Search

Converting greenhouse gases into valuable products has become a promising approach for achieving a carbon-neutral economy and sustainable development. However, the conversion efficiency depends on the energy yield of the substrate. In this study, we developed an electro-biocatalytic system by integrating electrochemical and microbial processes to upcycle CO2 into a valuable product (ectoine) using renewable energy. This system initiates the electrocatalytic reduction of CO2 to methane, an energy-dense molecule, which then serves as an electrofuel to energize the growth of an engineered methanotrophic cell factory for ectoine biosynthesis. The scalability of this system was demonstrated using an array of ten 25 cm2 electrochemical cells equipped with a high-performance carbon-supported isolated copper catalyst. The system consistently generated methane at the cathode under a total partial current of approximately -37 A (~175 mmolCH4 h-1) and O2 at the anode under a total partial current of approximately 62 A (~583 mmolO2 h-1). This output met the requirements of a 3-L bioreactor, even at maximum CH4 and O2 consumption, resulting in the high-yield conversion of CO2 to ectoine (1146.9 mg L-1). This work underscores the potential of electrifying the biosynthesis of valuable products from CO2, providing a sustainable avenue for biomanufacturing and energy storage., (© 2024 Wiley‐VCH GmbH.)

Proton exchange membrane water electrolysers promise to usher in a new era of clean energy, but they remain a formidable obstacle in designing active and durable electrocatalysts for the acidic oxygen evolution reaction (OER). In this study, a protonated iridium oxide embedded with single-atom dispersed ruthenium atoms (H 3.8 Ir 1- x Ru x O 4 ) that demonstrates exceptional activity and stability in acidic water oxidation is introduced. The single Ru dopants favorably induce localized oxygen vacancies in the Ir─O lattice, synergistically strengthening the adsorption of OOH* intermediates and enhancing the intrinsic OER activity. In addition, the preferential oxidation of Ru and the electronegativity of the oxygen vacancies significantly stabilize the Ir─O active sites, improving the OER stability. Consequently, the H 3.8 Ir 1─ x Ru x O 4 catalyst shows an overpotential of 255 mV at 10 mA cm -2 and displays exceptional catalytic endurance in acidic electrolytes, surpassing 1100 h, representing a remarkable one-order-of-magnitude increase in stability compared to that of pristine H 3.8 IrO 4 . A proton exchange membrane electrolyser utilizing the H 3.8 Ir 1- x Ru x O 4 catalyst as an anode exhibits stable performance for more than 1280 h under a high current density of 2 A cm -2 ., (© 2024 Wiley‐VCH GmbH.)

Bacterial infections and long-term inflammation cause serious secondary damage to chronic diabetic wounds and hinder the wound healing processes. Currently, multifunctional hydrogels have shown promising effects in chronic wound repair. However, traditional hydrogels only keep the wound moist and protect it from bacterial infection, and cannot provide mechanical force to contract the wound edges to achieve facilitated wound closure. Here, an asymmetric composite dressing was created by combining biaxially oriented nanofibers and hydrogel, inspired by the double-layer structure of the traditional Chinese medicinal plaster patch, for managing chronic wounds. Specifically, electrospun Poly-(lactic acid-co-trimethylene carbonate) (PLATMC) nanofibers and methacrylate gelatin (GelMa) hydrogel loaded with Epinecidin-1@chitosan (Epi-1@CS) nanoparticles are assembled as the temperature-responsive self-contracting nanofiber/hydrogel (TSNH) composite dressing. The substrate layer of PLATMC nanofibers combines topological morphology with material properties to drive wound closure through temperature-triggered contraction force. The functional layer of GelMa hydrogel is loaded with Epi-1@CS nanoparticles that combine satisfactory cytocompatibility, and antioxidant, anti-inflammatory, and antibacterial properties. Strikingly, in vivo , the TSNH dressing could regulate the diabetic wound microenvironment, thereby promoting collagen deposition, facilitating angiogenesis, and reducing the inflammatory response, which promotes the rapid healing of chronic wounds. This study highlights the potential of synergizing mechanical and biochemical signals in enhancing chronic wound treatment. Overall, this TSNH composite dressing is provided as a reliable approach to solving the long-standing problem of chronically infected wound healing., 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., (© 2024 The Authors.)

The [1,2]- and [2,3]-Stevens rearrangements are one of the most fascinating chemical bond reorganization strategies in organic chemistry, and they have been demonstrated in a wide range of applications, representing a fundamental reaction tactic for the synthesis of nitrogen compounds in chemical community. However, their applicabilities are limited by the scarcity of efficient, general, and straightforward methods for generating ammonium ylides. Herein, we report a general difluorocarbene-induced tertiary amine-involved [1,2]- and [2,3]-Stevens rearrangements stemmed from in situ generated difluoromethyl ammonium ylides, which allows for the rearrangements of versatile tertiary amines bearing either allyl, benzyl, or propargyl groups, resulting in the corresponding products in one reaction under the same reaction conditions with a general way. Broad substrate scope, simple operation, mild reaction conditions and late-stage modification of natural products highlight the advantages of this strategy, meanwhile, this general rearrangement reaction is believed to bring opportunities for the transformations of nitrogen ylides and the assembly of valuable tertiary amines and amino acids. This will further enrich the reaction repertoire of difluorocarbene species, facilitate the development of reactions involving difluoromethyl ammonium salts, and provide an avenue for the development of this type of rearrangement reactions., (© 2024. The Author(s).)

Molecular metal compounds have demonstrated excellent catalytic activity and product selectivity in the H 2 evolution reaction (HER) and the CO 2 reduction reaction (CO 2 RR). The heterogenization of molecular catalysts is regarded as an effective approach to improve their applicability. In this work, the molecular catalytic units [Cp*Ir(Bpy)Cl] + and [Ru(Bpy)(CO) 2 Cl 2 ] are constructed in situ on the bipyridine sites of the covalent organic framework for photocatalytic HER and CO 2 RR, respectively. Inheriting the impressive performance of molecular catalysts, the functionalized TpBpy-M exhibits excellent catalytic activity and product selectivity. Under visible light irradiation, the H 2 production rate of TpBpy-Ir is about 760 μmol g -1 h -1 , which is 6.7 times higher than that of TpBpy without built-in catalytic sites. Also, the HCOOH production rate of TpBpy-Ru is 271 μmol g -1 h -1 , with an impressive selectivity of 88%. Control experiments validated that this improvement is attributed to the incorporation of molecular catalytic units into the framework. Photoluminescence spectroscopy measurements and theoretical calculation consistently demonstrate that, under illumination, the photosensitizer [Ru(Bpy) 3 ]Cl 2 is excited and transfers electrons to the catalytic sites in TpBpy-M, which then catalyzes the reduction of H + and CO 2 .

