The utilization of nuclear power will persist as a prominent energy source in the foreseeable future.However,it presents substantial challenges concerning waste disposal and the potential emission of untreated radioac...The utilization of nuclear power will persist as a prominent energy source in the foreseeable future.However,it presents substantial challenges concerning waste disposal and the potential emission of untreated radioactive substances,such as radioactive 129I and 131I.The transportation of radioactive iodine poses a significant threat to both the environment and human health.Nevertheless,effectively,rapidly removing iodine ion from water using porous adsorbents remains a crucial challenge.In this work,three kinds of multiple sites porous organic polymers(POPs,POP-1,POP-2,and POP-3)have been developed using a monomer pre-modification strategy for highly efficient and fast I_(3) absorption from water.It is found that the POPs exhibited exceptional performance in terms of I3 adsorption,achieving a top-performing adsorption capacity of 5.25 g g^(-1) and the fastest average adsorption rate(K_(80%)=4.25 g g^(-1) h^(-1))with POP-1.Moreover,POP-1 exhibited exceptional capacity for the removal of I3 fromflowing aqueous solutions,with 95%removal efficiency observed even at 0.0005 mol L^(-1).Such results indicate that this material has the potential to be utilized for the emergency preparation of potable water in areas contaminated with radioactive iodine.The adsorption process can be effectively characterized by the Freundlich model and the pseudo-second-order model.The exceptional I_(3) absorption capacity is primarily attributed to the incorporation of a substantial number of active adsorption sites,including bromine,carbonyl,and amide groups.展开更多
Efficient recognition and selective capture of NH_(3)is not only beneficial for increasing the productivity of the synthetic NH_(3)industry but also for reducing air pollution.For this purpose,a group of deep eutectic...Efficient recognition and selective capture of NH_(3)is not only beneficial for increasing the productivity of the synthetic NH_(3)industry but also for reducing air pollution.For this purpose,a group of deep eutectic solvents(DESs)consisting of glycolic acid(GA)and phenol(PhOH)with low viscosities and multiple active sites was rationally designed in this work.Experimental results show that the GA^(+)PhOH DESs display extremely fast NH_(3)absorption rates(within 51 s for equilibrium)and high NH_(3)solubility.At 313.2 K,the NH_(3)absorption capacities of GA^(+)PhOH(1:1)reach 6.75 mol/kg(at 10.7 kPa)and 14.72 mol/kg(at 201.0 kPa).The NH_(3)solubility of GA^(+)PhOH DESs at low pressures were minimally changed after more than 100 days of air exposure.In addition,the NH_(3)solubility of GA^(+)PhOH DESs remain highly stable in 10 consecutive absorption-desorption cycles.More importantly,NH_(3)can be selectively captured by GA^(+)PhOH DESs from NH_(3)/CO_(2)/N_(2)and NH_(3)/N_(2)/H_(2)mixtures.1H-NMR,Fourier transform infrared and theoretical calculations were performed to reveal the intrinsic mechanism for the efficient recognition of NH_(3)by GA^(+)PhOH DESs.展开更多
The efficient separation and collection of ammonia(NH_(3))during NH_(3) synthesis process is essential to improve the economic efficiency and protect the environment.In this work,ethanolammonium hydrochloride(EtOHACl)...The efficient separation and collection of ammonia(NH_(3))during NH_(3) synthesis process is essential to improve the economic efficiency and protect the environment.In this work,ethanolammonium hydrochloride(EtOHACl)and phenol(PhOH)were used to prepare a novel class of deep eutectic solvents(DESs)with multiple active sites and low viscosities.The NH_(3) separation performance of EtOHACl+PhOH DESs was analyzed completely.It is figured out that the NH_(3) absorption rates in EtOHACl+PhOH DESs are very fast.The NH_(3) absorption capacities are very high and reach up to 5.52 and 10.74 mol·kg1 at 11.2 and 100.4 kPa under 298.2 K,respectively.In addition,the EtOHACl+PhOH DESs present highly selective absorption of NH_(3) over N_(2) and H_(2) and good regenerative properties after seven cycles of absorption/desorption.The intrinsic separation mechanism of NH_(3) by EtOHACl+PhOH DESs was further revealed by spectroscopic analysis and quantum chemistry calculations.展开更多
