Selectivity Control by Relay Catalysis in CO and CO2 Hydrogenation to Multicarbon Compounds.

ConspectusThe hydrogenative conversion of both CO and CO2 into high-value multicarbon (C2+) compounds, such as olefins, aromatic hydrocarbons, ethanol, and liquid fuels, has attracted much recent attention. The hydrogenation of CO is related to the chemical utilization of various carbon resources including shale gas, biomass, coal, and carbon-containing wastes via syngas (a mixture of H2 and CO), while the hydrogenation of CO2 by green H2 to chemicals and liquid fuels would contribute to recycling CO2 for carbon neutrality. The state-of-the-art technologies for the hydrogenation of CO/CO2 to C2+ compounds primarily rely on a direct route via Fischer-Tropsch (FT) synthesis and an indirect route via two methanol-mediated processes, i.e., methanol synthesis from CO/CO2 and methanol to C2+ compounds. The direct route would be more energy- and cost-efficient owing to the reduced operation units, but the product selectivity of the direct route via FT synthesis is limited by the Anderson-Schulz-Flory (ASF) distribution. Selectivity control for the direct hydrogenation of CO/CO2 to a high-value C2+ compound is one of the most challenging goals in the field of C1 chemistry, i.e., chemistry for the transformation of one-carbon (C1) molecules.We have developed a relay-catalysis strategy to solve the selectivity challenge arising from the complicated reaction network in the hydrogenation of CO/CO2 to C2+ compounds involving multiple intermediates and reaction channels, which inevitably lead to side reactions and byproducts over a conventional heterogeneous catalyst. The core of relay catalysis is to design a single tandem-reaction channel, which can direct the reaction to the target product controllably, by choosing appropriate intermediates (or intermediate products) and reaction steps connecting these intermediates, and arranging optimized yet matched catalysts to implement these steps like a relay. This Account showcases representative relay-catalysis systems developed by our group in the past decade for the synthesis of liquid fuels, lower (C2-C4) olefins, aromatics, and C2+ oxygenates from CO/CO2 with selectivity breaking the limitation of conventional catalysts. These relay systems are typically composed of a metal or metal oxide for CO/CO2/H2 activation and a zeolite for C-C coupling or reconstruction, as well as a third or even a fourth catalyst component with other functions if necessary. The mechanisms for the activation of H2 and CO/CO2 on metal oxides, which are distinct from that on the conventional transition or noble metal surfaces, are discussed with emphasis on the role of oxygen vacancies. Zeolites catalyze the conversion of intermediates (including hydrocracking/isomerization of heavier hydrocarbons, methanol-to-hydrocarbon reactions, and carbonylation of methanol/dimethyl ether) in the relay system, and the selectivity is mainly controlled by the Brønsted acidity and the shape-selectivity or the confinement effect of zeolites. We demonstrate that the thermodynamic/kinetic matching of the relay steps, the proximity and spatial arrangement of the catalyst components, and the transportation of intermediates/products in sequence are the key issues guiding the selection of each catalyst component and the construction of an efficient relay-catalysis system. Our methodology would also be useful for the transformation of other C1 molecules via controlled C-C coupling, inspiring more efforts toward precision catalysis.

Spinel Nanostructures for the Hydrogenation of CO2 to Methanol and Hydrocarbon Chemicals.

Composite oxides have been widely applied in the hydrogenation of CO/CO2 to methanol or as the component of bifunctional oxide-zeolite for the synthesis of hydrocarbon chemicals. However, it is still challenging to disentangle the stepwise formation mechanism of CH3OH at working conditions and selectively convert CO2 to hydrocarbon chemicals with narrow distribution. Here, we investigate the reaction network of the hydrogenation of CO2 to methanol over a series of spinel oxides (AB2O4), among which the Zn-based nanostructures offer superior performance in methanol synthesis. Through a series of (quasi) in situ spectroscopic characterizations, we evidence that the dissociation of H2 tends to follow a heterolytic pathway and that hydrogenation ability can be regulated by the combination of Zn with Ga or Al. The coordinatively unsaturated metal sites over ZnAl2Ox and ZnGa2Ox originating from oxygen vacancies (OVs) are evidenced to be responsible for the dissociative adsorption and activation of CO2. The evolution of the reaction intermediates, including both carbonaceous and hydrogen species at high temperatures and pressures over the spinel oxides, has been experimentally elaborated at the atomic level. With the integration of a series of zeolites or zeotypes, high selectivities of hydrocarbon chemicals with narrow distributions can be directly produced from CO2 and H2, offering a promising route for CO2 utilization.

