Effect of Facet on Local Electron Density of Oxygen Vacancy in Catalysts for Nitrogen Electro-Reduction.

Oxygen-vacancy (Ov) engineering is an effective strategy to manipulate the electronic configuration of catalysts for electrochemical nitrogen reduction reaction (eNRR). The influence of the stable facet on the electronic configuration of Ov is widely studied, however, the effect of the reactive facet on the local electron density of Ov is unveiled. In this work, an eNRR electrode R(111)-TiO2/HGO is provided with a high proportion exposed reactive facet (111) of rutile-TiO2 (denoted as R(111)-TiO2) nanocrystals with Ov anchored in hierarchically porous graphite oxide (HGO) nanofilms. The R(111)-TiO2/HGO exhibits excellent eNRR performance with an NH3 yield rate of 20.68 µg h-1 cm-2, which is ≈20 times the control electrode with the most stable facet (110) exposed (R(110)-TiO2/HGO). The experimental data and theoretical simulations reveal that the crystal facet (111) has a positive effect on regulating the local electron density around the oxygen vacancy and the two adjacent Ti-sites, promoting the π-back-donation, minimizing the eNRR barrier, and transforming the rate determination step to *NNH→*NNHH. This work illuminates the effect of crystal facet on the performance of eNRR, and offers a novel strategy to design efficient eNRR catalysts.

[Low disease activity and remission status of systemic lupus erythematosus in a real-world study].

OBJECTIVE: To investigate the rates of low disease activity and clinical remission in patients with systemic lupus erythematosus (SLE) in a real-world setting, and to analyze the related factors of low disease activity and clinical remission. METHODS: One thousand patients with SLE were enrolled from 11 teaching hospitals. Demographic, clinical and laboratory data, as well as treatment regimes were collec-ted by self-completed questionnaire. The rates of low disease activity and remission were calculated based on the lupus low disease activity state (LLDAS) and definitions of remission in SLE (DORIS). Charac-teristics of patients with LLDAS and DORIS were analyzed. Multivariate Logistic regression analysis was used to evaluate the related factors of LLDAS and DORIS remission. RESULTS: 20.7% of patients met the criteria of LLDAS, while 10.4% of patients achieved remission defined by DORIS. Patients who met LLDAS or DORIS remission had significantly higher proportion of patients with high income and longer disease duration, compared with non-remission group. Moreover, the rates of anemia, creatinine elevation, increased erythrocyte sedimentation rate (ESR) and hypoalbuminemia was significantly lower in the LLDAS or DORIS group than in the non-remission group. Patients who received hydroxychloroquine for more than 12 months or immunosuppressant therapy for no less than 6 months earned higher rates of LLDAS and DORIS remission. The results of Logistic regression analysis showed that increased ESR, positive anti-dsDNA antibodies, low level of complement (C3 and C4), proteinuria, low household income were negatively related with LLDAS and DORIS remission. However, hydroxychloroquine usage for longer than 12 months were positively related with LLDAS and DORIS remission. CONCLUSION: LLDAS and DORIS remission of SLE patients remain to be improved. Treatment-to-target strategy and standar-dized application of hydroxychloroquine and immunosuppressants in SLE are recommended.

Single Crystal Seed Induced Epitaxial Growth Stabilizes α-FAPbI3 in Perovskite Solar Cells.

FAPbI3 stands out as an ideal candidate for the photoabsorbing layer of perovskite solar cells (PSCs), showcasing outstanding photovoltaic properties. Nonetheless, stabilizing photoactive α-FAPbI3 remains a challenge due to the lower formation energy of the competitive photoinactive δ-phase. In this study, we employ tetraethylphosphonium lead tribromide (TEPPbBr3) single crystals as templates for the epitaxial growth of PbI2. The strategic use of TEPPbBr3 optimizes the evolution of intermediates and the crystallization kinetics of perovskites, leading to high-quality and phase-stable α-FAPbI3 films. The TEPPbBr3-modified perovskite exhibits optimized carrier dynamics, yielding a champion efficiency of 25.13% with a small voltage loss of 0.34 V. Furthermore, the target device maintains 90% of its initial PCE under maximum power point (MPP) tracking over 1000 h. This work establishes a promising pathway through single crystal seed based epitaxial growth for achieving satisfactory crystallization regulation and phase stabilization of α-FAPbI3 perovskites toward high-efficiency and stable PSCs.

