Novel Isoalantolactone-Based Derivatives as Potent NLRP3 Inflammasome Inhibitors: Design, Synthesis, and Biological Characterization.

The NLRP3 inflammasome has been recognized as a promising therapeutic target in drug discovery for inflammatory diseases. Our initial research identified a natural sesquiterpene isoalantolactone (IAL) as the active scaffold targeting NLRP3 inflammasome. To improve its activity and metabolic stability, a total of 64 IAL derivatives were designed and synthesized. Among them, compound 49 emerged as the optimal lead, displaying the most potent inhibitory efficacy on nigericin-induced IL-1ß release in THP-1 cells, with an IC50 value of 0.29 µM, approximately 27-fold more potent than that of IAL (IC50: 7.86 µM), and exhibiting higher metabolic stability. Importantly, 49 remarkably improved DSS-induced ulcerative colitis in vivo. Mechanistically, we demonstrated that 49 covalently bound to cysteine 279 in the NACHT domain of NLRP3, thereby inhibiting the assembly and activation of NLRP3 inflammasome. These results provided compelling evidence to further advance the development of more potent NLRP3 inhibitors based on this scaffold.

Unraveling the Molecular Size Effect on Surface Engineering of Perovskite Solar Cells.

Surface engineering in perovskite solar cells, especially for the upper surface of perovskite, is widely studied. However, most of these studies have primarily focused on the interaction between additive functional groups and perovskite point defects, neglecting the influence of other parts of additive molecules. Herein, additives with -NH3 + functional group are introduced at the perovskite surface to suppress surface defects. The chain lengths of these additives vary to conduct a detailed investigation into the impact of molecular size. The results indicate that the propane-1,3-diamine dihydroiodide (PDAI2 ), which possesses the most suitable size, exhibited obvious optimization effects. Whereas the molecules, methylenediamine dihydroiodide (MDAI2 ) and pentane-1,5-diamine dihydroiodide (PentDAI2 ) with unsuitable size, lead to a deterioration in device performance. The PDAI2 -treated devices achieved a certified power conversion efficiency (PCE) of 25.81% and the unencapsulated devices retained over 80% of their initial PCE after 600 h AM1.5 illumination.

Template-Assisted Synthesis of a Large-Area Ordered Perovskite Nanowire Array for a High-Performance Photodetector.

One-dimensional (1D) organic-inorganic hybrid perovskite nanowires (NWs) with well-defined structures possess superior optical and electrical properties for optoelectronic applications. However, most of the perovskite NWs are synthesized in air, which makes the NWs susceptible to water vapor, resulting in large amounts of grain boundaries or surface defects. Here, a template-assisted antisolvent crystallization (TAAC) method is designed to fabricate CH3NH3PbBr3 NWs and arrays. It is found that the as-synthesized NW array has designable shapes, low crystal defects, and ordered alignment, which is attributed to the sequestration of water and oxygen in air by the introduction of acetonitrile vapor. The photodetector based on the NWs exhibits an excellent response to light illumination. Under the illumination of a 532 nm laser with 0.1 µW and a bias of -1 V, the responsivity and detectivity of the device reach 1.55 A/W and 1.21 × 1012 Jones, respectively. The transient absorption spectrum (TAS) shows a distinct ground state bleaching signal only at 527 nm, which corresponds to the absorption peak induced by the interband transition of CH3NH3PbBr3. Narrow absorption peaks (a few nanometers) indicate that the energy-level structures of CH3NH3PbBr3 NWs only have a few impurity-level-induced transitions leading to additional optical loss. This work provides an effective and simple strategy to achieve high-quality CH3NH3PbBr3 NWs, which exhibit potential application in photodetection.

Fabrication of Transferable and Micro/Nanostructured Superhydrophobic Surfaces Using Demolding and iCVD Processes.

Superhydrophobic surfaces possess enormous potential in various applications on account of their versatile functionalities. However, artificial superhydrophobic surfaces with ultralow solid/liquid adhesion often require complicated structure fabrication and surface fluorination processes. Here, we designed a superhydrophobic surface possessed of micro/nanoscale structures by employing facile and low-cost demolding and initiated chemical vapor deposition (iCVD) processes. The achieved micro/nanostructured superhydrophobic surface has a maximum static contact angle of ∼170°, a roll-off angle and contact angle hysteresis below 1°, ultralow solid/liquid adhesion for water droplets, and maintains excellent superhydrophobicity after exposure to strongly corrosive species, like strong acid/base and salt solutions, for 60 h. This reasonability-designed method of creating the superhydrophobic surface could provide valuable guidelines for the manufacture of transferable superhydrophobic surfaces and facilitate potential applications extending from optoelectronic devices to self-cleaning materials, such as solar cells, windows, and electronic displays.

