (PANa-PVA-IL) is prepared using a hygroscopic IL, 1-ethyl-3-methylimidazolium chloride, as an additive for twin-chain PANa-PVA. PANa-PVA-IL exhibits a high conductivity of 306.9 mS cm-1 and a water uptake of 2515 wt% at room temperature. Moreover, a low-cost bifunctional catalyst, namely, Co9 S8 nanoparticles anchored on N- and S-co-doped activated carbon black pearls 2000 (Co9 S8 -NSABP), is synthesized, which demonstrates a low O2 reversibility potential gap of 0.629 V. FZABs based on PANa-PVA-IL and Co9 S8 -NSABP demonstrate high discharge capacities of 1.67 mAh cm-2 per cycle and long cycle lives of 330 h. Large-scale flexible rechargeable Zn-air pouch cells exhibit total capacities of 1.03 Ah and energy densities of 246 Wh kgcell -1 . This study provides new information about hydrogels with high ionic conductivities and water uptakes and should facilitate the application of FZABs in wearable electronics.

Deciphering the Morphology Change and Performance Enhancement for Perovskite Solar Cells Induced by Surface Modification.

Organic-inorganic perovskite solar cells (PSCs) have achieved great attention due to their expressive power conversion efficiency (PCE) up to 25.7%. To improve the photovoltaic performance of PSCs, interface engineering between the perovskite and hole transport layer (HTL) is a widely used strategy. Following this concept, benzyl trimethyl ammonium chlorides (BTACls) are used to modify the wet chemical processed perovskite film in this work. The BTACl-induced low dimensional perovskite is found to have a bilayer structure, which efficiently decreases the trap density and improves the energy level alignment at the perovskite/HTL interface. As a result, the BTACl-modified PSCs show an improved PCE compared to the control devices. From device modeling, the reduced charge carrier recombination and promoted charge carrier transfer at the perovskite/HTL interface are the cause of the open-circuit (Voc ) and fill factor (FF) improvement, respectively. This study gives a deep understanding for surface modification of perovskite films from a perspective of the morphology and the function of enhancing photovoltaic performance.

Dually Modified Wide-Bandgap Perovskites by Phenylethylammonium Acetate toward Highly Efficient Solar Cells with Low Photovoltage Loss.

Wide-bandgap perovskites as a class of promising top-cell materials have shown great promise in constructing efficient perovskite-based tandem solar cells, but their intrinsic relatively low radiative efficiency results in a large open-circuit voltage (VOC) deficit and thereby limits the whole device performance. Reducing film flaws or optimizing interfacial energy level alignments in wide-bandgap perovskite devices can efficiently inhibit nonradiative recombination to boost device VOC and efficiency. However, the simultaneous regulation on both sides and their underlying mechanism are less explored. Herein, a bifunctional modification approach is proposed to optimize the wide-bandgap perovskite surface with an ultrathin layer of phenylethylammonium acetate (PEAAc) to synchronously decrease the surface imperfection and mitigate the interfacial energy barrier. This treatment effectively heals under-coordinated surface defects through the formation of chemical interaction between the perovskite and PEAAc, bringing about a much slower charge trapping process and dramatically decreasing nonradiative recombination losses. Meanwhile, the passivation-induced upshifted Fermi level of the perovskite contributes to accelerated electron extraction and larger Fermi-level splitting under illumination. Consequently, the PEAAc-modified wide-bandgap (1.68 eV) device achieves an optimal efficiency of 20.66% with a high VOC of 1.25 V, among the highest reported VOC values for wide-bandgap perovskite devices, enormously outperforming that (18.86% and 1.18 V) of the device without passivation. In addition, the radiative limit of VOC for both cells is determined to be 1.42 V, delivering nonradiative recombination losses of 0.24 and 0.17 V for the control and PEAAc-modified devices, respectively. These results highlight the significance of the bifunctional modification strategy in achieving high-performance wide-bandgap perovskite devices.

Thermal-Radiation-Driven Ultrafast Crystallization of Perovskite Films Under Heavy Humidity for Efficient Inverted Solar Cells.

Fabricating perovskite solar cells (PSCs) in air is conducive to low-cost commercial production; nevertheless, it is rather difficult to achieve comparable device performance as that in an inert atmosphere because of the poor moisture toleration of perovskite materials. Here, the perovskite crystallization process is systematically studied using two-step sequential solution deposition in an inert atmosphere (glovebox) and air. It is found that moisture can stabilize solvation intermediates and prevent their conversion into perovskite crystals. To address this issue, thermal radiation is used to accelerate perovskite crystallization for integrated perovskite films within 10 s in air. The as-formed perovskite films are compact, highly oriented with giant grain size, superior photoelectric properties, and low trap density. When the films are applied to PSC devices, a champion power conversion efficiency (PCE) of 20.8% is obtained, one of the best results for air-processed inverted PSCs under high relative humidity (60 ± 10%). This work substantially assists understanding and modulation to perovskite crystallization kinetics under heavy humidity. Also, the ultrafast conversion strategy by thermal radiation provides unprecedented opportunities to manufacture high-quality perovskite films for low-temperature, eco-friendly, and air-processed efficient inverted PSCs.

