Ethylene glycol(EG)plays a pivotal role as a primary raw material in the polyester industry,and the syngas-to-EG route has become a significant technical route in production.The carbon monoxide(CO)gas-phase catalytic ...Ethylene glycol(EG)plays a pivotal role as a primary raw material in the polyester industry,and the syngas-to-EG route has become a significant technical route in production.The carbon monoxide(CO)gas-phase catalytic coupling to synthesize dimethyl oxalate(DMO)is a crucial process in the syngas-to-EG route,whereby the composition of the reactor outlet exerts influence on the ultimate quality of the EG product and the energy consumption during the subsequent separation process.However,measuring product quality in real time or establishing accurate dynamic mechanism models is challenging.To effectively model the DMO synthesis process,this study proposes a hybrid modeling strategy that integrates process mechanisms and data-driven approaches.The CO gas-phase catalytic coupling mechanism model is developed based on intrinsic kinetics and material balance,while a long short-term memory(LSTM)neural network is employed to predict the macroscopic reaction rate by leveraging temporal relationships derived from archived measurements.The proposed model is trained semi-supervised to accommodate limited-label data scenarios,leveraging historical data.By integrating these predictions with the mechanism model,the hybrid modeling approach provides reliable and interpretable forecasts of mass fractions.Empirical investigations unequivocally validate the superiority of the proposed hybrid modeling approach over conventional data-driven models(DDMs)and other hybrid modeling techniques.展开更多
The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))a...The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))are measured by employing an ion imaging mass spectrometer and two ion-pair dissociation channels(C^(+)+O^(+)and C^(2+)+O^(+))are identified.The absolute cross sections for producing individual ions and their total,as well as for the ion-pair dissociation channels are obtained by normalizing the data of CO^(+)to that of Ar^(+)from CO-Ar mixture target with a fixed 1:1 ratio.The overall errors are evaluated by considering various kinds of uncertainties.A comprehensive comparison is made with the available data,which shows a good agreement with each other over the energy ranges that are overlapped.This work presents new cross-section data with electron energies above 1000 eV.展开更多
All of the experimentally known electronic states of the Cr group metal monoxides(Cr O,Mo O,and WO)have been presented in the paper.The optical spectra of the Cr O molecule have been investigated in the gas phase thro...All of the experimentally known electronic states of the Cr group metal monoxides(Cr O,Mo O,and WO)have been presented in the paper.The optical spectra of the Cr O molecule have been investigated in the gas phase through a combination of the laser-induced fluorescence(LIF)excitation and single-vibronic-level(SVL)emission spectroscopy in the supersonic expansion.The rotational constants of the vibronic electronic states,including X^(5)Π_(-1)(v=0–3),B^(5)Π_(-1)(v=0–10),and B~5Π_1(v=1,5),and the vibrational constants of the spin–orbit components X^(5)Π_(-1,0,1)have been obtained.The molecular constants of the Mo O and WO molecules have been summarized by reviewing the previous spectroscopic studies,and a comprehensive energy level diagram of the Cr group metal monoxides has been constructed.By comparing the electronic configurations,bond lengths,and vibrational frequencies of all the transition metal monoxides in the ground electronic state,the significance of the relativistic effect in the bonding of the 5d transition metal monoxides has been discussed.The related spectroscopic data of the Cr O molecule are available at https://doi.org/10.57760/sciencedb.j00113.00085.展开更多
BACKGROUND Coronavirus disease 2019(COVID-19),which recently spread throughout the entire world,is still a significant health issue.Additionally,the most common cause of risky poisoning in emergency services is carbon...BACKGROUND Coronavirus disease 2019(COVID-19),which recently spread throughout the entire world,is still a significant health issue.Additionally,the most common cause of risky poisoning in emergency services is carbon monoxide(CO)poisoning.Both disorders seem to merit more research as they have an impact on all bodily systems via the lungs.AIM To determine how arterial blood gas and carboxyhemoglobin(COHb)levels affect the clinical and prognostic results of individuals requiring