Impermeable inorganic “walls” sandwiching perovskite layer toward inverted and indoor photovoltaic devices

Interfaces between the perovskite active layer and the charge-transport layers (CTLs) play a critical role in both efficiency and stability of halide-perovskite photovoltaics. One of the major concerns is that surface defects of perovskite could cause detrimental nonradiative recombination and material degradation. In this work, we addressed this challenging problem by inserting ultrathin alkali-fluoride (AF) films between the tri-cation lead-iodide perovskite layer and both CTLs. This bilateral inorganic “walls” strategy makes use of both physical-blocking and chemical-anchoring functionalities of the continuous, uniform and compact AF framework: on the one hand, the uniformly distributed alkali-iodine coordination at the perovskite-AF interfaces effectively suppresses the formation of iodine-vacancy defects at the surfaces, thus reducing the trap-assisted recombination at the perovskite-CTL interfaces and therewith the open-voltage loss; on the other hand, the impermeable AF buffer layers effectively prevent the bidirectional ion migration at the perovskite-CTLs interfaces even under harsh working conditions. As a result, a power-conversion efficiency (PCE) of 22.02% (certified efficiency 20.4%) with low open-voltage deficit (<0.4 V) was achieved for the low-temperature processed inverted planar perovskite solar cells. Exceptional operational stability (500 h, ISOS-L-2) and thermal stability (1000 h, ISOS-D-2) were obtained. Meanwhile, a 35.7% PCE was obtained under dim-light source (1000 lux white LED light) with the optimized device, which is among the best records in perovskite indoor photovoltaics

High performance flexible solid-state asymmetric supercapacitors from MnO2/ZnO core shell nanorods//specially reduced graphene oxide

With a view to developing flexible solid-state asymmetric supercapacitors, we have specially designed and nanoscopically engineered two types of electrodes: a MnO2/ZnO core-shell nanorod array and a HI-reduced graphene oxide assembly, both deposited in situ on a carbon cloth. These materials were thoroughly characterized by structural and spectroscopic techniques. The flexible solid-state asymmetric supercapacitors with cathodes and anodes made of these materials have demonstrated superior performance characteristics. They can be cycled in a wide potential window of 0-1.8 V for 5000 cycles with only 1.5% capacitance loss. The demonstrated volumetric energy density of 0.234 mW h cm(-3) and volumetric power density of 0.133 W cm(-3) are much higher than those of similar devices reported previously in the literature

A Quasi-Quantum Well Sensitized Solar Cell with Accelerated Charge Separation and Collection

Semiconductor-sensitized solar cell (SSSC) represents a new generation of device aiming to achieve easy fabrication and cost-effective performance. However, the power of the semiconductor sensitizers has not been fully demonstrated in SSSC, making it actually overshadowed by dye-sensitized solar cell (DSSC). At least part of the problem is related to the inefficient charge separation and severe recombination with the current technologies, which calls on rethinking about how to better engineer the semiconductor sensitizer structure in order to enhance the power conversion efficiency (PCE). Herein we report on using for the first time a quasi-quantum well (QW) structure (ZnSe/CdSe/ZnSe) as the sensitizer, which is quasi-epitaxially deposited on ZnO tetrapods. Such a novel photoanode architecture has attained 6.20% PCE, among the highest reported to date for this type of SSSCs. Impedance spectra have revealed that the ZnSe/CdSe/ZnSe QW structure has a transport resistance only a quarter that of, but a recombination resistance twice that of the ZnSe/CdSe heterojunction (HJ) structure, yielding much longer electron diffusion length, consistent with the resulting higher photovoltage, photocurrent, and fill factor. Time resolved photoluminescence spectroscopy indicates dramatically reduced electron transfer from ZnO to the QW sensitizer, a feature which is conducive to charge separation and collection. This study together with the impedance spectra and intensity modulated photocurrent spectroscopies supports a core/shell two channel transport mechanism in this type of solar cells and further suggests that the electron transport along sensitizer can be considerably accelerated by the QW structure employed

Engineering Ternary Copper-Cobalt Sulfide Nanosheets as High-performance Electrocatalysts toward Oxygen Evolution Reaction

The rational design and development of the low-cost and effective electrocatalysts toward oxygen evolution reaction (OER) are essential in the storage and conversion of clean and renewable energy sources. Herein, a ternary copper-cobalt sulfide nanosheets electrocatalysts (denoted as CuCoS/CC) for electrochemical water oxidation has been synthesized on carbon cloth (CC) via the sulfuration of CuCo-based precursors. The obtained CuCoS/CC reveals excellent electrocatalytic performance toward OER in 1.0 M KOH. It exhibits a particularly low overpotential of 276 mV at current density of 10 mA cm&#8722;2, and a small Tafel slope (58 mV decade&#8722;1), which is superior to the current commercialized noble-metal electrocatalysts, such as IrO2. Benefiting from the synergistic effect of Cu and Co atoms and sulfidation, electrons transport and ions diffusion are significantly enhanced with the increase of active sites, thus the kinetic process of OER reaction is boosted. Our studies will serve as guidelines in the innovative design of non-noble metal electrocatalysts and their application in electrochemical water splittin

Epitaxial Growth of ZnO Nanodisks with Large Exposed Polar Facets on Nanowire Arrays for Promoting Photoelectrochemical Water Splitting