Ultralong Bistable, Electrolytic MnO2-Based, Electrochromic Battery Enabled by Porous, Low-Barrier, Hydroxylated TiO2 Interface.

Electrochromic (EC) battery technology shows great potential in future "zero-energy building" by controlling outdoor solar transmission to tune heat gain as well as storing the consumed energy to reuse across other building systems. However, challenges still exist in exploring an electrochemical system to satisfy requirements on both ultra-long optical memory (also called bistability) without continuous power supply and high energy density. Herein, an EC battery is proposed to demonstrate ultra-long bistability (>760 h) based on the reversible deposition and dissolution of manganese oxide (MnO2) without the addition of any mediators. A porous low-barrier hydroxylated titanium dioxide (TiO2) interface is incorporated to synergistically enrich Mn2+-affinity active sites for deposition and effectively reduce the electron transport barrier of MnO2 for dissolution, thereby significantly improving the reversibility, high optical modulation (60.2% at 400 nm), and energy density (352 mAh m-2). The modification strategy is also verified on the cathode-less button cells with a much higher average coulombic efficiency (99.9%) compared to the batteries without the porous hydroxylated TiO2 interface (74.6%). These achievements lay a foundation for advancements in both electrochromism and Zn-Mn aqueous batteries.

Preparing Coordination Polymers with Acentric-Centric Structural Arrangements Related to SHG Response.

Three coordination polymers were successfully constructed in this work by applying biligands and were distinctly characterized through single crystal X-ray diffraction. The compounds crystallized in acentric and centric space groups under the direction of coordination bonds and adopted 1-dimensional link and 2-dimensional layer structures, as well as different coordination geometries for metal atoms. All compounds exhibited good thermal stability and luminescence properties, and compound 2 exhibited a good second harmonic generation (SHG) response. The method used in this work offers a feasible approach to using biligand and changing metal salt to obtain the microstructures of coordination materials with specific properties.

Study on OSA screening and influencing factors in community-based elderly hypertensive patients based on single-lead wearable ECG devices.

PURPOSE: Assessing whether single-lead ECG can be effectively and relatively inexpensively used in large-scale OSA screening, and identifying factors influencing moderate-to-severe OSA among elderly hypertensive patients without atypical symptoms in primary care. METHODS: The study gathered data from 15 medical institutions in Ningxia between January and December 2022 using cloud platforms. The dataset included basic information and 72-h ECG monitoring for 2573 hypertensive patients over 65. OSA screening was conducted using the single-lead wearable ECG devices based on the ACAT algorithm. A multivariable logistic regression identified the main factors affecting OSA severity in these patients, and the AUC was used to assess the model's predictive accuracy. RESULTS: The study found an OSA detection rate of 87.10%, with 55.42% being moderate to severe cases. Key risk factors associated with developing moderate-to-severe OSA included cardiac irregularities like supraventricular extrasystole and atrioventricular block, male gender, lifestyle factors like alcohol consumption and smoking, and health indicators such as SDNN ≤ 100 ms, abnormal LF/HF ratio, BMI, and age. The model's accuracy for predicting OSA, indicated by a ROAUC of 0.625, was moderate. Factors like gender, tea consumption, stroke history, and ventricular tachycardia were also independently linked to OSA severity. CONCLUSION: This study combines single-lead wearable ECG devices with the ACAT algorithm for OSA screening in Ningxia, China. Initial screening identified 87.10% of participants as having OSA, with 55.42% being moderate to severe cases. This suggests a convenient, low-cost, and repeatable ECG-based method for OSA screening, potentially improving early detection and management of OSA by identifying potential risk factors.

