Zhanhua Wei

High-Rate, Ultralong Cycle-Life Lithium/Sulfur Batteries Enabled by Nitrogen-Doped Graphene

Nitrogen-doped graphene (NG) is a promising conductive matrix material for fabricating high-performance Li/S batteries. Here we report a simple, low-cost, and scalable method to prepare an additive-free nanocomposite cathode in which sulfur nanoparticles are wrapped inside the NG sheets (S@NG). We show that the Li/S@NG can deliver high specific discharge capacities at high rates, that is, ∼ 1167 mAh g(-1) at 0.2 C, ∼ 1058 mAh g(-1) at 0.5 C, ∼ 971 mAh g(-1) at 1 C, ∼ 802 mAh g(-1) at 2 C, and ∼ 606 mAh g(-1) at 5 C. The cells also demonstrate an ultralong cycle life exceeding 2000 cycles and an extremely low capacity-decay rate (0.028% per cycle), which is among the best performance demonstrated so far for Li/S cells. Furthermore, the S@NG cathode can be cycled with an excellent Coulombic efficiency of above 97% after 2000 cycles. With a high active S content (60%) in the total electrode weight, the S@NG cathode could provide a specific energy that is competitive to the state-of-the-art Li-ion cells even after 2000 cycles. The X-ray spectroscopic analysis and ab initio calculation results indicate that the excellent performance can be attributed to the well-restored C-C lattice and the unique lithium polysulfide binding capability of the N functional groups in the NG sheets. The results indicate that the S@NG nanocomposite based Li/S cells have a great potential to replace the current Li-ion batteries.

High-Performance Hole-Extraction Layer of Sol-Gel-Processed NiO Nanocrystals for Inverted Planar Perovskite Solar Cells**

Hybrid organic/inorganic perovskite solar cells have been rapidly evolving with spectacular successes in both nanostructured and thin-film versions. Herein, we report the use of a simple sol-gel-processed NiO nanocrystal (NC) layer as the hole-transport layer in an inverted perovskite solar cell. The thin NiO NC film with a faceted and corrugated surface enabled the formation of a continuous and compact layer of well-crystallized CH3 NH3 PbI3 in a two-step solution process. The hole-extraction and -transport capabilities of this film interfaced with the CH3 NH3 PbI3 film were higher than those of organic PEDOT:PSS layers. The cell with a NiO NC film with a thickness of 30-40 nm exhibited the best performance, as a thinner layer led to a higher leakage current, whereas a thicker layer resulted in a higher series resistance. With the NiO film, we observed a cell efficiency of 9.11 %, which is by far the highest reported for planar perovskite solar cells based on an inorganic hole-extracting layer.

Hybrid Halide Perovskite Solar Cell Precursors: Colloidal Chemistry and Coordination Engineering behind Device Processing for High Efficiency

The precursor of solution-processed perovskite thin films is one of the most central components for high-efficiency perovskite solar cells. We first present the crucial colloidal chemistry visualization of the perovskite precursor solution based on analytical spectra and reveal that perovskite precursor solutions for solar cells are generally colloidal dispersions in a mother solution, with a colloidal size up to the mesoscale, rather than real solutions. The colloid is made of a soft coordination complex in the form of a lead polyhalide framework between organic and inorganic components and can be structurally tuned by the coordination degree, thereby primarily determining the basic film coverage and morphology of deposited thin films. By utilizing coordination engineering, particularly through employing additional methylammonium halide over the stoichiometric ratio for tuning the coordination degree and mode in the initial colloidal solution, along with a thermal leaching for the selective release of excess methylammonium halides, we achieved full and even coverage, the preferential orientation, and high purity of planar perovskite thin films. We have also identified that excess organic component can reduce the colloidal size of and tune the morphology of the coordination framework in relation to final perovskite grains and partial chlorine substitution can accelerate the crystalline nucleation process of perovskite. This work demonstrates the important fundamental chemistry of perovskite precursors and provides genuine guidelines for accurately controlling the high quality of hybrid perovskite thin films without any impurity, thereby delivering efficient planar perovskite solar cells with a power conversion efficiency as high as 17% without distinct hysteresis owing to the high quality of perovskite thin films.

Efficient Photoelectrochemical Water Splitting with Ultrathin films of Hematite on Three-Dimensional Nanophotonic Structures

Photoelectrochemical (PEC) solar water splitting represents a clean and sustainable approach for hydrogen (H2) production and substantial research are being performed to improve the conversion efficiency. Hematite (α-Fe2O3) is considered as a promising candidate for PEC water splitting due to its chemical stability, appropriate band structure, and abundance. However, PEC performance based on hematite is hindered by the short hole diffusion length that put a constraint on the active layer thickness and its light absorption capability. In this work, we have designed and fabricated novel PEC device structure with ultrathin hematite film deposited on three-dimensional nanophotonic structure. In this fashion, the nanophotonic structures can largely improve the light absorption in the ultrathin active materials. In addition, they also provide large surface area to accommodate the slow surface water oxidation process. As the result, high current density of 3.05 mA cm(-2) at 1.23 V with respect to the reversible hydrogen electrode (RHE) has been achieved on such nanophotonic structure, which is about three times of that for a planar photoelectrode. More importantly, our systematic analysis with experiments and modeling revealed that the design of high performance PEC devices needs to consider not only total optical absorption, but also the absorption profile in the active material, in addition to electrode surface area and carrier collection.