Two methods currently available for evaluating the probability of Multiple Site Damage(MSD)occurrence were studied in this paper.One of the methods is a probabilistic analysis approach based on the statistical theory ...Two methods currently available for evaluating the probability of Multiple Site Damage(MSD)occurrence were studied in this paper.One of the methods is a probabilistic analysis approach based on the statistical theory and fatigue characteristics of each structural detail,and the other is an approach which defines the initial damage scenario by means of Monte-Carlo simulation,and multiple initial crack scenarios are randomly generated.A modified method based on the Monte-Carlo simulation was proposed in this paper,in which the random fluctuation of the stress was considered to give more accurate evaluation results.In the presented method,the probability of MSD occurrence in a structural element containing multiple details was calculated based on the Monte-Carlo simulation and the p-S-N curve of a single structural detail.Fatigue tests were accomplished using specimens containing 21-similar-details to obtain the fatigue life corresponding to MSD occurrence.Tests on single-detail specimens and static calibration tests were also conducted to get the basic fatigue properties of the material and the degree of stress fluctuation.The aforementioned three methods were compared and validated via the test results.The influence of the stress random fluctuation degree on the probability of MSD occurrence and influence of the distribution types on evaluating the MSD occurrence probability were discussed.展开更多
Homocysteine(Hcy), cysteine(Cys) and glutathione(GSH) play crucial roles in redox homeostasis during mitochondria functions. Simultaneous differentiation and visualization of mitochondrial biothiols dynamics are signi...Homocysteine(Hcy), cysteine(Cys) and glutathione(GSH) play crucial roles in redox homeostasis during mitochondria functions. Simultaneous differentiation and visualization of mitochondrial biothiols dynamics are significant for understanding cell metabolism and their related diseases. Herein, a multisitebinding fluorescent probe(MCP) was developed for simultaneous sensing of mitochondrial Cys, GSH and Hcy from three fluorescence channels for the first time. This novel probe exhibited rapid fluorescence turn-on, good water-solubility, high selectivity and large spectral separation for discriminating Cys, GSH and Hcy with 131-, 96-, 748-fold fluorescence increasement at 471, 520, 567 nm through different excitation wavelengths, respectively. Importantly, this probe was successfully applied to simultaneous monitoring of mitochondrial Cys, GSH, and Hcy in live cells and zebrafish from three fluorescence channels,promoting the understanding of the functions of Hcy, Cys and GSH.展开更多
The development of highly active and stable bifunctional electrocatalysts in acidic media is crucial to hydrogen production by proton exchange membrane.In this study,we designed a RuO_(2)-IrO_(2)heterostructure cataly...The development of highly active and stable bifunctional electrocatalysts in acidic media is crucial to hydrogen production by proton exchange membrane.In this study,we designed a RuO_(2)-IrO_(2)heterostructure catalyst coupled by carbon quantum dots(CQDs).The catalyst showed excellent electrocatalytic performance for water splitting under acidic conditions.The overpotentials of oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)were as low as 180 and 15 mV at 10 mA/cm^(2)in 0.5 M H_(2)SO_(4),respectively.The acid electrolytic cell developed with RuO_(2)-IrO_(2)@CQDs as anode and cathode operated stably at 10 m A/cm^(2)for 120 h.In situ measurements and theoretical calculation reveal that the unique lattice oxygen mechanism path of RuO_(2)-IrO_(2)@CQDs can bypass the OOH^(*)intermediate and breaks the linear relationship of adsorbent evolution mechanism path,resulting in higher OER catalytic activity.展开更多
The electrochemical reaction rate strongly depends on the pH of the solution and the relatively sluggish alkaline hydrogen evolution reaction(HER)process,attributed to alterations in the type of proton donor and bindi...The electrochemical reaction rate strongly depends on the pH of the solution and the relatively sluggish alkaline hydrogen evolution reaction(HER)process,attributed to alterations in the type of proton donor and binding energy,has consistently presented a significant challenge.Here,we report a new method for boosting alkaline HER via spontaneous built-in electric field strategy employed on cobalt phosphide nanofibers(NFs)electrocatalyst.The anion-cation dual-introduction of V and N on the NFs not only increases the electrochemical surface area but also enhances the catalytic activity,thereby elevating the performance of alkaline HER.An investigation strategy combining experiments and calculations revealed the charge transfer law between multiple active components and the enhanced regulation mechanism of alkaline HER process,ultimately achieving a nearly twice increase in reaction overpotential of the as-fabricated catalyst at-10 mA·cm^(-2).This new approach provides a potential strategy for improving the efficiency of core catalyst for energy conversion technologies.展开更多