emergency treatment who have both COVID-19 and CO poisoning.METHODS Between January 2018 and December 2021,479 CO-poisoning patients participated in this single-center,retrospective study.Patients were primarily divided into two groups for analysis:Pre-pandemic and pandemic periods.Additionally,the pandemic era was divided into categories based on the presence of COVID-19 and,if present,the clinical severity of the infection.The hospital information system was used to extract patient demographic,clinical,arterial blood gas,COVID-19 polymerase chain reaction,and other laboratory data.RESULTS The mean age of the 479 patients was 54.93±11.51 years,and 187(39%)were female.226(47%)patients were in the pandemic group and 143(30%)of them had a history of COVID-19.While the mean potential of hydrogen(pH)in arterial blood gas of all patients was 7.28±0.15,it was 7.35±0.10 in the pre-pandemic group and 7.05±0.16 in the severe group during the pandemic period(P<0.001).COHb was 23.98±4.19%in the outpatients and 45.26%±3.19%in the mortality group(P<0.001).Partial arterial oxygen pressure(PaO2)was 89.63±7.62 mmHg in the pre-pandemic group,and 79.50±7.18 mmHg in the severe group during the pandemic period(P<0.001).Despite the fact that mortality occurred in 35(7%)of all cases,pandemic cases accounted for 30 of these deaths(85.7%)(P<0.001).The association between COHb,troponin,lactate,partial arterial pressure of carbon dioxide,HCO3,calcium,glucose,age,pH,PaO2,potassium,sodium,and base excess levels in the pre-pandemic and pandemic groups was statistically significant in univariate linear analysis.CONCLUSION Air exchange barrier disruption caused by COVID-19 may have pulmonary consequences.In patients with a history of pandemic COVID-19,clinical results and survival are considerably unfavorable in cases of CO poisoning.展开更多
Carbon monoxide (CO) poisoning is a frequent cause of emergency room admissions, especially during winter days, the symptoms are varied ranging from a simple headache to a serious cardiac and neurological impairment t...Carbon monoxide (CO) poisoning is a frequent cause of emergency room admissions, especially during winter days, the symptoms are varied ranging from a simple headache to a serious cardiac and neurological impairment that can be deadly. Diagnosis is based on the circumstances of occurrence as well as the dosage of carboxyhemoglobin in the blood. Exposure to CO has serious consequences, neurological and cardiac manifestations are not negligible and vary from repolarization disorders to heart attack. Treatment is urgent with normobaric or hyperbaric oxygen therapy. We report a case of a 2-year male child admitted to the emergency room for CO intoxication with an intracardiac thrombus subsequently complicated by an ischemic stroke with a fatal outcome in order to highlight this complication rarely described in literature.展开更多
This paper presents a system approach of mass balance calculations of ozone and other species under diffusion-convection-reaction processes to study the impacts of major ozone-depleting chemicals, chlorine (Cl) and ch...This paper presents a system approach of mass balance calculations of ozone and other species under diffusion-convection-reaction processes to study the impacts of major ozone-depleting chemicals, chlorine (Cl) and chlorine monoxide (ClO), and the effect of photolysis on ozone concentrations, ozone depletion, total ozone abundance, and ozone layer along the altitude in the stratosphere. The calculated ozone concentrations and profile of the layer followed a similar trend and were generally in good agreement with the measurements above the tropical area. The calculated peak of the layer was at the same mid-stratosphere at Z = 30 km with a peak concentration and total ozone abundance about 20% higher than the measured peak concentration of 8.0 ppm and total abundance of 399 DU. In the presence of Cl and ClO, the calculated ozone concentrations and total abundance were substantially reduced. Cl generally depleted more uniformly of ozone across the altitude, while ClO reduced substantially the ozone in the upper stratosphere and thus shifted the peak of the layer to a much lower elevation at Z = 14 km. Although both ClO and Cl are active ozone-depleting chemicals, ClO was found to have a more pronounced impact on ozone depletion and distribution than Cl. The possible explanations of these interesting phenomena were discussed and elaborated. The approach and calculations in this paper were shown to be useful in providing an initial insight into the structure and behavior of the complex ozone layer.展开更多