Sublethal effects and reproductive hormesis of emamectin benzoate on Plutella xylostella.

The diamondback moth (DBM), Plutella xylostella L., is an important pest of cruciferous vegetables, and population control mainly depends on chemical pesticides. Emamectin benzoate is a highly effective insecticide used for controlling DBM. However, it is unknown how the sublethal effects of low concentration residues of emamectin benzoate on DBM. So the population development sublethal effects of emamectin benzoate, at LC5, LC10, and LC20 with concentrations of 0.014 mg/L, 0.024 mg/L and 0.047 mg/L, respectively, on adult DBM and their progeny were investigated in this study. The pupal weight, pupal period, female fecundity, and vitellin content of the F0 DBM generation increased significantly compared to the control. And the single female oviposition number of DBM was increased by 20.21% with LC20 treatment. The pupation rate, adult longevity and ovariole length of the treatment groups decreased significantly. The fecundity of DBM in the treatment groups increased, and this increased the population by a presumptive 13.84%. Treatment also led to the shortening of ovarioles and the reduction of egg hatching, and increased pupal weight in the F1 generation. We concluded that the effects of sublethal/low concentration emamectin benzoate on the different life stages of DBM were variable, and the reproductive hormesis on DBM adults were attractive findings.

Synergistic Effects of Bipolar Additives on Grain Boundary-Mediated Charge Transport for Efficient Carbon-Based Inorganic Perovskite Solar Cells.

Carbon-based all-inorganic CsPbIxBr3-x perovskite solar cells offer high stability against heat and humidity and a suitable band gap for tandem and semitransparent photovoltaics. In CsPbIxBr3-x perovskite films, the defects at grain boundaries (GBs) cause charge trapping, reducing the efficiency of the cell. Electronic deactivation of GB has been a conventional strategy to suppress the trapping, but at the cost of charge carrier transport through the boundaries. Here, we turn the GBs into benign charge transport pathways with the aid of bipolar charge transport semiconductors, namely, Ti3C2TX (MXene) and Spiro-OMeTAD, respectively. Thanks to the synergistic effects of both n- and p-type transport media, the charge transport is improved and balanced at the GBs. As a result, the cells achieve an efficiency of 12.7%, the highest among all low-temperature-processed carbon-based inorganic perovskite solar cells. Benign GBs also lead to enhanced light and aging stabilities. Our work demonstrates a proof-of-concept strategy of benign electronic modulation of GBs for solution-processed perovskite solar cells.

Optically Rough and Physically Flat Transparent Conductive Substrates with Strong Far-Field Scattering.

Optically rough and physically flat transparent conductive (OR-PF) substrates facilitate the performance improvement of optoelectronic devices and functional glasses via simultaneously enabling high-quality growth of functional layers and effective light management. This paper studies the effect of the interface morphology of the hole array pattern (HAP) and the pillar array pattern (PAP) on the far-field scattering properties of OR-PF substrates fabricated by spin-coating Al-doped ZnO (AZO) on nanoimprint-patterned glasses for improving the performance of superstrate-type thin-film solar cells. Theoretical calculation based on bidirectional scattering distribution function predicts that HAP with a period of 1.5 µm and a diameter of 1.3 µm [HAP(P1.5D1.3)] and the PAP(P1.0D0.5) interface morphology have a haze ratio in transmission (HT) of around 64% and a scatter angle of larger than 34°. The fabricated AZO/HAP(P1.5D1.3) and AZO/PAP(P1.0D0.5) show a flat surface with a σrms of less than 9 nm, a high visible light transmittance of over 86%, a sheet resistance of about 30 Ω/sq, and strong far-field scattering. In particular, AZO/PAP(P1.0D0.5) possesses an average HT of over 11% at the wavelength range of 600-850 nm and an angular intensity distribution of over 1.5% at an azimuthal angle of around 55°, indicating stronger far-field scattering than the conventional pyramid-textured B-doped ZnO (BZO/F). Compared to the flat substrate, AZO/PAP generates an implied Jsc gain of 16.2% in a CH3NH3PbI3 photoactive layer with a thickness of 300 nm under normal incidence at the wavelength range of 550-800 nm. For 60° incidence, AZO/PAP(P1.0D0.5) enables an implied Jsc gain of 2.3% with respect to BZO/F. As applied to the front electrode of CH3NH3PbI3 thin-film solar cells, compared to BZO/F, AZO/PAP(P1.0D0.5) would enable a gain of up to 16.7 and 11.2% in photoelectric conversion efficiency for the 0 and 60° incidence, respectively.

