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Objective: To evaluate the protective effects of gentiopicroside (GPS) against reactive oxygen species (ROS)-induced NOD-like receptor family, pyrin domain containing 3 (NLRP3) inflammasome activation in endothelial cells, aiming to reduce atherosclerosis., Methods: Eight-week-old male ApoE-deficient mice were randomly divided into 2 groups (n=10 per group): the vehicle group and the GPS treatment group. Both groups were fed a high-fat diet for 16 weeks. GPS (40 mg/kg per day) was administered by oral gavage to the GPS group, while the vehicle group received an equivalent volume of the vehicle solution. At the end of the treatment, blood and aortic tissues were collected for assessments of atherosclerosis, lipid profiles, oxidative stress, and molecular expressions related to NLRP3 inflammasome activation, ROS production, and apoptosis. Additionally, in vitro experiments on human aortic endothelial cells treated with oxidized low-density lipoprotein (ox-LDL) were conducted to evaluate the effects of GPS on NLRP3 inflammasome activation, pyroptosis, apoptosis, and ROS production, specifically examining the role of the sirtuin 1 (SIRT1)/nuclear factor erythroid 2-related factor 2 (Nrf2) pathway. SIRT1 and Nrf2 inhibitors were used to confirm the pathway's role., Results: GPS treatment significantly reduced atherosclerotic lesions in the en face aorta (P<0.01), as well as in the thoracic and abdominal aortic regions, and markedly decreased sinus lesions within the aortic root (P<0.05 or P<0.01). Additionally, GPS reduced oxidative stress markers and proinflammatory cytokines, including interleukin (IL)-1 β and IL-18, in lesion areas (P<0.05, P<0.01). In vitro, GPS inhibited ox-LDL-induced NLRP3 activation, as evidenced by reduced NLRP3 (P<0.01), apoptosis-associated speck-like protein containing a CARD, cleaved-caspase-1, and cleaved-gasdermin D expressions (all P<0.01). GPS also decreased ROS production, apoptosis, and pyroptosis, with the beneficial effects being significantly reversed by SIRT1 or Nrf2 inhibitors., Conclusion: GPS exerts an antiatherogenic effect by inhibiting ROS-dependent NLRP3 inflammasome activation via the SIRT1/Nrf2 pathway., Competing Interests: Conflicts of Interest. The authors declare no conflict of interest., (© 2024. The Chinese Journal of Integrated Traditional and Western Medicine Press and Springer-Verlag GmbH Germany, part of Springer Nature.)

Reports on highly efficient silver(I)-based thermally activated delayed fluorescence (TADF) materials are scarce due to challenges in molecular design, although these materials show great potential for photoluminescent and electroluminescent applications. Herein, a silver(I)-iodine cluster, namely Ag 2 I 2 (dppb-Ac) 2 , is synthesized by employing a donor-acceptor (D-A) type bisphosphine ligand. Due to the introduction of electron-donating iodine ligands, Ag 2 I 2 (dppb-Ac) 2 exhibits an emissive singlet state characterized by (metal + iodine)-to-ligand charge transfer and intra-ligand charge transfer transitions, as well as a small singlet-triplet energy gap. Additionally, its non-planar, highly distorted D-A structure efficiently separates adjacent molecules in aggregated state. As a result, Ag 2 I 2 (dppb-Ac) 2 exhibits efficient TADF and suppressed luminescence concentration quenching in thin films. For instance, the 10 wt%-doped PMMA film and neat film of Ag 2 I 2 (dppb-Ac) 2 display bright bluish-green and green emission, peaking at 506 and 532 nm, with photoluminescence quantum yields (PLQYs) of 70% and 52%, and lifetimes of 18.9 and 7.9 μs, respectively. The high PLQYs and efficiently suppressed emission concentration quenching of Ag 2 I 2 (dppb-Ac) 2 in films are outstanding among reported Ag(I)-based TADF emitters.

Due to the presence of H 2 O within the solvated sheath of [Zn(H 2 O) 6 ] 2+ as well as reactive free water in the electrolyte bulk phase, the extended cycling of aqueous zinc-ion batteries (AZIBs) is significantly affected by detrimental side reactions and the growth of Zn dendrites. This study significantly enhances the long-term cycling stability of AZIBs by introducing a small amount of disodium malate (DM) into a 2 m ZnSO 4 electrolyte solution. DM involvement in the solvation sheath of Zn 2+ reduces the desolvation energy of Zn 2+ , thereby mitigating the corrosion and hydrogen evolution reaction (HER) of the negative electrode surface by [Zn(H 2 O) 6 ] 2+ ions. Additionally, DM adsorption on the zinc surface retards the reduction kinetics of Zn 2+ at anode, promoting uniform distribution and predominant deposition on the flat (002) crystal plane, thus reducing dendrite formation. The assembled Zn||Zn symmetric cell exhibits stable cycling for over 500 h at 10 mA cm -2 and 5 mAh cm -2 . The Zn||VO 2 full cells with DM additive exhibits an ultralong cycling lifespan without capacity loss., (© 2024 Wiley‐VCH GmbH.)

Vision Transformers have been the most popular network architecture in visual recognition recently due to the strong ability of encode global information. However, its high computational cost when processing high-resolution images limits the applications in downstream tasks. In this paper, we take a deep look at the internal structure of self-attention and present a simple Transformer style convolutional neural network (ConvNet) for visual recognition. By comparing the design principles of the recent ConvNets and Vision Transformers, we propose to simplify the self-attention by leveraging a convolutional modulation operation. We show that such a simple approach can better take advantage of the large kernels ( ≥ 7×7) nested in convolutional layers and we observe a consistent performance improvement when gradually increasing the kernel size from 5×5 to 21×21. We build a family of hierarchical ConvNets using the proposed convolutional modulation, termed Conv2Former. Our network is simple and easy to follow. Experiments show that our Conv2Former outperforms existent popular ConvNets and vision Transformers, like Swin Transformer and ConvNeXt in all ImageNet classification, COCO object detection and ADE20 k semantic segmentation.