Silicon monoxide(SiO)is regarded as a potential candidate for anode materials of lithium-ion batteries(LIBs).Unfortunately,the application of SiO is limited by poor initial Coulombic efficiency(ICE)and unsteady solid ...Silicon monoxide(SiO)is regarded as a potential candidate for anode materials of lithium-ion batteries(LIBs).Unfortunately,the application of SiO is limited by poor initial Coulombic efficiency(ICE)and unsteady solid electrolyte interface(SEI),which induce low energy,short cycling life,and poor rate properties.To address these drawbacks of SiO,we achieve in-situ construction of robust and fast-ion conducting F,N-rich SEI layer on prelithiated micro-sized SiO(P-μSiO)via the simple and continuous treatment ofμSiO in mild lithium 4,4′-dimethylbiphenyl solution and nonflammable hexafluorocyclotriphosphazene solution.Chemical prelithiation eliminates irreversible capacity through pre-forming inactive lithium silicates.Meanwhile,the symbiotic F,N-rich SEI with good mechanical stability and fast Li^(+)permeability is conductive to relieve volume expansion ofμSiO and boost the Li+diffusion kinetics.Consequently,the P-μSiO realizes an impressive electrochemical performance with an elevated ICE of 99.57%and a capacity retention of 90.67%after 350 cycles.Additionally,the full cell with P-μSiO anode and commercial LiFePO_(4) cathode displays an ICE of 92.03%and a high reversible capacity of 144.97 mA h g^(-1).This work offers a general construction strategy of robust and ionically conductive SEI for advanced LIBs.展开更多
The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped c...The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped carbon xerogel(Cu-N-C) are successfully developed varying the copper amount and the nature of the copper precursor, for the efficient CO_(2)RR. The electrocatalytic performance of Cu-N-C materials is assessed by a rotating ring-disc electrode(RRDE), technique still rarely explored for CO_(2)RR. For comparison, products are also characterized by online gas chromatography in a H-cell. The as-synthesized Cu-NC catalysts are found to be active and highly CO selective at low overpotentials(from -0.6 to -0.8 V vs.RHE) in 0.1 M KHCO_(3), while H_(2) from the competitive water reduction appears at larger overpotentials(-0.9 V vs. RHE). The optimum copper acetate-derived catalyst containing Cu-N_(4) moieties exhibits a CO_(2)-to-CO turnover frequency of 997 h^(-1) at -0.9 V vs. RHE with a H_(2)/CO ratio of 1.8. These results demonstrate that RRDE configuration can be used as a feasible approach for identifying electrolysis products from CO_(2)RR.展开更多
In recent years,exploring the relationship between community structure and node centrality in complex networks has gained significant attention from researchers,given its fundamental theoretical significance and pract...In recent years,exploring the relationship between community structure and node centrality in complex networks has gained significant attention from researchers,given its fundamental theoretical significance and practical implications.To address the impact of network communities on target nodes and effectively identify highly influential nodes with strong propagation capabilities,this paper proposes a novel influential spreaders identification algorithm based on density entropy and community structure(DECS).The proposed method initially integrates a community detection algorithm to obtain the community partition results of the networks.It then comprehensively considers the internal and external density entropies and degree centrality of the target node to evaluate its influence.Experimental validation is conducted on eight networks of varying sizes through susceptible–infected–recovered(SIR)propagation experiments and network static attack experiments.The experimental results demonstrate that the proposed method outperforms five other node centrality methods under the same comparative conditions,particularly in terms of information spreading capability,thereby enhancing the accurate identification of critical nodes in networks.展开更多