Risk Factors and Predictive Efficacy of Visceral Pleural Invasion in Lung Adenocarcinoma Patients with mGGN type.

Objective: To explore the risk factors and predictive effects of visceral pleural invasion in lung adenocarcinoma patients with mGGN type, in order to identify high-risk groups of visceral pleural invasion early, and to provide more references for targeted intervention and individualized treatment adjustment of high-risk groups based on the analysis of risk factors. Methods: The clinical data of 135 patients with mGGN-type lung adenocarcinoma who received surgical treatment in our hospital from January 2018 to December 2022 were selected from our hospital's medical record database for retrospective analysis. The patient information was entered by a two-person summary and analyzed after verification.The patients were divided into invasion group (60 cases) and non-invasion group (75 cases) according to the invasion of pleural viscera, which was helpful to analyze the difference of clinical features between the two groups. The independent risk factors for visceral pleural invasion in patients with mGGN lung adenocarcinoma were evaluated using univariate and multivariate factor methods, and receiver operating characteristic (ROC) curves were drawn to evaluate the clinical efficacy of these risk factors above alone and in combination in predicting of visceral pleural invasion risk. The larger the area under ROC curve, the higher the corresponding sensitivity and specificity, and the greater the predictive value for the risk of visceral pleural invasion in mGGN lung adenocarcinoma patients. Results: Univariate analysis showed that gender, family history of hypertension, location of focus, maximum diameter of solid component, proportion of solid component, pleural indentation, burr sign, bronchial and nodular route may be related to visceral pleural invasion in lung adenocarcinoma patients with mGGN type (P < .05). Multivariate Logistic regression analysis showed that pleural indentation (OR=2.49, 95%CI:1.17~4.58, P < .001) and abnormal broncho-nodular travel (OR=3.06, 95%CI: 1.35~7.02, P = .01) were the independent risk factors for visceral pleural invasion in lung adenocarcinoma patients with mGGN type (P < .05). ROC curve analysis results showed that pleural indentation (AUC=0.70, 95%CI: 0.65~0.79, P = .02), abnormal bronchial and nodular running relationship (AUC=0.74, 95%CI: 0.69~0.81, P = .01) could both be used to predict the visceral pleural invasion risk in lung adenocarcinoma patients with mGGN type, and combined prediction efficacy of both indexes (AUC=0.90, 95%CI: 0.85~0.97, P < .001) was better than single index. Conclusion: The occurrence of visceral pleural infiltration in patients with mGGN lung adenocarcinoma is related to the relationship between pleural indentation and bronchus and nodules. Combined with the above indicators, the risk of visceral pleural infiltration in patients can be effectively predicted, and early intervention and treatment can be performed on high-risk patients accordingly to effectively prevent and treat visceral pleural infiltration.

Hyperkalemia burden and treatment patterns in Chinese patients on hemodialysis: final analysis of a prospective multicenter cohort study (PRECEDE-K).

OBJECTIVES: Patients with end-stage renal disease (ESRD) on hemodialysis (HD) are at risk for hyperkalemia (HK), associated with cardiac arrhythmia and sudden death. Data on the burden of HK and management techniques among HD patients in China are still scarce. This study assessed the treatment modalities, recurrence, and prevalence of HK in Chinese HD patients. METHODS: In this prospective cohort study conducted from May 2021 to July 2022, patients aged ≥18 years who had ESRD and were on HD were enrolled from 15 centers in China (up to 6 months). RESULTS: Overall, 600 patients were enrolled. At the baseline visit, mean (± standard deviation) urea reduction ratio was 68.0% ± 9.70 and Kt/V was 1.45 ± 0.496. Over 6 months, 453 (75.5%) patients experienced HK, of whom 356 (78.6%) recurred. Within 1, 2, 3, 4, 5, and 6 months, 203 (44.8%), 262 (57.8%), 300 (66.2%), 326 (72.0%), 347 (76.6%), and 356 (78.6%) patients had at least one HK recurrence event, respectively. The proportions of patients with ≥1, 2, 3, 4, 5, or 6 HK recurrence events were 356 (78.6%), 306 (67.5%), 250 (55.2%), 208 (45.9%), 161 (35.5%), and 110 (24.3%), respectively. Among the 453 patients who experienced HK, only 24 (5.3%) were treated with potassium binders: seven (1.5%) with sodium polystyrene sulfonate, 13 (2.9%) with calcium polystyrene sulfonate, and six (1.3%) with sodium zirconium cyclosilicate. CONCLUSION: Since HK is a chronic illness, long-term care is necessary. Patients on HD should have effective potassium management on non-dialysis days, yet our real-world population rarely used potassium binders. TRIAL REGISTRATION: ClinicalTrials.gov Identifier NCT04799067.