Quantum Dot Interface-Mediated CsPbIBr2 Film Growth and Passivation for Efficient Carbon-Based Solar Cells.

CsPbIxBry-based all-inorganic perovskite materials are a potential candidate for stable semitransparent and tandem structured photovoltaic devices. However, poor film (morphological and crystalline) quality and interfacial recombination lead consequently to a decline in the photoelectric conversion performance of the applied solar cells. In this work, we incorporated PbS quantum dots (QDs) at the interface of electron transporting layer (ETL) SnO2 and perovskite to modulate the crystallization of CsPbIBr2 and the interfacial charge dynamics in carbon-based solar cells. The as-casted PbS QDs behave as seeds for lattice-matching the epitaxial growth of pinhole-free CsPbIBr2 films. The modified films with reduced defect density exhibit facilitated carrier transfer and suppressed charge recombination at the ETL/perovskite interface, contributing to an enhanced device efficiency from 7.00 to 9.09% and increased reproducibility and ambient stability. This strategic method of QD-assisted lattice-matched epitaxial growth is promising to prepare high-quality perovskite films for efficient perovskite solar cells.

Spatioselective Growth on Homogenous Semiconductor Substrates by Surface State Modulation.

Nanofabrication schemes usually suffer challenges in direct growth on complex nanostructured substrates. We provide a new technology that allows for the convenient, selective growth of complex nanostructures directly on three-dimensional (3D) homogeneous semiconductor substrates. The nature of the selectivity is derived from surface states modulated electrochemical deposition. Metals, metal oxides, and compound semiconductor structures can be prepared with high fidelity over a wide scale range from tens of nanometers to hundreds of microns. The utility of the process for photoelectrochemical applications is demonstrated by selectively decorating the sidewalls and tips of silicon microwires with cuprous oxide and cobalt oxides catalysts, respectively. Our findings indicate a new selective fabrication concept applied for homogeneous 3D semiconductor substrates, which is of high promise in community of photoelectronics, photoelectrochemistry, photonics, microelectronics, etc.

High-Performance Phototransistors Based on MnPSe3 and Its Hybrid Structures with Au Nanoparticles.

Layered metal thiophosphates with a general formula MPX3 (M is a group VIIB or VIII element and X is a chalcogen) have emerged as a novel member in a two-dimensional (2D) family with fascinating physical and chemical properties. Herein, the photoelectric performance of the few-layer MnPSe3 was studied for the first time. The multilayer MnPSe3 shows p-type conductivity and its field-effect transistor delivers an ultralow dark current of about 0.1 pA. The photoswitching ratio reaches ∼103 at a wavelength of 375 nm, superior to that of other thiophosphates. A responsivity and detectivity of 392.78 mA/W and 2.19 × 109 Jones, respectively, have been demonstrated under irradiation of 375 nm laser with a power intensity of 0.1 mW/cm2. In particular, the photocurrent can be remarkably increased up to 30 times by integrating a layer of Au nanoparticle array at the bottom of the MnPSe3 layer. The metal-semiconductor interfacial electric field and the strain-induced flexoelectric polarization field caused by the underlying nanorugged Au nanoparticles are proposed to contribute together to the significant current improvement.

Synthesis and evaluation of new compounds bearing 3-(4-aminopiperidin-1-yl)methyl magnolol scaffold as anticancer agents for the treatment of non-small cell lung cancer via targeting autophagy.

Magnolol and honokiol are the two major active ingredients with similar structure and anticancer activity from traditional Chinese medicine Magnolia officinalis, and honokiol is now in a phase I clinical trial (CTR20170822) for advanced non-small cell lung cancer (NSCLC). In search of potent lead compounds with better activity, our previous study has demonstrated that magnolol derivative C2, 3-(4-aminopiperidin-1-yl)methyl magnolol, has better activity than honokiol. Here, based on the core of 3-(4-aminopiperidin-1-yl)methyl magnolol, we synthesized fifty-one magnolol derivatives. Among them, compound 30 exhibited the most potent antiproliferative activities on H460, HCC827, H1975 cell lines with the IC50 values of 0.63-0.93 µM, which were approximately 10- and 100-fold more potent than those of C2 and magnolol, respectively. Besides, oral administration of 30 and C2 on an H460 xenograft model also demonstrated that 30 has better activity than C2. Mechanism study revealed that 30 induced G0/G1 phase cell cycle arrest, apoptosis and autophagy in cancer cells. Moreover, blocking autophagy by the autophagic inhibitor enhanced the anticancer activity of 30in vitro and in vivo, suggesting autophagy played a cytoprotective role on 30-induced cancer cell death. Taken together, our study implied that compound 30 combined with autophagic inhibitor could be another choice for NSCLC treatment in further investigation.

