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1.
Angew Chem Int Ed Engl ; : e202412590, 2024 Aug 24.
Artículo en Inglés | MEDLINE | ID: mdl-39180505

RESUMEN

As the initial synthesized colloidal quantum dots (CQDs) are generally capped with insulating ligands, ligand exchange strategies are essential in the fabrication of CQD films for solar cells, which can regulate the surface chemical states of CQDs to make them more suitable for thin-film optoelectronic devices. However, uncontrollable surface adsorption of water molecules during the ligand exchange process introduces new defect sites, thereby impairing the resultant device performance, which attracts more efforts devoted to it but remains a puzzle. Here, we develop a solvent-engineering-assisted ligand exchange strategy to revamp the surface adsorption, improve the exchange efficiency, and modulate the surface chemistry for the environmentally friendly lead-free silver bismuth disulfide (AgBiS2) CQDs. The optimized AgBiS2 CQD solar cells deliver an outstanding champion power conversion efficiency (PCE) of up to 8.95% and improved long-term stability. Our strategy is less environment-dependent and can produce solar cells with negligible performance variance for several batches across several months. Our work demonstrates the critical role of solvents for ligand exchange in the surface chemistry of CQDs and the realization of high-performance photovoltaic devices in a highly reproducible manner.

2.
Nano Lett ; 24(34): 10418-10425, 2024 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-39158928

RESUMEN

Surface ligand chemistry is vital to control the synthesis, diminish surface defects, and improve the electronic coupling of quantum dots (QDs) toward emerging applications in optoelectronic devices. Here, we successfully develop highly homogeneous and dispersed AgBiS2 QDs, focus on the control of interdot spacing, and substitute the long-chain ligands with ammonium iodide in solution. This results in improved electronic coupling of AgBiS2 QDs with excellent surface passivation, which greatly facilitates carrier transport within the QD films. Based on the stable AgBiS2 QD dispersion with the optimal ligand state, a homogeneous and densely packed QD film is prepared by a facile one-step coating process, delivering a champion power conversion efficiency of approximately 8% in the QD solar cells with outstanding shelf life stability. The proposed surface engineering strategy holds the potential to become a universal preprocessing step in the realm of high-performance QD optoelectronic devices.

3.
Materials (Basel) ; 17(13)2024 Jul 07.
Artículo en Inglés | MEDLINE | ID: mdl-38998436

RESUMEN

The catalytic capabilities of metals in degrading azo dyes have garnered extensive interest; however, selecting highly efficient metals remains a significant challenge. We have developed a Zn-Ca-based metallic glass composite which shows outstanding degradation efficiency for Direct Blue 6. This alloy comprises a Zn2Ca crystalline phase and an amorphous matrix, allowing for the degradation of azo dyes within minutes in a wide temperature range of 0-60 °C. Kinetic calculations reveal an exceptionally low activation energy of 8.99 kJ/mol. The rapid degradation is attributed to the active element Ca and the unique amorphous structure of the matrix, which not only facilitates abundant redox conditions but also minimizes the hydrolysis of the active element. The newly developed metallic glass composite exhibits a notably higher azo dye degradation rate compared to those of general metallic glasses, offering a new avenue for the rapid degradation of azo dyes. This paper holds significant importance for the development of novel azo dye wastewater treatment agents.

4.
ACS Nano ; 18(11): 8157-8167, 2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38456777

RESUMEN

Perovskite light-emitting diodes (PeLEDs) are the next promising display technologies because of their high color purity and wide color gamut, while two classical emitter forms, i.e., polycrystalline domains and quantum dots, are encountering bottlenecks. Weak carrier confinement of large polycrystalline domains leads to inadequate radiative recombination, and surface ligands on quantum dots are the main annihilation sites for injected carriers. Here, pinpointing these issues, we screened out an amphoteric agent, namely, 2-(2-aminobenzoyl)benzoic acid (2-BA), to precisely control the in situ growth of FAPbI3 (FA: formamidine) nanodomains with enhanced space confinement, preferred crystal orientation, and passivated trap states on the transport-layer substrate. The amphoteric 2-BA performs bidentate chelating functions on the formation of ultrasmall perovskite colloids (<1 nm) in the precursor, resulting in a smoother FAPbI3 emitting layer. Based on monodispersed and homogeneous nanodomain films, a near-infrared PeLED device with a champion efficiency of >22% plus enhanced T80 operational stability was achieved. The proposed perovskite nanodomain film tends to be a mainstream emitter toward the performance breakthrough of PeLED devices covering visible wavelengths beyond infrared.

