A randomized controlled trial of Baduanjin exercise to reduce the risk of atherosclerotic cardiovascular disease in patients with prediabetes.

To investigate the effectiveness of long-term Baduanjin and aerobic training on the 10-year risk of atherosclerotic cardiovascular disease in prediabetic patients. This study was single-blind randomized controlled trial. A total of 98 participants with prediabetes were randomly divided into three groups: the BDJ (n = 34), AT (n = 32), and control (n = 32) groups. Participants in the BDJ and AT groups underwent one year of supervised group exercise, consisting of 60 min/session every other day. The primary outcomes were metabolic control and the 10-year risk of ASCVD. The secondary outcome was a change in blood glucose status. After the intervention, various metabolic indexes were significantly improved in the two exercise groups relative to the control group and baseline measurements (p < 0.05). Compared with no exercise, BDJ and AT had significant preventive and protective effects against the risk of ASCVD in patients with prediabetes (p < 0.001). The overall effects of the two exercise groups were similar (p > 0.05). Long-term BDJ training can effectively reduce the risk of type 2 diabetes mellitus (T2DM) and its cardiovascular complications in prediabetic patients. The effect of BDJ is similar to that of moderate-intensity aerobic exercise.

MAPbI3 Photodetectors with 4.7 MHz Bandwidth and Their Application in Organic Optocouplers.

The photodetector based on methylammonium lead iodide (MAPbI3) is a promising device for wide wavelength range (380-780 nm) sensitivity. However, its industrial application is limited by the relatively low response speed to the light signal, which has received little attention. Only a few reports show low-bandwidth characteristics (less than 1 MHz at 0.1 cm2). Here, when a cosolvent strategy to manipulate the thickness and the crystallinity of the MAPbI3 film is adopted, photodetectors with a -3 dB bandwidth of 4.7 MHz are achieved (at 0.16 cm2 photo detecting area). The performance is significantly better than most of the organic and hybrid photodetectors reported so far. Based on this photodetector and an organic light-emitting diode (OLED), an organic optocoupler system with 1 MHz response frequency is successfully set up. Our results suggest that thickness-manipulated cosolvent strategy is a promising method in high-speed MAPbI3-based photodetectors.

Interpenetrating interfaces for efficient perovskite solar cells with high operational stability and mechanical robustness.

The perovskite solar cell has emerged rapidly in the field of photovoltaics as it combines the merits of low cost, high efficiency, and excellent mechanical flexibility for versatile applications. However, there are significant concerns regarding its operational stability and mechanical robustness. Most of the previously reported approaches to address these concerns entail separate engineering of perovskite and charge-transporting layers. Herein we present a holistic design of perovskite and charge-transporting layers by synthesizing an interpenetrating perovskite/electron-transporting-layer interface. This interface is reaction-formed between a tin dioxide layer containing excess organic halide and a perovskite layer containing excess lead halide. Perovskite solar cells with such interfaces deliver efficiencies up to 22.2% and 20.1% for rigid and flexible versions, respectively. Long-term (1000 h) operational stability is demonstrated and the flexible devices show high endurance against mechanical-bending (2500 cycles) fatigue. Mechanistic insights into the relationship between the interpenetrating interface structure and performance enhancement are provided based on comprehensive, advanced, microscopic characterizations. This study highlights interface integrity as an important factor for designing efficient, operationally-stable, and mechanically-robust solar cells.

Stabilizing Perovskite Light-Emitting Diodes by Incorporation of Binary Alkali Cations.

The poor stability of perovskite light-emitting diodes (PeLEDs) is a key bottleneck that hinders commercialization of this technology. Here, the degradation process of formamidinium lead iodide (FAPbI3 )-based PeLEDs is carefully investigated and the device stability is improved through binary-alkalication incorporation. Using time-of-flight secondary-ion mass spectrometry, it is found that the degradation of FAPbI3 -based PeLEDs during operation is directly associated with ion migration, and incorporation of binary alkali cations, i.e., Cs+ and Rb+ , in FAPbI3 can suppress ion migration and significantly enhance the lifetime of PeLEDs. Combining experimental and theoretical approaches, it is further revealed that Cs+ and Rb+ ions stabilize the perovskite films by locating at different lattice positions, with Cs+ ions present relatively uniformly throughout the bulk perovskite, while Rb+ ions are found preferentially on the surface and grain boundaries. Further chemical bonding analysis shows that both Cs+ and Rb+ ions raise the net atomic charge of the surrounding I anions, leading to stronger Coulomb interactions between the cations and the inorganic framework. As a result, the Cs+ -Rb+ -incorporated PeLEDs exhibit an external quantum efficiency of 15.84%, the highest among alkali cation-incorporated FAPbI3 devices. More importantly, the PeLEDs show significantly enhanced operation stability, achieving a half-lifetime over 3600 min.

