Rational design of defected carbons adjacent to nitrogen(N)dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon.Meanwhile,the combined effect of heteroatom doping and defect engineering can efficiently increase the oxygen reduction reaction(ORR)ability of inactive carbons through charge redistribution.Herein,we report that an enhanced built-in electric field caused by the combined effect of N-doping and carbon defects in the two-dimensional(2D)mesoporous N-doped carbon nanoflakes(NCNF)is a promising technique for improving ORR performance.As a result,the NCNF exhibits more promising ORR activity than Pt/C and similar per-formance with reported robust catalysts.Comprehensive experimental and theoretical investigations suggest that topologically defected carbon adjacent to the graphitic valley nitrogen is a real active site,rendering optimal energy for the adsorption of ORR intermediates and lowering the total energy barrier for ORR.Also,NCNF-based Zn-air batteries exhibited an excellent power density and specific capacity of~121.10 mW cm-2 and~679.86 mA h gZn-1,respectively.This study not only offers new insights into defected carbons with graphitic valley N for ORR but also proposes novel catalyst design principles and provides a solid grasp of the built-in electric field effect on the ORR performance of defective catalysts.
Photovoltaic technology is a prominent source of renewable energy, but maintenance costs and efficiency attenuation of large photovoltaic devices are significant issues due to their vast energy conversion area. To reduce costs and facilitate maintenance, superhydrophobic surfaces with self‐cleaning properties have been developed for photovoltaic glass. In this study, transparent ZnO nanoarrays (NAs) are synthesized on photovoltaic glass, with Eu 3+ doping enhancing the ultraviolet radiation resistance of photovoltaic devices and slightly increasing visible transmittance. A TiO 2 passivation layer is introduced on the ZnO NAs surface to enhance acid resistance and mitigate corrosion caused by acidic rainwater. Fluoroalkylsilane (POTS) modification achieves superhydrophobicity with a water contact angle of 160.25°, as demonstrated by droplet rolling experiments. Micro‐interaction of superhydrophobic properties is further investigated by force curve measurement using atomic force microscope, showing almost no nanometer water moisture on the superhydrophobic surface, but conspicuous water moisture on the control glass surface. Finally, simulated models and practical silicon crystal solar cells fabricated using the self‐cleaning glass show excellent acid rain resistance, self‐cleaning, and long service life properties, with no power conversion efficiency degeneration during a 40‐day outdoor application test.
Lithium-free anode dual-ion batteries have attracted extensive studies due to their simple configuration, reduced cost, high safety and enhanced energy density. For the first time, a novel Li-free DIB based on a carbon paper anode (Li-free CGDIB) is reported in this paper. Carbon paper anodes usually have limited application in DIBs due to their poor electrochemical performance. Herein, by using a lithium bis(fluorosulfonyl)imide (LiFSI)-containing electrolyte, the battery shows outstanding electrochemical performance with a capacity retention of 96% after 300 cycles at 2C with a stable 98% coulombic efficiency and 89% capacity retention after 500 cycles at 5C with a stable coulombic efficiency of 98.5%. Moreover, the electrochemical properties of the CGDIB were investigated with a variety of in situ characterization techniques, such as in situ EIS, XRD and online differential electrochemical mass spectrometry (OEMS). The multifunctional effect of the LiFSI additive on the electrochemical properties of the Li-free CGDIB was also systematically analyzed, including generating a LiF-rich interfacial film, prohibiting Li dendrite growth effectively and forming a defective structure of graphite layers. This design strategy and fundamental analysis show great potential and lay a theoretical foundation for facilitating the further development of DIBs with high energy density.
An organic–inorganic hybrid electrolyte based on a cyclic Ti-oxo cluster as the inorganic core and naphthalene-based organic ammonium bromide salts as the electrolyte was developed with easy synthesis and low cost. The new hybrid electrolyte exhibits excellent solubility in methanol, aligned work function, good conductivity, and amorphous state in thin film, enabling its successful application as a cathode interlayer in organic solar cells with a high power conversion efficiency of 17.19 %. This work demonstrates that the hybrid electrolytes are a new kind of semiconductor, exhibiting promising applications in organic electronics.
Perovskite solar cells (PSCs) have attracted great interest in recent decade, however, stability issue and large‐scale application still remain as roadblocks to their practical applications. To settle aforementioned issues, metal diffusion and ion migration should be controlled to improve long‐term operational stability. Herein, cubic zinc metatitanate (ZTO) is optimized and improved by segregating with surface sulfidation. The sulfurized electron transporting layer, label as ZTO‐ZnS, based PSCs achieved an amazing power conversion efficiency (PCE) of 21.3%. A large‐area module (8.0 cm2 active area) based on ZTO‐ZnS is also developed with 15.9% PCE. Furthermore, combining with inorganic CuI hole transporting layer and carbon counter electrode, metal diffusion, and ion migration effect are eliminated drastically in ZTO‐ZnS‐based PSCs. The combined PSC devices can easily keep more than 85% initial PCE after 1 000 h at 85 °C in air with a relative humidity of 85% under maximum power point and continuous AM 1.5G illumination. The persistence in stability is investigated and revealed fully by energy dispersive spectrometer analysis, attributing to the PSC structure which blocks the metal diffusion and ion migration in the devices. A big step forward industrialization and commercialization for PSCs is made.