5.
Adv Mater ; 36(21): e2311145, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38334458

RESUMEN

High-quality perovskite films are essential for achieving high performance of optoelectronic devices; However, solution-processed perovskite films are known to suffer from compositional and structural inhomogeneity due to lack of systematic control over the kinetics during the formation. Here, the microscopic homogeneity of perovskite films is successfully enhanced by modulating the conversion reaction kinetics using a catalyst-like system generated by a foaming agent. The chemical and structural evolution during this catalytic conversion is revealed by a multimodal synchrotron toolkit with spatial resolutions spanning many length scales. Combining these insights with computational investigations, a cyclic conversion pathway model is developed that yields exceptional perovskite homogeneity due to enhanced conversion, having a power conversion efficiency of 24.51% for photovoltaic devices. This work establishes a systematic link between processing of precursor and homogeneity of the perovskite films.

6.
Nature ; 625(7995): 516-522, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-38233617

RESUMEN

Perovskite solar cells (PSCs) comprise a solid perovskite absorber sandwiched between several layers of different charge-selective materials, ensuring unidirectional current flow and high voltage output of the devices1,2. A 'buffer material' between the electron-selective layer and the metal electrode in p-type/intrinsic/n-type (p-i-n) PSCs (also known as inverted PSCs) enables electrons to flow from the electron-selective layer to the electrode3-5. Furthermore, it acts as a barrier inhibiting the inter-diffusion of harmful species into or degradation products out of the perovskite absorber6-8. Thus far, evaporable organic molecules9,10 and atomic-layer-deposited metal oxides11,12 have been successful, but each has specific imperfections. Here we report a chemically stable and multifunctional buffer material, ytterbium oxide (YbOx), for p-i-n PSCs by scalable thermal evaporation deposition. We used this YbOx buffer in the p-i-n PSCs with a narrow-bandgap perovskite absorber, yielding a certified power conversion efficiency of more than 25%. We also demonstrate the broad applicability of YbOx in enabling highly efficient PSCs from various types of perovskite absorber layer, delivering state-of-the-art efficiencies of 20.1% for the wide-bandgap perovskite absorber and 22.1% for the mid-bandgap perovskite absorber, respectively. Moreover, when subjected to ISOS-L-3 accelerated ageing, encapsulated devices with YbOx exhibit markedly enhanced device stability.

7.
Adv Mater ; 36(2): e2305238, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37665975

RESUMEN

The limited conductivity of existing transparent conducting oxide (TCO) greatly restricts the further performance improvement of perovskite solar cells (PSCs), especially for large-area devices. Herein, buried-metal-grid tin-doped indium oxide (BMG ITO) electrodes are developed to minimize the power loss caused by the undesirable high sheet resistance of TCOs. By burying 140-nm-thick metal grids into ITO using a photolithography technique, the sheet resistance of ITO is reduced from 15.0 to 2.7 Ω sq-1 . The metal step of BMG over ITO has a huge impact on the charge carrier transport in PSCs. The PSCs using BMG ITO with a low metal step deliver power conversion efficiencies (PCEs) significantly better than that of their counterparts with higher metal steps. Moreover, compared with the pristine ITO-based PSCs, the BMG ITO-based PSCs show a smaller PCE decrease when scaling up the active area of devices. The parallel-connected large-area PSCs with an active area of 102.8 mm2 reach a PCE of 22.5%. The BMG ITO electrodes are also compatible with the fabrication of inverted-structure PSCs and organic solar cells. The work demonstrates the great efficacy of improving the conductivity of TCO by BMG and opens up a promising avenue for constructing highly efficient large-area PSCs.