Printable CsPbBr3 perovskite quantum dot ink for coffee ring-free fluorescent microarrays using inkjet printing.

Printable perovskite quantum dot (QD) ink is very important for achieving high quality coffee ring-free fluorescent microarrays for different kinds of emerging perovskite optoelectronic applications using inkjet printing. In this work, we prepared a printable CsPbBr3 perovskite QD ink by mixing high-boiling point dodecane with low-boiling point toluene as a solvent. The evaporation rate, viscosity and surface tension of the ink were carefully optimized by tuning the volume ratio of these two solvents for forming appropriate Marangoni flow, so as to balance the capillary flow and eliminate the coffee ring effect further. Successfully, CsPbBr3 perovskite microarrays with uniform surface, low roughness and no coffee rings were achieved by inkjet printing the optimized perovskite QD ink on a PVK (poly-(9-vinylcarbazole)) layer. Furthermore, we patterned the CsPbBr3 perovskite QD ink, and the printed patterns were only visible under ultraviolet (UV) light, which can be applied in invisible anti-counterfeiting labels and encryption in the future.

Efficient and stable emission of warm-white light from lead-free halide double perovskites.

Lighting accounts for one-fifth of global electricity consumption1. Single materials with efficient and stable white-light emission are ideal for lighting applications, but photon emission covering the entire visible spectrum is difficult to achieve using a single material. Metal halide perovskites have outstanding emission properties2,3; however, the best-performing materials of this type contain lead and have unsatisfactory stability. Here we report a lead-free double perovskite that exhibits efficient and stable white-light emission via self-trapped excitons that originate from the Jahn-Teller distortion of the AgCl6 octahedron in the excited state. By alloying sodium cations into Cs2AgInCl6, we break the dark transition (the inversion-symmetry-induced parity-forbidden transition) by manipulating the parity of the wavefunction of the self-trapped exciton and reduce the electronic dimensionality of the semiconductor4. This leads to an increase in photoluminescence efficiency by three orders of magnitude compared to pure Cs2AgInCl6. The optimally alloyed Cs2(Ag0.60Na0.40)InCl6 with 0.04 per cent bismuth doping emits warm-white light with 86 ± 5 per cent quantum efficiency and works for over 1,000 hours. We anticipate that these results will stimulate research on single-emitter-based white-light-emitting phosphors and diodes for next-generation lighting and display technologies.

Electric Bias Induced Degradation in Organic-Inorganic Hybrid Perovskite Light-Emitting Diodes.

For organic-inorganic perovskite to be considered as the most promising materials for light emitting diodes and solar cell applications, the active materials must be proven to be stable under various conditions, such as ambient environment, heat and electrical bias. Understanding the degradation process in organic-inorganic perovskite light emitting diodes (PeLEDs) is important to improve the stability and the performance of the device. We revealed that electrical bias can greatly influence the luminance and external quantum efficiency of PeLEDs. It was found that device performance could be improved under low voltage bias with short operation time, and decreased with continuous operation. The degradation of perovskite film under high electrical bias leads to the decrease of device performance. Variations in the absorption, morphology and element distribution of perovskite films under different electrical bias revealed that organic-inorganic perovskites are unstable at high electrical bias. We bring new insights in the PeLEDs which are crucial for improving the stability.

Cs2PbI2Cl2, All-Inorganic Two-Dimensional Ruddlesden-Popper Mixed Halide Perovskite with Optoelectronic Response.