Cesium Cyclopropane Acid-Aided Crystal Growth Enables Efficient Inorganic Perovskite Solar Cells with a High Moisture Tolerance.

While all-inorganic halide perovskites (iHPs) are promising photovoltaic materials, the associated water sensitivity of iHPs calls for stringent humidity control to reach satisfactory photovoltaic efficiencies. Herein, we report a moisture-insensitive perovskite formation route under ambient air for CsPbI2 Br-based iHPs via cesium cyclopropane acids (C3 ) as a compound introducer. With this approach, appreciably enhanced crystallization quality and moisture tolerance of CsPbI2 Br are attained. The improvements are attributed to the modified evaporation enthalpy of the volatile side product of DMA-acid initiated by Cs-acids. As such, the water-involving reaction is directed toward the DMA-acids, leaving the target CsPbI2 Br perovskites insensitive to ambient humidity. We highlight that by controlling the C3 concentration, the dependence of power conversion efficiency (PCE) in CsPbI2 Br devices on the humidity level during perovskite film formation becomes favorably weakened, with the PCEs remaining relatively high (>15 %) associated with improved device stability for RH levels changed from 25 % to 65 %. The champion solar cells yield an impressive PCE exceeding 17 %, showing small degradations (<10 %) for 2000 hours of shell storage and 300 hours of 85/85 (temperature/humidity) tests. The demonstrated C3 -based strategy provides an enabler for improving the long-sought moisture-stability of iHPs toward high photovoltaic device performance.

The rise of quasi-2D Dion-Jacobson perovskites for photovoltaics.

With the advance of nanotechnology, the past couple of years have witnessed the fast development of quasi two-dimensional (2D) halide perovskites, which exhibit outstanding long-term stability against moisture and heat, compared with their three-dimensional (3D) counterparts. As one of the most common structures in 2D halide perovskites, quasi-2D Dion-Jacobson (DJ) perovskites show multiple-quantum-well structures with n layers of [BX6]4- octahedral inorganic sheets sandwiched by two layers of diammonium spacers, thus exhibiting superior structural stability due to the elimination of van der Waals gaps. Thanks to the achievement of high power conversion efficiency accompanied by impressive stability, quasi-2D DJ perovskite solar cells (PSCs) have recently drawn extensive attention in the field. This review first introduces the fundamental understanding of quasi-2D DJ halide perovskites, including their superior stability, high exciton binding energy, and compositional flexibility and tunable properties. We then summarize detailed strategies to prepare high-quality quasi-2D DJ perovskites for PSCs, encompassing compositional engineering, solvent engineering, additive addition, and annealing processes. Moreover, the surface/interface modification and 2D-3D hybrid perovskite heterojunction are also discussed, for providing strategies to optimize the fabrication of quasi-2D DJ PSCs. Lastly, current challenges and perspectives toward the future development of quasi-2D DJ perovskites for photovoltaics are outlined.

Semitransparent Organic Solar Cells with Homogeneous Transmission and Colorful Reflection Enabled by an ITO-Free Microcavity Architecture.

Semitransparent organic photovoltaics (ST-OPVs), owing to the merits of high power generation, thermal insulation, and aesthetic features, have become a promising candidate for intellectual building- integrated photovoltaic windows. However, the traditional optical evaluation only focuses on the transmission properties and ignores the reflection behaviors. And the lack of quantitative descriptions for array appearance hinders implementation of ST-OPV based large-area modules. To tackle with these issues, an indium tin oxide (ITO)-free optical microcavity architecture into ST-OPVs for achieving high homogeneity in transmittance with controllable reflective appearances through tunning the thickness of individual component layers is introduced. A set of parameters based on optical characteristics of sub-units to provide a quantitative description for the transmittance brightness, transmissive and reflective color purity, and versatility of optical arrays, is further proposed. The optical simulations reveal that reflection modulation from blue to red colors can be realized for devices based on various bulk-heterojunction material systems through regulating the thickness of active layers and antireflection coatings. This work offers a viable design strategy for ST-OPVs toward applications in next-generation smart photovoltaic windows.