Fast and efficient exciton utilization is a crucial solution and highly desirable for achieving high-performance blue organic light-emitting diodes (OLEDs). However, the rate and efficiency of exciton utilization in traditional OLEDs, which employ fully closed-shell materials as emitters, are inevitably limited by spin statistical limitations and transition prohibition. Herein, a new sensitization strategy, namely doublet-sensitized fluorescence (DSF), is proposed to realize high-performance deep-blue electroluminescence. In the DSF-OLED, a doublet-emitting cerium(III) complex, Ce-2, is utilized as sensitizer for multi-resonance thermally activated delayed fluorescence emitter ν-DABNA. Experimental results reveal that holes and electrons predominantly recombine on Ce-2 to form doublet excitons, which subsequently transfer energy to the singlet state of ν-DABNA via exceptionally fast (over 10 8  s -1 ) and efficient (≈100%) Förster resonance energy transfer for deep-blue emission. Due to the circumvention of spin-flip in the DSF mechanism, near-unit exciton utilization efficiency and remarkably short exciton residence time of 1.36 µs are achieved in the proof-of-concept deep-blue DSF-OLED, which achieves a Commission Internationale de l'Eclairage coordinate of (0.13, 0.14), a high external quantum efficiency of 30.0%, and small efficiency roll-off of 14.7% at a luminance of 1000 cd m -2 . The DSF device exhibits significantly improved operational stability compared with unsensitized reference device., (© 2024 Wiley‐VCH GmbH.)

Carbazole-based COFs were synthesized and applied as the sulfur-host in cathode materials for lithium-sulfur batteries (LSBs), which effectively mitigate the shuttle effect of lithium polysulfides. A high initial capacity of 1232 mAh g -1 at 0.1C is achieved, while also showing excellent capacity retention and stability in cyclic experiments. This work highlights the potential application of carbazole-based COFs for LSBs.

Designing all-inorganic double perovskites through element mixing is a promising strategy to enhance their optoelectronic performance and structural stability. The complex interplay between multilevel structures and optoelectronic properties in element-mixed double perovskites necessitates further in-depth theoretical exploration. In this study, we employ screening strategies and multiscale simulations combining first-principles methods and device-scale continuum models to identify two novel element-mixed compounds, Rb 2 AgInCl 3 I 3 and Cs 2 AgInCl 3 I 3 , as promising candidates for photovoltaic applications. These compounds exhibit favorable structural factors and suitable direct band gaps. Theoretical investigations using first-principles methods with the HSE06 functional reveal direct band gaps of 0.98 and 1.26 eV for Rb 2 AgInCl 3 I 3 and Cs 2 AgInCl 3 I 3 , respectively, with corresponding optical absorption coefficients exceeding 10 5 cm -1 in the visible light range. Cs 2 AgInCl 3 I 3 features high charge mobilities of approximately 20 cm 2 ·V -1 ·s -1 and a notable single-junction spectroscopic limited maximum efficiency (SLME) of 25.54%. Further analysis using the device-scale continuum model simulated the nonradiative recombination effects on power conversion efficiency, integrating quantum-mechanically calculated optoelectronic properties. These theoretical investigations, which bridge composition engineering with multiscale simulations, provide valuable insights into screening novel, lead-free, halogen - mixed double metal perovskite optoelectronic devices, highlighting their potential for high-performance solar energy applications.

Objective: To investigate the long-term therapeutic effects and safety of renal denervation (RDN) on hypertensive patients with different cardiovascular risks, as well as its impact on adverse events, cardiovascular death and all-cause mortality. Methods: This was a single-center, single-arm, real-world retrospective study. Patients with refractory hypertension who underwent RDN at Tianjin First Central Hospital from July 6, 2011 to December 23, 2015 were enrolled and divided into either a high or intermediate-low risk group based on baseline cardiovascular risk. The treatment responsiveness of hypertensive patients with different cardiovascular stratification to RDN was assessed by comparing the results of office blood pressure, home blood pressure, and 24-h ambulatory blood pressure monitoring at 1, 5, and 11 years after RDN. Long-term safety of RDN was assessed by creatinine, and estimated glomerular filtration rate (eGFR) at 1 and 11 years after RDN. In addition, the total defined daily dose (DDD) of antihypertensive medications and the incidence of long-term adverse events, cardiovascular deaths, and all-cause deaths after RDN were followed up 11 years after RDN in person or by telephone. Results: A total of 62 patients with refractory hypertension, aged (50.2±15.0) years, of whom 35 (56.5%) were male, were included. There were 35 cases in high-risk group and 27 cases in low and medium risk group. The decrease in clinic systolic blood pressure (high risk vs. low-medium risk: (-38.0±15.1) mmHg vs. (-25.0±16.6) mmHg(1 mmHg=0.133kPa), P =0.002), home self-measured systolic blood pressure ((-28.4±12.7) mmHg vs. (-19.7±13.1) mmHg, P =0.011) and clinic systolic blood pressure 11 years after RDN ((-43.0±18.4) mmHg vs. (-27.8±17.9) mmHg, P =0.003) in the high-risk group was significantly higher than that in the low-medium risk group. The differences in heart rate and the decrease in total DDD number of antihypertensive drugs between the two groups were not statistically significant (all P >0.05). Creatinine and eGFR levels in the two groups at 1 and 11 years after RDN were not statistically significant when compared with the baseline values (all P >0.05). The cumulative cardiovascular mortality rate was 1.6% (1/62) and 8.1% (5/62), and the cumulative all-cause mortality rate was 3.2% (2/62) and 11.3% (7/62) at 5 and 11 years after RDN, respectively. The differences in the incidence rate of adverse events, cardiovascular mortality, and all-cause mortality rate between the two groups were not statistically significant (all P >0.05). Conclusions: RDN has long-term antihypertensive effect and good safety. Hypertensive patients who belong to the high-risk stratification of cardiovascular risk may respond better to RDN treatment.

