Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we r...Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.展开更多
Developing a green economy is key to achieving the 2030 Sustainable Development Goals. This paper uses the SBM-GML index, which includes non-desired outputs, to measure the trend of regional green economic efficiency ...Developing a green economy is key to achieving the 2030 Sustainable Development Goals. This paper uses the SBM-GML index, which includes non-desired outputs, to measure the trend of regional green economic efficiency changes and analyze the impact mechanism and realization path of industrial transformation on green economic efficiency. The research results show that advanced industrial structure has a positive influence on green economic efficiency nationwide, while energy utilization structure and energy utilization efficiency have positive partial intermediary effects in the influence path;industrial structure rationalization is also significantly positively related to green economic efficiency nationwide, and the mediating effect of energy utilization is positive. The impact of industrial transformation on green economic efficiency has regional heterogeneity, and the mediating effect of energy use also differs. Among them, the impact effect in the eastern region is basically consistent with the national sample, but is negative in the central and western regions. This paper proposes countermeasures in terms of adjusting the industrial structure, improving energy efficiency, and perfecting industrial and energy policies, which can provide theoretical and practical references for promoting the transformation and upgrading of regional industrial structure, optimizing energy utilization, and advancing the efficiency of the national and regional green economy.展开更多
Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental pollution.Currently,the vast majority of the...Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental pollution.Currently,the vast majority of the world's hydrogen is produced by reforming fossil fuels;however,this hydrogen-making technology is not sustainable or environmentally friendly because ofits high energy consumption and large carbon emissions.Renewables-driven water splitting(2H_(2)0-2H_(2)+0_(2))becomes an extensively studied scheme for sustain-able hydrogen production.Conventional water electrolysis requires an input voltage higher than 1.23 V and forms a gas mixture of H_(2)/O_(2),which results in high electricity consumption,potential safety hazards,and harmful reactive oxygen species.By virtue of the auxiliary redox mediators(RMs)as the robust H^(+)/e^(-)reservoir,decoupled electrolysis splits water at a much lower potential and evolves O_(2)(H_(2)O+RMS_(ox)-O_(2)+H-RMS_(red))and H_(2)(H-RMS_(red)-H_(2)+RMS_(ox))at separate times,rates,and spaces,thus pro-ducing the puretarget hydrogen gas safely.Decoupled electrolysis has accelerated the development ofwater electrolysis technology for H_(2) production.However,itis still lack of a comprehensive and in-depth review in this field based on different types of RMs.This review highlights the basic principles and critical progress of this emerging water electrolysis mode over the past decade.Several representative examples are then dis-played in detail according to the differences in the RMs.The rational choice and design of RMs have also been emphasized.Subsequently,novel applications of decoupled water splitting are briefly discussed,including the manufacture of valuable chemicals,Cl_(2) production,pollutant degradation,and other half-reactions in artificial photosynthesis.Finally,thekey characteristics and disadvantages of each type of mediator are sum-marized in depth.In addition,we present an outlook for future directions in decoupled water splitting.Thus,the flexibility in the design of mediators provides huge space for improving this electrochemical technology.@2024 Science Press and Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by ELSEVIER B.V.and Science Press.All rights reserved.展开更多
Decoupled Catalytic Hydrogen Evolution from a Molecular Metal Oxide Redox Mediator in Water Splitting B.Rausch,M.D.Symes,G.Chisholm,L.Cronin Science345（2014）6202.以杂多酸H4[SiW12O40]的还原加氢代替水分解中的氢析出反...Decoupled Catalytic Hydrogen Evolution from a Molecular Metal Oxide Redox Mediator in Water Splitting B.Rausch,M.D.Symes,G.Chisholm,L.Cronin Science345（2014）6202.以杂多酸H4[SiW12O40]的还原加氢代替水分解中的氢析出反应,然后将还原产物H6[SiW12O40]在隔离的空间与Pt催化剂接触释放出H2.Synergistic Geometric and Electronic Effects for Electrochemical Reduction of Carbon Dioxide Using Gold-Copper Bimetallic Nanoparticles。展开更多
人机交互语言工具是电信网管的重要组成部分,是网管系统中使用频率最高的模块之一,命令参数的显示控制是它的实现难点.基于Mediator模式的参数控制法分离了参数表示和逻辑控制,它让每个参数专心处理自身表示,由中介者控制显示逻辑,解除...人机交互语言工具是电信网管的重要组成部分,是网管系统中使用频率最高的模块之一,命令参数的显示控制是它的实现难点.基于Mediator模式的参数控制法分离了参数表示和逻辑控制,它让每个参数专心处理自身表示,由中介者控制显示逻辑,解除了参数间的耦合关系.这种实现方法,集中了对参数的控制,减少了耦合,有利于各参数的复用,易于逻辑关系扩展,提高了命令解析效率.实际测试表明,在PIII 1.0 G CPU环境下,解析一条命令的平均时间只需0.14 s.该方法为开发网管人机交互语言工具或处理对象强耦合问题提供了一种有参考价值的实现方法.展开更多