In recent years, the utilization of medical devices has gradually increased and implantation procedures have become common treatments. However, patients are susceptible to the risk of implant infections. This study utilized chemical grafting to immobilize polyethylenimine (QPEI) and hyaluronic acid (HA) on the surface of the mesh to improve biocompatibility while being able to achieve antifouling antimicrobial effects. From the in vitro testing, PP-PDA-Q-HA exhibited a high antibacterial ratio of 93% against S. aureus , 93% against E. coli , and 85% against C. albicans . In addition, after five rounds of antimicrobial testing, the coating continued to exhibit excellent antimicrobial properties; PP-PDA-Q-HA also inhibits the formation of bacterial biofilms. In addition, PP-PDA-Q-HA has good hemocompatibility and cytocompatibility. In vivo studies in animal implantation infection models also demonstrated the excellent antimicrobial properties of PP-PDA-Q-HA. Our study provides a promising strategy for the development of antimicrobial surface medical materials with excellent biocompatibility.

Using their own triazine groups as natural receptors, the introduction of various donor units to construct donor-receptor configuration in covalent triazine frameworks (CTFs) has been shown to be an effective strategy to improve photocatalytic activity. In this work, the effect of donor unit content (D-content) on the photoelectric properties and photocatalytic activity of CTFs was thoroughly investigated. Four analogous CTFs with different D-content have been rationally designed and synthesized, in which the bithiophene (Btp) as the donor unit and triazine as the acceptor unit. And CTF-Btp with the highest D-content showed the best photocatalytic activity. The experimental and theoretical results indicated this improvement is attributed to stronger visible light absorption capacity and higher photoinduced charge carrier separation efficiency. This study elucidates the relationship between the structural features of CTFs with varying D-content and their photocatalytic activity, offering a promising strategy for developing efficient photocatalysts., (© 2023 Wiley-VCH GmbH.)

MSP is a rare and atypical form of benign granulomatous inflammation characterised by tumour-like local proliferation of spindle-shaped histiocytes containing acid-fast positive mycobacteria, which should be differentiated from neoplastic lesions. A 26-year-old Chinese man complained an intermittent and mild right lower abdominal pain for 5 months in May 2022.Histopathology of biopsy samples showed Mycobacterial spindle cell pseudotumor (MSP). The test of Mycobacterium tuberculosis detected by polymerase chain reaction using intestinal tissue slice was negative. The metagenomic next-generation sequencing (BGI-Shenzhen) using formalin-fixation and paraffin-embedded intestine samples confirmed Mycobacterium tuberculosis complex (MTBC).

Rheumatoid arthritis (RA) is an inflammatory disease. Curcumin can inhibit NF-κB and reduce the expression of inflammation-related genes. Aim: To evaluate the potential development of 6d in the clinical treatment of inflammatory diseases such as RA. Methods: Using a skeleton fusion strategy to synthesize curcumin analogues for 6d . This work evaluates anti-inflammatory activity by conducting anti-arthritis experiments (adjuvant-induced RA models) on rats. Western blot and ELISA were used to detect the expression of inflammatory-related proteins and cytokines. Molecular docking analysis confirmed the binding effect of 6d with active sites. Conclusion: 6d inhibits NF-κB has a protective effect on arthritis caused by RA.

In recent years, numerous 1,2-R shift (R = aliphatic or aryl) based on tetracoordinate boron species have been well investigated. In the contrary, the corresponding radical migrations, especially 1,2-boryl radical shift for the construction of organoborons is still in its infancy. Given the paucity and significance of such strategies in boron chemistry, it is urgent to develop other efficient and alternative synthetic protocols to enrich these underdeveloped radical 1,2-boron migrations, before their fundamental potential applications could be fully explored at will. Herein, we have demonstrated a visible-light-induced photoredox neutral decarboxylative radical cross-coupling reaction, which undergoes a radical 1,2-boron shift to give a translocated C-radical for further capture of versatile radical acceptors. The mild reaction conditions, good functional-group tolerance, and broad β-boryl NHPI esters scope as well as versatile radical acceptors make this protocol applicable in modification of bioactive molecules. It can be expected that this methodology will be a very useful tool and an alternative strategy for the construction of primary organoborons via a novel radical 1,2-boron shift mode., (© 2023. Springer Nature Limited.)

The influence of grain structure and quenching rates on the exfoliation corrosion (EXCO) susceptibility of 7085 alloy was studied using immersion tests, optical microscopy (OM), scanning electron microscopy (SEM), electron backscatter diffraction (EBSD), and scanning transmission electron microscopy (STEM). The results show that as the cooling rate decreases from 1048 °C/min to 129 °C/min; the size of grain boundary precipitates (GBPs); the width of precipitate-free zones (PFZ); and the content of Zn, Mg, and Cu in GBPs rise, leading to an increase in EXCO depth and consequently higher EXCO susceptibility. Meanwhile, there is a linear relationship between the average corrosion depth and the logarithm of the cooling rate. Corrosion cracks initiate at the grain boundaries (GBs) and primarily propagate along the HAGBs. In the bar grain (BG) sample at lower cooling rates, crack propagation along the sub-grain boundaries (SGBs) was observed. Compared to equiaxed grain (EG) samples, the elongated grain samples exhibit larger GBPs, a wider PFZ, and minor compositional differences in the GBPs, resulting in higher EXCO susceptibility.

Transition metal mediated C-X (X = H, halogen) bond activation provides an impressive protocol for building polyaromatic hydrocarbons (PAHs) in C-C bond coupling and annulation; however, mimicking both the reaction model and Lewis acid mediator simultaneously in a hetero-PAH system for selective C-P bond cleavage faces unsolved challenges. At present, developing the C-P bond activation protocol of the phosphonic backbone using noble-metal complexes is a predominant passway for the construction of phosphine catalysts and P-center redox-dependent photoelectric semiconductors, but non-noble metal triggered methods are still elusive. Herein, we report Mn(iii)-mediated C-P bond activation and intramolecular cyclization of diphosphines by a redox-directed radical phosphonium process, generating phosphahelicene cations or phosphoniums with nice regioselectivity and substrate universality under mild conditions. Experiments and theoretical calculations revealed the existence of the unusual radical mechanism and electron-deficient character of novel phosphahelicenes. These rigid quaternary bonding skeletons facilitated versatile fluorescence with good tunability and excellent efficiency. Moreover, the enantiomerically enriched crystals of phosphahelicenes emitted intense circularly polarized luminescence (CPL). Notably, the modulated CPL of racemic phosphahelicenes was induced by chiral transmission in the cholesteric mesophase, showing ultrahigh asymmetry factors of CPL (+0.51, -0.48). Our findings provide a new approach for the design of emissive phosphahelicenes towards chiral emitters and synthesized precursors., Competing Interests: The authors declare no conflict of interest., (This journal is © The Royal Society of Chemistry.)