Facile Synthesis of Defect-Modified Thin-Layered and Porous g-C3N4 with Synergetic Improvement for Photocatalytic H2 Production.

Modulating and optimizing the diverse parameters of photocatalysts synergistically as well as exerting these advantages fully in photocatalytic reactions are crucial for the sufficient utilization of solar energy but still face various challenges. Herein, a novel and facile urea- and KOH-assisted thermal polymerization (UKATP) strategy is first developed for the preparation of defect-modified thin-layered and porous g-C3N4 (DTLP-CN), wherein the thickness of g-C3N4 was dramatically decreased, and cyano groups, nitrogen vacancies, and mesopores were simultaneously introduced into g-C3N4. Importantly, the roles of thickness, pores, and defects can be targetedly modulated and optimized by changing the mass ratio of urea, KOH, and melamine. This can remarkably increase the specific area, improve the light-harvesting capability, and enhance separation efficiency of photoexcited charge carriers, strengthening the mass transfer in g-C3N4. Consequently, the photocatalytic hydrogen evolution efficiency of the DTLP-CN (1.557 mmol h-1 g-1, λ > 420 nm) was significantly improved more than 48.5 times with the highest average apparent quantum yield (AQY) of 18.5% and reached as high as 0.82% at 500 nm. This work provides an effective strategy for synergistically regulating the properties of g-C3N4, and opens a new horizon to design g-C3N4-based catalysts for highly efficient solar-energy conversion.

Realization of Moisture-Resistive Perovskite Films for Highly Efficient Solar Cells Using Molecule Incorporation.

The development of highly crystalline perovskite films with large crystal grains and few surface defects is attractive to obtain high-performance perovskite solar cells (PSCs) with good device stability. Herein, we simultaneously improve the power conversion efficiency (PCE) and humid stability of the CH3NH3PbI3 (CH3NH3 = MA) device by incorporating small organic molecule IT-4F into the perovskite film and using a buffer layer of PFN-Br. The presence of IT-4F in the perovskite film can successfully improve crystallinity and enhance the grain size, leading to reduced trap states and longer lifetime of the charge carrier, and make the perovskite film hydrophobic. Meanwhile, as a buffer layer, PFN-Br can accelerate the separation of excitons and promote the transfer process of electrons from the active layer to the cathode. As a consequence, the PSCs exhibit a remarkably improved PCE of 20.55% with reduced device hysteresis. Moreover, the moisture-resistive film-based devices retain about 80% of their initial efficiency after 30 days of storage in relative humidity of 10-30% without encapsulation.

Nonfullerene Ternary Organic Solar Cell with Effective Charge Transfer between Two Acceptors.

High power conversion efficiency can be realized by using a ternary bulk heterojunction with complementary absorption spectra in organic solar cells. However, as the development of nonfullerene acceptors with a broad absorption spectrum makes the absorption efficiency of the photovoltaic devices close to optimal, such a strategy needs modifying. In particular, charge transfer between the two acceptors is necessary to be considered. Herein, we purposely design a ternary system based on PTB7-Th:COi8DFIC:ITIC-4F. Though the presence of ITIC-4F in PTB7-Th:COi8DFIC could not broaden the absorption spectrum obviously, the formed cascade-energy-level alignment is beneficial for promoting and balancing exciton separation and charge transport between the donor and two acceptors and even between the acceptors. Insights into the charge transport route in the completed system are provided via using the techniques including photoluminescence spectroscopy and pump-probe photoconductivity spectroscopy. This work provides a new idea for designing highly efficient ternary organic solar cells.

Optimizing the component ratio of PEDOT:PSS by water rinse for high efficiency organic solar cells over 16.7.

For the state-of-the-art organic solar cells (OSCs), PEDOT:PSS is the most popularly used hole transport material for the conventional structure. However, it still suffers from several disadvantages, such as low conductivity and harm to ITO due to the acidic PSS. Herein, a simple method is introduced to enhance the conductivity and remove the additional PSS by water rinsing the PEDOT:PSS films. The photovoltaic devices based on the water rinsed PEDOT:PSS present a dramatic improvement in efficiency from 15.98% to 16.75% in comparison to that of the untreated counterparts. Systematic characterization and analysis reveal that although part of the PEDOT:PSS is washed away, it still leaves a smoother film and the ratio of PEDOT to PSS is higher than before in the remaining films. It can greatly improve the conductivity and reduce the damage to substrates. This study demonstrates that finely modifying the charge transport materials to improve conductivity and reduce defeats has great potential for boosting the efficiency of OSCs.