Selective Oxidation of Methane to Methanol over Au/H-MOR.

Selective oxidation of methane to methanol by dioxygen (O2) is an appealing route for upgrading abundant methane resource and represents one of the most challenging reactions in chemistry due to the overwhelmingly higher reactivity of the product (methanol) versus the reactant (methane). Here, we report that gold nanoparticles dispersed on mordenite efficiently catalyze the selective oxidation of methane to methanol by molecular oxygen in aqueous medium in the presence of carbon monoxide. The methanol productivity reaches 1300 µmol gcat-1 h-1 or 280 mmol gAu-1 h-1 with 75% selectivity at 150 °C, outperforming most catalysts reported under comparable conditions. Both hydroxyl radicals and hydroperoxide species participate in the activation and conversion of methane, while it is shown that the lower affinity of methanol on gold mainly accounts for higher methanol selectivity.

Synergistic Interaction of Dual-Polymer Networks Containing Viologens-Anchored Poly(ionic liquid)s Enabling Long-Life and Large-Area Electrochromic Organogels.

Viologens-based electrochromic (EC) devices with multiple color changes, rapid response time, and simple all-in-one architecture have aroused much attention, yet suffer from poor redox stability caused by the irreversible aggregation of free radical viologens. Herein, the semi-interpenetrating dual-polymer network (DPN) organogels are introduced to improve the cycling stability of viologens-based EC devices. The primary cross-linked poly(ionic liquid)s (PILs) covalently anchored with viologens can suppress irreversible face-to-face contact between radical viologens. The secondary poly(vinylidenefluoride-co-hexafluoropropylene) (PVDF-HFP) chains with strong polar groups of -F can not only synergistically confine the viologens by the strong electrostatic effect, but also improve the mechanical performance of the organogels. Consequently, the DPN organogels show excellent cycling stability (87.5% retention after 10 000 cycles) and mechanical flexibility (strength of 3.67 MPa and elongation of 280%). Three types of alkenyl viologens are designed to obtain blue, green, and magenta colors, demonstrating the universality of the DPN strategy. Large-area EC devices (20 × 30 cm) and EC fibers based on organogels are assembled to demonstrate promising applications in green and energy-saving buildings and wearable electronics.

Stretchable, Electrochemically-Stable Electrochromic Devices Based on Semi-Embedded Ag@Au Nanowire Network.

Stretchable electrochromic (EC) devices that can adapt the irregular and dynamic human surfaces show promising applications in wearable display, adaptive camouflage, and visual sensation. However, challenges exist in lacking transparent conductive electrodes with both tensile and electrochemical stability to assemble the complex device structure and endure harsh electrochemical redox reactions. Herein, a wrinkled, semi-embedded Ag@Au nanowire (NW) networks are constructed on elastomer substrates to fabricate stretchable, electrochemically-stable conductive electrodes. The stretchable EC devices are then fabricated by sandwiching a viologen-based gel electrolyte between two conductive electrodes with the semi-embedded Ag@Au NW network. Because the inert Au layer inhibits the oxidation of Ag NWs, the EC device exhibits much more stable color changes between yellow and green than those with pure Ag NW networks. In addition, since the wrinkled semi-embedded structure is deformable and reversibly stretched without serious fractures, the EC devices still maintain excellent color-changing stability under 40% stretching/releasing cycles.