Simultaneously achieving a high photoluminescence quantum yield (PLQY), ultrashort exciton lifetime, and suppressed concentration quenching in thermally activated delayed fluorescence (TADF) materials is desirable yet challenging. Here, a novel acceptor-donor-acceptor type TADF emitter, namely, 2BO-sQA, wherein two oxygen-bridged triarylboron (BO) acceptors are arranged with cofacial alignment and positioned nearly orthogonal to the rigid dispirofluorene-quinolinoacridine (sQA) donor is reported. This molecular design enables the compound to achieve highly efficient (PLQYs up to 99%) and short-lived (nanosecond-scale) blue TADF with effectively suppressed concentration quenching in films. Consequently, the doped organic light-emitting diodes (OLEDs) base on 2BO-sQA achieve exceptional electroluminescence performance across a broad range of doping concentrations, maintaining maximum external quantum efficiencies (EQEs) at over 30% for doping concentrations ranging from 10 to 70 wt%. Remarkably, the nondoped blue OLED achieves a record-high maximum EQE of 26.6% with a small efficiency roll-off of 14.0% at 1000 candelas per square meter. By using 2BO-sQA as the sensitizer for the multiresonance TADF emitter ν-DABNA, TADF-sensitized fluorescence OLEDs achieve high-efficiency deep-blue emission. These results demonstrate the feasibility of this molecular design in developing TADF emitters with high efficiency, ultrashort exciton lifetime, and minimal concentration quenching., (© 2024 Wiley‐VCH GmbH.)

This study details the rational design and synthesis of Cu 2 ZnSnS 4 (CZTS)-doped anatase (A) heterostructures, utilizing earth-abundant elements to enhance the efficiency of solar-driven water splitting. A one-step hydrothermal method was employed to fabricate a series of CZTS-A heterojunctions. As the concentration of titanium dioxide (TiO 2 ) varied, the morphology of CZTS shifted from floral patterns to sheet-like structures. The resulting CZTS-A heterostructures underwent comprehensive characterization through photoelectrochemical response assessments, optical measurements, and electrochemical impedance spectroscopy analyses. Detailed photoelectrochemical (PEC) investigations demonstrated notable enhancements in photocurrent density and incident photon-to-electron conversion efficiency (IPCE). Compared to pure anatase electrodes, the optimized CZTS-A heterostructures exhibited a seven-fold increase in photocurrent density and reached a hydrogen production efficiency of 1.1%. Additionally, the maximum H 2 production rate from these heterostructures was 11-times greater than that of pure anatase and 250-times higher than the original CZTS after 2 h of irradiation. These results underscore the enhanced PEC performance of CZTS-A heterostructures, highlighting their potential as highly efficient materials for solar water splitting. Integrating Cu 2 ZnSnS 4 nanoparticles (NPs) within TiO 2 (anatase) heterostructures implied new avenues for developing earth-abundant and cost-effective photocatalytic systems for renewable energy applications.

Carbon Quantum dots (CQDs) are widely studied because of their good optical and electronic characteristics and because they can easily generate photocarriers. Nitrogen-doped CQDs (NCQDs) may exhibit improved hydrophilic, optical, and electron-transfer properties, which are conducive to photocatalytic hydrogen evolution. In this paper, NCQD-modified ZnS catalysts were successfully prepared. Under the irradiation of the full spectrum, the H 2 evolution rate of the optimal catalyst 0.25 wt % NCQDs/ZnS achieves 5.70 mmol g -1 h -1 , which is 11.88, 43.84, and 5.14 times the values of ZnS (0.48 mmol g -1 h -1 ), NCQDs (0.13 mmol g -1 h -1 ), and CQDs/ZnS (1.11 mmol g -1 h -1 ), respectively. Furthermore, it shows good stability, indicating that the modification of NCQDs prevents the photocorrosion and oxidation of ZnS. The enhanced performance is due to NCQD loading, which promotes the separation of photogenerated carriers, optimizes the structures, and increases the specific surface area. This work highlights the fact that NCQD-modified ZnS may afford a new strategy to synthesize ZnS-based photocatalysts with enhanced H 2 production performance.

Thermally activated delayed fluorescence (TADF) emitters based on the triptycene skeleton demonstrate exceptional performance, superior stability, and low efficiency roll-off. Understanding the interplay between the luminescent properties of triptycene-TADF molecules and their assembly environments, along with their excited-state characteristics, necessitates a comprehensive theoretical exploration. Herein, we predict the photophysical properties of triptycene-TADF molecules in a thin film environment using the quantum mechanics/molecular mechanics method and quantify their substantial dependency on the heavy atom effects and reorganization energies using the Marcus-Levich theory. Our calculated photophysical properties for two recently reported molecules closely align with experimental values. We design three novel triptycene-TADF molecules by incorporating chalcogen elements (O, S, and Se) to modify the acceptor units. These newly designed molecules exhibit reduced reorganization energies and enhanced reverse intersystem crossing (RISC) rates. The heavy atom effect amplifies spin-orbit coupling, thereby facilitating the RISC process, particularly at a remarkably high rate of ∼10 9 s -1 .

Nitroxinil (NIT) is a widely using veterinary medicine to protect cattle and sheep yet may threaten human health when ingested through food chain. Developing fluorescent analytical methods in ratiometric manners was essential for the on-site detection and in-situ monitoring of NIT but still challenging. Here, we improved the indicator-displacement assay (IDA)-based method and designed the first ratiometric fluorescent probe for NIT by using an albumin host and an Aggregation-induced emission (AIE) guest. This probe exhibited fast response (10 s), high sensitivity (limit of detection: 4.6 ppb), good selectivity (over twelve medicines) and eye-discriminable fluorescent color change (green-red) upon responding to NIT. Based on these properties, this probe enabled quantitative determination of NIT in real food samples, on-site analysis via a paper-based test strip, and fluorescence imaging of NIT in living cells., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023. Published by Elsevier Ltd.)