Most non-native speakers do have difficulty in developing native-like oracy due to vast differences in pronunciation between L1 and L2, adult ESL learners in particular. As Peter and Susan pointed in Teaching American...Most non-native speakers do have difficulty in developing native-like oracy due to vast differences in pronunciation between L1 and L2, adult ESL learners in particular. As Peter and Susan pointed in Teaching American English Pronunciation(1992), there are specific problem syllables with different language groups. As an ESL teacher from China, I assume it necessary to find out whether these sounds really trouble Chinese students in the ESL class I observed. I am going to pick out the most frequently occurred problem sounds and take notes how the teacher deal with them in class. In this paper, based on classroom observation and interviews, I analyzed problematic English vowels and consonants from Chinese learners, and the corresponding mediations for ESL teacher.展开更多
BACKGROUND： Sepsis and secondary multiple organ failure in critically ill patients are the major cause of death, but the pathogenesis of sepsis is not clear, especially the dysfunction of the immune system. In this p...BACKGROUND： Sepsis and secondary multiple organ failure in critically ill patients are the major cause of death, but the pathogenesis of sepsis is not clear, especially the dysfunction of the immune system. In this paper, we review the response and regulation of the immune system and the functions of a variety of inflammatory mediators in sepsis. DATA SOURCES Studies were identified by searching MEDLINE and PubMed for articles using the keywords ＂sepsis＂, ＂immune response＂, and ＂inflammatory mediator＂ up to October 2010. Additional papers were identified by a manual search of the references from the key articles.RESULTS： This systematic review was conducted of： 1） the immune response; 2） immune regulation; 3） inflammatory mediators; 4） high-mobility group box 1 protein; 5） the complement system; and 6） the autonomic nervous system. There are no therapeutic approaches available for sepsis that target inflammatory response; the mortality of sepsis has not been significantly reduced. Sepsis is complex and dynamic, and it has a group of heterogeneous syndromes.CONCLUSIONS： Since different patients with sepsis have different etiology, susceptibility, and responses, treatment should be prescribed individually.展开更多
Background Good interpersonal relationships can improve the negative mood and, to a certain extent, may help relieve dysmenorrhea symptoms. However, there has been no study examining the role of interpersonal relation...Background Good interpersonal relationships can improve the negative mood and, to a certain extent, may help relieve dysmenorrhea symptoms. However, there has been no study examining the role of interpersonal relationships in dysmenorrhea and how they may interact with negative emotions. Aims To investigate the connection between negative affect and dysmenorrhea, and the role of interpersonal relationships plays in this relationship. Methods The Cox Menstrual Symptom Scale (CMSS), short-form of Depression Anxiety Stress Scale, Interpersonal Comprehensive Diagnostic Scale and UCLA (University of California at Los Angeles) Loneliness Scale were applied to 855 adolescent nursing students to collect information on severity and frequency of dysmenorrheal symptoms, negative emotions (including depression, anxiety and stress), interpersonal problems and subjective experience of loneliness among them, and the relationship among these variables was examined. Results (1) Both the severity and frequency of dysmenorrhea were positively correlated with negative emotions, loneliness experience and interpersonal problems, while negatively correlated with age at menarche.(2) The negative emotions, romantic relationship and menarche age, but not loneliness and interpersonal problems, significantly contributed to both the severity and frequency of dysmenorrhea.(3) Mediation analysis revealed that the effects of loneliness and interpersonal problems on dysmenorrhea were totally mediated by negative emotions. Conclusions This investigation indicates that the relationship between interpersonal relationships and dysmenorrhea is mediated by negative emotions.展开更多
