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1.
Infect Dis Poverty ; 13(1): 29, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38622750

RESUMO

BACKGROUND: Culex pipiens pallens and Culex pipiens quinquefasciatus are the dominant species of Culex mosquitoes in China and important disease vectors. Long-term use of insecticides can cause mutations in the voltage-gated sodium channel (vgsc) gene of mosquitoes, but little is known about the current status and evolutionary origins of vgsc gene in different geographic populations. Therefore, this study aimed to determine the current status of vgsc genes in Cx. p. pallens and Cx. p. quinquefasciatus in China and to investigate the evolutionary inheritance of neighboring downstream introns of the vgsc gene to determine the impact of insecticides on long-term evolution. METHODS: Sampling was conducted from July to September 2021 in representative habitats of 22 provincial-level administrative divisions in China. Genomic DNA was extracted from 1308 mosquitoes, the IIS6 fragment of the vgsc gene on the nerve cell membrane was amplified using polymerase chain reaction, and the sequence was used to evaluate allele frequency and knockdown resistance (kdr) frequency. MEGA 11 was used to construct neighbor-joining (NJ) tree. PopART was used to build a TCS network. RESULTS: There were 6 alleles and 6 genotypes at the L1014 locus, which included the wild-type alleles TTA/L and CTA/L and the mutant alleles TTT/F, TTC/F, TCT/S and TCA/S. The geographic populations with a kdr frequency less than 20.00% were mainly concentrated in the regions north of 38° N, and the geographic populations with a kdr frequency greater than 80.00% were concentrated in the regions south of 30° N. kdr frequency increased with decreasing latitude. And within the same latitude, the frequency of kdr in large cities is relatively high. Mutations were correlated with the number of introns. The mutant allele TCA/S has only one intron, the mutant allele TTT/F has three introns, and the wild-type allele TTA/L has 17 introns. CONCLUSIONS: Cx. p. pallens and Cx. p. quinquefasciatus have developed resistance to insecticides in most regions of China. The neighboring downstream introns of the vgsc gene gradually decreased to one intron with the mutation of the vgsc gene. Mutations may originate from multiple mutation events rather than from a single origin, and populations lacking mutations may be genetically isolated.


Assuntos
Culex , Culicidae , Inseticidas , Piretrinas , Canais de Sódio Disparados por Voltagem , Animais , Inseticidas/farmacologia , Íntrons/genética , Mosquitos Vetores/genética , Culex/genética , Mutação , Canais de Sódio Disparados por Voltagem/genética , Resistência a Inseticidas/genética
2.
PLoS Negl Trop Dis ; 18(1): e0011883, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-38198451

RESUMO

Rocky Mountain spotted fever is a tick-borne disease that is highly dangerous but often overlooked by the public. To prevent the spread of the disease, it is important to understand the distribution patterns of its vectors' suitable areas. This study aims to explore the potential global suitability of areas for the vectors of Rocky Mountain spotted fever, including Dermacentor variabilis and Amblyomma cajennense under both historical and future climate scenarios. The study also seeks to investigate the impact of climatic factors on the distribution patterns of these vectors. Data on species distribution were downloaded from the Global Biodiversity Information Facility, Web of Science and PubMed database. The climatic variables were downloaded from WorldClim Global Climate Database. The Maximum Entropy Model was used to evaluate the contribution of monthly precipitation, monthly maximum temperature, monthly minimum temperature, elevation, and nineteen other climatic variables to vector survival, as well as to predict the suitable area for the vectors. We found that D. variabilis is distributed in North America, while A. cajennense is mainly distributed in South America, but all other continents except Antarctica have a suitable distribution. D. variabilis is more likely to survive in temperate regions, and A. cajennense is more likely to survive in tropical zones. D. variabilis is more sensitive to temperature, whereas A. cajennense is sensitive to both temperature and precipitation, and A. cajennense prefers tropical regions with hot and humid characteristics. The high suitable areas of both vectors were almost expanded in the ssp5-8.5 scenario, but not so much in the ssp1-2.6 scenario. Highly suitable areas with vectors survival should be strengthened with additional testing to prevent related diseases from occurring, and other highly suitable areas should be alert for entry and exit monitoring to prevent invasion and colonization of vectors.