ZnIn 2 S 4 /ZnO heterostructures have been achieved by a simple in-situ growth solvothermal method. Under full spectrum irradiation, the optimal photocatalyst 2ZnIn 2 S 4 /ZnO exhibits H 2 evolution rate of 13,638 (water/ethanol = 1:1) and 3036 (water) μmol·g -1 h -1 , which is respectively 4 and 5 times higher than that of pure ZnIn 2 S 4 . In situ illumination X-ray photoelectron spectroscopy (ISI-XPS) analysis and density functional theory (DFT) calculations show that the electrons of ZnIn 2 S 4 are removed to ZnO through hybridization and form an internal electric field between ZnIn 2 S 4 and ZnO. The optical properties of the catalyst and the effect of internal electric field (IEF) can increase photo-generated electrons (e - )-holes (h + ) transport rate and enhance light collection, resulting in profitable photocatalytic properties. The photoelectrochemical and EPR results show that a stepped (S-scheme) heterojunction is formed in the ZnIn 2 S 4 /ZnO redox center, which greatly promotes separation of e - -h + pairs and efficient H 2 evolution. This research offers an effective method for constructing an efficient S-Scheme photocatalytic system for H 2 evolution., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)

The development of orange-red/red thermally activated delayed fluorescence (TADF) materials with both high emission efficiencies and short lifetimes is highly desirable for electroluminescence (EL) applications, but remains a formidable challenge owing to the strict molecular design principles. Herein, two new orange-red/red TADF emitters, namely AC-PCNCF3 and TAC-PCNCF3, composed of pyridine-3,5-dicarbonitrile-derived electron-acceptor (PCNCF3) and acridine electron-donors (AC/TAC) are developed. These emitters in doped films exhibit excellent photophysical properties, including high photoluminescence quantum yields of up to 0.91, tiny singlet-triplet energy gaps of 0.01 eV, and ultrashort TADF lifetimes of less than 1 µs. The TADF-organic light-emitting diodes employing the AC-PCNCF3 as emitter achieve orange-red and red EL with high external quantum efficiencies of up to 25.0% and nearly 20% at doping concentrations of 5 and 40 wt%, respectively, both accompanied by well-suppressed efficiency roll-offs. This work provides an efficient molecular design strategy for developing high-performance red TADF materials., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

A novel binuclear Cu(I) halide complex, Cu 2 I 2 (DPPCz) 2 , which emits efficient thermally activated delayed fluorescence (TADF), is reported. The crystal of this complex spontaneously undergoes ligand rotation and coordination-configuration transformation, converting to its isomer without any external stimulation.

The development of highly efficient orange and red thermally activated delayed fluorescence (TADF) materials for constructing full-color and white organic light-emitting diodes (OLEDs) remains insufficient because of the formidable challenges in molecular design, such as the severe radiationless decay and the intrinsic trade-off between the efficiencies of radiative decay and reverse intersystem crossing (RISC). Herein, we design two high-efficiency orange and orange-red TADF molecules by constructing intermolecular noncovalent interactions. This strategy could not only ensure high emission efficiency via suppression of the nonradiative relaxation and enhancement of the radiative transition but also create intermediate triplet excited states to ensure the RISC process. Both emitters exhibit typical TADF characteristics, with a fast radiative rate and a low nonradiative rate. Photoluminescence quantum yields (PLQYs) of the orange (TPA-PT) and orange-red (DMAC-PT) materials reach up to 94 and 87%, respectively. Benefiting from the excellent photophysical properties and stability, OLEDs based on these TADF emitters realize orange to orange-red electroluminescence with high external quantum efficiencies reaching 26.2%. The current study demonstrates that the introduction of intermolecular noncovalent interactions is a feasible strategy for designing highly efficient orange to red TADF materials.

The development of efficient deep-blue emitters with thermally activated delayed fluorescence (TADF) properties is a highly significant but challenging task in the field of organic light-emitting diode (OLED) applications. Herein, we report the design and synthesis of two new 4,10-dimethyl-6H,12H-5,11-methanodibenzo[ b,f ][1,5]diazocine ( TB )-derived TADF emitters, TB-BP-DMAC and TB-DMAC , which feature distinct benzophenone ( BP )-derived acceptors but share the same dimethylacridin ( DMAC ) donors. Our comparative study reveals that the amide acceptor in TB-DMAC exhibits a significantly weaker electron-withdrawing ability in comparison to that of the typical benzophenone acceptor employed in TB-BP-DMAC . This disparity not only causes a noticeable blue shift in the emission from green to deep blue but also enhances the emission efficiency and the reverse intersystem crossing (RISC) process. As a result, TB-DMAC emits efficient deep-blue delay fluorescence with a photoluminescence quantum yield (PLQY) of 50.4% and a short lifetime of 2.28 μs in doped film. The doped and non-doped OLEDs based on TB-DMAC display efficient deep-blue electroluminescence with spectral peaks at 449 and 453 nm and maximum external quantum efficiencies (EQEs) of 6.1% and 5.7%, respectively. These findings indicate that substituted amide acceptors are a viable option for the design of high-performance deep-blue TADF materials.

Thermally activated delayed fluorescence (TADF) materials with both high photoluminescence quantum yield (PLQY) and fast reverse intersystem crossing (RISC) are strongly desired to realize efficient and stable organic light-emitting diodes (OLEDs). Control of excited-state dynamics via molecular design plays a central role in optimizing the PLQY and RISC rate of TADF materials but remains challenging. Here, 3 TADF emitters possessing similar molecular structures, similar high PLQYs (89.5% to 96.3%), and approximate energy levels of the lowest excited singlet states (S 1 ), but significantly different spin-flipping RISC rates (0.03 × 10 6 s -1 vs. 2.26 × 10 6 s -1 ) and exciton lifetime (297.1 to 332.8 μs vs. 6.0 μs) were systematically synthesized to deeply investigate the feasibility of spin-flip between charge-transfer excited states ( 3 CT- 1 CT) transition. Experimental and theoretical studies reveal that the small singlet-triplet energy gap together with low RISC reorganization energy between the 3 CT and 1 CT states could provide an efficient RISC through fast spin-flip 3 CT- 1 CT transition, without the participation of an intermediate locally excited state, which has previously been recognized as being necessary for realizing fast RISC. Finally, the OLED based on the champion TADF emitter achieves a maximum external quantum efficiency of 27.1%, a tiny efficiency roll-off of 4.1% at 1,000 cd/m 2 , and a high luminance of 28,150 cd/m 2 , which are markedly superior to those of the OLEDs employing the other 2 TADF emitters., (Copyright © 2023 Donghai Zhang et al.)

Peroxyoxalate chemiluminescence (PO-CL) is one of the most popular cold light sources, yet the drawback of aggregation-caused quenching limits their use. Here, we report a new kind of efficient bifunctional emitter derived from salicylic acid, which not only exhibits typical aggregation-induced emission (AIE) character but also has the ability to catalyze the CL process under basic conditions based on base sensitivity. By taking advantage of these unique features, we successfully confine the CL process on the surface of solid bases and provide a high-contrast visualization of CL emission. This method allows most of the common basic salts like sodium carbonate to be invisible encryption information ink and PO-CL solution to be a decryption tool to visualize the hidden information. The current study opens up an appealing way for the development of multifunction CL emitters for information encryption and decryption applications.