Electrocatalytic Reduction of CO2 Coupled with Organic Conversion to Selectively Synthesize High-Value Chemicals.

The electrochemical process of coupling electrocatalytic CO2 reduction and organic conversion reaction can effectively reduce the reaction overpotential and obtain value-added chemicals. Moreover, because of the diversity of substrates and the designability of coupling forms, more and more attention has been paid to this field. This review systematically summarizes the research progress of coupling electrolysis in recent years, (1) co-electrolysis of CO2 and organics at the cathode to obtain specific products with high selectivity, (2) replacing traditional anodic oxygen evolution reaction (OER) with other valuable oxidation reactions to improve energy utilization efficiency and economic benefits of CO2 conversion, (3) in an electrolytic cell without membrane, the cathode and anode jointly transform CO2 and organics to redox products. We hope that the examples and insights on coupling electrolysis introduced in this review can inspire researchers to further explore and innovate in this direction.

Central GLP-1 Resistance Induced by Severe Traumatic Brain Injury Was Associated with Persistent Hyperglycemia in Humans.

INTRODUCTION: Whether central glucagon-like peptide 1 (GLP-1)/GLP-1 receptor system mediated peripheral glucose homeostasis in patients with traumatic brain injury (TBI) is not clear. We aim to determine if plasma GLP-1 level could distinguish the non-survivors from the survivors during the first 14 days after TBI that could prognose 6 months mortality. METHODS: Metabolic, inflammatory, and hematologic profiles were examined in 73 patients with TBI in neurological intensive care unit. Factors that discriminate non-survivors from survivors were determined by two-way ANOVA. Biomarkers associated with mortality were determined by binary logistic regression and Cox proportional hazard regression. RESULTS: The non-survivors had higher infectious SOFA scores (p < 0.001), lower first 3 days' body temperature (p = 0.017), greater chance of cerebral hernia (p = 0.048), and decompressive craniectomy (p = 0.001) than the survivors. Higher 14-day plasma GLP-1 (p < 0.0001), glucose (p = 0.002), and IL-6 (p = 0.005) levels, in contrast with lower insulin level at days 4-7 (p = 0.020) were found in non-survivors than in survivors. Except the survivors who had an increased 14-day platelet number (p < 0.001), the two groups did not differ in hematological profile and intestinal barrier function. Although GLP-1 correlated closely with IL-6 in both the groups, it correlated with neither insulin nor glucose in each group. GLP-1 on days 8-10 and IL-6 on days 1-3 were positively, while insulin on days 4-7 was negatively associated with mortality. CONCLUSION: Persistent higher GLP-1 level in non-survivors over the survivors may present more severe central resistance to endogenous GLP-1 in non-survivors, which may be associated with progressive hyperglycemia with increased mortality in TBI.

Hyperkalaemia prevalence and dialysis patterns in Chinese patients on haemodialysis: an interim analysis of a prospective cohort study (PRECEDE-K).