Assuntos
Febre Maculosa das Montanhas Rochosas , Doenças Transmitidas por Carrapatos , Humanos , Febre Maculosa das Montanhas Rochosas/epidemiologia , Mudança Climática , Biodiversidade , América do Norte
3.
Adv Mater ; 35(40): e2304716, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37392073

RESUMO

Indirect electrocatalytic conversion of cheap organic raw materials via the activation of S─H and N─H bonds into the value-added S─N/S─S bonds chemicals for industrial rubber production is a promising strategy to realize the atomic economic reaction, during which the kinetic inhibition that is associated with the electron transfer at the electrode/electrolyte interface in traditional direct electrocatalysis can be eliminated to achieve higher performance. In this work, a series of di-copper-substituted phosphotungstatebased foams (PW10 Cu2 @CMC) are fabricated with tunable loadings (17 to 44 wt%), which can be successfully applied in indirect electrocatalytic syntheses of sulfenamides and disulfides. Specifically, the optimal PW10 Cu2 @CMC (44 wt%) exhibits excellent electrocatalytic performance for the construction of S─N/S─S bonds (yields up to 99%) coupling with the efficient production of H2 (≈50 µmol g-1  h-1 ). Remarkably, it enables the scale-up production (≈14.4 g in a batch experiment) and the obtained products can serve as rubber vulcanization accelerators with superior properties to traditional industrial rubber additives in real industrial processes. This powerful catalysis system that can simultaneously produce rubber vulcanization accelerator and H2 may inaugurate a new electrocatalytic avenue to explore polyoxometalate-based foam catalysts in electrocatalysis field.

4.
J Comput Chem ; 44(4): 581-593, 2023 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-36326119

RESUMO

Si69 and Si75, typical commodities of silane coupling agents, are often employed in tire recipes to work as the bridges connecting silica and polymers, with which rolling resistance and wet traction are enhanced without loss in abrasion resistance. In this article, the reactivities of Si69 and Si75 with silica and various rubbers were theoretically investigated by using density functional theory (DFT). When the agents were coupled with silica, not only the acid+water condition but also the pure acid condition was confirmed to readily trigger the condensation reactions. The corresponding Gibbs free energy barriers were related to the charge distributions of reaction regions. As the agents suffered from the homolysis of central SS bonds, the generated single-S-tailer radicals (RS·) showed significantly higher reactivities of both the radical addition and the α-H transfer reactions with rubbers, due to the stronger radical philicities of the terminal sulfur radicals with larger condensed local softnesses [s0 (S)]. When the agents underwent the heterolysis of central SS bonds, the terminal sulfur anions with smaller s- (S) indices, however, facilitated the nucleophilic addition reactions with rubbers. Several derivative indices based on the condensed local softnesses were also proposed here to shed light on the reactivities from the viewpoint of the relationship between energy barriers and electronic characteristics. The above findings pave the way for the design of new kinds of silane coupling agents using computer-aided techniques, and meanwhile, provide references for the practical application of Si69 and Si75 to the silica/rubbers systems.

5.
Molecules ; 27(14)2022 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-35889275

RESUMO

Soluble sulfur (S8) and insoluble sulfur (IS) have different application fields, and molecular dynamics simulation can reveal their differences in solubility in solvents. It is found that in the simulated carbon disulfide (CS2) solvent, soluble sulfur in the form of clusters mainly promotes the dissolution of clusters through van der Waals interaction between solvent molecules (CS2) and S8, and the solubility gradually increases with the increase in temperature. However, the strong interaction between polymer chains of insoluble sulfur in the form of polymer hinders the diffusion of IS into CS2 solvent, which is not conducive to high-temperature dissolution. The simulated solubility parameter shows that the solubility parameter of soluble sulfur is closer to that of the solvent, which is consistent with the above explanation that soluble sulfur is easy to dissolve.