Carbon monoxide(CO)and nitric oxide(NO)are signal molecules that enhance plant adaptation to environmental stimuli.Auxin is an essential phytohormone for plant growth and development.CO and NO play crucial roles in mo...Carbon monoxide(CO)and nitric oxide(NO)are signal molecules that enhance plant adaptation to environmental stimuli.Auxin is an essential phytohormone for plant growth and development.CO and NO play crucial roles in modulating the plant’s response to iron deficiency.Iron deficiency leads to an increase in the activity of heme oxygenase(HO)and the subsequent generation of CO.Additionally,it alters the polar subcellular distribution of Pin-Formed 1(PIN1)proteins,resulting in enhanced auxin transport.This alteration,in turn,leads to an increase in NO accumulation.Furthermore,iron deficiency enhances the activity of ferric chelate reductase(FCR),as well as the expression of the Fer-like iron deficiency-induced transcription factor 1(FIT)and the ferric reduction oxidase 2(FRO2)genes in plant roots.Overexpression of the long hypocotyl 1(HY1)gene,which encodes heme oxygenase,or the CO donor treatment resulted in enhanced basipetal auxin transport,higher FCR activity,and the expression of FIT and FRO2 genes under Fe deficiency.Here,a potential mechanism is proposed:CO and NO interact with auxin to address iron deficiency stress.CO alters auxin transport,enhancing its accumulation in roots and up-regulating key iron-related genes like FRO2 and IRT1.Elevated auxin levels affect NO signaling,leading to greater sensitivity in root development.This interplay promotes FCR activity,which is crucial for iron absorption.Together,these molecules enhance iron uptake and root growth,revealing a novel aspect of plant physiology in adapting to environmental stress.展开更多
电催化CO_(2)还原反应(Electrocatalytic CO_(2)reduction reaction, CO_(2)RR)在解决全球变暖和能源危机方面有着巨大的应用潜力,但目前催化效率低、催化产物多样等问题限制了CO_(2)RR反应的商业化应用。采用一锅法、碳化法制备了一系...电催化CO_(2)还原反应(Electrocatalytic CO_(2)reduction reaction, CO_(2)RR)在解决全球变暖和能源危机方面有着巨大的应用潜力,但目前催化效率低、催化产物多样等问题限制了CO_(2)RR反应的商业化应用。采用一锅法、碳化法制备了一系列不同镍含量的镍单原子催化剂,利用XRD、XPS、ICP-OES、HRTEM、HAADF-STEM、XAS等方法对镍单原子催化剂的形貌结构、原子价态、金属含量等方面进行表征,并通过电催化还原产物的法拉第效率(Faraday efficiency, FE)和电流密度(Current density,J)来评价其电催化性能。此外,还研究了电解实验装置的改变对升电催化性能的提升。实验结果表明,随着Ni单原子催化剂的Ni金属负载量增加,产物CO的FECO和JCO均增加。催化剂中Zn1Ni2-CN表现出了优异的CO_(2)RR催化性能,在H型电解池中,在-0.7 V vs. RHE电位下FECO达到89%,在-0.9 V vs. RHE下JCO达到6.99 mA·cm^(-2)。在流动电解池中,大范围电位变化下(-0.4~-1.2 V vs. RHE)FECO均保持在99%以上,且在-1.2 V vs. RHE电位下产物电流密度JCO达到174.5 mA·cm^(-2)。展开更多
基金supported in part by the National Key Research and Development Program of China(2022YFB3305300)the National Natural Science Foundation of China(62173178).
文摘Ethylene glycol(EG)plays a pivotal role as a primary raw material in the polyester industry,and the syngas-to-EG route has become a significant technical route in production.The carbon monoxide(CO)gas-phase catalytic coupling to synthesize dimethyl oxalate(DMO)is a crucial process in the syngas-to-EG route,whereby the composition of the reactor outlet exerts influence on the ultimate quality of the EG product and the energy consumption during the subsequent separation process.However,measuring product quality in real time or establishing accurate dynamic mechanism models is challenging.To effectively model the DMO synthesis process,this study proposes a hybrid modeling strategy that integrates process mechanisms and data-driven approaches.The CO gas-phase catalytic coupling mechanism model is developed based on intrinsic kinetics and material balance,while a long short-term memory(LSTM)neural network is employed to predict the macroscopic reaction rate by leveraging temporal relationships derived from archived measurements.The proposed model is trained semi-supervised to accommodate limited-label data scenarios,leveraging historical data.By integrating these predictions with the mechanism model,the hybrid modeling approach provides reliable and interpretable forecasts of mass fractions.Empirical investigations unequivocally validate the superiority of the proposed hybrid modeling approach over conventional data-driven models(DDMs)and other hybrid modeling techniques.
基金Project supported by the National Key Research and Development Program of China (Grant No.2022YFA1602502)the National Natural Science Foundation of China (Grant No.12127804)the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant Nos.XDB34000000)。
文摘The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))are measured by employing an ion imaging mass spectrometer and two ion-pair dissociation channels(C^(+)+O^(+)and C^(2+)+O^(+))are identified.The absolute cross sections for producing individual ions and their total,as well as for the ion-pair dissociation channels are obtained by normalizing the data of CO^(+)to that of Ar^(+)from CO-Ar mixture target with a fixed 1:1 ratio.The overall errors are evaluated by considering various kinds of uncertainties.A comprehensive comparison is made with the available data,which shows a good agreement with each other over the energy ranges that are overlapped.This work presents new cross-section data with electron energies above 1000 eV.