8.
Materials (Basel) ; 16(19)2023 Sep 27.
Artículo en Inglés | MEDLINE | ID: mdl-37834567

RESUMEN

In recent years, Zn and its alloys have become some of the most promising degradable metals as in vivo implants due to their acceptable biocompatibility and more suitable degradation rate compared with Mg-based and Fe-based alloys. However, the degradation rate of Zn-based materials after implantation in the body for orthopedic applications is relatively slow, leading to long-term retention of the implants after fulfilling their missions. Moreover, the excessive release of Zn2+ during the degradation process of Zn-based implants usually leads to high cytotoxicity and delayed osseointegration. To provide a feasible solution to the problem faced by Zn-based implants, a Zn-Ca composite was fabricated by an air pressure infiltration method in this work. The XRD pattern of the composite suggests that the composite is fully composed of Zn-Ca intermetallic compounds. The degradation tests in vitro show that the composite has a much higher degradation rate than pure Zn, and the high Ca content regions in the composite can preferentially degrade as sacrificial anodes. In addition, the composite can efficiently induce Ca-P deposition during immersion tests in Hank's solution. Cytotoxicity tests indicate that L-929 cells exhibit around 82% cell viability (Grade 1) even after being cultured in the 100% extract prepared from the Zn-Ca composite for 1 day and show excellent cell viability.

9.
Materials (Basel) ; 16(15)2023 Jul 28.
Artículo en Inglés | MEDLINE | ID: mdl-37570028

RESUMEN

Ti-based bulk metallic glass (BMG) alloys have attracted widespread attention due to their strong glass forming ability, high specific strength, and good corrosion resistance. However, the poor plasticity of BMGs limits their further application in the aerospace and aircraft fields, as well as others. We optimized the composition of SiC-reinforced, Ti-based metallic glass matrix composites (MGMCs) through finite element modeling (FEM). FEM of MGMCs containing irregularly shaped SiC particles with different contents was conducted. Stress and strain analyses were conducted to evaluate the effect of the particle volume fraction on the mechanical behavior of MGMCs, and an optimization value of 30% was obtained, which is conducive to plasticity improvement. Arc melting copper mold injection casting was used to verify the optimized SiC content. The results show that the electroless nickel plating treatment effectively improves the wettability between SiC particles and the amorphous matrix, enabling the successful preparation of SiC/MGMC with a volume fraction of 29.5% through traditional injection casting. The volume fraction of SiC plays a crucial role in the transition of fracture mode from splitting to shear in MGMCs. After adding lightweight SiC particles, the yield strength, plasticity, modulus, and specific strength were improved by 25%, 1471%, 46%, and 33%, indicating that the use of nickel-plated SiC particles in MGMCs is an effective strengthening and toughening method for BMGs.

10.
Materials (Basel) ; 16(16)2023 Aug 09.
Artículo en Inglés | MEDLINE | ID: mdl-37629832

RESUMEN

To solve the problem of the low coercivity of Nd-Fe-B-based nanowires impeding their application in magnetic storage media, highly ordered Nd-Fe-B/Fe-Co composite nanowires were fabricated in an anodic alumina template by means of the alternating electrochemical deposition method. In this paper, the effect of soft and hard magnetic phase compositing on the magnetic properties of Nd-Fe-B-based nanowires was investigated, and the coercivity improvement mechanism was demonstrated. The results show that after annealing at 600 °C for 2 h, Nd-Fe-B/Fe-Co nanowires crystallize into a multiphase structure containing a hard Nd2(Fe, Co)14B phase and soft NdB4, NdB6, Fe7Nd, and Fe7Co3 phases. It is characterized that the Nd2(Fe, Co)14B phase preferentially nucleates, followed by NdB4 + NdB6 + Fe7Nd, while Fe7Co3 has been formed in as-deposited nanowires. The existence of a Nd2(Fe, Co)14B phase with high anisotropy fields, the remanence enhancement effect produced by exchange coupling between hard-soft magnetic phases, and the pinning effect between different phases make the composite nanowires approximately exhibit single hard magnetic phase characteristics with coercivity and remanence ratio as high as 4203.25 Oe and 0.89. The results indicate that synthesizing Nd-Fe-B/Fe-Co exchange-coupled composite nanowires via alternating electrodeposition is an effective way to optimize the magnetic performance of Nd-Fe-B-based nanowires.