Nitrite (NO 2 - ) is one of the common salts in aqueous aerosols, and its photolytic products, nitric oxide (NO) and hydroxyl radical (OH), have potential for use in the oxidation of organic matter, such as dissolved formaldehyde, methanediol (CH 2 (OH) 2 ), which is regarded as the precursor of atmospheric formic acid. In this work, the simulation of UVA irradiation in an aqueous mixture of NaNO 2 /CH 2 (OH) 2 was carried out via continuous exposure with a 365 nm LED lamp, and the reaction evolutions were probed by in situ and real-time infrared and Raman spectroscopy, which provided multiplexity in the identification of the relevant species and the corresponding reaction evolution. Although performing infrared absorption measurements in aqueous solution seemed impracticable due to the strong interference of water, the multiplexity of the vibrational bands of parents and products in the non-interfered infrared regimes and the conjunction with Raman spectroscopy still make it possible to perform in situ and real-time characterization of the photolytic reaction in the aqueous phase, supplementary to chromatographic approaches. During the 365 nm irradiation, NO 2 - and CH 2 (OH) 2 gradually decreased, concomitant with the formation of nitrous oxide (N 2 O) and formate (HCOO - ) in the early period and carbonate (CO 3 2- ) in the late period, as revealed by the vibrational spectra. The losses or the gains of the aforementioned species increased with increases in the concentration of CH 2 (OH) 2 and the irradiation flux of the 365 nm UV light. The ionic product HCOO - was also confirmed by ion chromatography, but oxalate (C 2 O 4 2- ) was absent in the vibrational spectra and ion chromatogram. The reaction mechanism is reasonably proposed on the basis of the evolutions of the aforementioned species and the predicted thermodynamic favorableness.

Developing novel lead-free perovskite materials with suitable bandgaps and superior thermal stability is crucial to boost their applications in next-generation photovoltaic technologies. High throughput screening combined with the first principles method can accurately and effectively screen out promising perovskites. Herein, we select two lead-free all-inorganic halide double perovskite materials Cs 2 KMI 6 (M = Ga, In) from 1026 compounds with the criteria including appropriate structure factors, positive decomposition energies, and suitable direct bandgaps. We investigated the thermal and mechanical stability, geometric and electronic structures, photoelectric properties, and defect formation energies for both perovskites Cs 2 KMI 6 (M = Ga, In). They can exhibit excellent structural formability and stability through the analysis of structure factors, elastic constants, and stable chemical potential regions. In addition, we investigate the defect effects of Cs 2 KMI 6 (M = Ga, In) on the photovoltaic performance by evaluating the defect formation energies and transition energy levels. Based on the HSE06 functional, we calculated the energy band structures of these two compounds and demonstrate the direct bandgaps of 1.69 eV (HSE06) and 2.16 eV (HSE06) for Cs 2 KGaI 6 and Cs 2 KInI 6 , respectively. Moreover, we predicted excellent spectroscopic limited maximum efficiencies (SLMEs) of these two perovskites with high light absorption coefficients (around 10 5 cm -1 ), for instance, the SLME of Cs 2 KGaI 6 can reach as high as 28.39%.

Renal outer medullary potassium (ROMK) channel is an important K + excretion channel in the body, and K + secreted by the ROMK channels is most or all source of urinary potassium. Previous studies focused on the ROMK channels of thick ascending limb (TAL) and collecting duct (CD), while there were few studies on the involvement of ROMK channels of the late distal convoluted tubule (DCT2) in K + excretion. The purpose of the present study was mainly to record the ROMK channels current in renal DCT2 and observe the effect of high potassium diet on the ROMK channels by using single channel and whole-cell patch-clamp techniques. The results showed that a small conductance channel current with a conductance of 39 pS could be recorded in the apical membrane of renal DCT2, and it could be blocked by Tertiapin-Q (TPNQ), a ROMK channel inhibitor. The high potassium diet significantly increased the probability of ROMK channel current occurrence in the apical membrane of renal DCT2, and enhanced the activity of ROMK channel, compared to normal potassium diet (P < 0.01). Western blot results also demonstrated that the high potassium diet significantly up-regulated the protein expression levels of ROMK channels and epithelial sodium channel (ENaC), and down-regulated the protein expression level of Na + -Cl - cotransporter (NCC). Moreover, the high potassium diet significantly increased urinary potassium excretion. These results suggest that the high potassium diet may activate the ROMK channels in the apical membrane of renal DCT2 and increase the urinary potassium excretion by up-regulating the expression of renal ROMK channels.

Cerium element with a unique electric structure can be used to modify semiconductor photocatalysts to enhance their photocatalytic performances. In this work, Ce-doped TiO 2 (Ce/TiO 2 ) was successfully achieved using the sol-gel method. The structural characterization methods confirm that Ce was doped in the lattice of anatase TiO 2 , which led to a smaller grain size. The performance test results show that the Ce doped in anatase TiO 2 significantly enhances the charge transport efficiency and broadens the light absorption range, resulting in higher photocatalytic performance. The Ce/TiO 2 exhibited a photocurrent density of 10.9 μA/cm 2 at 1.0 V vs. Ag/AgCl, 2.5 times higher than that of pure TiO 2 (4.3 μA/cm 2 ) under AM 1.5 G light. The hydrogen (H 2 ) production rate of the Ce/TiO 2 was approximately 0.33 μmol/h/g, which is more than twice as much as that of the pure anatase TiO 2 (0.12 μmol/h/g). This work demonstrates the effect of Ce doping in the lattice of TiO 2 for enhanced photocatalytic hydrogen production.