Electrocatalytic synthesis of urea through C-N bond formation,converting carbon dioxide(CO_(2))and ni-trate(NO_(3)^(-)),presents a promising,less energy-intensive alternative to industrial urea production process.In t...Electrocatalytic synthesis of urea through C-N bond formation,converting carbon dioxide(CO_(2))and ni-trate(NO_(3)^(-)),presents a promising,less energy-intensive alternative to industrial urea production process.In this communication,we report the application of Mo_(2)C nanosheets-decorated carbon sheets(Mo_(2)C/C)as a highly efficient electrocatalyst for facilitating C-N coupling in ambient urea electrosynthesis.In CO_(2)-saturated 0.2 mol/L Na_(2)SO_(4)solution containing 0.05 mol/L NO_(3)^(-),the Mo_(2)C/C catalyst achieves an impres-sive urea yield of 579.13μg h^(-1)mg^(-1)with high Faradaic efficiency of 44.80%at-0.5 V versus the reversible hydrogen electrode.Further theoretical calculations reveal that the multiple Mo active sites enhance the formation of^(∗)CO and^(∗)NH_(2)intermediates and facilitate their C-N coupling.This research propels the use of Mo_(2)C-based electrodes in electrocatalysis and accentuates the capabilities of binary metal-based catalysts in C-N coupling reactions.展开更多
While the present structural integrity evaluation method is based on the philosophy of assumed similitude, Fatigue and Damage Tolerance(F&DT) evaluations for next generation of air-vehicles require high-fidelity p...While the present structural integrity evaluation method is based on the philosophy of assumed similitude, Fatigue and Damage Tolerance(F&DT) evaluations for next generation of air-vehicles require high-fidelity physical models within cyberspace. To serve the needs of F&DT evaluation in digital twin paradigm, a fatigue damage-cumulative model within peridynamic framework is proposed in this paper. Based on the concept of fatigue element block and damage accumulation law in form of Coffin-Manson relationship, the proposed model applies to both fatigue crack initiation and fatigue crack growth;fatigue crack growth rates under constant-amplitude and simple variable-amplitude block loading cases can be well predicted for three common structural materials without inputs of Paris law parameters. Additionally, the proposed model can also be easily extended to a probabilistic version;for verification, multiple-site-damage problems are simulated and the statistic nature of fatigue process in experiments can be well captured. In the end, main features of the proposed model are summarized, and distinctions from the other models are discussed. There may be a potential for the peridynamic damage-cumulative model proposed in this work to numerically predict fatigue problems in digital twin paradigm for future generations of aerospace vehicles.展开更多
Enrichment of trace bioactive constituents and metabolites from complex biological samples is challenging.This study presented a one-pot synthesis of magnetic polydopamine nanoparticles(Fe3O4@-SiO2@PDA NPs)with multip...Enrichment of trace bioactive constituents and metabolites from complex biological samples is challenging.This study presented a one-pot synthesis of magnetic polydopamine nanoparticles(Fe3O4@-SiO2@PDA NPs)with multiple recognition sites for the magnetic dispersive solid-phase extraction(MDSPE)of ginsenosides from rat plasma treated with white ginseng.The extracted ginsenosides were characterized by combining an ultra-high-performance liquid chromatography coupled to a highresolution mass spectrometry with supplemental UNIFI libraries.Response surface methodology was statistically used to optimize the extraction procedure of the ginsenosides.The reusability of Fe3O4@-SiO2@PDA NPs was also examined and the results showed that the recovery rate exceeded 80%after recycling 6 times.Furthermore,the proposed method showed greater enrichment efficiency and could rapidly determine and characterize 23 ginsenoside prototypes and metabolites from plasma.In comparison,conventional methanol method can only detect 8 ginsenosides from the same plasma samples.The proposed approach can provide methodological reference for the trace determination and characterization of different bioactive ingredients and metabolites of traditional Chinese medicines and food.展开更多