Sepsis is an infection induced systemic inflammatory response syndrome and is a major cause of morbidity as well as mortality in intensive care units. A growing body of evidence suggests that the activation of a proin...Sepsis is an infection induced systemic inflammatory response syndrome and is a major cause of morbidity as well as mortality in intensive care units. A growing body of evidence suggests that the activation of a proinflammatory cascade is responsible for the development of immune dysfunction, susceptibility to severe sepsis and septic shock. The present theories of sepsis as a dysregulated inflammatory response and immune function, as manifested by excessive release of inflammatory mediators such as high mobility group box 1 protein （HMGB1）, are supported by increasing studies employing animal models and clinical observations of sepsis. HMGB1, originally described as a DNA-binding protein and released passively by necrotic cells and actively by macrophages/monocytes, has been discovered to be one of essential cytokines that mediates the response to infection, injury and inflammation. A growing number of studies still focus on the inflammation-regulatory function and its contribution to infectious and inflammatory disorders, recent data suggest that HMGB1 formation can also markedly influence the host cell-mediated immunity, including T lymphocytes and macrophages. Here we review emerging evidence that support extracellular HMGB1 as a late mediator of septic complications, and discuss the therapeutic potential of several HMGBl-targeting agents in experimental sepsis. In addition, with the development of traditional Chinese medicine in recent years, it has been proven that traditional Chinese herbal materials and their extracts have remarkable effective in treating severe sepsis. In this review, we therefore provide some new concepts of HMGBl-targeted Chinese herbal therapies in sepsis.展开更多
While the sulfur conversion reaction kinetics in Li–S batteries is nowadays improved by the use of appropriate electrocatalysts,it remains a challenge for the batteries to perform well under the lean electrolyte cond...While the sulfur conversion reaction kinetics in Li–S batteries is nowadays improved by the use of appropriate electrocatalysts,it remains a challenge for the batteries to perform well under the lean electrolyte condition where polysulfide shuttle,electrode passivation and the loss of electrolyte due to side reactions,are aggravated.These challenges are addressed in this study by the tandem use of a polysulfide conversion catalyst and a redox–targeting mediator in a gel sulfur cathode.Specifically,the gel cathode reduces the polysulfide mobility and hence the polysulfide shuttle and the passivation of the lithium anode by the crossover polysulfides.The redox mediator restrains the deposition of inactive sulfur species in the cathode thereby enabling the Fe–N and Co–N co–doped carbon catalyst to prolong its catalytic activity.Consequently,the integrated catalytic system is able to increase the discharge capacity of high–loading (6.8 mg cm^(-2)) lean–electrolyte (4.0μL mg^(-1)) Li–S batteries from~630 to~1316 m Ah g^(-1),concurrently with an improvement of the cycle life (600 cycles with 46%capacity retention at 1.0 m A cm^(-2)).Redox mediator assisted catalysis in a gel cathode is therefore an effective strategy to extend the application of the sulfur conversion catalyst in lean electrolyte Li–S batteries.展开更多
Autoimmune disease management presents a significant challenge to medical science. Environmental factors potentially increase the risk of developing inflammatory and autoimmune diseases, such as multiple sclerosis, rh...Autoimmune disease management presents a significant challenge to medical science. Environmental factors potentially increase the risk of developing inflammatory and autoimmune diseases, such as multiple sclerosis, rheumatoid arthritis, and lupus. Among various environmental stresses, cigarette smoke and hypoxia have both been reported to lead to an enhanced risk of inflammatory and autoimmune diseases. In this review, we shed light on all reported mechanisms whereby cigarette smoke and a hypoxic environment can induce inflammatory and autoimmune diseases and discuss how hypoxic conditions influence the cigarette smoke-induced threat of inflammatory and autoimmune disease development. Cigarette smoke and hypoxia both lead to increased oxidative stress and production of reactive oxygen species and other free radicals, which have various effects including the generation of autoreactive pro-inflammatory T cells and autoantibodies, reductions in T regulatory(Treg) cell activity, and enhanced expression of pro-inflammatory mediators [e.g., interleukin-6(IL-6), interleukin-4(IL-4) and interleukin-8(IL-8)]. Accordingly, smoking and hypoxic environments may synergistically act as potent environmental risk factors for inflammatory and autoimmune diseases. To our knowledge, no studies have reported the direct association of cigarette smoke and hypoxic environments with the risk of developing inflammatory and autoimmune diseases. Future studies exploring the risk of autoimmune disease development in smokers at high altitudes, particularly military personnel and mountaineers who are not acclimatized to high-altitude regions, are required to obtain a better understanding of disease risk as well as its management.展开更多