The two-dimensional Ruddlesden-Popper (RP) phases are an important class of halide perovskites with versatile optoelectronic properties. So far, only organic-inorganic hybrid RP phases involving long organic spacers were reported in this class. Here, we report an all-inorganic RP phase lead halide perovskite, Cs2PbI2Cl2 (1, I4/ mmm space group; a = 5.6385(8) Å, c = 18.879(4) Å), synthesized by a solid-state method. The compound exhibits a band gap of Eg ∼ 3.04 eV and photoconductivity. We find an anomalous band gap evolution in Cs2Pb1- xSn xI2Cl2 solid solutions. Our combined density functional theory and experimental study supports the thermodynamically stable nature of 1 as a unique ordered phase in the Cs2PbX4 (X = Cl, Br, I) system. The calculations suggest that 1 is a direct bandgap semiconductor with relatively small effective carrier mass along the in-plane direction, consistent with the experimentally observed in-plane UV-light photoresponse. We also demonstrate that 1 is promising for radiation detection capable of α-particle counting. Moreover, 1 shows markedly ambient and thermal stability.

A Droplet-Reactor System Capable of Automation for the Continuous and Scalable Production of Noble-Metal Nanocrystals.

Noble-metal nanocrystals with well-controlled shapes or morphologies are of great interest for a variety of applications. To utilize these nanomaterials in consumer products, one has to produce the colloidal nanocrystals in large quantities while maintaining good control over their physical parameters and properties. Droplet reactors have shown great potential for the continuous and scalable production of colloidal nanocrystals with controlled shapes. However, the efficiencies of most previously reported systems are still limited because of the complex post-treatment procedures. For example, the mixture of silicone oil and an aqueous suspension of solid products has to be separated by leveraging their miscibility and difference in density, while the solid products often need to be purified and concentrated by centrifugation. Herein, we report the design and construction of a droplet-reactor system that include new features such as a homemade unit for the automatic separation of silicone oil from the aqueous phase as well as a cross-flow filtration unit for the effective purification and concentration of the nanocrystals. Using various types of Pd nanocrystals as examples, we have demonstrated the feasibility of using this system to automatically produce and collect samples with uniform sizes and well-controlled shapes.

CH3NH3Pb1-x Eu x I3 mixed halide perovskite for hybrid solar cells: the impact of divalent europium doping on efficiency and stability.

The crucial role of the impact of divalent europium doping in perovskite solar cells is investigated in this work. We selected europium (Eu2+, 117 pm) to replace lead (Pb2+, 119 pm) because their ion radii are really comparable. This appropriate substitution has shown great potential to achieve high stability and enhance the power conversion efficiency of the solar cells. Through adjusting the doping concentration of europium, the perovskite solar cells corresponding average efficiency greatly increased. Furthermore, compared with the CH3NH3PbI3 perovskite film, the attenuation of power conversion efficiency of europium doped perovskite film slowed down 4.7 times at room temperature. Therefore, we put forward a useful method for the optimization of organic-inorganic perovskite solar cells.

Stable α/δ phase junction of formamidinium lead iodide perovskites for enhanced near-infrared emission.

Although formamidinium lead iodide (FAPbI3) perovskite has shown great promise in the field of perovskite-based optoelectronic devices, it suffers the complications of a structural phase transition from a black perovskite phase (α-FAPbI3) to a yellow non-perovskite phase (δ-FAPbI3). Generally, it is pivotal to avoid δ-FAPbI3 since only α-FAPbI3 is desirable for photoelectric conversion and near-infrared (NIR) emission. However, herein, we firstly exploited the undesirable δ-FAPbI3 to enable structurally stable, pure FAPbI3 films with a controllable α/δ phase junction at low annealing temperature (60 °C) through stoichiometrically modified precursors (FAI/PbI2 = 1.1-1.5). The α/δ phase junction contributes to a striking stabilization of the perovskite phase of FAPbI3 at low temperature and significantly enhanced NIR emission at 780 nm, which is markedly different from pure α-FAPbI3 (815 nm). In particular, the optimal α/δ phase junction with FAI/PbI2 = 1.2 exhibited preferable long-term stability against humidity and high PLQY of 6.9%, nearly 10-fold higher than that of pure α-FAPbI3 (0.7%). The present study opens a new approach to realize highly stable and efficient emitting perovskite materials by utilizing the phase junctions.

An Origami Perovskite Photodetector with Spatial Recognition Ability.