Carbon Nitride with Rationally Designed π-Conjugated Structure for Bright Blue-Violet Light-Emitting Diodes.

Carbon nitride consisting of the broken π-conjugated structure (bc-CN) is designed as the emitting layer in a blue-violet light emitting diode (LED). The bc-CN is prepared by a metal-oxide (MgO) template-assisted method, in which the low reaction temperature and nano MgO jointly control the degree of polymerization to form cyano groups and broken π-conjugation in the bc-CN nanosheets (bc-CN NS) which emit intense blue-violet photoluminescence at 412 nm. The broken π-conjugated heptazine-ring structure in the bc-CN NS mitigates non-radiation energy loss and promotes the d*-LP transition. As a result, a high quantum efficiency of 73.1% is achieved. The excellent dispersing ability of the bc-CN NS enables solution-based fabrication of the light emitting diode (LED). The LED exhibits intense electroluminescence of 236 cd m-2 at 412 nm with an external quantum efficiency of 0.46%. The broken π-conjugation modulates the optical properties of the polymerized carbon nitride semiconductor giving rise to intense blue-violet electroluminescence, which is very desirable for printable and wide-color-gamut display devices.

Integrated Ideal-Bandgap Perovskite/Bulk-Heterojunction Solar Cells with Efficiencies > 24.

Here, the authors report a highly efficient integrated ideal-bandgap perovskite/bulk-heterojunction solar cell (IPBSC) with an inverted architecture, featuring a near infrared (NIR) polymer DTBTI-based bulk-heterojunction (BHJ) layer atop guanidinium bromide (GABr)-modified FA0.7 MA0.3 Pb0.7 Sn0.3 I3 perovskite film as the photoactive layer. The IPBSC shows cascade-like energy level alignment between the charge-extractionlayer/perovskite/BHJ and efficient passivation effect of BHJ on perovskite. Thanks to the well-matched energy level alignment and high-quality ideal bandgap-based perovskite film, an efficient charge transfer occurs between the charge-extraction-layer/perovskite/BHJ. Moreover, the NIR polymer DTBTI on the perovskite film leads to an improved NIR light response for the IPBSC. In addition, the O, S and N atoms in the DTBTI polymer yield a strong interaction with perovskite, which is conducive to reducing the defects of the perovskite and suppressing charge recombination. As a result, the solar cell achieves a power conversion efficiency (PCE) of 24.27% (certificated value at 23.4% with 0.283-volt voltage loss), currently the recorded efficiency for both IPBSCs and Pb-Sn alloyed PSCs, and which is over the highest efficiency of perovskite-organic tandem solar cell. Moreover, the thermal, humidity and long-term operational stabilities of the IPBSCs are also significantly improved compared with the control PSCs.

In situ fabrication of dry/gel bilayer Ti3C2Tx films for high-rate micro-supercapacitors.

A H2SO4-Ti3C2Tx ion-gel is in situ fabricated to prevent the restacking of Ti3C2Tx for high-rate micro-supercapacitors. The ion-gel pillared by an electrolyte possesses an enlarged interlayer spacing facilitating ion transport. Furthermore, a bilayer structure is designed with dry Ti3C2Tx for fast electron conduction. The bilayer Ti3C2Tx film shows improved capacitance from 49% to 73% of the initial capacitance at a high scan rate of 200 mV s-1, along with excellent cycle stability. This study opens up a concise and efficient way for high-performance micro-supercapacitors.

Simultaneous Tuning of Alkyl Chains and End Groups in Non-fused Ring Electron Acceptors for Efficient and Stable Organic Solar Cells.

Fine-tuning the alkyl chains and end groups of non-fused ring electron acceptors (NFREAs) plays vital roles in the promotion of charge transfer (CT) and power conversion efficiency (PCE). In this work, we developed a series of A-D-A'-D-A-type NFREAs, which possess the same terminals (A), the cyclopentadithiophene unit (D), and the thieno[3,4-c]pyrrole-4,6-dione (A'). Despite the subtle difference in side chains and halogenated end groups, the six acceptors exhibit a considerable difference in the efficiency and device stability of the organic solar cells (OSCs). Among the molecules, chlorinated NFREAs show a broader light absorption than the fluorinated ones do. Compared with C8C8-4F (1-octylnonyl and fluorination) and C6C4-4Cl (2-butyloctyl and chlorination), C8C8-4Cl (1-octylnonyl and chlorination) exhibits a lower highest occupied molecular orbital level, higher electron mobility, and denser molecular packing. The OSCs based on PM6:C8C8-4Cl yield the best PCE of 14.11%, which is attributed to the faster charge transport, high miscibility, and preferable morphology. Moreover, the PM6:C8C8-4Cl devices retain 91.1% of the initial PCE after being placed in air with 67% relative humidity for 50 days. This work shows that the simultaneous optimization of side chains and end groups facilitates the CT and improves the stability in the OSCs, offering a novel view into the molecular design of A-D-A'-D-A-type NFREAs.