Digital coherent receivers adopting joint clock recovery and adaptive equalization (JCA) can avoid failures of the adaptive equalizer (AEQ) or clock recovery algorithm (CRA) due to clock asynchrony and chromatic dispersion (CD). But in the previous JCA scheme, the AEQ has a heavy computational load as it has to generate two samples per symbol (SPS) for the subsequent timing phase error detector (TPED) which is the core of the CRA. Furthermore, the previous JCA scheme cannot compensate for receiver skew or accommodate Nyquist signals with small roll-off factors (ROFs). These shortcomings hinder its practical applications in ultrahigh-speed short-reach coherent transmission requiring low power consumption, high spectral efficiency, whilst being sensitive to receiver skew. To solve this problem, we propose a new JCA scheme by integrating a two-section real-valued (RV) AEQ with an all-digital feedback CRA based on a baud-rate TPED versatile for different ROFs. Experiments for 61-GBaud dual-polarization (DP) Nyquist 16QAM signals with an ROF of 0.01 show that, compared with the previous JCA scheme, the proposed scheme can reduce the AEQ computational load by about 70% for 10-km transmission, whilst improving the receiver sensitivity by more than 1.7 dB for a receiver skew of 1.5 ps. As far as we know, the proposed JCA scheme is the most comprehensive and efficient solution for ultrahigh-speed short-reach coherent transmission where CD, receiver skew, clock asynchrony, and Nyquist signals with small ROFs have to be dealt with.

Electrochemical conversion of CO 2 to formic acid using Bismuth catalysts is one the most promising pathways for industrialization. However, it is still difficult to achieve high formic acid production at wide voltage intervals and industrial current densities because the Bi catalysts are often poisoned by oxygenated species. Herein, we report a Bi 3 S 2 nanowire-ascorbic acid hybrid catalyst that simultaneously improves formic acid selectivity, activity, and stability at high applied voltages. Specifically, a more than 95% faraday efficiency was achieved for the formate formation over a wide potential range above 1.0 V and at ampere-level current densities. The observed excellent catalytic performance was attributable to a unique reconstruction mechanism to form more defective sites while the ascorbic acid layer further stabilized the defective sites by trapping the poisoning hydroxyl groups. When used in an all-solid-state reactor system, the newly developed catalyst achieved efficient production of pure formic acid over 120 hours at 50 mA cm -2 (200 mA cell current)., (© 2023. Springer Nature Limited.)

Introduction: The development of highly effective wound dressings is crucial for successful clinical applications. Achieving wound closure, preventing infection, and minimizing scarring are key objectives in wound healing. Drawing inspiration from the regenerative mechanisms observed in embryonic tissue repair, we designed a series of wound-contractible dressings with exceptional antibacterial properties., Methods: This was achieved by encapsulating quaternized silicone (QP12) and poly( N -isopropylacrylamide-co- N -hydroxymethylacrylamide-co-octadecyl acrylate) (PNNS) within electrospun nanofibers of poly(ε-caprolactone) (PCL)., Results and Discussion: The resulting nanofibrous dressings demonstrated remarkable thermo-responsive self-contraction and tissue adhesion capabilities, enabling secure adherence to the skin and active wound closure. Notably, these nanofibers exhibited potent antibacterial activity against both Gram-positive and Gram-negative bacteria. Furthermore, they possessed desirable properties such as hydrophilicity, biocompatibility and mechanical properties resembling human skin. A full-thickness skin defect model evaluation revealed that these temperature-sensitive nanofibers expedited wound closure, enhanced wound healing, and suppressed scar formation. This result was evidenced by reduced infiltration of inflammatory cells, well-organized collagen arrangement, and improved vascularization. In summary, we propose that these wound-contractible nanofibers, with their antibacterial and anti-scarring properties, hold great promise as an advanced solution for skin wound repair., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2023 Qi, Li, Wang, Hou and Li.)

Through isothermal hot compression experiments at various strain rates and temperatures, the thermal deformation behavior of Zn-2.0Cu-0.15Ti alloy is investigated. The Arrhenius-type model is utilized to forecast flow stress behavior. Results show that the Arrhenius-type model accurately reflects the flow behavior in the entire processing region. The dynamic material model (DMM) reveals that the optimal processing region for the hot processing of Zn-2.0Cu-0.15Ti alloy has a maximum efficiency of about 35%, in the temperatures range (493-543 K) and a strain rate range (0.01-0.1 s -1 ). Microstructure analysis demonstrates that the primary dynamic softening mechanism of Zn-2.0Cu-0.15Ti alloy after hot compression is significantly influenced by temperature and strain rate. At low temperature (423 K) and low strain rate (0.1 s -1 ), the interaction of dislocations is the primary mechanism for the softening Zn-2.0Cu-0.15Ti alloys. At a strain rate of 1 s -1 , the primary mechanism changes to continuous dynamic recrystallization (CDRX). Discontinuous dynamic recrystallization (DDRX) occurs when Zn-2.0Cu-0.15Ti alloy is deformed under the conditions of 523 K/0.1 s -1 , while twinning dynamic recrystallization (TDRX) and CDRX are observed when the strain rate is 10 s -1 .

A clock recovery algorithm (CRA) suitable for non-integer oversampled Nyquist signals with a small roll-off factor (ROF) is appealing to short-reach high-speed inter-datacenter transmission systems which need to cut down the transceiver power consumption and cost by reducing the oversampling factor (OSF) and using cheap low-bandwidth components. However, due to the lack of a suitable timing phase error detector (TPED), CRAs proposed now fail for non-integer OSFs below two and small ROFs close to zero and are not hardware-efficient. To solve these problems, we propose a low-complexity TPED by modifying the time-domain quadratic signal and reselecting the synchronization spectral component. We demonstrate that the proposed TPED, in combination with a piece-wise parabolic (PWP) interpolator, can significantly improve the performance of feedback CRAs for non-integer oversampled Nyquist signals with a small ROF. Numerical simulations and experiments show that, based on the improved CRA, the receiver sensitivity penalty can keep below 0.5 dB when the OSF is reduced from 2 to 1.25 and the ROF is varied from 0.1 to 0.001 for 45 GBaud dual-polarization Nyquist 16QAM signals.

Electrochemically reducing CO 2 to more reduced chemical species is a promising way that not only enables the conversion of intermittent energy resources to stable fuels, but also helps to build a closed-loop anthropogenic carbon cycle. Among various electrocatalysts for electrochemical CO 2 reduction, multifunctional metal-organic frameworks (MOFs) have been employed as highly efficient and selective heterogeneous electrocatalysts due to their ultrahigh porosity and topologically diverse structures. Up to now, great progress has been achieved in the design and synthesis of highly active and selective MOF-related catalysts for electrochemical CO 2 reduction reaction (CO 2 RR), and their corresponding reaction mechanisms have been thoroughly studied. In this review, we summarize the recent progress of applying MOFs and their derivatives in CO 2 RR, with a focus on the design strategies for electrocatalysts and electrolyzers. We first discussed the reaction mechanisms for different CO 2 RR products and introduced the commonly applied electrolyzer configurations in the current CO 2 RR system. Then, an overview of several categories of products (CO, HCOOH, CH 4 , CH 3 OH, and multi-carbon chemicals) generated from MOFs or their derivatives via CO 2 RR was discussed. Finally, we offer some insights and perspectives for the future development of MOFs and their derivatives in electrochemical CO 2 reduction. We aim to provide new insights into this field and further guide future research for large-scale applications., (© 2023. The Author(s).)