Assuntos
Dissulfeto de Carbono , Simulação de Dinâmica Molecular , Polímeros , Solubilidade , Solventes , Enxofre
6.
Front Psychiatry ; 13: 737972, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35370838

RESUMO

Background: Depression-related mortality and morbidity pose growing public health burdens worldwide. Although the therapeutic effect of exogenous melatonin on depression has been investigated, findings remain inconsistent. We conducted this systematic review and meta-analysis to clarify the effectiveness of melatonin in the treatment of depression, including primary and secondary depression symptoms. Methods: We searched the online databases of PubMed, EMBASE, and the Cochrane Library for original studies published up to May 2021. We used STATA 14.0 software to synthesize the results of included studies. To evaluate the effectiveness of melatonin, we calculated the standardized mean differences (SMDs) and 95% confidence intervals (CIs) of depression scores between the melatonin and placebo groups. Results: Our literature search returned 754 publications, among which 19 studies with 1,178 patients (715 women, 463 men; mean age: 56.77 years) met inclusion criteria. Melatonin dosages ranged from 2 to 25 mg per day; treatment durations were between 10 days and 3.5 years. Our synthesized results showed that melatonin was not found significantly beneficial for alleviating depressive symptoms (SMD = -0.17, 95% CI = [-0.38, 0.05]). Subgroup analysis demonstrated that the decrease in depression scores measured with the Beck Depression Inventory (BDI) was significant (SMD = -0.52, 95% CI = [-0.73, -0.31]). Conclusions: There is very limited evidence for effects of melatonin on depression.

7.
Biology (Basel) ; 11(1)2022 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-35053104

RESUMO

Ixodes scapularis is a vector of tick-borne diseases. Climate change is frequently invoked as an important cause of geographic expansions of tick-borne diseases. Environmental variables such as temperature and precipitation have an important impact on the geographical distribution of disease vectors. We used the maximum entropy model to project the potential geographic distribution and future trends of I. scapularis. The main climatic variables affecting the distribution of potential suitable areas were screened by the jackknife method. Arc Map 10.5 was used to visualize the projection results to better present the distribution of potential suitable areas. Under climate change scenarios, the potential suitable area of I. scapularis is dynamically changing. The largest suitable area of I. scapularis is under SSP3-7.0 from 2081 to 2100, while the smallest is under SSP5-8.5 from 2081 to 2100, even smaller than the current suitable area. Precipitation in May and September are the main contributing factors affecting the potential suitable areas of I. scapularis. With the opportunity to spread to more potential suitable areas, it is critical to strengthen surveillance to prevent the possible invasion of I. scapularis.

8.
Infect Dis Poverty ; 11(1): 12, 2022 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-35074010

RESUMO

BACKGROUND: Overseas imported dengue fever is an important factor in local outbreaks of this disease in the mainland of China. To better prevent and control such local outbreaks, the epidemiological characteristics and temporal-spatial distribution of overseas imported dengue fever cases in provincial-level administrative divisions (PLADs) where dengue fever is outbreak in the mainland of China were explored. METHODS: Using the Chinese National Notifiable Infectious Disease Reporting Information System (CNNDS), we identified overseas imported dengue fever cases in dengue fever outbreak areas in the mainland of China from 2005 to 2019 to draw the epidemic curve and population characteristic distribution of overseas imported cases in each PLAD. Based on spatial autocorrelation analysis of ArcGIS 10.5 and temporal-spatial scanning analysis of SaTScan 9.5, we analyzed the temporal-spatial distribution of overseas imported dengue fever in dengue fever outbreak areas in the mainland of China. RESULTS: A total of 11,407 imported cases, mainly from Southeast Asia, were recorded from 2005 to 2019 in these 13 PLADs. Of which 62.1% were imported into Yunnan and Guangdong Provinces. Among the imported cases, there were more males than females, mainly from the 21-50 age group. The hot spots were concentrated in parts of Yunnan, Guangdong and Fujian Provinces. We found the cluster of infected areas were expanding northward. CONCLUSIONS: Based on the analysis of overseas imported dengue cases in 13 PLADs of the mainland of China from 2005 to 2019, we obtained the epidemiological characteristics and spatial distribution of imported dengue cases. Border controls need to pay attention to key population sectors, such as 21-50 years old men and education of key populations on dengue prevention. There is a need to improve the awareness of the prevention and control of imported cases in border areas. At the same time, northern regions cannot relax their vigilance.