BACKGROUND: Hyperkalaemia is a known risk factor for cardiac arrhythmia and mortality in patients on haemodialysis. Despite standard adequate haemodialysis, hyperkalaemia is common in patients with end-stage renal disease (ESRD) at interdialytic intervals. Data on hyperkalaemia burden and its effects on dialysis patterns and serum potassium (sK) fluctuations in patients on haemodialysis in China remain limited. The prospective, observational cohort study (PRECEDE-K; NCT04799067) investigated the prevalence, recurrence, and treatment patterns of hyperkalaemia in Chinese patients with ESRD on haemodialysis. METHODS: Six hundred adult patients were consecutively enrolled from 15 secondary and tertiary hospitals in China. In this interim analysis, we report the baseline characteristics of the cohort, the prevalence of predialysis hyperkalaemia (sK > 5.0 mmol/L), and the trends in serum-dialysate potassium gradient and intradialytic sK shift at Visit 1 (following a long interdialytic interval [LIDI]). RESULTS: At baseline, most patients (85.6%) received three-times weekly dialysis; mean duration was 4.0 h. Mean urea reduction ratio was 68.0% and Kt/V was 1.45; 60.0% of patients had prior hyperkalaemia (previous 6 months). At Visit 1, mean predialysis sK was 4.83 mmol/L, and 39.6% of patients had hyperkalaemia. Most patients (97.7%) received a dialysate potassium concentration of 2.0 mmol/L. The serum-dialysate potassium gradient was greater than 3 mmol/L for over 40% of the cohort (1- < 2, 2- < 3, 3- < 4, and ≥ 4 mmol/L in 13.6%, 45.1%, 35.7%, and 5.2% of patients, respectively; mean: 2.8 mmol/L). The intradialytic sK reduction was 1- < 3 mmol/L for most patients (0- < 1, 1- < 2, 2- < 3, and ≥ 3 mmol/L in 24.2%, 62.2%, 12.8%, and 0.9% of patients, respectively; mean: 1.4 mmol/L). CONCLUSIONS: Hyperkalaemia after a LIDI was common in this real-world cohort of Chinese patients despite standard adequate haemodialysis, and led to large serum-dialysate potassium gradients and intradialytic sK shifts. Previous studies have shown hyperkalaemia and sK fluctuations are highly correlated with poor prognosis. Effective potassium-lowering treatments should be evaluated for the improvement of long-term prognosis through the control of hyperkalaemia and sK fluctuations. TRIAL REGISTRATION: ClinicalTrials.gov, NCT04799067.

Prognostic Significance of Plasma Insulin Level for Deep Venous Thrombosis in Patients with Severe Traumatic Brain Injury in Critical Care.

BACKGROUND: Whether insulin resistance underlies deep venous thrombosis (DVT) development in patients with severe traumatic brain injury (TBI) is unclear. In this study, the association between plasma insulin levels and DVT was analyzed in patients with severe TBI. METHODS: A prospective observational study of 73 patients measured insulin, glucose, glucagon-like peptide 1 (GLP-1), inflammatory factors, and hematological profiles within four preset times during the first 14 days after TBI. Ultrasonic surveillance of DVT was tracked. Two-way analysis of variance was used to determine the factors that discriminated between patients with and without DVT or with and without insulin therapy. Partial correlations of insulin level with all the variables were conducted separately in patients with DVT or patients without DVT. Factors associated with DVT were analyzed by multivariable logistic regression. Neurological outcomes 6 months after TBI were assessed. RESULTS: Among patients with a mean (± standard deviation) age of 53 (± 16 years), DVT developed in 20 patients (27%) on median 10.4 days (range 4-22), with higher Acute Physiology and Chronic Health Evaluation II scores but similar Sequential Organ Failure Assessment scores and TBI severity. Patients with DVT were more likely to receive insulin therapy than patients without DVT (60% vs. 28%; P = 0.012); hence, they had higher 14-day insulin levels. However, insulin levels were comparable between patients with DVT and patients without DVT in the subgroups of patients with insulin therapy (n = 27) and patients without insulin therapy (n = 46). The platelet profile significantly discriminated between patients with and without DVT. Surprisingly, none of the coagulation profiles, blood cell counts, or inflammatory mediators differed between the two groups. Patients with insulin therapy had significantly higher insulin (P = 0.006), glucose (P < 0.001), and GLP-1 (P = 0.01) levels and were more likely to develop DVT (60% vs. 15%; P < 0.001) along with concomitant platelet depletion. Insulin levels correlated with glucose, GLP-1 levels, and platelet count exclusively in patients without DVT. Conversely, in patients with DVT, insulin correlated negatively with GLP-1 levels (P = 0.016). Age (P = 0.01) and elevated insulin levels at days 4-7 (P = 0.04) were independently associated with DVT. Patients with insulin therapy also showed worse Glasgow Outcome Scale scores (P = 0.001). CONCLUSIONS: Elevated insulin levels in the first 14 days after TBI may indicate insulin resistance, which is associated with platelet hyperactivity, and thus increasing the risk of DVT.