A Binary Solution Strategy Enables High-Efficiency Quasi-2D Perovskite Solar Cells with Excellent Thermal Stability.

Quasi-two-dimensional (2D) perovskites are highly promising light-harvesting materials for commercialization of perovskite solar cells (PSCs) owing to the excellent materials stability. However, the coexistence of multiple n-value species in 2D perovskites often causes increased complexities in crystallization that can negatively affect the eventual photovoltaic performance. Herein, we present a binary solution based strategy via introducing nontoxic and widely accessible CH3COOH (HAc) as a co-solvent for preparing high-quality 2D perovskite films. Based on a 2D perovskite model system, (AA)2MA4Pb5I16 (n = 5), we show that the prenucleation and grain growth kinetics are appreciably modified with HAc, which benefits from the strong electron-donating ability of HAc with the key component of PbI2, leading to formation of favorable cluster aggregates and resultant modulation of crystal growth. With the HAc-based method, the devices yield a boosted photovoltaic efficiency of 18.55% with an impressive photovoltage of 1.26 V. The champion cells exhibit a supreme thermal stability, showing <3% efficiency degradation under continuous thermal aging for 800 h.

Crystallinity and Phase Control in Formamidinium-Based Dion-Jacobson 2D Perovskite via Seed-Induced Growth for Efficient Photovoltaics.

2D perovskites based on Formamidinium (FA) hold the potential for excellent stability and a broad absorption range, making them attractive materials for solar cells. However, FA-based 2D perovskites produced via one-step processing exhibit poor crystallinity and random quasi-quantum wells (QWs), leading to subpar photovoltaic performance. In this study, a seed-induced growth approach is introduced employing MAPbCl3 and BDAPbI4 in the deposition of FA-based Dion-Jacobson 2D perovskite films. This method yields high-quality perovskite films as the seeds preferentially precipitate and serve as templates for the epitaxial growth of FA-based counterparts, effectively suppressing the δ phase. Moreover, the epitaxial growth facilitated by uniformly dispersed seeds results in simultaneous crystallization from top to bottom, efficiently mitigating random phases (n = 2, 3, 4…) induced by the diffusion of organic cations and, in turn, minimizing energy loss. The impact of seed-induced growth on the crystallization and phase distribution of FA-based 2D perovskites is systematically investigated. As a result, the optimized FA-based 2D perovskite solar cell delivers an outstanding efficiency of 20.0%, accompanied by a remarkable fill factor of 0.823. Additionally, the unencapsulated device demonstrates exceptional stability, maintaining 98% of its initial efficiency after 1344 h of storage.

Lifetime over 10000 hours for organic solar cells with Ir/IrOx electron-transporting layer.

The stability of organic solar cells is a key issue to promote practical applications. Herein, we demonstrate that the device performance of organic solar cells is enhanced by an Ir/IrOx electron-transporting layer, benefiting from its suitable work function and heterogeneous distribution of surface energy in nanoscale. Notably, the champion Ir/IrOx-based devices exhibit superior stabilities under shelf storing (T80 = 56696 h), thermal aging (T70 = 13920 h), and maximum power point tracking (T80 = 1058 h), compared to the ZnO-based devices. It can be attributed to the stable morphology of photoactive layer resulting from the optimized molecular distribution of the donor and acceptor and the absence of photocatalysis in the Ir/IrOx-based devices, which helps to maintain the improved charge extraction and inhibited charge recombination in the aged devices. This work provides a reliable and efficient electron-transporting material toward stable organic solar cells.

Sulfonium-Cations-Assisted Intermediate Engineering for Quasi-2D Perovskite Solar Cells.