Perovskite solar cells (PSCs) have experienced considerable development in the past few years. The stability issue has become a focus of research efforts toward their commercial applications. The development and interface engineering of electron transport materials (ETMs) to build up stable interfaces with perovskites has been emerging as a powerful strategy to enhance PSCs' stability. Herein, cubic zinc metatitanate (ZTO) is identified as an excellent ETM with interface engineering treatment of dezincification for fabricating PSCs with much better overall performances than those fabricated from TiO 2 , a popularly used ETM. The high electron mobility of ZTO helps minimize the hysteresis. Together with the use of CuSCN as inorganic hole transport material and further protecting the PSCs with reduced graphene oxide, the ZTO‐based PSCs exhibit remarkable enhancement in stability, retaining 95% of initial power conversion efficiency under AM 1.5 G illumination at 85 °C and 85% relative humidity in air for 1000 h at open circuit.
We report a dendrite-free Li metal anode obtained by the synergistic effect of AgPF6–LiNO3 hybrid additives in the electrolyte. The constructed symmetric cell battery shows excellent cycling lifetime for >3000 h with only slight polarization.
Perovskite films prepared with CH3NH2 molecules under ambient conditions have led to rapid fabrication of perovskite solar cells (PSCs), but there remains a lack of mechanistic studies and inconsistencies with operability in their production. Here the crystal structure of CH3NH2-CH3NH3PbI3 was analyzed to involve hydrogen bonds (CH3NH2 center dot center dot center dot CH3NH3+) and has guided the facile, reproducible preparation of high-quality perovskite films under ambient conditions. Hydrogen bonds within CH3NH2 center dot center dot center dot CH3NH3+ dimers were found in the CH3NH2-CH3NH3PbI3 intermediates, accompanied by 1D-PbI3- chains (delta-phase). The weakly hydrogen-bonded CH3NH2 molecules were easily released from the CH3NH2-CH3NH3PbI3 intermediates, contributing to rapid, spontaneous phase transition from 1D-PbI3- (delta-phase) to 3D-PbI3- (alpha-phase). Further introduction of CH3NH3Cl into the CH3NH2-CH3NH3PbI3 intermediates led to interruption of 1D-PbI3- transition into 0D-Pb2I9-xClx5-(0 < x < 6), adjusting the phase transition route toward 3D-PbI3-. On the basis of the above understanding, CH3NH2 solution in ethanol and CH3NH3Cl were used for precursors and a best efficiency of 20.3% in PSCs was achieved. Large-scale modules (12 cm(2) aperture area) fabricated by a dip-coating technology exhibited an efficiency up to 16.0% and outstanding stability over 10 000 s under continuous output. The developed preparation method of perovskite precursors and insightful research into the methylamine-dimer-induced phase transition mechanism have enabled the production of high-quality perovskite films with robust operability, showing great potential for large-scale commercialization.
Dual-ion battery complements lithium-ion batteries in terms of the use of inexpensive materials and ease to construct cells. To improve the safety and energy density of dual-ion battery, in this paper, a novel MnO-graphite dual-ion battery is reported for the first time. Microporous MnO materials are used as anode, which exhibits a low conversion potential and a low voltage hysteresis. The MnO-graphite dual-ion battery can deliver a capacity of 104 mAh g-1 at 0.5C and exhibits good rate performances and cycling stability (capacity retention >93% after 300 cycles). A mechanism is proposed to explain the irreversibility in capacity during the initial cycle by using operando X-ray diffraction in combination with online electrochemical mass spectrometry and electrochemical impedance spectroscopy.
Lithium (Li) metal is a favorable anode for most energy storage equipment, thanks to its higher theoretical specific capacity. However, nonuniform Li nucleation/growth results in large-sized and irregular dendrites generated from the Li anode, which causes rapid capacity fade and serious safety hazard, hindering its widespread practical applications. In this paper, with the aid of a lithium nitrate (LiNO3) additive in a carbonate-based electrolyte, the Li anode shows low hysteresis for in excess of 1000 h at a current density of 0.5 mA cm-2. At the same time, a Li-graphite dual-ion battery exhibits an outstanding cycling stability at 5C; after 1000 cycles, 81% of the capacity is retained. After calculation, the Li-graphite dual-ion battery shows a competitive specific energy density of 243 Wh kg-1 at a power density of 234 W kg-1. Moreover, the linear sweep voltammetry test was first performed to analyze the Li nucleation/growth mechanism and explain the effect of the LiNO3 additive. The superior electrochemical properties of the Li-graphite dual-ion battery are ascribed to the formation of smooth Li composed of Li nanoparticles and a steady solid electrolyte interface film.
Perovskite solar cells (PSCs) have reached certified efficiencies of up to 23.7% but suffered from frailness and instability when exposed to ambient atmosphere. Zinc oxide (ZnO), when used as electron transport layer (ETL) on PSCs, gives rise to excellent electronic, optic, and photonic properties, yet the Lewis basic nature of ZnO surface leads to deprotonation of the perovskite layer, resulting in serious degradation of PSCs using ZnO as ETL. Here, we report a simple but effective strategy to convert ZnO surface into ZnS at the ZnO/perovskite interface by sulfidation. The sulfide on ZnO-ZnS surface binds strongly with Pb2+ and creates a novel pathway of electron transport to accelerate electron transfer and reduce interfacial charge recombination, yielding a champion efficiency of 20.7% with improved stability and no appreciable hysteresis. The model devices modified with sulfide maintained 88% of their initial performance for 1000 h under storage condition and 87% for 500 h under UV radiation. ZnS is demonstrated to act as both a cascade ETL and a passivating layer for enhancing the performance of PSCs.