Review on descaling and anti-scaling technology of heat exchanger in high-salt wastewater thermal desalination.

Thermal desalination evaporation of high-salt wastewater has been widely used in industry because of the proposed concept of 'zero liquid discharge'. However, due to the high content of Ca2+ and Mg2+ in high-salt wastewater, the heat exchanger, as the main treatment equipment, suffers from serious scaling problems. This review presents descaling and scale inhibition technologies of high-salt wastewater. The advantages and disadvantages of various technologies are summarized and analyzed to provide theoretical support for the research of descaling and anti-scaling of heat exchangers with high-salt wastewater. In future industrial development, the synergistic application of electromagnetic water treatment technology and scale inhibitors can significantly improve the anti-scaling effect, which can reach over 95% stably. Furthermore, the addition of a physical field can also expand the application range of scale inhibitors.

Differentiated expressed miRNAs in splenic monocyte induced by burn injury in mice.

To find potential biomarkers based on miRNA and their potential targets in splenic monocytes in burn-injured mice. Male Balb/c mice were subjected to sham or scalding injury of 15% total body surface area. Spenic CD11b+ monocytes were purified with magnetic beads. The monocytes were cultured in the presence of lipopolysaccharide. The proliferation of monocytes was detected by MTT assay, and the cytokines in the supernatant were examined by enzyme linked immunosorbent assay. The purified monocytes were also under total RNA extraction. The differential monocytic miRNAs expression between the sham and burn-injured mice was analysed by miRNA microarray. The activity of monocytes was comparable between the two groups (p > 0.05). However, monocytes from burn-injured mice secreted higher levels of tumour necrosis factor (TNF)-α and transforming growth factor-ß, but lower level of monocyte chemoattratctant protein-1. A total of 54 miRNAs were differentially expressed in monocytes from burn relative to sham-injured mice (fold >3). Further quantitative reverse transcription polymerase chain reaction confirmed that the expression of miR-146a was significantly down-regulated, while miR-3091-6p was up-regulated after burn injury. Using the combination of Miranda and TargetScan softwares, we found that mir-146a may regulate 180 potential target genes including TNF receptor related factor 6 (TRAF6), interleukin-1 receptor related kinase 1 (IRAK1) and CD28. Mir-3091-6p may regulate 39 potential targets, including SOCS7 (cytokine signal transduction inhibitor 7) and ARRB2 (arrestin, ß 2). The miRNAs expressed by monocytes after burn injury may be involved in the regulation of innate immune response in burn injury.

A Nanocomposite of Bismuth Clusters and Bi2 O2 CO3 Sheets for Highly Efficient Electrocatalytic Reduction of CO2 to Formate.

The renewable-electricity-driven CO2 reduction to formic acid would contribute to establishing a carbon-neutral society. The current catalyst suffers from limited activity and stability under high selectivity and the ambiguous nature of active sites. Herein, we report a powerful Bi2 S3 -derived catalyst that demonstrates a current density of 2.0 A cm-2 with a formate Faradaic efficiency of 93 % at -0.95 V versus the reversible hydrogen electrode. The energy conversion efficiency and single-pass yield of formate reach 80 % and 67 %, respectively, and the durability reaches 100 h at an industrial-relevant current density. Pure formic acid with a concentration of 3.5 mol L-1 has been produced continuously. Our operando spectroscopic and theoretical studies reveal the dynamic evolution of the catalyst into a nanocomposite composed of Bi0 clusters and Bi2 O2 CO3 nanosheets and the pivotal role of Bi0 -Bi2 O2 CO3 interface in CO2 activation and conversion.

Photo-Driven Iron-Induced Non-Oxidative Coupling of Methane to Ethane.