In this work, a simple one-step hydrothermal method was employed to prepare the Ce-doped Fe 2 O 3 ordered nanorod arrays (CFT). The Ce doping successfully narrowed the band gap of Fe 2 O 3 , which improved the visible light absorption performance. In addition, with the help of Ce doping, the recombination of electron/hole pairs was significantly inhibited. The external voltage will make the performance of the Ce-doped sample better. Therefore, the Ce-doped Fe 2 O 3 has reached superior photoelectrochemical (PEC) performance with a high photocurrent density of 1.47 mA/cm 2 at 1.6 V vs. RHE (Reversible Hydrogen Electrode), which is 7.3 times higher than that of pristine Fe 2 O 3 nanorod arrays (FT). The Hydrogen (H 2 ) production from PEC water splitting of Fe 2 O 3 was highly improved by Ce doping to achieve an evolution rate of 21 μmol/cm 2 /h.

The accumulation of the intermediate zeaxanthin and canthaxanthin in the astaxanthin biosynthesis pathway catalyzed by β-carotene hydroxylase ( crtZ ) and β-carotene ketolase ( crtW ) decreases the content of the astaxanthin. Here, we exploited directed evolution of the fusion of crtZ and crtW for improving astaxanthin biosynthesis in Saccharomyces cerevisiae . The results demonstrated that the fusion enzyme of crtZ-crtW with 2 X GGGGS peptides linker can effectively reduce the accumulation of intermediates and improves the content of astaxanthin. Compared with the control strain, the fusion enzyme of ketase and hydroxylase reduced zeaxanthin and canthaxanthin by 7 and 14 times and increased astaxanthin by 1.6 times, respectively. Moreover, 9 variant fusion mutants with improved astaxanthin production were generated through directed evolution. Combining these dominant mutants generated a variant, L95S + I206L, which increased the astaxanthin content of 3.8 times than the control strain. The AlphaFold2 assisted structural analysis indicated that these two mutations alter the interaction between the substrate and the enzymes pocket. Our research provided an efficient idea to reduce the accumulation of the intermediate products in complex biosynthesis pathway., Competing Interests: The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (© 2022 The Authors.)

The unique electronic structure of rare-earth elements makes their modified semiconductor photocatalysts show great advantages in solar energy conversion. Herein, the pollen-like N, P self-doped biochar-based rare-earth composite catalyst (Er/LP-C) has been successfully synthesized, which combines the advantages of biochar and Er and is used for the first time in the field of photocatalytic hydrogen production from ethanol-water mixtures. Experimental results confirmed that the performance of photocatalytic hydrogen production under the full spectrum is up to 33.70 μmol/g in 6 h; this is due to the introduction of Er, which improves the carrier concentration, separation and transfer efficiency, and the driving force for the reduction reaction., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

Herein, a simple and straightforward method to reduce dramatically the lifetime of a pure organic thermally activated delayed fluorescence (TADF) material VIA metal coordination is demonstrated. We designed a mononuclear silver complex [Ag(PPh 2 CH 3 )(TCzBN-PyPz)]BF 4 (1) with a new emissive TCzBN-PyPz ligand. Even though the ligand and the metal complex have very similar emissive efficiencies and maximal peaks, over three orders of magnitude shorter lifetime of 0.59 μs for the complex than 2074 μs for ligand were obtained. Compared to other methods, the present protocol seems to be simple and highly effective.

Organic light-emitting diodes (OLEDs) with tunable emission colors, especially white OLEDs, have rarely been observed with a single emitter in a single emissive layer. In this paper, we report a new compound featuring a D-A-D structure, 9,9'-(pyrimidine-2,5-diylbis(2,1-phenylene))bis(3,6-di-tert-butyl-9 H -carbazole) ( PDPC ). A nondoped OLED using this compound as a single emitter exhibits unique voltage-dependent dual emission. The emission colors range from blue to orange-red with an increase in voltage, during which white electroluminescence with a Commission Internationale De L'Eclairage (CIE) coordinate of (0.35, 0.29) and a color render index (CRI) value of 93 was observed. A comparative study revealed that the dual emission simultaneously originates from the monomers and excimers of the emitter. This study provides insight into understanding the multimer-excited mechanism and developing novel color-tunable OLEDs.

Oxides composed of an oxygen framework and interstitial cations are promising cathode materials for lithium-ion batteries. However, the instability of the oxygen framework under harsh operating conditions results in fast battery capacity decay, due to the weak orbital interactions between cations and oxygen (mainly 3d-2p interaction). Here, a robust and endurable oxygen framework is created by introducing strong 4s-2p orbital hybridization into the structure using LiNi 0.5 Mn 1.5 O 4 oxide as an example. The modified oxide delivers extraordinarily stable battery performance, achieving 71.4 % capacity retention after 2000 cycles at 1 C. This work shows that an orbital-level understanding can be leveraged to engineer high structural stability of the anion oxygen framework of oxides. Moreover, the similarity of the oxygen lattice between oxide electrodes makes this approach extendable to other electrodes, with orbital-focused engineering a new avenue for the fundamental modification of battery materials., (© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Porous biochar materials prepared with biomass as a precursor have received widespread attention. In this work, lotus pollen (LP) was used as the carbon source, a variety of the pollen carbon photocatalyst were prepared by a two-step roasting method. A series of characterizations were carried out on the prepared samples, and it was found that the average particle size was about 40 μm. They also exhibit a typical amorphous carbon structure and a porous structure with a network-like interconnected surface. The photocatalytic hydrogen production performances of lotus pollen carbon (LP-C) and commercial carbon black (CB) were measured under the full spectrum illumination. LP-C-600 showed the best hydrogen production performance (3.5 μmol·g -1 ·h -1 ). In addition, the photoelectrochemical (PEC) measurement results confirmed that the LP-C materials show better incident photon-current efficiency (IPCE) performance than the CB materials in the neutral electrolyte. This is because the unique surface wrinkling, hierarchical porous structure, and the N, P self-doping behavior of the LP-C samples are able to improve the light utilization efficiency and the carrier separation/transfer efficiency, thereby further improving the overall hydrogen production efficiency.