Uncontrolled bleeding and bacterial infections cause severe damage to the wounds and remain a clinical challenge. Here, we developed a nanofiber/sponge bilayered composite membrane (QCP) containing quaternized silicone (QP12) and quaternized chitosan (QCS12) by joint approaches of electrospinning and freeze-drying and investigated their potential for wound dressing. The QCP was composed of a sponge (QCC) containing collagen (COL) and QCS12 and a nanofibrous membrane (MQP) containing poly-ε-caprolactone (PCL) and QP12. The QCP composite membrane possessed feasible permeability (0.22 ± 0.01 g/(cm 2 ·24 h)), available thermal stability, suitable mechanical properties with natural skin, and in vivo hemostatic efficiency. The bonds of the N-quaternary and Schiff base endow composite membranes with significant anti-microbial invasion, potentially enhancing the wound healing process with an eligible microenvironment. Meanwhile, QCP evinced fine hemocompatibility, low cytotoxicity, negligible skin irritation, and other desirable biosafety as an excellent wound dressing. QCP promoted collagen deposition and re-epithelization to accelerate healing and suppress scars in the full-thickness acute wound models. Furthermore, the evaluation in the chronic skin incision model of diabetes mellitus manifested high healing efficiency with a certain resistance to bacterial infection of the composite membrane. Taken together, the QCP composite membrane may be a potential antibacterial and hemostatic wound dressing., 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 B.V. All rights reserved.)

The development of hydrogels as wound dressings has gained considerable attention due to their promising ability to promote wound healing. However, in many cases of clinical relevance, repeated bacterial infection, which might obstruct wound healing, usually occurs due to the lack of antibacterial properties of these hydrogels. In this study, we fabricated a new class of self-healing hydrogel with enhanced antibacterial properties based on dodecyl quaternary ammonium salt (Q12)-modified carboxymethyl chitosan (Q12-CMC), aldehyde group- modified sodium alginate (ASA), Fe 3+ via Schiff bases and coordination bonds (QAF hydrogels). The dynamic Schiff bases and coordination interactions conferred excellent self-healing abilities to the hydrogels, while the incorporation of dodecyl quaternary ammonium salt gave the hydrogels superior antibacterial properties. Additionally, the hydrogels displayed ideal hemocompatibility and cytocompatibility, crucial for wound healing. Our full-thickness skin wound studies demonstrated that QAF hydrogels could result in rapid wound healing with reduced inflammatory response, increased collagen disposition and improved vascularization. We anticipate that the proposed hydrogels, possessing both antibacterial and self-healing properties, will emerge as a highly desirable material for skin wound repair.

Marine organisms are threatened by various environmental contaminants, and nanoplastics (NPs) is one of the most concerned. Studied have shown that NPs has a certain impact on marine organisms, but the specific molecular mechanism is still unclear. At present, researches on the effect of NPs on marine life mostly focus on crustaceans, gastropods, and bivalves. In this study, cephalopod Sepia esculenta larvae were first used to investigate the potential immune response molecular mechanisms caused by PS-NPs (50 nm, 50 mg/L) short-term exposure (4 and 24 h). Through S. esculenta larvae transcriptome profile of gene expression analysis, 548 and 1990 genes showed differential expression at 4 and 24 h after NPs exposure, respectively. GO and KEGG enrichment analysis were performed to find immune related DEGs. Then, the interaction relationship between the immune related DEGs after NPs exposure was known through the constructed protein-protein interaction network. 20 hub genes were found on the base of KEGG pathway numbers involved and protein-protein interaction numbers. This research supply valuable genes for the study of cephalopod immune response caused by NPs, which can help us further uncover the molecular mechanisms of organism against NPs., Competing Interests: Declaration of competing interest We declare that we have no financial and personal relationships with other people or organizations., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Transition-metal-catalyzed Suzuki-Miyaura coupling has significantly advanced C-C bond formation and has been well recognized in organic synthesis, pharmaceuticals, materials science and other fields. In this rapid development, cross coupling without transition metal catalyst is a big challenge in this field, and using widely existing tertiary amines as electrophiles to directly couple with boronic acids has great hurdles yet significant application prospects. Herein, we report an efficient and general deaminative arylation and alkenylation of tertiary amines (propargyl amines, allyl amines and 1H-indol-3-yl methane amines) with ary and alkenylboronic acids enabled by difluorocarbene under transition-metal-free conditions. Preliminary mechanism experiments suggest that in situ formed difluoromethyl quaternary amine salt, nitrogen ylide and tetracoordinate boron species are the key intermediates, the subsequent 1,2-metallate shift and protodeboronation complete the new coupling reaction., (© 2022 Wiley-VCH GmbH.)

Background: In this study, we surveyed the prevalence of hepatitis B virus (HBV) surface antigen (HBsAg) and hepatitis C virus (HCV) antibody (anti-HCV) among inpatients with human immunodeficiency virus (HIV) infection and analyzed the correlated factors. Methods: We conducted a retrospective data collection of the HIV-infected inpatients in our hospital from January 2010 to December 2020. We utilized multivariate logistic regression to identify the correlated factors. Results: The proportion of patients screened for HBsAg was 81.8%, which increased from 66.7% in 2010 to 85.7% in 2020. The proportion of patients with anti-HCV screening was 73.9%, which increased from 58.3% in 2010 to 86.7% in 2020. The prevalence of HBsAg positivity was 10.9%, which decreased from 15.0% in the period of 2010−2015 to 9.0% during 2016−2020. Positive anti-HCV was identified in 4.1% of cases. Compared to 4.8% in the period of 2010−2015, there was a similar prevalence of anti-HCV at 3.1% during 2016−2020. Among the HBsAg-positive cases, HBV deoxyribonucleic acid was screened in 70.8% of cases. Among the anti-HCV positive cases, HCV ribonucleic acid (RNA) was screened in 90% of cases. Albumin < 30 g/L, thrombocytopenia and aspartate aminotransferase (AST) > 40 U/L were associated with HBsAg positivity. AST > 40 U/L and higher CD4-positive T lymphocyte counts were associated with HIV/HCV coinfection. Conclusions: The routine screening for both HBV and HCV among HIV-positive inpatients has been greatly improved in the past decade. However, screening for the complete HBV serological markers in HIV-positive inpatients and HCV genotyping among HCV RNA-positive cases leaves much to be desired. A concerted effort should be made to improve HBV vaccine compliance in the HIV-positive population and provide direct-acting antiviral therapies to HCV RNA-positive patients.

While stem cell transplantation has emerged as a promising approach to improving wound healing outcomes, the application of stem cells to date has been limited by the poor survival and retention of these cells once transplanted. The survival, development, and migratory activity of transplanted cells can be improved through the use of three-dimensional (3D) culture systems. Here, a novel alginate microsphere-collage hydrogel (AMS-Col gel) 3D culture system was developed and found to improve human umbilical cord mesenchymal stem cell (hUCMSC) survival, permitting their sustained release so as to promote wound healing. Through hematoxylin and eosin staining and Masson's trichrome staining, the prepared hUCMSCs-AMS-Col gel was found to exhibit wound healing activity. On day 7 following the hUCMSCs-AMS-Col gel treatment of model wounds, improved collagen fiber deposition and re-epithelialization were evident, with complete epithelial regeneration as of day 14 and near-total wound healing was evident as of day 21. This hUCMSCs-AMS-Col gel was also associated with increased VEGF and FGF2 expression. Together, these data indicate that AMS-Col gels are a promising and novel form of 3D cell culture system capable of improving hUCMSC-mediated wound healing, highlighting the potential clinical utility of this regenerative strategy., 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 © 2022 Elsevier B.V. All rights reserved.)