11.
ACS Omega ; 8(11): 10503-10511, 2023 Mar 21.
Artículo en Inglés | MEDLINE | ID: mdl-36969468

RESUMEN

Nickel and cobalt oxides are promising electrode materials for supercapacitors, but their poor conductivity and sluggish kinetics seriously hinder their application. Herein, a simple one-step calcination method was proposed to prepare carbon-incorporated NiO@Co3O4 (denoted as CNC) using a NiCo Prussian blue analogue (NiCo-PBA) as a precursor. The effect of calcination temperature on the electrochemical behavior of CNC was investigated. Benefiting from the relatively large specific surface area and porous structure characteristics, when used as an electrode for supercapacitors, the CNC obtained at 400 °C shows the typical features of a battery-type electrode, with a good specific capacitance of 208.5 F g-1 at 1 A g-1 and a rate capability of 70.8% at 30 A g-1. The hybrid supercapacitor (HSC) constructed with the optimum CNC electrode can provide a high energy density of 32.6 Wh kg-1 at the corresponding power density of 750.0 W kg-1 and an excellent cycling stability of 87.1% over 5000 cycles. This study provides a simple calcination method for preparing MOF-derived high-conductivity mixed metal oxide electrode materials for supercapacitors.

12.
Biomed Mater ; 18(2)2023 02 28.
Artículo en Inglés | MEDLINE | ID: mdl-36758244

RESUMEN

The development of novel antibacterial nano-materials with synergistic biological effects has attracted extensive interest of the researchers. In the study, 0.5 mol% Ag and 0.5 mol% Cu co-doped K2Ti6O13(0.5 Ag-0.5 Cu-KTO) nanomaterial was successfully synthesized using two-step method of sol-gel and hydrothermal synthesis. The crystal structure of 0.5 Ag-0.5 Cu-KTO was the same as that of monoclinic K2Ti6O13. Ag ions and Cu ions were uniformly loaded on K2Ti6O13by replacing partial Ti ions, so that these antibacterial ions could be slowly released. High specific surface area of 0.5 Ag-0.5 Cu-KTO (337.6 m2g-1) provided more surface active sites for Ag-Cu doping and adsorption. More negative surface zeta potential (-32.83 mV in phosphate buffer solution and -21.45 mV in physiological saline solution, respectively) would be beneficial to prevent the aggregation of the nanowires in physiological environment. Under the same doping amount, compared to 1.0 mol% Cu doped K2Ti6O13, 0.5 Ag-0.5 Cu-KTO exhibited better antibacterial performance against gram-positive and gram-negative bacteria at only 100 µg ml-1dose concentration, near to 1.0 mol% Ag doped K2Ti6O13(1.0 Ag-KTO). And 0.5 Ag-0.5 Cu-KTO showed more excellent biocompatibility than 1.0 Ag-KTO, which was attribute to the introduction of Cu ions effectively decreasing the hemolytic and cytotoxic risks from Ag ions. As expected, the synthesized 0.5 Ag-0.5 Cu-KTO nanowires demonstrated excellent structural stability, high antibacterial activity, good hemocompatibility and cytocompatibility owing to the synergistic effects of Cu and Ag ions. 0.5 Ag-0.5 Cu-KTO nanowires will be a promising antimicrobial candidate for biomedical applications.