Background Burn-out among doctors threatens their own health, and that of their patients. To identify risk factors of the doctor burn-out is vital to improving their health and increasing the quality of healthcare s...Background Burn-out among doctors threatens their own health, and that of their patients. To identify risk factors of the doctor burn-out is vital to improving their health and increasing the quality of healthcare services. This study aims to explore the relationship between work-family confict （WFC） and burn-out among Chinese doctors and the mediating role of coping styles in this relationship.Methods A cross-sectional survey was conducted in China, with a questionnaire packet which consisted of the Chinese Maslach Burnout Inventory （CMBI）, WFC Scale and the Simplifed Coping Style Questionnaire （SCSQ）. A total of 2530 doctors participated in the survey. Correlation analysis was performed to explore the relationship between CMBI, WFC and SCSQ scores. A linear regression model was set to determine the mediating role of coping styles on the relationship between WFC and burn-out.Results Doctors who had higher scores on work interfering with family confict, reported more emotional exhaustion （r=0.514, P〈0.001） and had a sense of accomplishment （r= 0.149, P〈0.001）. Simultaneously, family interfering with work （FIW） was positively associated with all dimensions of burn-out （r=0.213, 0.504, 0.088, respectively, P〈0.001）. Coping styles had partial, complete and even mediating effects on the relationship between WFC and burn-out among Chinese doctors.Conclusions WFC was correlated with burn-out, and coping style was a mediator in this relationship among Chinese doctors. Coping style was a positive resource against burn-out.展开更多
As promising anodes for sodium-ion batteries,metal sulfides ubiquitously suffer from low-rate and high-plateau issues,greatly hindering their application in full-cells.Herein,exemplifying carbon nanotubes(CNTs)-string...As promising anodes for sodium-ion batteries,metal sulfides ubiquitously suffer from low-rate and high-plateau issues,greatly hindering their application in full-cells.Herein,exemplifying carbon nanotubes(CNTs)-stringed metal sulfides superstructure(CSC)assembled by nano-dispersed SnS_(2) and CoS_(2) phases,cocktail mediation effect similar to that of high-entropy materials is initially studied in ether-based electrolyte to solve the challenges.The high nano-dispersity of metal sulfides in CSC anode underlies the cocktail-like mediation effect,enabling the circumvention of intrinsic drawbacks of different metal sulfides.By utilizing ether-based electrolyte,the reversibility of metal sulfides is greatly improved,sustaining a long-life effectivity of cocktail-like mediation.As such,CSC effectively overcomes low-rate flaw of SnS_(2) and highplateau demerit of CoS_(2),simultaneously realizes a high rate and a low plateau.In half-cells,CSC delivers an ultrahigh-rate capability of 327.6 mAh g^(−1) anode at 20 A g^(−1),far outperforming those of monometallic sulfides(SnS_(2),CoS_(2))and their mixtures.Compared with CoS_(2) phase and SnS_(2)/CoS_(2) mixture,CSC shows remarkably lowered average charge voltage up to ca.0.62 V.As-assembled CSC//Na1.5VPO4.8F0.7 full-cell shows a good rate capability(0.05~1.0 A g^(−1),120.3 mAh g^(−1) electrode at 0.05 A g^(−1))and a high average discharge voltage up to 2.57 V,comparable to full-cells with alloy-type anodes.Kinetics analysis verifies that the cocktail-like mediation effect largely boosts the charge transfer and ionic diffusion in CSC,compared with single phase and mixed phases.Further mechanism study reveals that alternative and complementary electrochemical processes between nano-dispersed SnS_(2) and CoS_(2) phases are responsible for the lowered charge voltage of CSC.This electrolyte/structure-dependent cocktail-like mediation effect effectively enhances the practicability of metal sulfide anodes,which will boost the development of high-rate/-voltage sodium-ion full batteries.展开更多