The coexistence of multi-component active sites like single-atom sites,diatomic sites(DAS)and nanoclusters is shown to result in superior performances in the hydrogen evolution reaction(HER).Metal diatomic sites are m...The coexistence of multi-component active sites like single-atom sites,diatomic sites(DAS)and nanoclusters is shown to result in superior performances in the hydrogen evolution reaction(HER).Metal diatomic sites are more complex than single-atom sites but their unique electronic structures can lead to significant enhancement of the HER kinetics.Although the synthesis and identification of DAS is usually challenging,we report a simple access to a diatomic catalyst by anchoring Co-Ru DAS on nitrogen-doped carbon supports along with Ru nanoparticles(NPs).Experimental and theoretical results revealed the atomic-level characteristics of Co-Ru sites,their strong electronic coupling and their synergy with Ru NPs within the catalyst.The unique electronic structure of the catalyst resulted in an excellent HER activity and stability in alkaline media.This work provides a valuable insight into a widely applicable design of diatomic catalysts with multi-component active sites for highly efficient HER electrocatalysis.展开更多
Objective: The coronavirus disease 2019 (COVID-19) epidemic resulting from severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) has still spread globally. The occurrence of the Delta variant, which is more inf...Objective: The coronavirus disease 2019 (COVID-19) epidemic resulting from severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) has still spread globally. The occurrence of the Delta variant, which is more infectious and spreads faster than earlier forms of the virus that causes COVID-19, makes infection prevention more challenging. Therefore, this study aimed to gain a comprehensive insight into the transmission routes of SARS-CoV-2 for curbing the propagation of SARS-CoV-2 in human populations.Methods: We studied a prospective cohort of 576 patients admitted consecutively to the First Affiliated Hospital of Guangzhou Medical University from January 21 to June 8, 2020. These patients were chosen based on their similar clinical phenotypes or imaging findings. There were 21 (3.6%) laboratory-confirmed COVID-19 patients (16 severe and 5 mild cases) and 555 non-COVID-19 patients. The antibody response and routes and duration of viral shedding were systematically evaluated in serial clinical specimens. Moreover, SARS-CoV-2 RNA was also detected in a mouth rinse, urine, and tear samples. This study was approved by the Medical Ethical Committee of The First Affiliated Hospital of Guangzhou Medical University (approval No. 2020-77).Results: SARS-CoV-2 mainly existed in sputum, nasal and throat swabs, and feces samples. Virus latency was longer in sputum and feces samples than in nasopharyngeal samples. IgG antibody response in respiratory samples was related to disease severity. Although droplets and aerosols are the major transmission routes for COVID-19, covert routes of transmission from asymptomatic patients, contaminated surfaces, and wastewater are also of interest.Conclusion: Our findings provide a solid foundation for developing prophylactic measures against SARS-CoV-2.展开更多
At present,excessive carbon dioxide(CO_(2))emission has become an increasingly prominent global energy and environmental issue.Therefore,effective methods to convert CO_(2) into fine chemicals are urgently required.He...At present,excessive carbon dioxide(CO_(2))emission has become an increasingly prominent global energy and environmental issue.Therefore,effective methods to convert CO_(2) into fine chemicals are urgently required.Herein,series of S-doped carbon-nitrogen(CNS-X)materials(where X denotes the ratio of thiourea and melamine substances ranging from 0.03 to 0.8)was prepared via the programmed temperature pyrolysis method,which thiourea(CH4N_(2)S)and melamine was used as the precursor of the catalysts.The sulfur source endow the CNS-X acidic sites,which cooperate synergistically with amino groups from the incomplete polymerization of melamine,leading to a bifunctional catalyst for cycloaddition reaction of CO_(2) with epoxides.These catalysts were characterized using X-ray diffraction,Fourier transform infrared spectroscopy,elemental analysis,X-ray photoelectron spectroscopy,and N_(2) adsorption-desorption techniques,confirming the successful integration of functional groups.The optimal thiourea doping concentration of 0.4 was certainly found to have considerably facilitated the efficient conversion of CO_(2) by the CNS-0.4 catalyst,in which the conversion of epichlorohydrin(ECH)could achieve over 90.0% and the selectivity of cyclic carbonate is 98.0% under 1.0 MPa at 140℃ for 10 h.The superior catalytic performance of CNS-0.4 was attributable to the synergistic effect arising from the co-existence of Lewis acidic and basic sites.Notably,using CNS-0.4 resulted in a high yield even after four reaction cycles.展开更多
基金support from the National Natural Science Foundation of China(No.22273016,22273017,22233006)Plan for Henan Province University Science and Technology Innovation Team(No.25IRTSTHN002)+1 种基金Young Backbone Teacher Training Program of Henan Province(2023GGJS036)the 111 project(No.D17007).