In this article, hierarchical porous carbon (HPC) with high surface area of 1604.9 m 2 /g is prepared by the pyrolysis of rubberwood sawdust using CaCO 3 as a hard template. The bio-oil pyrolyzed from the rubber sawdust, followed by the polymerization reaction to form resole phenolic resin, can be used as a carbon source to prepare HPC. The biomass-derived HPC shows a three-dimensionally interconnected morphology which can offer a continuous pathway for ionic transport. The symmetrical supercapacitors based on the as-prepared HPC were tested in 1.0 M tetraethylammonium tetrafluoroborate/propylene carbonate electrolyte. The results of electrochemical analysis show that the HPC-based supercapacitor exhibits a high specific capacitance of 113.3 F/g at 0.5 A/g with superior rate capability and cycling stability up to 5000 cycles. Hybrid lithium-ion capacitors (LICs) based on the HPC and Li 4 Ti 5 O 12 (LTO) were also fabricated. The LICs have a maximum energy density of 113.3 Wh/kg at a power density of 281 W/kg. Moreover, the LIC also displays a remarkable cycling performance with a retention of 92.8% after 3000 cycles at a large current density of 0.75 A/g, suggesting great potential application in the energy storage of the LIC.

Sensors that can specifically and accurately detect glycosaminoglycans are rare. Here, a dual-mode platform for fluorescence intensity and lifetime sensing of plasma heparin and fluorescence imaging of heparan sulfate proteoglycan-expressed cancer cells was developed by stabilizing the intramolecular charge transfer (ICT) state of dansyl acid-labeling AG73 (DA-AG73) peptide with glutathione-capped gold nanoclusters (GSH-AuNCs). DA-AG73 peptides, including an electron-donor dimethylamino group and an electron-withdrawing sulfonamide moiety in the labeled DA molecules, emitted weak fluorescence due to the formation of the twisted ICT excited state. The complexation of heparin with DA-AG73 peptides followed by interacting with the GSH-AuNCs could restrict the rotation of the dimethylamino groups of the labeled DA molecules, triggering the transition from their twisted ICT state to ICT excited state. As a result, the fluorescence intensity and lifetime of the labeled DA molecules in DA-AG73 peptides were gradually enhanced with increasing the heparin concentration. The proposed platform provided excellent selectivity toward heparin and heparan sulfate and exhibited two linear calibration curves for quantifying 20-800 nM and 20-1000 nM heparin in the fluorescence intensity and lifetime modes, respectively. The proposed platform was practically applied for the fluorescence intensity and lifetime determination of plasma heparin and for the selective imaging of heparan sulfate proteoglycan-expressed cells., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Organic molecules with thermally activated delayed fluorescence (TADF) and aggregation induced emission (AIE) properties have attracted increasing research interest due to their great potential applications in organic light emitting diodes (OLEDs), especially for those with multicolor mechanochromic luminescence (MCL) features. Theoretical research on the luminescence characteristics of organic TADF emitters based on the aggregation states is highly desired to quantify the relationship between the TADF properties and aggregation states. In this work, we study the 4,4'-(6-(9,9-dimethylacridine-10(9 H )-yl)quinoline-2,3-dibenzonitrile (DMAC-CNQ) emitter with TADF and AIE properties, and calculate the photophysical properties in gas, solid and amorphous states by using the quantum mechanics and molecular mechanics (QM/MM) method. Our simulations demonstrate that the aggregation states enhance obviously the reverse intersystem crossing rates and transition dipole moments of the DMAC-CNQ emitter, and suppress the non-radiative rates from the lowest excited singlet state (S 1 ) to ground state (S 0 ). Specifically, the molecular stacking of DMAC-CNQ in solid phases can mainly restrict the geometric torsion of the DMAC moiety for decreasing non-radiative decay rates, and the torsion of the CNQ moiety for increasing the reverse intersystem crossing rates. As a result, the calculated fluorescence efficiencies of the DMAC-CNQ emitter in the crystal and amorphous states are 67% and 26% respectively, and in good agreement with the experimental results.

The development of reliable and safe high-energy-density lithium-ion batteries is hindered by the structural instability of cathode materials during cycling, arising as a result of detrimental phase transformations occurring at high operating voltages alongside the loss of active materials induced by transition metal dissolution. Originating from the fundamental structure/function relation of battery materials, the authors purposefully perform crystallographic-site-specific structural engineering on electrode material structure, using the high-voltage LiNi 0.5 Mn 1.5 O 4 (LNMO) cathode as a representative, which directly addresses the root source of structural instability of the Fd 3 ¯ m structure. By employing Sb as a dopant to modify the specific issue-involved 16c and 16d sites simultaneously, the authors successfully transform the detrimental two-phase reaction occurring at high-voltage into a preferential solid-solution reaction and significantly suppress the loss of Mn from the LNMO structure. The modified LNMO material delivers an impressive 99% of its theoretical specific capacity at 1 C, and maintains 87.6% and 72.4% of initial capacity after 1500 and 3000 cycles, respectively. The issue-tracing site-specific structural tailoring demonstrated for this material will facilitate the rapid development of high-energy-density materials for lithium-ion batteries., (© 2021 Wiley-VCH GmbH.)

Small-molecule thermally activated delayed fluorescence (TADF) materials have been extensively developed to actualize efficient organic LEDs (OLEDs). However, organic small molecules generally compromise thin film quality and stability due to the tendency of crystallization, aggregation, and phase separation, which hence degrade the efficiency and long-term stability of the OLEDs. Here, for the first time, we exploit the unique molecular configuration of the bimesitylene scaffold to design two highly efficient TADF amorphous molecular materials with excellent thermal and morphological stabilities. The twisted and rigid bimesitylene scaffold thwarts regular molecular packing and crystallization, thereby guaranteeing homogeneous and stable amorphous thin films. Meanwhile, the highly twisted geometry of the bimesitylene scaffold efficiently breaks the molecular conjugation and thus conserves the high energies of the lowest locally excited triplet states ( 3 LE) above the lowest charge transfer states ( 1 CT and 3 CT), leading to small singlet-triplet energy splitting and fast reverse intersystem crossing. These TADF emitters exhibit high photoluminescence quantum yields of 0.90 and 0.69 and short TADF lifetimes of 4.94 and 1.44 μs in doped films, based on which the greenish-blue and greenish-yellow OLEDs achieve external quantum efficiencies of 23.2 and 16.2%, respectively, with small efficiency roll-off rates and perfect color stability.