Rechargeable lithium-oxygen(Li-O_(2))batteries are the next generation energy storage devices due to their ultrahigh theoretical capacity.Redox mediators(RMs)are widely used as a homogenous electrocatalyst in non-aque...Rechargeable lithium-oxygen(Li-O_(2))batteries are the next generation energy storage devices due to their ultrahigh theoretical capacity.Redox mediators(RMs)are widely used as a homogenous electrocatalyst in non-aqueous Li-O_(2)batteries to enhance their discharge capacity and reduce charge overpotential.However,the shuttle effect of RMs in the electrolyte solution usually leads to corrosion of the Li metal anode and uneven Li deposition on the anode surface,resulting in unwanted consumption of electrocatalysts and deterioration of the cells.It is therefore necessary to take some measures to prevent the shuttle effect of RMs and fully utilize the soluble electrocatalysts.Herein,we summarize the strategies to suppress the RM shuttle effect reported in recent years,including electrolyte additives,protective separators and electrode modification.The mechanisms of these strategies are analyzed and their corresponding requirements are discussed.The electrochemical properties of Li-O_(2)batteries with different strategies are summarized and compared.The challenges and perspectives on preventing the shuttle effect of RMs are described for future study.This review provides guidance for achieving shuttle-free redox mediation and for designing Li-O_(2)cells with a long cycle life,high energy efficiency and highly reversible electrochemical reactions.展开更多
The practical applications of lithium-sulfur(Li-S)battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode.One of the effective solutions dea...The practical applications of lithium-sulfur(Li-S)battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode.One of the effective solutions deals with concurrent management of both electrodes.Nevertheless,this direction remains in a nascent stage due to a lack of material selection and mechanism exploration.Herein,we devise a temperature-mediated direct chemical vapor deposition strategy to realize the controllable synthesis of three-dimensional boron/nitrogen dual-doped graphene(BNG)particulated architectures,which is employed as a light-weighted and multi-functional mediator for both electrodes in Li-S batteries.Benefiting from the“sulfiphilic”and“lithiophilic”features,the BNG modified separator not only enables boosted kinetics of polysulfide transformation to mitigate the shuttle effect but also endows uniform lithium deposition to suppress the dendritic growth.Theoretical calculations in combination with electro-kinetic tests and operando Raman analysis further elucidate the favorable sulfur and lithium electrochemistry of BNG at a molecular level.This work offers direct insight into the mediator design via controllable synthesis of graphene materials to tackle the fundamental challenges of Li-S batteries.展开更多
The ever-increasing demand for energy has stimulated the development of economical non-fossil fuels.As representative of clean energy,solar and wind have been identified as the most promising energy sources due to the...The ever-increasing demand for energy has stimulated the development of economical non-fossil fuels.As representative of clean energy,solar and wind have been identified as the most promising energy sources due to their abundance,cost efficiency,and environmental friendliness.The intrinsic intermittent of the clean energy leads to the urgent requirements large-scale energy storage technique.Redox flow batteries(RFBs)are attractive technology due to their independent control over energy and power.Insoluble redox-active flow battery is a new type of electrochemical energy storage technology that disperses redox-active particles in the electrolyte.Compared with traditional flow batteries,insoluble flow batteries have advantages of large energy density and are very promising in the development of large-scale energy storage systems.At present,three types of insoluble flow batteries have been explored:slurry-based flow batteries,metal/slurry hybrid,and redox-mediator-assisted flow batteries.This Review summarizes the research progress of insoluble flow batteries,and analyzes the key challenges from the fundamental research and practical application perspectives.展开更多
Lithium-sulfur(Li-S)batteries are promising energy storage devices owing to their high energy density and the low cost of sulfur.However,they are still far from being applied commercially because of the detrimental ca...Lithium-sulfur(Li-S)batteries are promising energy storage devices owing to their high energy density and the low cost of sulfur.However,they are still far from being applied commercially because of the detrimental capacity fade caused by the dissolution of lithium polysulfide(LPS)in liquid electrolyte.In this study,we introduced a new polymer binder having a redox-mediating function that assists in the reduction of soluble LPS to Li2S at the cathode to suppress the shuttle effect as well as enhance sulfur utilization.An amine group containing benzo(ghi)perylene imide(BPI)was synthesized and grafted onto poly(acrylic acid)to produce a redox-mediating polymer binder.An Li-S cell fabricated using the new redox-mediating polymer binder demonstrated a capacity decay retention of 0.036%per cycle up to 500 cycles at 0.5 C with a coulombic efficiency of 98%.展开更多
基金This study is supported by the National Key Research and Development Program of China(2017YFB0307500).
文摘Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.