High‐Efficiency All‐Polymer Solar Cells Based on a Pair of Crystalline Low‐Bandgap Polymers

All-polymer solar cells based on a pair of crystalline low-bandgap polymers (NT and N2200) are demonstrated to achieve a high short-circuit current density of 11.5 mA cm-2 and a power conversion efficiency of up to 5.0% under the standard AM1.5G spectrum with one sun intensity. The high performance of these NT:N2200-based cells can be attributed to the low optical bandgaps of the polymers and the reasonably high and balanced electron and hole mobilities of the NT:N2200 blends due to the crystalline nature of the two polymers.

Inkjet Printing and Instant Chemical Transformation of a CH3NH3PbI3/Nanocarbon Electrode and Interface for Planar Perovskite Solar Cells

A planar perovskite solar cell that incorporates a nanocarbon hole-extraction layer is demonstrated for the first time by an inkjet printing technique with a precisely controlled pattern and interface. By designing the carbon plus CH3NH3I ink to transform PbI2 in situ to CH3NH3PbI3, an interpenetrating seamless interface between the CH3NH3PbI3 active layer and the carbon hole-extraction electrode was instantly constructed, with a markedly reduced charge recombination compared to that with the carbon ink alone. As a result, a considerably higher power conversion efficiency up to 11.60% was delivered by the corresponding solar cell. This method provides a major step towards the fabrication of low-cost, large-scale, metal-electrode-free but still highly efficient perovskite solar cells.

Cost-efficient clamping solar cells using candle soot for hole extraction from ambipolar perovskites

Ambient-unstable hole transporters and expensive and complicated noble metal electrode deposition are incompatible with the large scale and low-cost production of perovskite solar cells and thus would hamper their commercialization. Herein we report a new modality of perovskite solar cells that do away with the use of conventional hole transporters by directly clamping a selective hole extraction electrode made of candle soot and a deliberately engineered perovskite photoanode. The key soot/perovskite interface, which promotes hole extraction and electron blocking by forming a Schottky junction, was established seamlessly by pre-wetting and reaction embedding the carbon particles. Femtosecond time-resolved photoluminescence revealed a high hole extraction rate at 1.92 ns−1. We have now achieved 11.02% efficiency, making an important step towards roll-to-roll production of perovskite solar cells.

High‐Performance Graphene‐Based Hole Conductor‐Free Perovskite Solar Cells: Schottky Junction Enhanced Hole Extraction and Electron Blocking

Multilayered graphene and single-layered graphene are assembled onto perovskite films in the form of Schottky junctions and ohmic contacts, respectively, for the production of a graphene-based hole transporting material-free perovskite solar cell. Multilayered graphene extracts charge selectively and efficiently, delivering a higher efficiency of 11.5% than single-layered graphene (6.7%).

Hysteresis-free multi-walled carbon nanotube-based perovskite solar cells with a high fill factor

Among the various perovskite solar cells, the carbon-based hole-transporter-free type is arguably the most promising for applications because of its low material/manufacturing cost, high efficiency and better long-term stability. However, the fill factor (FF) is typically below 0.75, limiting the cell performance. In this communication, through a comparison of systematic performance between the multi-walled carbon nanotube (MWCNT) and another two representative carbon materials, namely carbon black and graphite, we highlight two salient advantages of MWCNT-based devices: high FF and hysteresis-free performance. We owe the superior performance to the charge transport highway at the interface of MWCNT/perovskite. After preliminary optimization, we have achieved a PCE of 12.67% with a very impressive FF of 0.80, which is among the highest for carbon-based perovskite solar cells.

A three-dimensional hexagonal fluorine-doped tin oxide nanocone array: a superior light harvesting electrode for high performance photoelectrochemical water splitting

Photonic nanostructures hold great promise in promoting light harvesting. Here we report the first design and construction of a three-dimensional (3D) hexagonal nanocone array of fluorine-doped tin oxide (FTO) on glass as an excellent electrode for photoelectrochemical (PEC) water splitting. The PEC current density with suitably deposited Ti-doped hematite at 1.23 V vs. the reversible hydrogen electrode (RHE) was increased by 86% to 2.24 ± 0.02 mA cm−2 compared to that with the planar counterpart, mainly ascribable to the special light harvesting effect and the electrode surface area provided by 3D FTO. Upon the embedment of a gold layer to concentrate the incident light onto the hematite layer and the deposition of the Co–Pi catalyst with a modified procedure, the photocurrent experienced a large cathodic shift of onset potential by 360 mV and soared to a high value of 3.39 ± 0.01 mA cm−2 (at 1.23 V), yielding a power conversion efficiency of 0.70% at a potential as low as 0.88 V vs. RHE.