Asunto(s)
Antibacterianos , Nanocables , Antibacterianos/química , Titanio/química , Bacterias Gramnegativas , Bacterias Grampositivas , Iones
13.
Adv Mater ; 35(5): e2206345, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36443913

RESUMEN

Inverted-structure metal halide perovskite solar cells (PSCs) have attractive advantages like low-temperature processability and outstanding device stability. The two-step sequential deposition method shows the benefits of easy fabrication and decent performance repeatability. Nevertheless, it is still challenging to achieve high-performance inverted PSCs with similar or equal power conversion efficiencies (PCEs) compared to the regular-structure counterparts via this deposition method. Here, an improved two-step sequential deposition technique is demonstrated via treating the bottom organic hole-selective layer with the binary modulation system composed of a polyelectrolyte and an ammonium salt. Such improved sequential deposition method leads to the spontaneous refinement of up and buried interfaces for the perovskite films, contributing to high film quality with significantly reduced defect density and better charge transportation. As a result, the optimized PSCs show a large enhancement in the open-circuit voltage by 100 mV and a dramatic lift in the PCE from 18.1% to 23.4%, delivering the current state-of-the-art performances for inverted PSCs. Moreover, good operational and thermal stability is achieved upon the improved inverted PSCs. This innovative strategy helps gain a deeper insight into the perovskite crystal growth and defect modulation in the inverted PSCs based on the two-step sequential deposition method.

14.
Adv Mater ; 35(3): e2208178, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36305594

RESUMEN

Solar cells capable of light-harvesting during daytime and light-emission at night are multifunctional semiconductor devices with many potential applications. Here, it is reported that halide perovskite heterojunction interfaces can be refined to yield stable and efficient solar cells. The cell can also operate effectively as an ultralow-voltage light-emitting diode (LED) with a peak external quantum efficiency of electroluminescence (EQEEL ) of 3.3%. Spectroscopic and microscopic studies reveal that double-heterojunction refinement with wide-bandgap salts is key to densifying the packing of perovskite grains and enlarging the bandgaps of the perovskite surfaces that are in contact with charge-transport semiconductors. The refined perovskite enables a simple device with dual actions of solar cells and LEDs. This type of all-in-one device has the potential to be used in multifunctional harvesting-storage-utilization (HSU) systems.

15.
Sci Adv ; 8(35): eabo3733, 2022 Sep 02.
Artículo en Inglés | MEDLINE | ID: mdl-36054361

RESUMEN

There exists a considerable density of interaggregate grain boundaries (GBs) and intra-aggregate GBs in polycrystalline perovskites. Mitigation of intra-aggregate GBs is equally notable to that of interaggregate GBs as intra-aggregate GBs can also cause detrimental effects on the photovoltaic performances of perovskite solar cells (PSCs). Here, we demonstrate full-scale GB mitigation ranging from nanoscale intra-aggregate to submicron-scale interaggregate GBs, by modulating the crystallization kinetics using a judiciously designed brominated arylamine trimer. The optimized GB-mitigated perovskite films exhibit reduced nonradiative recombination, and their corresponding mesostructured PSCs show substantially enhanced device efficiency and long-term stability under illumination, humidity, or heat stress. The versatility of our strategy is also verified upon applying it to different categories of PSCs. Our discovery not only specifies a rarely addressed perspective concerning fundamental studies of perovskites at nanoscale but also opens a route to obtain high-quality solution-processed polycrystalline perovskites for high-performance optoelectronic devices.

16.
Phys Rev E ; 106(2-1): 024213, 2022 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-36109962

RESUMEN

Dark soliton is usually seen as one of the simplest topological solitons, due to phase shift across its intensity dip. We investigate phase characters of single-valley dark soliton (SVDS) and double-valley dark soliton (DVDS) in a single-mode optical fiber with third-order dispersion and delayed nonlinear response. Notably, two different phase shifts can produce an SVDS with the same velocity under some conditions, which is not admitted for a dark soliton with only the second-order dispersion and self-phase modulation, whose phase shift and velocity is a one-to-one match. This phase property of SVDS can be used to explain the generation of previously reported DVDS in Hirota equation and make DVDSs show two types of phase profiles. Moreover, the different topological vector potentials underlying the distinct phase profiles have been uncovered. We further explore the collision properties of the DVDSs by analyzing their topological phases. Strikingly, the inelastic collision can lead to the conversion between the two types of phase profiles for DVDS. The results reveal that inelastic or elastic collision can be judged by analyzing virtual topological magnetic fields.