基金supported by National Natural Science Foundation of China [grant numbers 42371194]。
文摘Developing a green economy is key to achieving the 2030 Sustainable Development Goals. This paper uses the SBM-GML index, which includes non-desired outputs, to measure the trend of regional green economic efficiency changes and analyze the impact mechanism and realization path of industrial transformation on green economic efficiency. The research results show that advanced industrial structure has a positive influence on green economic efficiency nationwide, while energy utilization structure and energy utilization efficiency have positive partial intermediary effects in the influence path;industrial structure rationalization is also significantly positively related to green economic efficiency nationwide, and the mediating effect of energy utilization is positive. The impact of industrial transformation on green economic efficiency has regional heterogeneity, and the mediating effect of energy use also differs. Among them, the impact effect in the eastern region is basically consistent with the national sample, but is negative in the central and western regions. This paper proposes countermeasures in terms of adjusting the industrial structure, improving energy efficiency, and perfecting industrial and energy policies, which can provide theoretical and practical references for promoting the transformation and upgrading of regional industrial structure, optimizing energy utilization, and advancing the efficiency of the national and regional green economy.
基金the financial support from the National Natural Science Foundation of China(52002146).
文摘Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental pollution.Currently,the vast majority of the world's hydrogen is produced by reforming fossil fuels;however,this hydrogen-making technology is not sustainable or environmentally friendly because ofits high energy consumption and large carbon emissions.Renewables-driven water splitting(2H_(2)0-2H_(2)+0_(2))becomes an extensively studied scheme for sustain-able hydrogen production.Conventional water electrolysis requires an input voltage higher than 1.23 V and forms a gas mixture of H_(2)/O_(2),which results in high electricity consumption,potential safety hazards,and harmful reactive oxygen species.By virtue of the auxiliary redox mediators(RMs)as the robust H^(+)/e^(-)reservoir,decoupled electrolysis splits water at a much lower potential and evolves O_(2)(H_(2)O+RMS_(ox)-O_(2)+H-RMS_(red))and H_(2)(H-RMS_(red)-H_(2)+RMS_(ox))at separate times,rates,and spaces,thus pro-ducing the puretarget hydrogen gas safely.Decoupled electrolysis has accelerated the development ofwater electrolysis technology for H_(2) production.However,itis still lack of a comprehensive and in-depth review in this field based on different types of RMs.This review highlights the basic principles and critical progress of this emerging water electrolysis mode over the past decade.Several representative examples are then dis-played in detail according to the differences in the RMs.The rational choice and design of RMs have also been emphasized.Subsequently,novel applications of decoupled water splitting are briefly discussed,including the manufacture of valuable chemicals,Cl_(2) production,pollutant degradation,and other half-reactions in artificial photosynthesis.Finally,thekey characteristics and disadvantages of each type of mediator are sum-marized in depth.In addition,we present an outlook for future directions in decoupled water splitting.Thus,the flexibility in the design of mediators provides huge space for improving this electrochemical technology.@2024 Science Press and Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by ELSEVIER B.V.and Science Press.All rights reserved.
文摘Decoupled Catalytic Hydrogen Evolution from a Molecular Metal Oxide Redox Mediator in Water Splitting B.Rausch,M.D.Symes,G.Chisholm,L.Cronin Science345（2014）6202.以杂多酸H4[SiW12O40]的还原加氢代替水分解中的氢析出反应,然后将还原产物H6[SiW12O40]在隔离的空间与Pt催化剂接触释放出H2.Synergistic Geometric and Electronic Effects for Electrochemical Reduction of Carbon Dioxide Using Gold-Copper Bimetallic Nanoparticles。
文摘人机交互语言工具是电信网管的重要组成部分,是网管系统中使用频率最高的模块之一,命令参数的显示控制是它的实现难点.基于Mediator模式的参数控制法分离了参数表示和逻辑控制,它让每个参数专心处理自身表示,由中介者控制显示逻辑,解除了参数间的耦合关系.这种实现方法,集中了对参数的控制,减少了耦合,有利于各参数的复用,易于逻辑关系扩展,提高了命令解析效率.实际测试表明,在PIII 1.0 G CPU环境下,解析一条命令的平均时间只需0.14 s.该方法为开发网管人机交互语言工具或处理对象强耦合问题提供了一种有参考价值的实现方法.
文摘Most non-native speakers do have difficulty in developing native-like oracy due to vast differences in pronunciation between L1 and L2, adult ESL learners in particular. As Peter and Susan pointed in Teaching American English Pronunciation(1992), there are specific problem syllables with different language groups. As an ESL teacher from China, I assume it necessary to find out whether these sounds really trouble Chinese students in the ESL class I observed. I am going to pick out the most frequently occurred problem sounds and take notes how the teacher deal with them in class. In this paper, based on classroom observation and interviews, I analyzed problematic English vowels and consonants from Chinese learners, and the corresponding mediations for ESL teacher.