Background: Previous studies have found that the dissemination pattern and delivery mechanism of information can provide crucial resources and empowerment for individuals to the promotion of health literacy. The present study investigates how health information sources are associated with health literacy among older adults in west China, and tries to explain the mechanisms underlying the link between health information sources and health literacy in the Chinese context., Methods: The cross-sectional study employed a representative sample of 812 urban citizens aged 60 and older in 2017 in Western China., Results: We found that health information sources including healthcare practitioners (B = 4.577, p < 0.001), neighbors (B = 2.545, p < 0.05), newspapers (B = 4.280, p < 0.001), and television (B = 4.638, p < 0.001) were positively associated with health literacy. Additionally, age (B = -1.781, p < 0.001) was negatively associated with health literacy, and the socio-economic status factors including minority (B = -10.005, p < 0.001), financial strain status of perceived very difficult (B = -10.537, p < 0.001), primary school (B = 11.461, p < 0.001), junior high school (B = 18.016, p < 0.001), polytechnic school or senior high school (B = 21.905, p < 0.001), college and above (B = 23.433, p < 0.001) were significantly linked to health literacy, and suffering from chronic diseases (B = 3.430, p < 0.01) was also positively related to health literacy., Conclusions: Health information sources including healthcare practitioners, neighbors, newspapers, and television have a strong influence on health literacy, which implies that the four main types of sources are the important patterns of health information dissemination in the reinforcement of health literacy. In addition, the present findings also indicate age, minority and disease differences in health literacy and confirm the influence of enabling factors including educational attainment and financial strain on health literacy. Based on these findings and their implications, specific evidence is presented for the reinforcement of health literacy in interpersonal and mass communication, and in the educational and financial settings in the Chinese context. The present results also suggest that the age-specific, minority-specific and disease-specific measures should be taken to promote health literacy among older adults.

Objectives: This study aimed to investigate the changes in serum levels of retinol-binding protein 4 (RBP4) with cerebral infarction, relationship of RBP4 with oxidative stress and carotid atherosclerosis, and its possible role in cerebral infarction., Materials and Methods: According to the results of cervical vascular ultrasound, the experimental group was divided into three groups: intima thickening group ( n = 31), stable plaque group ( n = 51), and unstable plaque group ( n = 54). Forty healthy subjects were selected as the control group. Their serum levels of RBP4, 8-iso-prostaglandin-F2alpha (8-iso-PGF2α), and catalase (CAT) were measured. Carotid vascular ultrasound was used to measure the plaque area and intima-media thickness (IMT)., Results: The serum RBP4 and 8-iso-PGF2α levels, IMT and plaque area in the control, intimal thickening, stable plaque, and unstable plaque groups increased, while the serum level of CAT decreased ( P < 0.001). The serum levels of RBP4 positively correlated with 8-iso-PGF2α, IMT, and plaque area and negatively correlated with CAT level. The area under the receiver operating characteristic curve was 0.778 in predicting unstable plaques., Conclusions: The serum levels of RBP4 were significantly elevated in elderly patients with cerebral infarction and correlated with oxidative stress injury and the degree of atherosclerosis. Serum RBP4 has diagnostic value for unstable plaques in carotid arteries., Competing Interests: Conflict of 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 article., (© 2022 Qingqing Wang et al., published by De Gruyter.)

A versatile digital coherent receiver capable of handling optical signals with different kinds of pulse shaping schemes (PSSs) is indispensable for future flexible and heterogeneous coherent optical communication networks. Therefore, a low-complexity timing phase error detector (TPED) versatile for all PSSs is of particular interest. In this paper, we propose a TPED suitable for both Nyquist signals with different roll-off factors and non-Nyquist signals. It requires two samples per symbol and involves no multiplications. As far as we know, it has the lowest computation complexity compared with the existing TPEDs used in coherent systems, while incurring no receiver sensitivity penalty. Numerical simulations and experiments are carried out to demonstrate the superior timing performance and PSS versatility of the proposed TPED in both open-loop and closed-loop working conditions. We also implement the novel TPED in a field programmable gate array (FPGA) and verify its real-time clock recovery performance using the 10 Gbaud very low roll-off Nyquist and non-Nyquist quadrature phase shift keying (QPSK) signals.

Background: Rhabdomyolysis is a serious and potentially life threatening condition that can be caused by drugs. We report a case of acute hepatitis B with rhabdomyolysis after treatment with rosuvastatin and entecavir., Case Presentation: A 72-year-old female was admitted to our hospital due to acute hepatitis B infection. She had taken atorvastatin for 3 months before being admitted to our hospital. After being administered entecavir (ETV) and rosuvastatin to replace atorvastatin, she suffered from muscle pain in both lower limbs and was diagnosed with rhabdomyolysis. After discontinuation of the two drugs, the patient's symptoms subsided and creatine kinase levels returned to normal. We hypothesize that the rhabdomyolysis was caused by the combination of rosuvastatin and ETV., Conclusions: We suggest that patients who use rosuvastatin and ETV be made aware of the complication of rhabdomyolysis., (© 2022. The Author(s).)

Backgound: Low-density lipoprotein (LDL) cholesterol can lead to the occurrence of atherosclerotic plaques, but patients with normal LDL still have atherosclerotic plaques in clinical practice. With the proposal of LDL subclass, this experiment investigated the relationship between the LDL content of different subclasses and the stability of carotid plaques., Methods: Plaque stability was suggested by carotid ultrasound results. 37 patients with stable plaques were classified into one group and 41 patients with unstable plaques were classified into another group. The data of age, glycosylated hemoglobin (Ghb), and homocysteine (Hcy) were collected. The contents of LDL subclasses were measured by LIPOPRINT system. The data of total cholesterol (TC), LDL cholesterol, and triglyceride (TG) were collected. The plaque stability was assessed by carotid artery color Doppler ultrasound and the intima-media thickness (IMT) was measured., Results: The levels of LDL-1 subclass 19.00 (13.00, 27.50) and LDL-2 subclass (21.62 ± 7.24) in the stable plaque group were higher than those in the unstable plaque group ( p < 0.05). The levels of LDL-3 subclass (12.24 ± 4.58), LDL-4 subclass 5.00 (2.00, 9.00), and sd-LDL 0 (0.00, 3.00) in the unstable plaque group were higher than those in the stable plaque group ( p < 0.05). LDL-1 subclass (adjusted OR = 0.923 and p < 0.05), and LDL-3 subclass (adjusted OR = 1.176 and p < 0.05) were independent risk factors for plaque stability., Conclusion: Elevated LDL1 is associated with stable plaques whereas LDL3 was found associated with unstable plaques., Competing Interests: Conflict of interest: Authors state no conflict of interest., (© 2022 Zhanhai Pan et al., published by De Gruyter.)