基金the National Key R&D Program of China(Grant No.2022YFA1602500)the National Natural Science Foundation of China(Grant No.12027809)Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB21030900)。
文摘All of the experimentally known electronic states of the Cr group metal monoxides(Cr O,Mo O,and WO)have been presented in the paper.The optical spectra of the Cr O molecule have been investigated in the gas phase through a combination of the laser-induced fluorescence(LIF)excitation and single-vibronic-level(SVL)emission spectroscopy in the supersonic expansion.The rotational constants of the vibronic electronic states,including X^(5)Π_(-1)(v=0–3),B^(5)Π_(-1)(v=0–10),and B~5Π_1(v=1,5),and the vibrational constants of the spin–orbit components X^(5)Π_(-1,0,1)have been obtained.The molecular constants of the Mo O and WO molecules have been summarized by reviewing the previous spectroscopic studies,and a comprehensive energy level diagram of the Cr group metal monoxides has been constructed.By comparing the electronic configurations,bond lengths,and vibrational frequencies of all the transition metal monoxides in the ground electronic state,the significance of the relativistic effect in the bonding of the 5d transition metal monoxides has been discussed.The related spectroscopic data of the Cr O molecule are available at https://doi.org/10.57760/sciencedb.j00113.00085.
文摘BACKGROUND Coronavirus disease 2019(COVID-19),which recently spread throughout the entire world,is still a significant health issue.Additionally,the most common cause of risky poisoning in emergency services is carbon monoxide(CO)poisoning.Both disorders seem to merit more research as they have an impact on all bodily systems via the lungs.AIM To determine how arterial blood gas and carboxyhemoglobin(COHb)levels affect the clinical and prognostic results of individuals requiring emergency treatment who have both COVID-19 and CO poisoning.METHODS Between January 2018 and December 2021,479 CO-poisoning patients participated in this single-center,retrospective study.Patients were primarily divided into two groups for analysis:Pre-pandemic and pandemic periods.Additionally,the pandemic era was divided into categories based on the presence of COVID-19 and,if present,the clinical severity of the infection.The hospital information system was used to extract patient demographic,clinical,arterial blood gas,COVID-19 polymerase chain reaction,and other laboratory data.RESULTS The mean age of the 479 patients was 54.93±11.51 years,and 187(39%)were female.226(47%)patients were in the pandemic group and 143(30%)of them had a history of COVID-19.While the mean potential of hydrogen(pH)in arterial blood gas of all patients was 7.28±0.15,it was 7.35±0.10 in the pre-pandemic group and 7.05±0.16 in the severe group during the pandemic period(P<0.001).COHb was 23.98±4.19%in the outpatients and 45.26%±3.19%in the mortality group(P<0.001).Partial arterial oxygen pressure(PaO2)was 89.63±7.62 mmHg in the pre-pandemic group,and 79.50±7.18 mmHg in the severe group during the pandemic period(P<0.001).Despite the fact that mortality occurred in 35(7%)of all cases,pandemic cases accounted for 30 of these deaths(85.7%)(P<0.001).The association between COHb,troponin,lactate,partial arterial pressure of carbon dioxide,HCO3,calcium,glucose,age,pH,PaO2,potassium,sodium,and base excess levels in the pre-pandemic and pandemic groups was statistically significant in univariate linear analysis.CONCLUSION Air exchange barrier disruption caused by COVID-19 may have pulmonary consequences.In patients with a history of pandemic COVID-19,clinical results and survival are considerably unfavorable in cases of CO poisoning.
文摘Carbon monoxide (CO) poisoning is a frequent cause of emergency room admissions, especially during winter days, the symptoms are varied ranging from a simple headache to a serious cardiac and neurological impairment that can be deadly. Diagnosis is based on the circumstances of occurrence as well as the dosage of carboxyhemoglobin in the blood. Exposure to CO has serious consequences, neurological and cardiac manifestations are not negligible and vary from repolarization disorders to heart attack. Treatment is urgent with normobaric or hyperbaric oxygen therapy. We report a case of a 2-year male child admitted to the emergency room for CO intoxication with an intracardiac thrombus subsequently complicated by an ischemic stroke with a fatal outcome in order to highlight this complication rarely described in literature.