A wrinkled structure with broadband and omnidirectional light-trapping abilities for improving the performance of organic solar cells with low defect density.

Fabricating thin film solar cells on the light-trapping structures is an effective way to improve the absorption of the active layer. Here, we report a non-fullerene organic solar cell based on a PBDB-T:ITIC active layer, a wrinkled metal rear electrode, and a MoO3/Ag/ZnS front transparent electrode. Optical characterization shows that the wrinkled metal structure can remarkably increase the absorption of the active layer in a broadband range. The resulting device shows a power conversion efficiency of 8.2%, which increases by 4.6% compared to that of the flat counterpart. Apart from higher absorption, the improved performance can also be ascribed to the efficient charge transport and collection in the device due to the lower defect density, larger interfacial area, and smaller active layer thickness. A device with a power conversion efficiency of 10.19% based on the flat ITO/glass substrate is also achieved. Accordingly, a power conversion efficiency of about 10.66% is predicted under the condition where the wrinkled rear electrode and the ITO front electrode are employed. In addition, the power conversion efficiency of the wrinkled device could increase by about 50.48% compared to that of the flat device under an incident angle of 60 °C, illustrating that a better omnidirectional ability is achieved.

Multiple-engineering controlled growth of tunable-bandgap perovskite nanowires for high performance photodetectors.

Controllable growth of perovskite nanowires is very important for various applications in optical and electrical devices. Although significant progress has been achieved in the solution method, a deep understanding of the mechanics of growing perovskite nanowires is still lacking. Herein, we developed an electrochemical method for growing the perovskite nanowires and studied the growth processes systematically. The initial nucleation and crystal growth could be controlled by simply varying the additive solvents, thus leading to two stable size ratio distributions of the perovskite nanowires. Further, with compositional engineering, the bandgap of the perovskites could be tuned from 1.59 eV to 3.04 eV. All the as-grown perovskite nanowires displayed a unique structure with high crystallization quality, contributing to a very high responsivity of 2.1 A W-1 and a large on/off ratio of 5 × 103 for the photodetectors based on the CH3NH3PbBr3 nanowires. All of these findings demonstrate that the optimized solution method offers a new approach to synthesize perovskite nanowires for applications in photoelectric devices.

Insights into Charge Separation and Transport in Ternary Polymer Solar Cells.

Although ternary polymer solar cells have more potential in realizing a high power conversion efficiency than the binary counterparts, the mechanism of exciton separation and charge transport in such complicated ternary systems is far from being understood. Herein, we focus on this issue and give a clear view on the detailed roles of the ternary components contributing to the device performance, through utilizing the technique of pump-probe photoconductivity spectroscopy combined with transient photoluminescence spectroscopy, for the first time for ternary polymer solar cells. The ternary photovoltaic devices are based on PBDB-T:ITIC:PC71BM and present a dramatic improvement in efficiency in comparison to that of the binary counterparts. Systematic investigation reveals that the excitons generated in ITIC could be separated at the interface of PBDB-T:ITIC rather than ITIC:PC71BM with holes injecting to PBDB-T. These holes together with those generated in PBDB-T contribute to the photocurrent of the devices. The aggregation of holes in PBDB-T would also weaken the exciton generation herein, and the electron injection to PC71BM and ITIC would also be influenced. The key role of PC71BM in the ternary devices is accepting the electrons from PBDB-T and transporting them to the cathode with a higher rate than that of ITIC. Thus, this article is of importance in constructing high-efficiency ternary polymer solar cells.

Insights into the Influence of Work Functions of Cathodes on Efficiencies of Perovskite Solar Cells.

Though various efforts on modification of electrodes are still undertaken to improve the efficiency of perovskite solar cells, attributing to the large scope of these methods, it is of significance to unveil the working principle systematically. Herein, inverted perovskite solar cells based on indium tin oxide (ITO)/poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS)/CH3 NH3 PbI3 /phenyl-C61-butyric acid methyl ester (PC61 BM)/buffer metal/Al are constructed. Through the choice of different buffer metals to tune work function of the cathode, the contact nature of the active layer with the cathode could be manipulated well. In comparison with the device using Au/Al as the electrode that shows an unfavorable band bending for conducting the excited electrons to the cathode, the one with Ca/Al presents a dramatically improved efficiency over 17.1%, ascribed to the favorable band bending at the interface of the cathode with the active layer. Details for tuning the band bending and the corresponding charge transfer mechanism are given in a systematic manner. Thus, a general guideline for constructing perovskite photovoltaic devices efficiently is provided.