The electrochemical N 2 reduction reaction (NRR) demonstrates a process of NH 3 synthesis from N 2 molecules under ambient conditions, which is environmentally friendly and recyclable. However, it requires an efficient electrocatalyst to activate inert N 2 molecules, which is still difficult to satisfy. Recently, as an active NRR electrocatalyst and a typical metal oxide, CeO 2 has featured ultrahigh thermal stability and the ability to apply heteroatom doping, which is an imperative approach importing oxygen vacancy by replacing metal ions with selective elements to greatly influence the activity of catalysts. Here, we analyze the unique properties of manganese dopants in modulating the activity of CeO 2 nanospheres for NRR. It attains a larger NH 3 yield of 27.79 μg h -1 mg cat -1 and a higher Faradaic efficiency of 9.1% than pure CeO 2 at -0.30 V in 0.1 M HCl, with high electrochemical and structure stability. With calculations by density functional theory, the performance enhancement of Mn-doped CeO 2 is also proved mathematically.

Developing ultrasensitive and user-friendly methods for the detection glucose has attracted more and more attention. By virtue of high selectivity and sensitivity, enzyme-based glucose sensor plays a key role in point-of-care sensing technology for detecting glucose concentration. In this study, Amplex Red (AR), as both indicator and mediator, was investigated to detect glucose in presence of glucose oxidase (GOx) enzymes using colorimetric and electrochemical methods. Without using any advanced techniques and sophisticated nanomaterials, 1 μM glucose can be easily detected through simply detecting the solution color with a visual colorimetric method. On the other hand, the electrochemical method can provide much higher sensitivity for the detection of glucose, which achieves a linear range spanning from 20 nM to 3.56 μM with a limit of 7.3 nM (signal-to-noise ratio SNR = 3). It is also found that the presence of other sugars such as fructose, lactose, and maltose have very limited interference effects on the detection of glucose. More importantly, a bare GC electrode was used in all these electrochemical measurements without any electrode surface modification, guaranteeing a simple and fast operation. The analytical platforms for the detection of glucose presented here not only provide simple, fast, and ultrasensitive methods, but also have the potential to advance the sensing technology in the application of other health diagnostic research areas. Amplex Red (AR) was reported as both an indicator and mediator for the sensitive and specific determination of glucose using the colorimetric and electrochemical methods. The detection limit was 1 μM glucose by the visual colorimetric methods. A bare glassy carbon electrode without any functional modification was employed for the detection as low as 20 nM glucose with LOD of 7.3 nm (SNR = 3) in the electrochemical method., (© 2021. Springer-Verlag GmbH Germany, part of Springer Nature.)

The lattice strain of a perovskite film is vital to the controllable growth and charge transport in perovskite solar cells (PSCs). In this work, a lead chloride (PbCl 2 ) assisted crystallization (LCAC) protocol is introduced for releasing the strain across the interface of a NiO x /perovskite, which induces a preferred ( h 00) crystal plane growth and grain homogenization. PSCs with LCAC show a facilitated charge extraction and suppressed nonradiative recombination. Thanks to the controlled film growth and strain-released interface, the inverted MAPbI 3 (MA = methylammonium) PSC devices with LCAC deliver a power conversion efficiency (PCE) over 20% with a short-circuit current density ( J sc ) of 23.60 mA cm -2 , which is obviously higher than that of the control device with a PCE of 18.36% and a J sc of 21.74 mA cm -2 . Meanwhile, the LCAC devices maintain 80% of their initial efficiency after being exposed to an ambient atmosphere with a relative humidity of 40% over 1000 h in the dark.

The present study aimed to observe the effect of socio-economic status on health information literacy and to identify whether there is a social gradient for health information literacy among urban older adults in Western China. This study employed a cross-sectional research design, and 812 urban participants aged 60 and older were enrolled in Western China. In the current study, only 16.7% of urban older adults reported having adequate health information literacy. Binary logistic regression analysis showed that socio-economic status factors including educational attainment, ethnicity, and financial strain were significantly and tightly associated with health information literacy. Additionally, other factors including suffering from chronic diseases, information-seeking activity, reading magazines and books, and watching television were also significantly linked to health information literacy. Consistent with existing studies, the findings indicate the health information literacy deficit and demonstrate the crucial impact of socio-economic status on health information literacy, which implies a social gradient in health information literacy. The importance of other factors related to health information literacy are discussed as well. The results suggest that reducing the health information literacy deficit and social gradient in health information literacy must be considered as an important priority when developing public health and health education strategies, programs, and actions among urban older adults in Western China.

Particle pollution has been a research topic attracting the attention of the researchers around the world because inhalable particles are hazardous to humans and the environment. The major resource of particle pollution is the combustion of coal and biomass. Dust collectors, electrostatic precipitators, and bag filters are required to remove particles from flue. Because of the large specific surface areas of inhalable particles, they easily agglomerate to form larger aggregates; therefore, improving the capture efficiency of dust collectors is of importance. Herein, chemical agglomeration agents were sprayed into a turbulent agglomeration chamber to improve the removal efficiency of inhalable particles. The results showed that the total removal efficiency of inhalable particles was 59.2% for the three-composition agglomeration agents of kappa carrageenans/Tween-80/NH 4 Cl (KC/TW/NH 4 Cl). The mean particle diameter increased from 2.8 μm before agglomeration to above 10.0 μm after agglomeration. In the agglomeration process, nonionic TW accelerates the wetting properties, in which the polymer, KC, or anion polyacrylamide, promotes prolongation of the contact time between droplets and particles. Two different removal mechanisms are proposed to explain the effect of chemical agglomeration agents. Immersion agglomeration described the agglomeration process of only fine particles, and distribution agglomeration supported the capture of large particles for fine ones in polydispersed aerosols., Competing Interests: The authors declare no competing financial interest.

The microstructures, mechanical properties, and thermal conductivity (TC) of Al-2Fe- x Co ( x = 0~0.8) alloys in as-cast, homogeneous annealed, and cool rolled states are systematically studied. Results indicate that appropriate Co modification ( x ≤ 0.5) simultaneously improves the thermal and mechanical properties of as-cast Al-2Fe alloys. The improvement of TC is attributed to ameliorating the morphology of primary Al 3 Fe phases from needles to short rods and fine particles, which decreases the scattering probability of free electrons during the electronic transmission. However, further increasing the Co content ( x = 0.8) decreases the TC due to the formation of a coarse plate-like Al 2 FeCo phase. Besides, the thermal conductivity of annealed Al-2Fe- x Co alloys is higher than that of as-cast alloys because of the elimination of lattice defects and spheroidization of Al 3 Fe phases. After cool rolling with 80 % deformation, thermal conductivity of alloys slightly increases due to the breaking down of Al 2 FeCo phases. The rolled Al-2Fe-0.3Co alloy exhibits the highest thermal conductivity, which is about 225 W/(m·K), approximately 11 % higher than the as-cast Al-2Fe sample. The ultimate tensile strength (UTS) and elongation (EL) of as-cast Al-2Fe-0.5Co (UTS: 138 MPa; EL: 22.0 %) are increased by 35 % and 69 %, respectively, compared with those of unmodified alloy (UTS: 102 MPa; EL: 13.0 %).