Assuntos
Dengue , Epidemias , Adulto , China/epidemiologia , Dengue/epidemiologia , Surtos de Doenças , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Análise Espacial , Adulto Jovem
9.
Front Public Health ; 10: 1018327, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36684875

RESUMO

Background: Peromyscopsylla hesperomys and Orchopeas sexdentatus are regarded to be representative plague vectors in the United States. The incidence of plague is rising globally, possibly due to climate change and environmental damage. Environmental factors such as temperature and precipitation have a significant impact on the temporal and spatial distribution of plague vectors. Methods: Maximum entropy models (MaxEnt) were utilized to predict the distributions of these two fleas and their trends into the future. The main environmental factors influencing the distribution of these two fleas were analyzed. A risk assessment system was constructed to calculate the invasion risk values of the species. Results: Temperature has a significant effect on the distribution of the potentially suitable areas for P. hesperomys and O. sexdentatus. They have the potential to survive in suitable areas of China in the future. The risk assessment system indicated that the risk level for the invasion of these two species into China was moderate. Conclusion: In order to achieve early detection, early interception, and early management, China should perfect its monitoring infrastructure and develop scientific prevention and control strategies to prevent the invasion of foreign flea vectors.


Assuntos
Peste , Sifonápteros , Animais , Peste/epidemiologia , Mudança Climática , China/epidemiologia , Medição de Risco
10.
Int J Hypertens ; 2021: 9672994, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34777859

RESUMO

OBJECTIVE: To understand the prevalence of hypertension in the population without awareness of hypertension in a rural area, a cross-sectional study was carried out. METHODS: Blood pressures were measured in residents over 60 years during the National Basic Public Health Service project carrying on in a rural town of Shandong province. Combined with detail information of the hypertension disease history, the status of prevalence of hypertension was calculated. Basic information and clinical laboratory examinations were analyzed with Student' t or t' or chi-square test for univariate analysis. Multinomial logistic analysis was used in exploring multiple variables. RESULTS: According to the individual history and blood pressure levels, the awareness rate of hypertension in the population over 60 years old was 50.3% (1285/2554, 95% CI: 48.3-52.3%). The prevalence of hypertension was 55.1% (1270/2304, 95% CI: 53.1-57.2%) in the population without awareness of hypertension, in which the proportion of stage 1 hypertension was 58.8% (747/1270), stage 2 hypertension was 28.9% (367/1270), and stage 3 hypertension was 12.3% (156/1270). The prevalence of hypertension in men was 54.4% (611/1124, 95% CI: 51.4-57.3%), which was almost the same as that in women (55.8%, 659/1180, 95% CI: 53.0-58.7%) (X 2 = 0.515, P=0.473). The prevalence of hypertension increased with age (X 2 trend = 11.848, P=0.001). Age, BMI, total cholesterol, triglyceride, and drinking rate were positively correlated with the prevalence of hypertension, that is, the higher the level of these factors, the higher the prevalence of hypertension; on the contrary, LDL and smoking rate might be negatively correlated with the prevalence of hypertension, which means, the higher the prevalence of hypertension, the lower the level of these two indicators. Binary and multinominal logistic results showed that age, BMI, and drinking had stronger effects on the higher blood pressure level. CONCLUSIONS: The awareness rate of hypertension among the elderly in a rural area needs to be further improved. In the prevention and control of hypertension, close attention should be paid to the group of elder, high BMI index, high levels of total cholesterol and triglyceride, and drinking habits.

11.
Biology (Basel) ; 10(11)2021 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-34827144

RESUMO

Glossina morsitans is a vector for Human African Trypanosomiasis (HAT), which is mainly distributed in sub-Saharan Africa at present. Our objective was to project the historical and future potentially suitable areas globally and explore the influence of climatic factors. The maximum entropy model (MaxEnt) was utilized to evaluate the contribution rates of bio-climatic factors and to project suitable habitats for G. morsitans. We found that Isothermality and Precipitation of Wettest Quarter contributed most to the distribution of G. morsitans. The predicted potentially suitable areas for G. morsitans under historical climate conditions would be 14.5 million km2, including a large area of Africa which is near and below the equator, small equatorial regions of southern Asia, America, and Oceania. Under future climate conditions, the potentially suitable areas are expected to decline by about -5.38 ± 1.00% overall, under all shared socioeconomic pathways, compared with 1970-2000. The potentially suitable habitats of G. morsitans may not be limited to Africa. Necessary surveillance and preventive measures should be taken in high-risk regions.