Quasi-2D Ruddlesden-Popper (RP) perovskites with superior stability are admirable candidates for perovskite solar cells (PSCs) toward commercialization. However, the device performance remains unsatisfactory due to the disordered crystallization of perovskites. In this work, the effects of sulfonium cations on the evolution of intermediates and photovoltaic properties of 2D RP perovskites are investigated. The introduction of sulfonium cations leads to preferred intermediate transformation and improved film quality of perovskites. The resulting devices deliver a champion efficiency of 19.08% at room temperature and 20.52% at 180 K, due to reduced recombination and enhanced charge transport. More importantly, the unencapsulated device maintains 84% of the initial efficiency under maximum power point (MPP) tracking at 40 °C for 1000 h. This work helps to gain a comprehensive understanding of the crystallization process of quasi-2D perovskites and provides a simple strategy to modulate the intermediates of perovskites.

Solvent Effect on Film Formation and Trap States of Two-Dimensional Dion-Jacobson Perovskite.

Two dimensional Dion-Jacobson (2D DJ) perovskite has emerged as a potential photovoltaic material because of its unique optoelectronic characteristics. However, due to its low structural flexibility and high formation energy, extra assistance is needed during crystallization. Herein, we study the solvent effect on film formation and trap states of 2D DJ perovskite. It is found that the nucleation process of 2D DJ perovskite can be retarded by extra coordination, which is proved by in situ optical spectra. As a benefit, out-of-plane oriented crystallization and ordered phase distribution are realized. Finally, in 1,5-pentanediammonium (PeDA) based 2D DJ perovskite solar cells (PSCs), one of the highest reported open-circuit voltage (VOC) values of 1.25 V with state-of-the-art efficiency of 18.41% is obtained due to greatly shallowed trap states and suppressed nonradiative recombination. The device also exhibits excellent heat tolerance, which maintains 80% of its initial efficiency after being kept under 85 °C after 3000 h.

Impact of Strain Relaxation on 2D Ruddlesden-Popper Perovskite Solar Cells.

Although the photovoltaic performance of perovskite solar cells (PSCs) has reached the commercial standards, the unsatisfactory stability limits their further application. Hydrophobic interface and encapsulation can block the damage of water and oxygen, while the instability induced by intrinsic residual strain remains inevitable. Here, the residual strain in a two-dimensional (2D) Ruddlesden-Popper (RP) perovskite film is investigated by X-ray diffraction and atomic force microscopy. It's found that the spacer cations contribute to the residual strain even though they are not in the inorganic cages. Benefited from strain relaxation, the film quality is improved, leading to suppressed recombination, promoted charge transport and enhanced efficiency. More significantly, the strain-released devices maintain 86 % of the initial efficiency after being kept in air with 85 % relative humidity (RH) for 1080 h, 82 % under maximum power point (MPP) tracking at 50 °C for 804 h and 86 % after continuous heating at 85 °C for 1080 h.

"N-π-N" Type Oligomeric Acceptor Achieves an OPV Efficiency of 18.19% with Low Energy Loss and Excellent Stability.

A novel "N-π-N" type oligomeric acceptor of 2BTP-2F-T, constructed by two small non-fullerene acceptor (NFA) units linked with a thiophene π bridge is reported. The 2BTP-2F-T not only combines the advantages of small NFA and polymeric acceptors (PYF-T-o) with similar units but also exhibits superior characteristics of high absorption coefficient and high electron moblity(µe) ) with less dependence on molecular packing. Using PM6 as the donor, a remarkable efficiency of 18.19% is obtained with an open circuit (Voc ) of 0.911 V, short current circuit (Jsc ) of 25.50 mA cm-2 , and fill factor (FF) of 78.3%, which is much better than that of the corresponding monomer (16.54%) and PYF-T-o (15.8%) based devices. The much-improved efficiency results from two aspects: 1) an enhanced FF due to the largely improved µe and well-controlled morphology ; 2) a higher value of (Jsc × Voc ) due to its higher absorption coefficient and efficient charge generation at a similar low energy loss. Furthermore, the PM6/2BTP-2F-T device possesses the longest T80 lifetime to light-soaking and comparable high thermal stability with PM6/PYF-T-o. The results indicate that the "N-π-N" type oligomeric acceptor has a great application prospect due to its superior high efficiency and improved stability in organic solar cells.