文摘The utilization of nuclear power will persist as a prominent energy source in the foreseeable future.However,it presents substantial challenges concerning waste disposal and the potential emission of untreated radioactive substances,such as radioactive 129I and 131I.The transportation of radioactive iodine poses a significant threat to both the environment and human health.Nevertheless,effectively,rapidly removing iodine ion from water using porous adsorbents remains a crucial challenge.In this work,three kinds of multiple sites porous organic polymers(POPs,POP-1,POP-2,and POP-3)have been developed using a monomer pre-modification strategy for highly efficient and fast I_(3) absorption from water.It is found that the POPs exhibited exceptional performance in terms of I3 adsorption,achieving a top-performing adsorption capacity of 5.25 g g^(-1) and the fastest average adsorption rate(K_(80%)=4.25 g g^(-1) h^(-1))with POP-1.Moreover,POP-1 exhibited exceptional capacity for the removal of I3 fromflowing aqueous solutions,with 95%removal efficiency observed even at 0.0005 mol L^(-1).Such results indicate that this material has the potential to be utilized for the emergency preparation of potable water in areas contaminated with radioactive iodine.The adsorption process can be effectively characterized by the Freundlich model and the pseudo-second-order model.The exceptional I_(3) absorption capacity is primarily attributed to the incorporation of a substantial number of active adsorption sites,including bromine,carbonyl,and amide groups.
基金supported by the National Natural Science Foundation of China(22008033)the Major Program of Qingyuan Innovation Laboratory.
文摘Efficient recognition and selective capture of NH_(3)is not only beneficial for increasing the productivity of the synthetic NH_(3)industry but also for reducing air pollution.For this purpose,a group of deep eutectic solvents(DESs)consisting of glycolic acid(GA)and phenol(PhOH)with low viscosities and multiple active sites was rationally designed in this work.Experimental results show that the GA^(+)PhOH DESs display extremely fast NH_(3)absorption rates(within 51 s for equilibrium)and high NH_(3)solubility.At 313.2 K,the NH_(3)absorption capacities of GA^(+)PhOH(1:1)reach 6.75 mol/kg(at 10.7 kPa)and 14.72 mol/kg(at 201.0 kPa).The NH_(3)solubility of GA^(+)PhOH DESs at low pressures were minimally changed after more than 100 days of air exposure.In addition,the NH_(3)solubility of GA^(+)PhOH DESs remain highly stable in 10 consecutive absorption-desorption cycles.More importantly,NH_(3)can be selectively captured by GA^(+)PhOH DESs from NH_(3)/CO_(2)/N_(2)and NH_(3)/N_(2)/H_(2)mixtures.1H-NMR,Fourier transform infrared and theoretical calculations were performed to reveal the intrinsic mechanism for the efficient recognition of NH_(3)by GA^(+)PhOH DESs.
基金supported by the National Natural Science Foundation of China(22221005 and 22008033).
文摘The efficient separation and collection of ammonia(NH_(3))during NH_(3) synthesis process is essential to improve the economic efficiency and protect the environment.In this work,ethanolammonium hydrochloride(EtOHACl)and phenol(PhOH)were used to prepare a novel class of deep eutectic solvents(DESs)with multiple active sites and low viscosities.The NH_(3) separation performance of EtOHACl+PhOH DESs was analyzed completely.It is figured out that the NH_(3) absorption rates in EtOHACl+PhOH DESs are very fast.The NH_(3) absorption capacities are very high and reach up to 5.52 and 10.74 mol·kg1 at 11.2 and 100.4 kPa under 298.2 K,respectively.In addition,the EtOHACl+PhOH DESs present highly selective absorption of NH_(3) over N_(2) and H_(2) and good regenerative properties after seven cycles of absorption/desorption.The intrinsic separation mechanism of NH_(3) by EtOHACl+PhOH DESs was further revealed by spectroscopic analysis and quantum chemistry calculations.