文摘This paper presents a system approach of mass balance calculations of ozone and other species under diffusion-convection-reaction processes to study the impacts of major ozone-depleting chemicals, chlorine (Cl) and chlorine monoxide (ClO), and the effect of photolysis on ozone concentrations, ozone depletion, total ozone abundance, and ozone layer along the altitude in the stratosphere. The calculated ozone concentrations and profile of the layer followed a similar trend and were generally in good agreement with the measurements above the tropical area. The calculated peak of the layer was at the same mid-stratosphere at Z = 30 km with a peak concentration and total ozone abundance about 20% higher than the measured peak concentration of 8.0 ppm and total abundance of 399 DU. In the presence of Cl and ClO, the calculated ozone concentrations and total abundance were substantially reduced. Cl generally depleted more uniformly of ozone across the altitude, while ClO reduced substantially the ozone in the upper stratosphere and thus shifted the peak of the layer to a much lower elevation at Z = 14 km. Although both ClO and Cl are active ozone-depleting chemicals, ClO was found to have a more pronounced impact on ozone depletion and distribution than Cl. The possible explanations of these interesting phenomena were discussed and elaborated. The approach and calculations in this paper were shown to be useful in providing an initial insight into the structure and behavior of the complex ozone layer.
基金financially supported by the National Natural Science Foundation of China(Nos.51972198 and 62133007)the Natural Science Foundation of Shandong Province(ZR2020JQ19)the Taishan Scholars Program of Shandong Province(Nos.tsqn201812002 and ts20190908)。
文摘Silicon monoxide(SiO)is regarded as a potential candidate for anode materials of lithium-ion batteries(LIBs).Unfortunately,the application of SiO is limited by poor initial Coulombic efficiency(ICE)and unsteady solid electrolyte interface(SEI),which induce low energy,short cycling life,and poor rate properties.To address these drawbacks of SiO,we achieve in-situ construction of robust and fast-ion conducting F,N-rich SEI layer on prelithiated micro-sized SiO(P-μSiO)via the simple and continuous treatment ofμSiO in mild lithium 4,4′-dimethylbiphenyl solution and nonflammable hexafluorocyclotriphosphazene solution.Chemical prelithiation eliminates irreversible capacity through pre-forming inactive lithium silicates.Meanwhile,the symbiotic F,N-rich SEI with good mechanical stability and fast Li^(+)permeability is conductive to relieve volume expansion ofμSiO and boost the Li+diffusion kinetics.Consequently,the P-μSiO realizes an impressive electrochemical performance with an elevated ICE of 99.57%and a capacity retention of 90.67%after 350 cycles.Additionally,the full cell with P-μSiO anode and commercial LiFePO_(4) cathode displays an ICE of 92.03%and a high reversible capacity of 144.97 mA h g^(-1).This work offers a general construction strategy of robust and ionically conductive SEI for advanced LIBs.
基金Grant PID2020-115848RB-C21 "STORELEC" projectTED2021-129694B-C22 "DEFY-CO2" project funded by MCIN/AEI/10.13039/501100011033+3 种基金LMP253_ (2)1 project funded by Gobierno de AragónGrant IJC2019-041874-I funded by the MCIN/AEI/10.13039/501100011033CSIC for her JAE Intro ICU 2021-ICB-04 grantthe Y2020/EMT-6419 "CEOTRES" project funded by the Comunidad Autonoma de Madrid。
文摘The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped carbon xerogel(Cu-N-C) are successfully developed varying the copper amount and the nature of the copper precursor, for the efficient CO_(2)RR. The electrocatalytic performance of Cu-N-C materials is assessed by a rotating ring-disc electrode(RRDE), technique still rarely explored for CO_(2)RR. For comparison, products are also characterized by online gas chromatography in a H-cell. The as-synthesized Cu-NC catalysts are found to be active and highly CO selective at low overpotentials(from -0.6 to -0.8 V vs.RHE) in 0.1 M KHCO_(3), while H_(2) from the competitive water reduction appears at larger overpotentials(-0.9 V vs. RHE). The optimum copper acetate-derived catalyst containing Cu-N_(4) moieties exhibits a CO_(2)-to-CO turnover frequency of 997 h^(-1) at -0.9 V vs. RHE with a H_(2)/CO ratio of 1.8. These results demonstrate that RRDE configuration can be used as a feasible approach for identifying electrolysis products from CO_(2)RR.