High Miscibility Compatible with Ordered Molecular Packing Enables an Excellent Efficiency of 16.2% in All-Small-Molecule Organic Solar Cells.

In all-small-molecule organic solar cells (ASM-OSCs), a high short-circuit current (Jsc ) usually needs a small phase separation, while a high fill factor (FF) is generally realized in a highly ordered packing system. However, small domain and ordered packing always conflicted each other in ASM-OSCs, leading to a mutually restricted Jsc and FF. In this study, alleviation of the previous dilemma by the strategy of obtaining simultaneous good miscibility and ordered packing through modulating homo- and heteromolecular interactions is proposed. By moving the alkyl-thiolation side chains from the para- to the meta-position in the small-molecule donor, the surface tension and molecular planarity are synchronously enhanced, resulting in compatible properties of good miscibility with acceptor BTP-eC9 and strong self-assembly ability. As a result, an optimized morphology with multi-length-scale domains and highly ordered packing is realized. The device exhibits a long carrier lifetime (39.8 µs) and fast charge collection (15.5 ns). A record efficiency of 16.2% with a high FF of 75.6% and a Jsc of 25.4 mA cm-2 in the ASM-OSCs is obtained. These results demonstrate that the strategy of simultaneously obtaining good miscibility with high crystallinity could be an efficient photovoltaic material design principle for high-performance ASM-OSCs.

Peculiar Steric Hindrance Assists Monoclinic Phase Formation toward High-Quality All-Inorganic Perovskites.

Bromine-containing metal halide all-inorganic perovskite CsPbI2Br exhibits excellent photoelectric performance and supreme thermal and structural stabilities; it is thus attractive for use as photoabsorbing layers in perovskite solar cells (PSCs). However, when steric hindrance molecules are introduced, the complicated phase transition mechanism and the difficult-to-control crystallization process in CsPbI2Br are not well understood. Here, we introduce a class of sterically hindered cesium naphthenate small molecules to control the crystallization process of CsPbI2Br films. Of interest, a new intermediate monoclinic phase has been discovered which leads to formation of dense and nonporous polycrystalline perovskite films. This phenomenon was also explained by density functional theory. The residues of steric hindrance molecules inside the CsPbI2Br film also improve its stability. We further show that as the ring number of cycloalkanes increases, the hindrance for the crystallization becomes more significant. Thus, by choosing the suitable steric hindrance, the optimal photovoltaic efficiency is 15.45%.

Recent advances in non-fullerene organic photovoltaics enabled by green solvent processing.

Solution-processed organic photovoltaic (OPV) as a new energy device has attracted much attention due to its huge potential in future commercial manufacturing. However, so far, most of the studies on high-performance OPV have been treated with halogenated solvents. Halogenated solvents not only pollute the environment, but are also harmful to human health, which will negatively affect the large-scale production of OPV in the future. Therefore, it is urgent to develop low-toxic or non-toxic non-halogen solvent-processable OPV. Compared with conventional fullerene OPVs, non-fullerene OPVs exist with stronger absorption, better-matched energy levels and lower energy loss. Processing photoactive layers with non-fullerenes as the acceptor material has broad potential advantages in non-halogenated solvents. This review introduces the research progress of non-fullerene OPV treated by three different kinds of green solvents as the non-halogenated and aromatic solvent, the non-halogenated and non-aromatic solvent, alcohol and water. Furthermore, the effects of different optimization strategies on the photoelectric performance and stability of non-fullerene OPV are analyzed in detail. The current optimization strategy can increase the power conversion efficiency of non-fullerene OPV processed with non-halogen solvents up to 17.33%, which is close to the performance of processing with halogen-containing solvents. Finally, the commercial potential of non-halogen solvent processing OPVs is discussed. The green solvent processing of non-fullerene-based OPVs will become a key development direction for the future of the OPV industry.

Strongly Reduced Non-Radiative Voltage Losses in Organic Solar Cells Prepared with Sequential Film Deposition.