Organic-inorganic metal halide perovskite solar cells (PSCs) have recently been considered as one of the most competitive contenders to commercial silicon solar cells in the photovoltaic field. The deposition process of a perovskite film is one of the most critical factors affecting the quality of the film formation and the photovoltaic performance. A hot-casting technique has been widely implemented to deposit high-quality perovskite films with large grain size, uniform thickness, and preferred crystalline orientation. In this review, we first review the classical nucleation and crystal growth theory and discuss those factors affecting the hot-casted perovskite film formation. Meanwhile, the effects of the deposition parameters such as temperature, thermal annealing, precursor chemistry, and atmosphere on the preparation of high-quality perovskite films and high-efficiency PSC devices are comprehensively discussed. The excellent stability of hot-casted perovskite films and integration with scalable deposition technology are conducive to the commercialization of PSCs. Finally, some open questions and future perspectives on the maturity of this technology toward the upscaling deposition of perovskite film for related optoelectronic devices are presented.

Industrially, artifical N 2 fixation to NH 3 mainly relies on the Haber-Bosch process which is operated in a harsh environment with large energy consumption and heavy serious greenhouse gas emission. Electrochemical N 2 reduction offers a carbon-neutral and energy-saving method for NH 3 synthesis under ambient conditions. Herein, we demonstrate the first use of ZrO 2 nanoparticles as an earth-abundant electrocatalyst for NH 3 synthesis from N 2 and water under ambient conditions. In 0.1 M HCl, the electrocatalyst presents a large NH 3 yield rate of 24.74 μg h -1 mg cat. -1 with a faradaic efficiency of 5.0% at -0.45 V vs. the reversible hydrogen electrode. It also demonstrates high electrochemical stability and excellent selectivity for NH 3 generation.

The fabrication of efficient and convenient photocatalytic H 2 evolution systems is a fascinating research topic in the field of solar energy conversion. A ternary self-assembled photocatalytic H 2 evolution system was fabricated through supramolecular host-guest chemistry. The system consisted of the H 2 evolution catalyst [Co(dmgH) 2 (4-ppy) 2 ]NO 3 (1; dmgH 2 =dimethylglyoxime, 4-ppy=4-phenylpyridine) and the photosensitizer Eosin Y (EY) assembled with the macrocyclic compound cucurbit[7]uril (CB[7]) to form the 1@CB[7]/EY complex through inclusion and exclusion interactions, respectively. The synchronous self-assembly drives an orthogonal arrangement of the 1@CB[7]/EY system. The inclusion complex 1@CB[7] was successfully characterized by 1 H NMR spectroscopy and single-crystal XRD. The exclusion process of CB[7] with EY was identified by NMR titration and the optimized geometry of the exclusion structure was determined by DFT calculations. The use of CB[7] resulted in a 6-fold increase in turnover number, a 3-fold increase in turnover frequency, and a 3-fold extension of lifetime for photocatalytic H 2 evolution as compared with the system in the absence of CB[7]. The improvement of the light-driven H 2 evolution activity was ascribed to the ability of CB[7] to link the photosensitizer and catalyst., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Background: We report a rare case of chronic brucellosis accompanied with myelodysplastic syndrome and neutrophilic dermatosis, which to the best of our knowledge, has never been reported., Case Presentation: A young man was admitted to our hospital complaining of recurrent fever, arthritis, rashes and anemia. He had been diagnosed with brucellosis 6 years prior and treated with multiple courses of antibiotics. He was diagnosed with myelodysplastic syndrome and neutrophilic dermatosis following bone marrow puncture and skin biopsy. After anti-brucellosis treatment and glucocorticoid therapy, the symptoms improved., Conclusions: Clinicians should consider noninfectious diseases when a patient who has been diagnosed with an infectious disease exhibits changing symptoms.

Titanium-based catalysts are needed to achieve electrocatalytic N 2 reduction to NH 3 with a large NH 3 yield and a high Faradaic efficiency (FE). One of the cheapest and most abundant metals on earth, iron, is an effective dopant for greatly improving the nitrogen reduction reaction (NRR) performance of TiO 2 nanoparticles in ambient N 2 -to-NH 3 conversion. In 0.5 m LiClO 4 , Fe-doped TiO 2 catalyst attains a high FE of 25.6 % and a large NH 3 yield of 25.47 μg h -1  mg cat -1 at -0.40 V versus a reversible hydrogen electrode. This performance compares favorably to those of all previously reported titanium- and iron-based NRR electrocatalysts in aqueous media. The catalytic mechanism is further probed with theoretical calculations., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The artificial N2 fixation to NH3 is dominated by the traditional Haber-Bosch process, which consumes large amounts of energy and natural gas with low energy efficiency and large amounts of CO2 emissions. Electrochemical N2 reduction is a promising and environmentally friendly route for artificial N2-to-NH3 fixation under milder conditions. Herein, we report that dendritic Cu acts as a highly active electrocatalyst to catalyze N2 to NH3 fixation under ambient conditions. When tested in 0.1 M HCl, such an electrocatalyst achieves a high faradaic efficiency of 15.12% and a large NH3 yield rate of 25.63 μg h-1 mgcat.-1 at -0.40 V versus a reversible hydrogen electrode. Notably, this catalyst shows high electrochemical stability and excellent selectivity toward NH3 synthesis.

Excellent nonlinear optical materials simultaneously meet the requirements of large SHG response, phase-matching capability, wide transparency windows, considerable energy band-gap, good thermal stability and structure stability. Herein, two new promising nonlinear optical (NLO) crystals LiM II (IO 3 ) 3 (M II =Zn and Cd) are rationally designed by the aliovalent substitution strategy from the commercialized α-LiIO 3 with the perfect parallel alignment of IO 3 groups. Compared with parent α-LiIO 3 and related A I 2 M IV (IO 3 ) 6 , the title compounds exhibit more stable covalent 3D structure, and overcome the racemic twinning problem of A I 2 M IV (IO 3 ) 6 . More importantly, both compounds inherit NLO-favorable structure merits of α-LiIO 3 and show larger SHG response (≈14× and ≈12×KDP), shorter absorption edge (294 and 297 nm) with wider energy band-gap (4.21 and 4.18 eV), good thermal stability (460 and 430 °C), phase-matching behaviors, wider optical transparency window and good structure stability, achieving an excellent balance of NLO properties., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Hot-casting is a promising technique of depositing high-quality organic-inorganic hybrid perovskite thin films with large crystal grain size. Here, we reported the that the crystallinity and grain size of perovskite films could be systematically tailored by modulating the stoichiometry of the precursor solution in the hot-casting process under ambient condition with a relative humidity of 40%. It was found that a slight excess of methylammonium iodide (MAI) in the precursor solution could effectively compensate the MAI loss due to the high substrate temperature. A significant increase in the grain size and crystallinity of the perovskite film was observed together with a decrease in defect density and a carrier concentration enhancement in MAI-rich samples. The corresponding devices exhibited a notable increase in fill factor (up to 80.70%) and short-circuit current density. In addition, in MAI-deficient samples, an enrichment of PbI 2 at the grain boundaries was directly observed by optical microscopy and laser confocal microscopy. Time-resolved photoluminescence spectroscopy revealed an increase in the charge carrier lifetime in the MAI-deficient samples, which was in line with the previous results with a small amount of excess PbI 2 in the perovskite film. This work highlights a new strategy to prepare high-quality perovskite thin films with excellent crystal quality under ambient condition.