12.
Diabetes Metab Syndr Obes ; 14: 4505-4512, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34795495

RESUMO

OBJECTIVE: To understand the prevalence and control of type 2 diabetes mellitus (T2DM) in a rural area, a cross-sectional study was carried out. METHODS: Blood glucose was determined in residents over 60 years during the National Basic Public Health Service project carrying on in a rural town of Shandong province. Combined with detail information of diabetic history, the prevalence rate of this disease was calculated with a cutoff of more than 7.0 mmol/L of fasting plasma glucose (FPG). Furthermore, according to FPG levels, the control rate of diabetes was evaluated. Basic information and clinical laboratory tests were analyzed with proper methods for univariate analysis. Multivariable logistic analysis was used to explore multiple variables associated with the control effect of T2DM. RESULTS: The prevalence rate of T2DM was 13.5% (95% CI 12.4%~14.7%) without age difference in residents over 60-year old (X 2= 1.078, P = 0.898). And the rate was higher in the female (16.1%, 95% CI 14.4%~17.8%) than that in the male (11.3%, 95% CI 9.7%~12.9%). The control rate of diabetes was 44.5% (95% CI 39.4-49.6%, cutoff <6.1 mmol/L for FPG) and 59.6% (95% CI 54.5-64.6%, cutoff <7.0 mmol/L for FPG), respectively. Most T2DM residents had balance foods, and a high proportion of drugs or insulin were used; however, the proportion of keeping exercise and modifying behaviors was low. Nearly 80% of the diabetic individuals used at least one drug or insulin. However, the more drugs or insulin used, the higher the FPG level was. CONCLUSION: A relative high level of T2DM prevailed in the rural area under fast economy-transforming. T2DM was controlled poor and measures should be further optimized to achieve ideal effect, especially for the use of anti-diabetic drugs.

13.
Biology (Basel) ; 10(10)2021 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-34681097

RESUMO

BACKGROUND: Anopheles philippinensis and Anopheles nivipes are morphologically similar and are considered to be effective vectors of malaria transmission in northeastern India. Environmental factors such as temperature and rainfall have a significant impact on the temporal and spatial distribution of disease vectors driven by future climate change. METHODS: In this study, we used the maximum entropy model to predict the potential global distribution of the two mosquito species in the near future and the trend of future distribution in China. Based on the contribution rate of environmental factors, we analyzed the main environmental factors affecting the distribution of the two mosquito species. We also constructed a disease vector risk assessment index system to calculate the comprehensive risk value of the invasive species. RESULTS: Precipitation has a significant effect on the distribution of potentially suitable areas for Anopheles philippinensis and Anopheles nivipes. The two mosquito species may spread in the suitable areas of China in the future. The results of the risk assessment index system showed that the two mosquito species belong to the moderate invasion risk level for China. CONCLUSIONS: China should improve the mosquito vector monitoring system, formulate scientific prevention and control strategies and strictly prevent foreign imports.

14.
Biology (Basel) ; 10(10)2021 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-34681156

RESUMO

Amblyomma americanum (the lone star tick) is a pathogen vector, mainly from eastern North America, that bites humans. With global integration and climate change, some ticks that are currently confined to a certain place may begin to spread out; some reports have shown that they are undergoing rapid range expansion. The difference in the potential geographic distribution of A. americanum under current and future climatic conditions is dependent on environment variables such as temperature and precipitation, which can affect their survival. In this study, we used a maximum entropy (MaxEnt) model to predict the potential geographic distribution of A. americanum. The MaxEnt model was calibrated at the native range of A. americanum using occurrence data and the current climatic conditions. Seven WorldClim climatic variables were selected by the jackknife method and tested in MaxEnt using different combinations of model feature class functions and regularization multiplier values. The best model was chosen based on the omission rate and the lowest Akaike information criterion. The resulting model was then projected onto the global scale using the current and future climate conditions modeled under four greenhouse gas emission scenarios.