Flexible photodetectors are attracting substantial attention because of their promising applications in bendable display and smart clothes which cannot be fulfilled by the existing rigid counterparts. In this work, we demonstrate a newly designed photodetector constructed on the common printing paper. Pencil trace was applied as the graphite electrode. With such a simple and convenient method, the as-prepared photodetector exhibited a satisfactory responsivity of 4.4 mA/W, on/off current ratio of 32, coupled with a high response speed of <10 ms. It also demonstrated excellent mechanical flexibility and durability. Most inspiringly, by an ingenious origami, we created the first perovskite photodetector with a 3D configuration. The cubic photodetector array displayed an excellent spatial recognition ability which could not be achieved in all the previously reported 2D photodetectors. Such a fusion of materials science and the art of origami provides a robust strategy for the design of low-cost flexible electronics, especially for the applications in 3D configurations.

High Performance of Perovskite Solar Cells via Catalytic Treatment in Two-Step Process: The Case of Solvent Engineering.

Currently, the potential mechanism of the solvent-assisted crystallization for mixed cations perovskite thin film (FAxMA1-xPbI3) prepared via two-step solution-process still remains obscure. Here, we clarified the molecular-competing-reacted process of NH2CH═NH2I (FAI) and CH3NH3I (MAI) with PbI2(DMSO)x complex in dimethyl sulfoxide (DMSO) and diethyl ether (DE) catalytic solvent system in the sequential two-step solution-process. The microscopic dynamics was characterized via the characterizations of in situ photoluminescence spectra. In addition, we found that the thermal stability of the perovskite films suffered from the residual solvent with high boiling point, for example, DMSO. The further DE treatment could promote the volatility process of DMSO and accelerate the crystallization process of perovskite films. The highest PCE over 19% with slight hysteresis effect was eventually obtained with a reproducible FA0.88MA0.12PbI3 solar cell, which displayed a constant power output within 100 s upon light soaking and stable PCE output within 30 d in the thermal stability test.

Insight into the CH3NH3PbI3/C interface in hole-conductor-free mesoscopic perovskite solar cells.

Perovskite solar cells (PSCs) with hole-conductor-free mesoscopic architecture have shown superb stability and great potential in practical application. The printable carbon counter electrodes take full responsibility of extracting holes from the active CH3NH3PbI3 absorbers. However, an in depth study of the CH3NH3PbI3/C interface properties, such as the structural formation process and the effect of interfacial conditions on hole extraction, is still lacking. Herein, we present, for the first time, an insight into the spatial confinement induced CH3NH3PbI3/C interface formation by in situ photoluminescence observations during the crystallization process of CH3NH3PbI3. The derived reaction kinetics allows a quantitative description of the perovskite formation process. In addition, we found that the interfacial contact between carbon and perovskite was dominant for hole extraction efficiency and associated with the photovoltaic parameter of short circuit current density (JSC). Consequently, we conducted a solvent vapor assisted process of PbI2 diffusion to carefully control the CH3NH3PbI3/C interface with less unreacted PbI2 barrier. The improvement of interface conditions thereby contributes to a high hole extraction proved by the charge extraction resistance and PL lifetime change, resulting in the increased JSC valve.

Synthesis of Pt-Ni Octahedra in Continuous-Flow Droplet Reactors for the Scalable Production of Highly Active Catalysts toward Oxygen Reduction.

A number of groups have reported the syntheses of nanosized Pt-Ni octahedra with remarkable activities toward the oxygen reduction reaction (ORR), a process key to the operation of proton-exchange membrane fuel cells. However, the throughputs of those batch-based syntheses are typically limited to a scale of 5-25 mg Pt per batch, which is far below the amount needed for commercial evaluation. Here we report the use of droplet reactors for the continuous and scalable production of Pt-Ni octahedra with high activities toward ORR. In a typical synthesis, Pt(acac)2, Ni(acac)2, and W(CO)6 were dissolved in a mixture of oleylamine, oleic acid, and benzyl ether, and then pumped into a polytetrafluoroethylene tube. When the solution entered the reaction zone at a temperature held in the range of 170-230 °C, W(CO)6 quickly decomposed to generate CO gas, naturally separating the reaction solution into discrete, uniform droplets. Each droplet then served as a reactor for the nucleation and growth of Pt-Ni octahedra whose size and composition could be controlled by changing the composition of the solvent and/or adjusting the amount of Ni(acac)2 added into the reaction solution. For a catalyst based on Pt2.4Ni octahedra of 9 nm in edge length, it showed an ORR mass activity of 2.67 A mgPt(-1) at 0.9 V, representing an 11-fold improvement over a state-of-the-art commercial Pt/C catalyst (0.24 A mgPt(-1)).