With nearly 100% yields for mobile charge carriers in organic solar cells (OSCs), the relatively large photovoltage loss (ΔVoc) is a critical barrier limiting the power conversion efficiency of OSCs. Herein, we aim to improve the open-circuit voltage (Voc) in OSCs with non-fullerene acceptors via sequential film deposition (SD). We show that ΔVoc in planar heterojunction (PHJ) devices prepared by the SD method can be appreciably mitigated, leading increases in Voc to 80 mV with regard to the Voc of bulk heterojunction devices. In PHJ OSCs, the energy level of intermolecular charge-transfer states is found to increase with a decrease in the level of aggregation in the solid state. These properties explain the enhanced electroluminescent quantum efficiency and resultant suppression of the voltage losses induced by nonradiative charge recombination and interfacial charge transfer. This work provides a promising strategy for tackling the heavily discussed photovoltage loss in OSCs.

Low infectious risk of re-positive COVID-19 patients: a single-center study.

OBJECTIVE: The aim of this study was to investigate the infectiousness of re-positive coronavirus disease 2019 (COVID-19) patients. METHODS: All nucleic acid testing (NAT) was performed using throat swabs, nasopharyngeal swabs, and anal swabs, which were tested by Fluorescent quantitative realtime PCR. Re-positive cases were defined as a discharged patient who re-tested positive by NAT. Micro-neutralization of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) was performed based on the methods for severe acute respiratory syndrome (SARS) and Middle East respiratory syndrome (MERS) viruses. IgM and IgG against the N protein of SARS-CoV-2 were determined by ELISA. RESULTS: A total 255 (16.04%) of 1590 COVID-19 patients were re-positive. The re-positive cases were more likely to occur in patients in the 20-39 years age group and in patients with disease of moderate severity. Quantitative PCR showed that cycle threshold (Ct) values and viral loads were both far lower than in the hospitalized COVID-19 patients. The viral load in re-positive cases was very low. Viral culture of the samples from re-positive patients showed no cytopathic effect, and NAT of the culture medium of viral cultures all exhibited negative results. CONCLUSION: The viral load in re-positive cases was very low; patients were not infectious and the risk of human-to-human transmission was extremely low. Discharged COVID-19 patients should undergo home health management for 3 weeks.

Cryo-EM reveals a previously unrecognized structural protein of a dsRNA virus implicated in its extracellular transmission.

Mosquito viruses cause unpredictable outbreaks of disease. Recently, several unassigned viruses isolated from mosquitoes, including the Omono River virus (OmRV), were identified as totivirus-like viruses, with features similar to those of the Totiviridae family. Most reported members of this family infect fungi or protozoans and lack an extracellular life cycle stage. Here, we identified a new strain of OmRV and determined high-resolution structures for this virus using single-particle cryo-electron microscopy. The structures feature an unexpected protrusion at the five-fold vertex of the capsid. Disassociation of the protrusion could result in several conformational changes in the major capsid. All these structures, together with some biological results, suggest the protrusions' associations with the extracellular transmission of OmRV.

Emergence of a non vaccine-cognate enterovirus A71 genotype C1 in mainland China.

BACKGROUND: EV-A71 is a common causative agent of hand foot and mouth disease. In mainland China, EV-A71 subgenotype C4 has been the sole circulating genotype since 2008, and was used in the production of multiple licensed vaccines. Here, we report the first detection EV-A71 C1 strains in China. METHODS: Full genomic sequence were obtained. The origin of the EV-A71 C1 strains were tracked down by Bayesian inferences. Recombination was analyzed using Simplot program. And the antigenicity were tested using the microneutralization test. RESULTS: The C1-GD2019 shared high identity with the C1-like lineage recently identified in Europe and was introduced into Guangdong in 2018-2019. Close genetic relatedness between the C1-GD2019 and Europe C1-like strains were observed except for the 3D-3'UTR region. The late showed high similarity with CVA genomes. Antigenic variance was found. The C1-GD2019 could not be effectively neutralized by EV-A71 C4a neutralizing antibody positive samples. CONCLUSION: This is the first report of EV-A71 subgenotype C1 isolated in China. It is a recombinant strain originating from C1-like strains recently identified in Europe and CVA strains. The different antigenicity between the C1 strains and C4a vaccine strains highlighted the importance on closely monitoring the EV-A71 C1 strains in China.