Single-crystalline and branched 1D arrays, ZnO nanowires/nanodisks (NWs/NDs) arrays, are fabricated to significantly enhance the performance of photoelectrochemical (PEC) water splitting. The epitaxial growth of the ZnO NDs with large exposed polar facets on ZnO NWs exhibits a laminated structure, which dramatically increases the light scattering capacity of the NWs arrays, especially in the wavelength region around 400 nm. The ND branching of the 1D arrays in the epitaxial fashion not only increase surface area and light utilization, but also support fast charge transport, leading to the considerable increase of photocurrent. Moreover, the tiny size NDs can facilitate charge separation and reduce charge recombination, while the large exposed polar facets of NDs reduce the external potential bias needed for water splitting. These advantages land the ZnO NWs/NDs arrays a four times higher power conversion efficiency than the ZnO NWs arrays. By sensitizing the ZnO NWs/NDs with CdS and CdSe quantum dots, the PEC performance can be further improved. This work advocates a trunk/leaf in forest concept for the single-crystalline NWs/NDs in array with enlarged exposure of polar facets, which opens the way for optimizing light harvesting and charge separation and transport, and thus the PEC water splitting

Magnetic-field-assisted aerosol pyrolysis synthesis of iron pyrite sponge-like nanochain networks as cost-efficient counter electrodes in dye-sensitized solar cells

Aerosol pyrolysis of Fe(CO)(5) in an atmosphere of sulfur vapor under a magnetic field is shown to controllably produce iron pyrite (FeS2) three-dimensional nanochain networks. The formation processes of the FeS2 nanochain networks are systematically studied: (1) thermal decomposition of Fe(CO)(5) followed by Fe nanoparticle assembly into one-dimensional chains and then three-dimensional networks under a magnetic field and (2) subsequent sulfurization in a sulfur vapor atmosphere to form a sponge-like thin film of FeS2 nanochain networks. A control experiment performed in the absence of magnetic field yielded randomly packed FeS2 nanoparticles, rather than the inter-connected nanochain networks. The nanochain networks and their surfactant-free surfaces brought about by our new synthesis will enable a host of photoelectric applications. For example, when used as the counter electrode in dye-sensitized solar cells, the FeS2 nanochain networks are almost as efficient as noble Pt, and more impressively, their catalytic activity faded by only 8% even after 2000 cycles. This work opens up fresh opportunities to make smart use of earth-abundant materials in areas of sustainable energy and environment

Building High-Efficiency CdS/CdSe-Sensitized Solar Cells with a Hierarchically Branched Double-Layer Architecture

We report a double-layer architecture for a photoanode of quantum-dot-sensitized solar cells (QDSSCs), which consists of a ZnO nanorod array (NR) underlayer and a ZnO nanotetrapod (TP) top layer. Such double-layer and branching strategies have significantly increased the power conversion efficiency (PCE) to as high as 5.24%, nearly reaching the record PCE of QDSSCs based on TiO₂. Our systematic studies have shown that the double-layer strategy could significantly reduce charge recombination at the interface between the charge collection anode (FTO) and ZnO nanostructure because of the strong and compact adhesion of the NRs and enhance charge transport due to the partially interpenetrating contact between the NR and TP layers, leading to improved open-circuit voltage (<i>V</i>_oc) and short-circuit current density (<i>J</i>_sc). Also, when the double layer was subjected to further branching, a large increase in <i>J</i>_sc and, to a lesser extent, the fill factor (FF) has resulted from increases in quantum-dot loading, enhanced light scattering, and reduced series resistance

High performance inverted structure perovskite solar cells based on a PCBM:polystyrene blend electron transport layer

Hybrid organic/inorganic perovskite solar cells are among the most competitive emerging photovoltaic technologies. Here, we report on NiO-based inverted structure perovskite solar cells with a high power conversion efficiency of 10.68%, which is achieved by adding a small percentage (1.5 wt%) of high molecular weight polystyrene (PS) into the PCBM electron transport layer (ETL). The addition of PS facilitates the formation of a highly smooth and uniform PCBM ETL that is more effective in preventing undesirable electron-hole recombination between the perovskite layer and the top electrode. As a result, the V-OC of the PCBM: PS-based cells is increased from 0.97 V to 1.07 V, which leads to significantly enhanced power conversion efficiencies of the solar cells. Our study provides a simple and low-cost approach to improving the ETL film quality and the performance of inverted perovskite solar cells

Carbon-Conjugated Co Complexes as Model Electrocatalysts for Oxygen Reduction Reaction

Single-atom catalysts are a family of heterogeneous electrocatalysts widely used in energy storage and conversion. The determination of the local structure of the active metal sites is challenging, which limits the establishment of the reliable structure-property relationship of single-atom catalysts. A carbon black-conjugated complex can be used as the model catalyst to probe the intrinsic activity of metal sites with certain local structures. In this work, we prepared carbon black-conjugated [Co(phenanthroline)Cl2], [Co(o-phenylenediamine)Cl2] and [Co(salophen)]. In these catalysts, the Co complexes with well-defined structures are anchored on the edge of carbon black by pyrazine moieties. The number of electrochemical accessible Co sites can be measured from the area of the redox peaks of pyrazine linkers in the cyclic voltammetry curve. Then, the intrinsic electrocatalytic activity of one Co site can be obtained. The catalytic performances of the three catalysts towards oxygen reduction reaction in alkaline conditions were measured. Carbon black-conjugated [Co(salophen)] showed the highest intrinsic activity with the turnover frequency of 0.72 s−1 at 0.75 V vs. the reversible hydrogen electrode. The strategy developed in this work can be used to explore and verify the possible local structure of active sites proposed for single-atom catalysts