文摘Two methods currently available for evaluating the probability of Multiple Site Damage(MSD)occurrence were studied in this paper.One of the methods is a probabilistic analysis approach based on the statistical theory and fatigue characteristics of each structural detail,and the other is an approach which defines the initial damage scenario by means of Monte-Carlo simulation,and multiple initial crack scenarios are randomly generated.A modified method based on the Monte-Carlo simulation was proposed in this paper,in which the random fluctuation of the stress was considered to give more accurate evaluation results.In the presented method,the probability of MSD occurrence in a structural element containing multiple details was calculated based on the Monte-Carlo simulation and the p-S-N curve of a single structural detail.Fatigue tests were accomplished using specimens containing 21-similar-details to obtain the fatigue life corresponding to MSD occurrence.Tests on single-detail specimens and static calibration tests were also conducted to get the basic fatigue properties of the material and the degree of stress fluctuation.The aforementioned three methods were compared and validated via the test results.The influence of the stress random fluctuation degree on the probability of MSD occurrence and influence of the distribution types on evaluating the MSD occurrence probability were discussed.
基金supported by the National Natural Science Foundation of China (Nos. 21877035 and 21977028)Research Foundation of Education Bureau of Hunan Province (No. 18B004)。
文摘Homocysteine(Hcy), cysteine(Cys) and glutathione(GSH) play crucial roles in redox homeostasis during mitochondria functions. Simultaneous differentiation and visualization of mitochondrial biothiols dynamics are significant for understanding cell metabolism and their related diseases. Herein, a multisitebinding fluorescent probe(MCP) was developed for simultaneous sensing of mitochondrial Cys, GSH and Hcy from three fluorescence channels for the first time. This novel probe exhibited rapid fluorescence turn-on, good water-solubility, high selectivity and large spectral separation for discriminating Cys, GSH and Hcy with 131-, 96-, 748-fold fluorescence increasement at 471, 520, 567 nm through different excitation wavelengths, respectively. Importantly, this probe was successfully applied to simultaneous monitoring of mitochondrial Cys, GSH, and Hcy in live cells and zebrafish from three fluorescence channels,promoting the understanding of the functions of Hcy, Cys and GSH.
基金supported by the Natural Science Foundation of Shandong Province ZR2024MB087the National Natural Science Foundation of China(No.52122308,51973200,52202050,and 21905253)+3 种基金the Natural Science Foundation of Henan(202300410372)the Joint Fund of Science and Technology R&D Plan of Henan Province(232301420042)the China Postdoctoral Science Foundation(2022TQ0286)the Center for Modern Analysis and Gene Sequencing of Zhengzhou University for supporting this project。
文摘The development of highly active and stable bifunctional electrocatalysts in acidic media is crucial to hydrogen production by proton exchange membrane.In this study,we designed a RuO_(2)-IrO_(2)heterostructure catalyst coupled by carbon quantum dots(CQDs).The catalyst showed excellent electrocatalytic performance for water splitting under acidic conditions.The overpotentials of oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)were as low as 180 and 15 mV at 10 mA/cm^(2)in 0.5 M H_(2)SO_(4),respectively.The acid electrolytic cell developed with RuO_(2)-IrO_(2)@CQDs as anode and cathode operated stably at 10 m A/cm^(2)for 120 h.In situ measurements and theoretical calculation reveal that the unique lattice oxygen mechanism path of RuO_(2)-IrO_(2)@CQDs can bypass the OOH^(*)intermediate and breaks the linear relationship of adsorbent evolution mechanism path,resulting in higher OER catalytic activity.
基金financially supported by the National Natural Science Foundation of China(No.52304335)China Postdoctoral Science Foundation(No.2023TQ0303)+3 种基金the Postdoctoral Fellowship Program of CPSF(No.GZC20232450)the Project of Zhongyuan Critical Metals Laboratory(Nos.GJJSGFYQ202305 and GJJSGFJQ202302)the Youth Science and technology innovation of Henan Province(No.23HASTIT009)Henan Province Youth Talent Support Program(2022)。
文摘The electrochemical reaction rate strongly depends on the pH of the solution and the relatively sluggish alkaline hydrogen evolution reaction(HER)process,attributed to alterations in the type of proton donor and binding energy,has consistently presented a significant challenge.Here,we report a new method for boosting alkaline HER via spontaneous built-in electric field strategy employed on cobalt phosphide nanofibers(NFs)electrocatalyst.The anion-cation dual-introduction of V and N on the NFs not only increases the electrochemical surface area but also enhances the catalytic activity,thereby elevating the performance of alkaline HER.An investigation strategy combining experiments and calculations revealed the charge transfer law between multiple active components and the enhanced regulation mechanism of alkaline HER process,ultimately achieving a nearly twice increase in reaction overpotential of the as-fabricated catalyst at-10 mA·cm^(-2).This new approach provides a potential strategy for improving the efficiency of core catalyst for energy conversion technologies.