文摘BACKGROUND： Sepsis and secondary multiple organ failure in critically ill patients are the major cause of death, but the pathogenesis of sepsis is not clear, especially the dysfunction of the immune system. In this paper, we review the response and regulation of the immune system and the functions of a variety of inflammatory mediators in sepsis. DATA SOURCES Studies were identified by searching MEDLINE and PubMed for articles using the keywords ＂sepsis＂, ＂immune response＂, and ＂inflammatory mediator＂ up to October 2010. Additional papers were identified by a manual search of the references from the key articles.RESULTS： This systematic review was conducted of： 1） the immune response; 2） immune regulation; 3） inflammatory mediators; 4） high-mobility group box 1 protein; 5） the complement system; and 6） the autonomic nervous system. There are no therapeutic approaches available for sepsis that target inflammatory response; the mortality of sepsis has not been significantly reduced. Sepsis is complex and dynamic, and it has a group of heterogeneous syndromes.CONCLUSIONS： Since different patients with sepsis have different etiology, susceptibility, and responses, treatment should be prescribed individually.
基金the Sichuan Provincial Science and Technology Department (2017JY0324)Joint Project of Southwest Medical University and Sichuan Luzhou (2017LZXNYD-Z02)+3 种基金Natural Science Foundation of China (81701322)Humanity and Social Science Youth Foundation of Ministry of Education of China (17YJC190001,17YJC190009)the joint project of Southwest Medical University & Affiliated Hospital of Southwest Medical University (2015-QB-003)Sichuan Applied Psychology Research Center Project (CSXL-172012).
文摘Background Good interpersonal relationships can improve the negative mood and, to a certain extent, may help relieve dysmenorrhea symptoms. However, there has been no study examining the role of interpersonal relationships in dysmenorrhea and how they may interact with negative emotions. Aims To investigate the connection between negative affect and dysmenorrhea, and the role of interpersonal relationships plays in this relationship. Methods The Cox Menstrual Symptom Scale (CMSS), short-form of Depression Anxiety Stress Scale, Interpersonal Comprehensive Diagnostic Scale and UCLA (University of California at Los Angeles) Loneliness Scale were applied to 855 adolescent nursing students to collect information on severity and frequency of dysmenorrheal symptoms, negative emotions (including depression, anxiety and stress), interpersonal problems and subjective experience of loneliness among them, and the relationship among these variables was examined. Results (1) Both the severity and frequency of dysmenorrhea were positively correlated with negative emotions, loneliness experience and interpersonal problems, while negatively correlated with age at menarche.(2) The negative emotions, romantic relationship and menarche age, but not loneliness and interpersonal problems, significantly contributed to both the severity and frequency of dysmenorrhea.(3) Mediation analysis revealed that the effects of loneliness and interpersonal problems on dysmenorrhea were totally mediated by negative emotions. Conclusions This investigation indicates that the relationship between interpersonal relationships and dysmenorrhea is mediated by negative emotions.
文摘Sepsis is an infection induced systemic inflammatory response syndrome and is a major cause of morbidity as well as mortality in intensive care units. A growing body of evidence suggests that the activation of a proinflammatory cascade is responsible for the development of immune dysfunction, susceptibility to severe sepsis and septic shock. The present theories of sepsis as a dysregulated inflammatory response and immune function, as manifested by excessive release of inflammatory mediators such as high mobility group box 1 protein （HMGB1）, are supported by increasing studies employing animal models and clinical observations of sepsis. HMGB1, originally described as a DNA-binding protein and released passively by necrotic cells and actively by macrophages/monocytes, has been discovered to be one of essential cytokines that mediates the response to infection, injury and inflammation. A growing number of studies still focus on the inflammation-regulatory function and its contribution to infectious and inflammatory disorders, recent data suggest that HMGB1 formation can also markedly influence the host cell-mediated immunity, including T lymphocytes and macrophages. Here we review emerging evidence that support extracellular HMGB1 as a late mediator of septic complications, and discuss the therapeutic potential of several HMGBl-targeting agents in experimental sepsis. In addition, with the development of traditional Chinese medicine in recent years, it has been proven that traditional Chinese herbal materials and their extracts have remarkable effective in treating severe sepsis. In this review, we therefore provide some new concepts of HMGBl-targeted Chinese herbal therapies in sepsis.