Photo-driven CH4 conversion to multi-carbon products and H2 is attractive but challenging, and the development of efficient catalytic systems is critical. Herein, we construct a solar-energy-driven redox cycle for combining CH4 conversion and H2 production using iron ions. A photo-driven iron-induced reaction system was developed, which is efficient at selective coupling of CH4 as well as conversion of benzene and cyclohexane under mild conditions. For CH4 conversion, 94 % C2 selectivity and a C2 H6 formation rate of 8.4 µmol h-1 is achieved. Mechanistic studies reveal that CH4 coupling is induced by hydroxyl radical, which is generated by photo-driven intermolecular charge migration of an Fe3+ complex. The delicate coordination structure of the [Fe(H2 O)5 OH]2+ complex ensures selective C-H bond activation and C-C coupling of CH4 . The produced Fe2+ can be used to reduce the potential for electrolytic H2 production, and then turns back into Fe3+ , forming an energy-saving and sustainable recyclable system.

Electrochemical Actuators with Multicolor Changes and Multidirectional Actuation.

Electrochemical (EC) actuators have garnered significant attention in recent years, yet there are still some critical challenges to limit their application range, such as responsive time, multifunctionality, and actuating direction. Herein, an EC actuator with a back-to-back structure is fabricated by stacking two membranes with bilayer V2 O5 nanowires/single-walled carbon nanotubes (V2 O5 NWs/SWCNTs) networks, and shows a synchronous high actuation amplitude (about ±9.7 mm, ±28.4°) and multiple color changes. In this back-to-back structure, the inactive SWCNTs layer is used as a conductive current collector, and the bilayer network is attached to a porous polymer membrane. The dual-responsive processes of V2 O5 nanowires (V2 O5 NWs) actuation films and actuators are also deeply investigated through in situ EC X-ray diffraction and Raman spectroscopy. The results show that the EC actuation of the V2 O5 NWs/SWCNTs film is highly related to the redox behavior of the pseudocapacitive V2 O5 NWs layer. At last, both V2 O5 NWs and W18 O49 nanowires (W18 O49 NWs)-based EC actuators are constructed to demonstrate the multicolor changes and multidirectional actuation induced by the opposite lattice changes of V2 O5 NWs and W18 O49 NWs during ionic de-/intercalation, guiding the design of multifunctional EC actuators in the future.

Exendin-4 Exacerbates Burn-Induced Mortality in Mice by Switching to Th2 Response.

INTRODUCTION: To determine if Exendin-4 could be a therapeutic agent for burn-induced hyperglycemia. MATERIALS AND METHODS: Male Balb/c mice received a bolus of Exendin-4 intraperitoneally immediately after 15% total body surface area scald injury. Tail glucose levels were recorded and T-cell functions were analyzed at 4 h and 24 h postburn (pb). Pancreatic pathology was observed consecutively. The secretions of cytokines were detected in serum, spleen, and lung. Apoptosis of splenic CD3+ T-cells was examined by terminal deoxynucleotidyl transferase-mediated dUTP nick-end labeling and flow cytometry. RESULTS: Although Exendin-4 could attenuate burn-induced hyperglycemia in mice at 4 h pb, it accelerated their survival dose dependently with progressive depletion of splenocyte number. T-cell function underwent two-phasic changes following Exendin-4 treatment. Compared to placebo mice, T-cell from Exendin-4-treated mice was manifested with increased proliferation, while decreased IL-2 secretion and lower ratio of IL-4/IFN-γ at 4 h pb. However, at 24 h pb, it showed decreased proliferation, while increased IL-2 secretion and higher ratio of IL-4/IFN-γ. Exendin-4 could elicit higher circulating IL-6 and IL-10 levels at 4 h pb, which were pronounced in the lung at 24 h pb. In the meanwhile, severe inflammation could be found in the pancreas. At 24 h pb, the numbers of terminal deoxynucleotidyl transferase-mediated dUTP nick-end labeling or caspase-3 positive cells and the apoptosis of CD3+ T-cells were significantly increased in the spleens of Exendin-4 mice relative to placebo mice. CONCLUSIONS: These data support a pathogenic role of Exendin-4 signaling during thermal injury, warning against its clinical application in acute insults.