基金Project supported by the National Natural Science Foundation of China(Grant No.61803264)。
文摘In recent years,exploring the relationship between community structure and node centrality in complex networks has gained significant attention from researchers,given its fundamental theoretical significance and practical implications.To address the impact of network communities on target nodes and effectively identify highly influential nodes with strong propagation capabilities,this paper proposes a novel influential spreaders identification algorithm based on density entropy and community structure(DECS).The proposed method initially integrates a community detection algorithm to obtain the community partition results of the networks.It then comprehensively considers the internal and external density entropies and degree centrality of the target node to evaluate its influence.Experimental validation is conducted on eight networks of varying sizes through susceptible–infected–recovered(SIR)propagation experiments and network static attack experiments.The experimental results demonstrate that the proposed method outperforms five other node centrality methods under the same comparative conditions,particularly in terms of information spreading capability,thereby enhancing the accurate identification of critical nodes in networks.
基金Open Project of Jiangsu Key Laboratory for Eco-Agricultural Biotechnology around Hongze Lake,Grant Number HZHLAB2201.
文摘Carbon monoxide(CO)and nitric oxide(NO)are signal molecules that enhance plant adaptation to environmental stimuli.Auxin is an essential phytohormone for plant growth and development.CO and NO play crucial roles in modulating the plant’s response to iron deficiency.Iron deficiency leads to an increase in the activity of heme oxygenase(HO)and the subsequent generation of CO.Additionally,it alters the polar subcellular distribution of Pin-Formed 1(PIN1)proteins,resulting in enhanced auxin transport.This alteration,in turn,leads to an increase in NO accumulation.Furthermore,iron deficiency enhances the activity of ferric chelate reductase(FCR),as well as the expression of the Fer-like iron deficiency-induced transcription factor 1(FIT)and the ferric reduction oxidase 2(FRO2)genes in plant roots.Overexpression of the long hypocotyl 1(HY1)gene,which encodes heme oxygenase,or the CO donor treatment resulted in enhanced basipetal auxin transport,higher FCR activity,and the expression of FIT and FRO2 genes under Fe deficiency.Here,a potential mechanism is proposed:CO and NO interact with auxin to address iron deficiency stress.CO alters auxin transport,enhancing its accumulation in roots and up-regulating key iron-related genes like FRO2 and IRT1.Elevated auxin levels affect NO signaling,leading to greater sensitivity in root development.This interplay promotes FCR activity,which is crucial for iron absorption.Together,these molecules enhance iron uptake and root growth,revealing a novel aspect of plant physiology in adapting to environmental stress.
文摘电催化CO_(2)还原反应(Electrocatalytic CO_(2)reduction reaction, CO_(2)RR)在解决全球变暖和能源危机方面有着巨大的应用潜力,但目前催化效率低、催化产物多样等问题限制了CO_(2)RR反应的商业化应用。采用一锅法、碳化法制备了一系列不同镍含量的镍单原子催化剂,利用XRD、XPS、ICP-OES、HRTEM、HAADF-STEM、XAS等方法对镍单原子催化剂的形貌结构、原子价态、金属含量等方面进行表征,并通过电催化还原产物的法拉第效率(Faraday efficiency, FE)和电流密度(Current density,J)来评价其电催化性能。此外,还研究了电解实验装置的改变对升电催化性能的提升。实验结果表明,随着Ni单原子催化剂的Ni金属负载量增加,产物CO的FECO和JCO均增加。催化剂中Zn1Ni2-CN表现出了优异的CO_(2)RR催化性能,在H型电解池中,在-0.7 V vs. RHE电位下FECO达到89%,在-0.9 V vs. RHE下JCO达到6.99 mA·cm^(-2)。在流动电解池中,大范围电位变化下(-0.4~-1.2 V vs. RHE)FECO均保持在99%以上,且在-1.2 V vs. RHE电位下产物电流密度JCO达到174.5 mA·cm^(-2)。