15.
ACS Appl Mater Interfaces ; 13(7): 8488-8496, 2021 Feb 24.
Artigo em Inglês | MEDLINE | ID: mdl-33576236

RESUMO

Ultrasmall Ru nanoparticles is expected as a potential alternative to Pt for efficient hydrazine oxidation (HzOR). However, preparation of ultrasmall and well-distributed Ru nanoparticles usually suffered from the steps of modification of supports, coordination, reduction with strong reducing reagents (e.g., NaBH4) or pyrolysis, imposing the complexity. Based on the self-reducibility of C-OH group and physical adsorption ability of commercial Ketjen black (KB), we developed an efficient, stable and robust Ru-based electrocatalyst (A-Ru-KB) by coupling impregnation of KB in RuCl3 solution and simple in situ electrochemical activation strategy, which endowed the formation of ultrasmall and well-distributed Ru nanoparticles. Benefiting from an enhanced exposure of Ru sites and the faster mass transport, A-Ru-KB achieved 63.4 and 3.9-fold enhancements of mass activity compared with Pt/C and Ru/C, respectively, accompanied by a ∼144 mV lower onset potential and faster catalytic kinetics than Pt/C. In the hydrazine fuel cell, the open-circuit voltage and maximal mass power density of A-Ru-KB was 130 mV and ∼3.8-fold higher than those of Pt/C, respectively, together with the long-term stability. This work would provide a facile and sustainable approach for large-scale production of other robust metal (electro)catalysts with ultrasmall nanosize for various energy conversion and electrochemical organic synthesis.

16.
ACS Appl Mater Interfaces ; 12(51): 57134-57140, 2020 Dec 23.
Artigo em Inglês | MEDLINE | ID: mdl-33300776

RESUMO

Manipulating the strain effect of Ag without any foreign metals to boost its intrinsic oxygen reduction reaction (ORR) activity is intriguing, but it remains a challenge. Herein, we developed a class of Ag-based electrocatalysts with tunable strain structures for efficient ORR via ligand-assisted competitive decomposition of Ag-organic complexes (AgOCs). Benefiting from the superior coordination capability, 4,4'-bipyridine as a ligand triggered a stronger competition with NaBH4 for Ag ions during reduction-induced decomposition of AgOCs in comparison with the counterparts of the pyrazine ligand and the NO3- anion, which moderately modulated the compressive strain structure to upshift the d-band center of the catalyst and increase the electron density of Ag. Accordingly, the O2 adsorption was obviously improved, and the stronger repulsion effect between the Ag sites and the 4e ORR product, i.e., the electron-rich OH-, was generated to promote the desorption of OH- via the Ag-OH bond cleavage, which enabled more Ag sites to be regenerated after ORR. Both of these led to an enhancement to the intrinsic ORR activity of the Ag-based catalyst. This competitive decomposition of metal-organic complex strategy would provide a facile method to design other catalysts with the well-tuned strain structures for energy conversion and heterocatalysis.

17.
ACS Appl Mater Interfaces ; 12(34): 38183-38191, 2020 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-32799446

RESUMO

Pursuing nonprecious doped carbon with Pt-like electrocatalytic N2H4 oxidation activity for hydrazine fuel cells (HzFCs) remains a challenge. Herein, we present a Fe/N-doped carbon (Fe-NC) catalyst with mesopore-rich channel and highly dispersed Fe-N sites incorporated in N-doped carbon, as an analogue of hydrazine dehydrogenase (HDH), showing the structure-dependent activity for electrocatalytic oxidation of N2H4. The maximal turnover frequency of the N2H4 oxidation reaction (HzOR) over the Fe-N sites (62870 h-1) is 149-fold that over the pyridinic-N sites of N-doped carbon. The Fe mass activity of HzOR and maximal power density of HzFCs driven by Fe-NC approximately surpass those of Pt/C by 2.3 and 2.2 times, respectively. Theoretical calculation reveals that the Fe-N sites improve the dehydrogenation process of HzOR-related intermediates. One of the roles of the mesoporous structure in Fe-NC resembles that of a substrate channel in HDH for enhancing the transport of N2H4 besides exposing Fe-N sites and improving storage capacity of HzOR-related species.