Enhanced optoelectronic quality of perovskite thin films with hypophosphorous acid for planar heterojunction solar cells.

Solution-processed metal halide perovskite semiconductors, such as CH3NH3PbI3, have exhibited remarkable performance in solar cells, despite having non-negligible density of defect states. A likely candidate is halide vacancies within the perovskite crystals, or the presence of metallic lead, both generated due to the imbalanced I/Pb stoichiometry which could evolve during crystallization. Herein, we show that the addition of hypophosphorous acid (HPA) in the precursor solution can significantly improve the film quality, both electronically and topologically, and enhance the photoluminescence intensity, which leads to more efficient and reproducible photovoltaic devices. We demonstrate that the HPA can reduce the oxidized I2 back into I(-), and our results indicate that this facilitates an improved stoichiometry in the perovskite crystal and a reduced density of metallic lead.

High-Performance Planar-Type Photodetector on (100) Facet of MAPbI3 Single Crystal.

Recently, the discovery of organometallic halide perovskites provides promising routes for fabricating optoelectronic devices with low cost and high performance. Previous experimental studies of MAPbI3 optoelectronic devices, such as photodetectors and solar cells, are normally based on polycrystalline films. In this work, a high-performance planar-type photodetector fabricated on the (100) facet of a MAPbI3 single crystal is proposed. We demonstrate that MAPbI3 photodetector based on single crystal can perform much better than that on polycrystalline-film counterpart. The low trap density of MAPbI3 single crystal accounts for the higher carrier mobility and longer carrier diffusion length, resulted in a significant performance increasement of MAPbI3 photodetector. Compared with similar planar-type photodetectors based on MAPbI3 polycrystalline film, our MAPbI3 single crystal photodetector showed excellent performance with good stability and durability, broader response spectrum to near-infrared region, about 10(2) times higher responsivity and EQE, and approximately 10(3) times faster response speed. These results may pave the way for exploiting high-performance perovskites photodetectors based on single crystal.

Controllable Grain Morphology of Perovskite Absorber Film by Molecular Self-Assembly toward Efficient Solar Cell Exceeding 17%.

The highly developed crystallization process with respect to perovskite thin films is favorable for efficient solar cells. Here, an innovative intermolecular self-assembly approach was employed to retard the crystallization of PbI2 in dimethylformamide (DMF) by additional solvent of dimethyl sulfoxide (DMSO), which was proved to be capable of coordinating with PbI2 by coordinate covalent bond. The obtained PbI2(DMSO)x (0 ≤ x ≤ 1.86) complexes tend to be closely packed by means of intermolecular self-assembly. Afterward, an intramolecular exchange of DMSO with CH3NH3I (MAI) enabled the complexes to deform their shape and finally to reorganize to be an ultraflat and dense thin film of CH3NH3PbI3. The controllable grain morphology of perovskite thin film allows obtaining a power conversion efficiency (PCE) above 17% and a stabilized power output above 16% within 240 s by controlling DMSO species in the complex-precursor system (CPS). The present study gives a reproductive and facile strategy toward high quality of perovskite thin films and efficient solar cells.

Improved charge transport and injection in a meso-superstructured solar cell by a tractable pre-spin-coating process.

In meso-superstructured solar cells (MSSCs), the state-of-the-art perovskite acts as both the light harvester and electron transporter due to its ambipolar properties. The inefficient pore filling and infiltration of perovskite directly affect the continuous distribution of perovskite in mesoporous Al2O3, resulting in discontinuous carrier transport in the mesoporous structure and insufficient electron injection to the compact TiO2 layer. Herein, we introduce a simple pre-spin-coating process to improve the infiltration and pore filling of perovskite, which results in higher light absorption and enhanced electron injection, as seen in UV-vis spectra and photoluminescence (PL) spectra, respectively. We first apply time of flight (TOF) experiments to characterize charge transport in MSSCs, and the results reveal that more continuous charge transport pathways are formed with the pre-spin-coating process. This effective method, with ease of processing, demonstrates obviously improved photocurrents, reaching an efficiency as high as 14%, and promotes the application of lead halide perovskite materials in the photovoltaics field.