17.
Phys Rev E ; 105(5-1): 054202, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-35706226

RESUMEN

Weak Gaussian perturbations on a plane wave background could trigger lots of rogue waves (RWs), due to modulational instability. Numerical simulations showed that these RWs seemed to have similar unit structure. However, to the best of our knowledge, there are no relative results to prove that these RWs have the similar patterns for different perturbations, partly due to that it is hard to measure the RW pattern automatically. In this work, we address these problems from the perspective of computer vision via using deep neural networks. We propose a rogue wave detection network (RWD-Net) model to automatically and accurately detect RWs in the images, which directly indicates they have the similar computer vision patterns. For this purpose, we herein meanwhile have designed and release the corresponding dataset, termed as rogue wave dataset-10K (RWD-10K), which has 10191 RW images with bounding box annotations for each RW unit. In our detection experiments, we get 99.29% average precision on the test splits of the proposed dataset. Finally, we derive our metric, termed as the density of RW units, to characterize the evolution of Gaussian perturbations and obtain the statistical results on them.

18.
Materials (Basel) ; 15(3)2022 Jan 26.
Artículo en Inglés | MEDLINE | ID: mdl-35160886

RESUMEN

A Zn-3Mg-1Ti alloy was fabricated by ultrasonic treatment of Zn-Mg alloy melt using a Ti ultrasonic radiation rod. The microstructure, phase structure, mechanical properties, degradation property, and in vitro cytotoxicity were investigated systematically. The obtained Zn-3Mg-1Ti alloy is composed of the Zn, Mg2Zn11, and TiZn16. Owing to the grain refinement and second phase reinforcement, the mechanical properties of Zn-3Mg-1Ti alloy is improved. In addition, the Zn-3Mg-1Ti alloy exhibits minimal cytotoxicity compared to pure Zn and Zn-1Ti alloy. Electrochemical tests show that the Zn-3Mg-1Ti alloy has an appropriate degradation rate in Hank's solution.

19.
Materials (Basel) ; 15(2)2022 Jan 06.
Artículo en Inglés | MEDLINE | ID: mdl-35057126

RESUMEN

The mechanical properties of iron-rich Al-Si alloy is limited by the existence of plenty of the iron-rich phase (ß-Al5FeSi), whose unfavorable morphology not only splits the matrix but also causes both stress concentration and interface mismatch with the Al matrix. The effect of the cooling rate on the tensile properties of Fe-rich Al-Si alloy was studied by the melt spinning method at different rotating speeds. At the traditional casting cooling rate of ~10 K/s, the size of the needle-like ß-Al5FeSi phase is about 80 µm. In contrast, the size of the ß-Al5FeSi phase is reduced to 500 nm and the morphology changes to a granular morphology with the high cooling rate of ~104 K/s. With the increase of the cooling rate, the morphology of the ß-Al5FeSi phase is optimized, meanwhile the tensile properties of Fe-rich Al-Si alloy are greatly improved. The improved tensile properties of the Fe-rich Al-Si alloy is attributed to the combination of Fe-rich reinforced particles and the granular silicon phase provided by the high cooling rate of the melt spinning method.

20.
J Am Chem Soc ; 144(4): 1700-1708, 2022 Feb 02.
Artículo en Inglés | MEDLINE | ID: mdl-35041406

RESUMEN

The benefits of excess PbI2 on perovskite crystal nucleation and growth are countered by the photoinstability of interfacial PbI2 in perovskite solar cells (PSCs). Here we report a simple chemical polishing strategy to rip PbI2 crystals off the perovskite surface to decouple these two opposing effects. The chemical polishing results in a favorable perovskite surface exhibiting enhanced luminescence, prolonged carrier lifetimes, suppressed ion migration, and better energy level alignment. These desired benefits translate into increased photovoltages and fill factors, leading to high-performance mesostructured formamidinium lead iodide-based PSCs with a champion efficiency of 24.50%. As the interfacial ion migration paths and photodegradation triggers, dominated by PbI2 crystals, were eliminated, the hysteresis of the PSCs was suppressed and the device stability under illumination or humidity stress was significantly improved. Moreover, this new surface polishing strategy can be universally applicable to other typical perovskite compositions.

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