Aim: To evaluate the application of anterior segment-optical coherence tomography (AS-OCT) in posterior capsule opacification (PCO) severity assessment and analyse the relationship between PCO severity and intraocular lens (IOL) characters., Methods: PCO patients were prospectively recruited. Cross-sectional images of the anterior segment at horizontal and vertical meridians were acquired with AS-OCT. The area of the IOL-PC (posterior capsular) space and PCO severity (area, thickness, and density at 3 mm and 5 mm IOL optic regions) were measured. The relationship between PCO severity and visual acuity, comparisons of PCO severity and IOL-PC space using varied IOL designs were analysed., Results: One hundred PCO eyes were enrolled. IOL-PC space, PCO thickness and area were positively correlated with axial length. In addition, PCO area and thickness were positively correlated with visual acuity when it was ≤0.52 logMAR. The cut-off level of visual acuity should be 0.52 logMAR. With varied IOL designs, 3-piece C haptic IOL showed a smaller PCO area and thickness than the 1-piece 3 haptic IOL and 1-piece 4 haptic IOL. PCO area and thickness values for an IOL with a diameter ≤11.0 mm was greater than for an IOL with a diameter of 12.5 mm, and the differences were statistically significant. PCO area and thickness increased when IOL haptic angulation increased (from 0 to 12 degrees)., Conclusion: In PCO eyes, cut-off level of visual acuity is 0.52 logMAR. With more severe PCO, visual acuity maybe not enough to describe the visual function impairment. PCO severity and IOL-PC space are significantly correlated with axial length and IOL design and material., (International Journal of Ophthalmology Press.)

Interactive and responsive materials are dynamic molecular systems that are capable of modulating their behavior and adapting to environment autonomously. Photochromic materials are among the fascinating class of dynamic responsive systems and widely used in molecular switches and optoelectronic devices. However, the phototriggered color changing largely relies on the conformation transformation of the photochromic motif, which significantly limited their usage in organic liquid solutions. Herein, we demonstrate a photochromic organic supramolecular system by using electron-rich N,N-dimethylacetamide (DMA) and electron-deficient naphthalenediimide (NDI) as a donor and acceptor, respectively. In the binary system, the photo-induced electron transfer through lone pair···π interactions pathway leads to dynamic photochromic response not only in the solution but also in the crystalline aggregated state. Furthermore, by incorporating the supramolecules in the polymer matrix, the transparent polymeric film also exhibits rapid photochromic response, which makes it a promisingly interactive and adaptive photochromic material., Competing Interests: The authors declare no competing interests., (© 2021 The Author(s).)

Covalent organic frameworks (COFs), a fast-growing field in crystalline porous materials, have achieved tremendous success in structure development and application exploration over the past decade. The vast majority of COFs reported to date are designed according to the basic concept of reticular chemistry, which is rooted in the idea that building blocks are fully connected within the frameworks. We demonstrate here that sub-stoichiometric construction of 2D/3D COFs can be accomplished by the condensation of a hexagonal linker with 4-connected building units. It is worth noting that the partially connected frameworks were successfully reticulated for 3D COFs for the first time, representing the highest BET surface area among imine-linked 3D COFs to data. The unreacted benzaldehydes in COF frameworks can enhance C 2 H 2 and CO 2 adsorption capacity and selectivities between C 2 H 2 /CH 4 and C 2 H 2 /CO 2 for sub-stoichiometric 2D COFs, while the reserved benzaldehydes control the interpenetrated architectures for the 3D case, achieving a rare non-interpenetrated pts topology for 3D COFs. This work not only paves a new avenue to build new COFs and endows residual function groups with further applications but also prompts redetermination of reticular frameworks in highly connected and symmetrical COFs.

Carbon-coated Li 4 Ti 5 O 12 (LTO) has been prepared using polyimide (PI) as a carbon source via the thermal imidization of polyamic acid (PAA) followed by a carbonization process. In this study, the PI with different structures based on pyromellitic dianhydride (PMDA), 4,4'-oxydianiline (ODA), and p -phenylenediamine ( p -PDA) moieties have been synthesized. The effect of the PI structure on the electrochemical performance of the carbon-coated LTO has been investigated. The results indicate that the molecular arrangement of PI can be improved when the rigid p -PDA units are introduced into the PI backbone. The carbons derived from the p -PDA-based PI show a more regular graphite structure with fewer defects and higher conductivity. As a result, the carbon-coated LTO exhibits a better rate performance with a discharge capacity of 137.5 mAh/g at 20 C, which is almost 1.5 times larger than that of bare LTO (94.4 mAh/g).

Three strongly emissive Cu(i) complexes [Cu(tBupzmpy)(POP)]BF4(1), [Cu(Phpzmpy)(POP)]BF4(2) and [Cu(Adpzmpy)(POP)]BF4(3) (tBupzmpy = 2-(5-(tert-butyl)-1H-pyrazol-3-yl)-6-methylpyridine, Phpzmpy = 2-methyl-6-(5-phenyl-1H-pyrazol-3-yl)pyridine, Adpzmpy = 2-(5-((3R,5R)-adamantan-1-yl)-1H-pyrazol-3-yl)-6-methylpyridine, and POP = bis[2-(diphenylphosphino)phenyl]ether) were synthesized and characterized. These complexes exhibit bright bluish-green photoluminescence in the solid state with quantum yields of 91% (1), 71% (2) and 77% (3) and lifetimes of 13.4 μs (1), 32.9 μs (2) and 34.1 μs (3) at room temperature. The results of theoretical calculations, coupled with the temperature dependence of the spectroscopic properties and emission decay behaviors, reveal that the title Cu(i) complexes emit efficient thermally activated delayed fluorescence (TADF) from excited states involving metal-to-ligand charge transfer (MLCT) transitions and ligand-to-ligand charge transfer (LLCT) transitions. The emissive-state characteristics and emission properties of the investigated Cu(i) complexes were tuned effectively by changing the steric and electronic structures of the diimine ligands.

In the present work, we have introduced a series of stable radical-doped coordination compounds composed of donor-acceptor structures and shown to produce organic radicals in situ as a result of unconventional lone pair-π interactions in ambient conditions. Inconspicuous lone pair-π and C-Hπ interactions were shown to play a key role in self-assembly as well as the charge transfer process, resulting in a long-lived charge-separated state able to generate organic radicals. The resultant species displayed broad-spectrum antimicrobial activity, including against multi-drug-resistant bacteria. This study unveiled the promise of reactive organic radical-doped materials as a new platform for developing antimicrobial agents that can overcome antibiotic resistance.