The production of ammonia (NH 3 ) in the industrial scale basically relies on the traditional technology of Haber-Bosch, which is operated under harsh conditions with high energy consumption and a huge number of greenhouse gas emissions. Electrochemical N 2 reduction reaction (NRR) is a promising route for artificial N 2 -to-NH 3 fixation with less energy consumption. However, an effective electrocatalyst, as a prerequisite of the NRR, is of significance. Here, we report that a spinel LiMn 2 O 4 nanofiber acts as a noble-metal-free electrocatalyst for NH 3 synthesis with excellent performance under ambient conditions. The electrocatalyst, which was tested in 0.1 M HCl, has an excellent Faradaic efficiency of 7.44% and a NH 3 yield of 15.83 μg h -1 mg cat. -1 at -0.50 V versus reversible hydrogen electrode. Moreover, it also possesses excellent electrochemical and structure stability.

In this study, Fe-bearing Mg-3%Al alloys were inoculated by combining carbon with or without Ca. Both processes can significantly refine the grain size of Mg-3%Al alloys. The highest refining efficiency can be obtained by carbon combined with Ca. The synergistic grain refining efficiency can be attributed to the constitutional undercooling produced by the addition of Ca. Two kinds of carbon-containing nuclei with duplex-phase particles and cluster particles were observed in the carbon-inoculated alloys. A thermodynamic model was established to disclose the formation mechanisms of the duplex-phase particles and Al 4 C 3 cluster particles. This thermodynamic model is based on the change of Gibbs free energy for the formation of these two kinds of particles. The calculated results show that these two particles can form spontaneously, since the change of Gibbs free energy is negative. However, the Gibbs free change of the duplex-phase particle is more negative than the Al 4 C 3 cluster particle. This indicates that the adsorption process is more spontaneous than the cluster process, and tiny Al 4 C 3 particles are preferred to form duplex-phase particle, rather than gathering to form an Al 4 C 3 cluster particle. In addition, the addition of Ca can reduce the interfacial energy between the Al 4 C 3 phase and the Al-Fe phase and promote the formation of duplex-phase particles.

To evaluate the influence of transition metal substituents on the characteristics of CH 3 NH 3 PbI 3 /TiO 2 , we investigated the geometrical and electronic properties of transition metal-substituted CH 3 NH 3 PbI 3 /TiO 2 by first-principles calculations. The results suggested that the substitution of Ti 4+ at the five-fold coordinated (Ti 5c ) sites by transition metals is energetically favored. The substituted interface has enhanced visible light sensitivity and photoelectrocatalytic activity by reducing the transition energies. The transition metal substitution can effectively tune the band gap of the interface, which significantly improves the photo-reactivity. The substituted systems are expected to be more efficient in separating the photo-generated electrons-holes and active in the visible spectrum., Competing Interests: The authors declare no conflict of interest.

The synthesis of NH3 heavily relies on the Haber-Bosch process suffering from a large amount of CO2 emission and energy consumption. Possessing eco-friendly and sustainable characteristics, electrochemical reduction is considered as a promising candidate for artificial N2 fixation under ambient conditions, but efficient electrocatalysts are crucial for the N2 reduction reaction (NRR). In this communication, we report that perovskite La2Ti2O7 nanosheets behave as an efficient NRR electrocatalyst with excellent selectivity under ambient conditions. In 0.1 M HCl, this catalyst achieves a high NH3 yield rate of 25.15 μg h-1 mgcat.-1 with a faradaic efficiency of 4.55% at -0.55 V vs. a reversible hydrogen electrode. Notably, it also shows high electrochemical stability.

Background: The oblique-supine position for percutaneous nephrolithotomy (PCNL) has advantages, but the position fixation methods are inadequate. This study aimed to analyze the PCNL outcomes using a patented self-made frame for oblique-supine position., Methods: This was a prospective study of patients scheduled to undergo PCNL at 2 hospitals in China between November 2009 and December 2016. The patients underwent PCNL in the oblique-supine position using the self-made position frame (n = 94). Operative time, stone clearance rate, intraoperative average systolic pressure, intraoperative average heart rate, intraoperative average airway pressure, intraoperative average intrapelvic pressure, and complications were observed., Results: The patients were 45.3 ± 19.7 years old and 71% were male. Stones were of the size 2.5 ± 1.1 cm. The operative time was 95.6 min and the stone clearance rate was 81.9%. Intraoperative systolic blood pressure was 15.13 ± 1.68 kPa. Intraoperative airway pressure was 15.5 ± 2.3 cm H2O. Postoperative fever was observed in 3.2% of the patients. None had organ injury. Postoperative stay was 4.8 ± 0.6 days. The nephrostomy tube was routinely removed on the 5th day after surgery and the patients were discharged on the following day., Conclusion: The self-made surgical position frame met the position requirements for the oblique-supine PCNL operation. This surgical position frame deserves clinical application and promotion., (© 2019 S. Karger AG, Basel.)

Objective: To investigate the value of 'swallow-tail' sign and putaminal hypointensity on 3 T susceptibility-weighted imaging (SWI) for distinguishing multiple system atrophy (MSA) from idiopathic Parkinson's disease (IPD)., Methods: Three groups - 39 MSA patients, 18 IPD patients,and 31 healthy controls (HCs) - were administered a 3 T SWI sequence to evaluate 'swallow-tail' sign and putaminal hypointensity using visual scales from 0 to 2 and 0 to 3 scores, respectively. The diagnostic accuracy of the two signs separately and combined was calculated using a receiver operating characteristic curve, with clinical diagnosis as the gold standard., Results: The scores of 'swallow-tail' sign were lower in IPD than in MSA or in HCs, as well as for putaminal hypointensity in IPD or HCs than in MSA (p < 0.05). The sensitivity and specificity of 'swallow-tail' sign and putaminal hypointensity were 87.9% and 83.3%, and 35.9% and 100%, respectively, in the respective patient groups. The area under the curve of combined signs was increased from 0.85 ('swallow tail') or 0.68 (putaminal hypointensity) to 0.93., Conclusion: The combination of 'swallow-tail' sign and putaminal hypointensity can increase the accuracy of discriminating between MSA and IPD., Key Points: • Differential diagnosis of MSA and IPD is still challenging in clinical practice. • Absence of 'swallow-tail' sign is a valuable biomarker for IPD on SWI. • Putaminal hypointensity is a valuable biomarker for MSA on SWI. • Combined 'swallow- tail' sign and putaminal hypointensity increase diagnostic accuracy.