Assuntos
Materiais Biomiméticos/química , Carbono/química , Hidrazinas/química , Ferro/química , Materiais Biomiméticos/metabolismo , Catálise , Teoria da Densidade Funcional , Oxirredução , Oxirredutases/química , Oxirredutases/metabolismo , Piridinas/química
18.
ACS Appl Mater Interfaces ; 12(4): 4833-4842, 2020 Jan 29.
Artigo em Inglês | MEDLINE | ID: mdl-31914316

RESUMO

Development of low-cost and efficient (electro)catalysts with tunable 2e/4e oxygen reduction reaction (ORR) selectivity toward energy conversion, biomimetic catalysis, and biosensing has attracted growing interest. Herein, we reported that carbon nanohybrids with O- or N-coordinated Cu (Cu-OC or Cu-NC) showed superior activity for 2e and 4e electrocatalytic ORR with selectivities of 84.0% and 97.2%, respectively. Experimental evidence demonstrated that the strong electron-rich O-doped carbon in Cu-OC donated electrons to Cu2+, weakening the binding strength of H2O2 at Cu-O centers and facilitating the 2e ORR pathway for selective production of H2O2. However, the poor electron-donor ability of the N-doped carbon in Cu-NC made Cu-N sites more electron deficient due to the reduced electron transfer from N-doped carbon to Cu2+, promoting 4e ORR by enhancing adsorption of O2 and the ORR intermediates. The high 4e ORR activity of Cu-NC rendered its potential for application in a Zn-air battery and oxidase-mimicking activity for 3,3',5,5'-tetramethylbenzidine (TMB) and ascorbic acid (AA) oxidation. The maximal velocity (Vmax) of TMB and AA oxidation over Cu-NC was higher than some natural oxidases and noble-metal-based artificial enzymes. The lower activation energy for AA oxidation over Cu-NC resulted in a 263-fold higher oxidative rate than TMB, further prompting nonenzymatic sensing of AA by the competitive oxidation strategy.

19.
J Hazard Mater ; 385: 121527, 2020 03 05.
Artigo em Inglês | MEDLINE | ID: mdl-31708287

RESUMO

Regulation of defects and surface acidic sites of photocatalysts is an efficient approach to improve the photocatalytic activity. Ultrathin 2D-ZnO photocatalysts were prepared to uncover the synergetic effects of defects and surface acidic sites on the photocatalytic activity. The reaction constant for photocatalytic degradation of MB upon ZnO-S is 2.26, 2.82, 12.2 times higher than that of SH-500, SO-500, and ZnO-R, respectively. The results revealed that the surface defects, hydroxyl group and chemisorbed water played pivotal roles in the generation of reactive oxygen species (ROS). Although the limited improvement of visible absorption was achieved after introduction of oxygen vacancy (VO), the overall photocatalytic activity decreased due to the reduced ROS production capacity shown by density functional theory (DFT) calculations. Hydroxyl radical is the key ROS in degradation of organics, and electron contributes a little bigger than hole in the generation of hydroxyl radical. Importantly, the decrease in surface acidic sites resulted in the decreased photocatalytic activity, proven by the dynamics of photoinduced carriers. This study reveals that the improved photocatalytic activity of 2D-ZnO photocatalysts can be attributed to the synergetic effects of surface defects and acidic sites rather than the enhanced visible absorption resulted from the VO introduction.

20.
Nanomicro Lett ; 9(4): 42, 2017.
Artigo em Inglês | MEDLINE | ID: mdl-30393737

RESUMO

Stretchable electronic sensing devices are defining the path toward wearable electronics. High-performance flexible strain sensors attached on clothing or human skin are required for potential applications in the entertainment, health monitoring, and medical care sectors. In this work, conducting copper electrodes were fabricated on polydimethylsiloxane as sensitive stretchable microsensors by integrating laser direct writing and transfer printing approaches. The copper electrode was reduced from copper salt using laser writing rather than the general approach of printing with pre-synthesized copper or copper oxide nanoparticles. An electrical resistivity of 96 µΩ cm was achieved on 40-µm-thick Cu electrodes on flexible substrates. The motion sensing functionality successfully demonstrated a high sensitivity and mechanical robustness. This in situ fabrication method leads to a path toward electronic devices on flexible substrates.

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