基金support from the Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province(No.JC2018004).
文摘Electrocatalytic synthesis of urea through C-N bond formation,converting carbon dioxide(CO_(2))and ni-trate(NO_(3)^(-)),presents a promising,less energy-intensive alternative to industrial urea production process.In this communication,we report the application of Mo_(2)C nanosheets-decorated carbon sheets(Mo_(2)C/C)as a highly efficient electrocatalyst for facilitating C-N coupling in ambient urea electrosynthesis.In CO_(2)-saturated 0.2 mol/L Na_(2)SO_(4)solution containing 0.05 mol/L NO_(3)^(-),the Mo_(2)C/C catalyst achieves an impres-sive urea yield of 579.13μg h^(-1)mg^(-1)with high Faradaic efficiency of 44.80%at-0.5 V versus the reversible hydrogen electrode.Further theoretical calculations reveal that the multiple Mo active sites enhance the formation of^(∗)CO and^(∗)NH_(2)intermediates and facilitate their C-N coupling.This research propels the use of Mo_(2)C-based electrodes in electrocatalysis and accentuates the capabilities of binary metal-based catalysts in C-N coupling reactions.
基金supported by the National Natural Science Foundation of China (No. 11672012)。
文摘While the present structural integrity evaluation method is based on the philosophy of assumed similitude, Fatigue and Damage Tolerance(F&DT) evaluations for next generation of air-vehicles require high-fidelity physical models within cyberspace. To serve the needs of F&DT evaluation in digital twin paradigm, a fatigue damage-cumulative model within peridynamic framework is proposed in this paper. Based on the concept of fatigue element block and damage accumulation law in form of Coffin-Manson relationship, the proposed model applies to both fatigue crack initiation and fatigue crack growth;fatigue crack growth rates under constant-amplitude and simple variable-amplitude block loading cases can be well predicted for three common structural materials without inputs of Paris law parameters. Additionally, the proposed model can also be easily extended to a probabilistic version;for verification, multiple-site-damage problems are simulated and the statistic nature of fatigue process in experiments can be well captured. In the end, main features of the proposed model are summarized, and distinctions from the other models are discussed. There may be a potential for the peridynamic damage-cumulative model proposed in this work to numerically predict fatigue problems in digital twin paradigm for future generations of aerospace vehicles.
基金This work was supported by grants from the National Natural Science Foundation of China Key Program(NO.81530094)General Program(NO.81573574,81873193)the Science and Technology Development Project of Jilin Province(20190201283JC).
文摘Enrichment of trace bioactive constituents and metabolites from complex biological samples is challenging.This study presented a one-pot synthesis of magnetic polydopamine nanoparticles(Fe3O4@-SiO2@PDA NPs)with multiple recognition sites for the magnetic dispersive solid-phase extraction(MDSPE)of ginsenosides from rat plasma treated with white ginseng.The extracted ginsenosides were characterized by combining an ultra-high-performance liquid chromatography coupled to a highresolution mass spectrometry with supplemental UNIFI libraries.Response surface methodology was statistically used to optimize the extraction procedure of the ginsenosides.The reusability of Fe3O4@-SiO2@PDA NPs was also examined and the results showed that the recovery rate exceeded 80%after recycling 6 times.Furthermore,the proposed method showed greater enrichment efficiency and could rapidly determine and characterize 23 ginsenoside prototypes and metabolites from plasma.In comparison,conventional methanol method can only detect 8 ginsenosides from the same plasma samples.The proposed approach can provide methodological reference for the trace determination and characterization of different bioactive ingredients and metabolites of traditional Chinese medicines and food.
基金the National Natural Science Foundation of China(No.22271203)the State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry(No.KF2021005)the Collaborative Innovation Center of Suzhou Nano Science and Technology,the Priority Academic Program Development of Jiangsu Higher Education Institutions,and the Project of Scientific and Technologic Infrastructure of Suzhou(No.SZS201905).
文摘The coexistence of multi-component active sites like single-atom sites,diatomic sites(DAS)and nanoclusters is shown to result in superior performances in the hydrogen evolution reaction(HER).Metal diatomic sites are more complex than single-atom sites but their unique electronic structures can lead to significant enhancement of the HER kinetics.Although the synthesis and identification of DAS is usually challenging,we report a simple access to a diatomic catalyst by anchoring Co-Ru DAS on nitrogen-doped carbon supports along with Ru nanoparticles(NPs).Experimental and theoretical results revealed the atomic-level characteristics of Co-Ru sites,their strong electronic coupling and their synergy with Ru NPs within the catalyst.The unique electronic structure of the catalyst resulted in an excellent HER activity and stability in alkaline media.This work provides a valuable insight into a widely applicable design of diatomic catalysts with multi-component active sites for highly efficient HER electrocatalysis.
基金This work was supported by the Science and Technology Development Fund,Macao SAR(Nos.FDCT 0044/2018/AFJ and 0002/2019/APD).
文摘Objective: The coronavirus disease 2019 (COVID-19) epidemic resulting from severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) has still spread globally. The occurrence of the Delta variant, which is more infectious and spreads faster than earlier forms of the virus that causes COVID-19, makes infection prevention more challenging. Therefore, this study aimed to gain a comprehensive insight into the transmission routes of SARS-CoV-2 for curbing the propagation of SARS-CoV-2 in human populations.Methods: We studied a prospective cohort of 576 patients admitted consecutively to the First Affiliated Hospital of Guangzhou Medical University from January 21 to June 8, 2020. These patients were chosen based on their similar clinical phenotypes or imaging findings. There were 21 (3.6%) laboratory-confirmed COVID-19 patients (16 severe and 5 mild cases) and 555 non-COVID-19 patients. The antibody response and routes and duration of viral shedding were systematically evaluated in serial clinical specimens. Moreover, SARS-CoV-2 RNA was also detected in a mouth rinse, urine, and tear samples. This study was approved by the Medical Ethical Committee of The First Affiliated Hospital of Guangzhou Medical University (approval No. 2020-77).Results: SARS-CoV-2 mainly existed in sputum, nasal and throat swabs, and feces samples. Virus latency was longer in sputum and feces samples than in nasopharyngeal samples. IgG antibody response in respiratory samples was related to disease severity. Although droplets and aerosols are the major transmission routes for COVID-19, covert routes of transmission from asymptomatic patients, contaminated surfaces, and wastewater are also of interest.Conclusion: Our findings provide a solid foundation for developing prophylactic measures against SARS-CoV-2.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(Nos.2023A1515110260 and 2023A1515140049)Special Projects in Key Areas of the Guangdong Provincial Department of Education(No.2024ZDZX2093).
文摘At present,excessive carbon dioxide(CO_(2))emission has become an increasingly prominent global energy and environmental issue.Therefore,effective methods to convert CO_(2) into fine chemicals are urgently required.Herein,series of S-doped carbon-nitrogen(CNS-X)materials(where X denotes the ratio of thiourea and melamine substances ranging from 0.03 to 0.8)was prepared via the programmed temperature pyrolysis method,which thiourea(CH4N_(2)S)and melamine was used as the precursor of the catalysts.The sulfur source endow the CNS-X acidic sites,which cooperate synergistically with amino groups from the incomplete polymerization of melamine,leading to a bifunctional catalyst for cycloaddition reaction of CO_(2) with epoxides.These catalysts were characterized using X-ray diffraction,Fourier transform infrared spectroscopy,elemental analysis,X-ray photoelectron spectroscopy,and N_(2) adsorption-desorption techniques,confirming the successful integration of functional groups.The optimal thiourea doping concentration of 0.4 was certainly found to have considerably facilitated the efficient conversion of CO_(2) by the CNS-0.4 catalyst,in which the conversion of epichlorohydrin(ECH)could achieve over 90.0% and the selectivity of cyclic carbonate is 98.0% under 1.0 MPa at 140℃ for 10 h.The superior catalytic performance of CNS-0.4 was attributable to the synergistic effect arising from the co-existence of Lewis acidic and basic sites.Notably,using CNS-0.4 resulted in a high yield even after four reaction cycles.
基金financially supported by National Natural Science Foundation of China(22172077,T2322013)the Scientific Research Foundation of Chemistry and Chemical Engineering Guangdong Laboratory(2011001)the support by the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(2018M3D1A1058624,2019R1A2C3010479)。