基金the financial support provided by the National University of Singapore。
文摘While the sulfur conversion reaction kinetics in Li–S batteries is nowadays improved by the use of appropriate electrocatalysts,it remains a challenge for the batteries to perform well under the lean electrolyte condition where polysulfide shuttle,electrode passivation and the loss of electrolyte due to side reactions,are aggravated.These challenges are addressed in this study by the tandem use of a polysulfide conversion catalyst and a redox–targeting mediator in a gel sulfur cathode.Specifically,the gel cathode reduces the polysulfide mobility and hence the polysulfide shuttle and the passivation of the lithium anode by the crossover polysulfides.The redox mediator restrains the deposition of inactive sulfur species in the cathode thereby enabling the Fe–N and Co–N co–doped carbon catalyst to prolong its catalytic activity.Consequently,the integrated catalytic system is able to increase the discharge capacity of high–loading (6.8 mg cm^(-2)) lean–electrolyte (4.0μL mg^(-1)) Li–S batteries from~630 to~1316 m Ah g^(-1),concurrently with an improvement of the cycle life (600 cycles with 46%capacity retention at 1.0 m A cm^(-2)).Redox mediator assisted catalysis in a gel cathode is therefore an effective strategy to extend the application of the sulfur conversion catalyst in lean electrolyte Li–S batteries.
文摘Autoimmune disease management presents a significant challenge to medical science. Environmental factors potentially increase the risk of developing inflammatory and autoimmune diseases, such as multiple sclerosis, rheumatoid arthritis, and lupus. Among various environmental stresses, cigarette smoke and hypoxia have both been reported to lead to an enhanced risk of inflammatory and autoimmune diseases. In this review, we shed light on all reported mechanisms whereby cigarette smoke and a hypoxic environment can induce inflammatory and autoimmune diseases and discuss how hypoxic conditions influence the cigarette smoke-induced threat of inflammatory and autoimmune disease development. Cigarette smoke and hypoxia both lead to increased oxidative stress and production of reactive oxygen species and other free radicals, which have various effects including the generation of autoreactive pro-inflammatory T cells and autoantibodies, reductions in T regulatory(Treg) cell activity, and enhanced expression of pro-inflammatory mediators [e.g., interleukin-6(IL-6), interleukin-4(IL-4) and interleukin-8(IL-8)]. Accordingly, smoking and hypoxic environments may synergistically act as potent environmental risk factors for inflammatory and autoimmune diseases. To our knowledge, no studies have reported the direct association of cigarette smoke and hypoxic environments with the risk of developing inflammatory and autoimmune diseases. Future studies exploring the risk of autoimmune disease development in smokers at high altitudes, particularly military personnel and mountaineers who are not acclimatized to high-altitude regions, are required to obtain a better understanding of disease risk as well as its management.
基金special fund for public welfare industry of health grant(200802150)(JSYRKJ2010-C1-001Jiangsu Provincial Medical Humanities and Social Science committee(No:JSYRKJ2010-C1-001)+1 种基金Philosophy and Social Science Special Project in Nanjing Medical University(No:2013NJZS40)Key Project supported by Medical Science and Technology Development Foundation Nanjing Department of Healt(No.YKK17246,YKK16241)
文摘Background Burn-out among doctors threatens their own health, and that of their patients. To identify risk factors of the doctor burn-out is vital to improving their health and increasing the quality of healthcare services. This study aims to explore the relationship between work-family confict （WFC） and burn-out among Chinese doctors and the mediating role of coping styles in this relationship.Methods A cross-sectional survey was conducted in China, with a questionnaire packet which consisted of the Chinese Maslach Burnout Inventory （CMBI）, WFC Scale and the Simplifed Coping Style Questionnaire （SCSQ）. A total of 2530 doctors participated in the survey. Correlation analysis was performed to explore the relationship between CMBI, WFC and SCSQ scores. A linear regression model was set to determine the mediating role of coping styles on the relationship between WFC and burn-out.Results Doctors who had higher scores on work interfering with family confict, reported more emotional exhaustion （r=0.514, P〈0.001） and had a sense of accomplishment （r= 0.149, P〈0.001）. Simultaneously, family interfering with work （FIW） was positively associated with all dimensions of burn-out （r=0.213, 0.504, 0.088, respectively, P〈0.001）. Coping styles had partial, complete and even mediating effects on the relationship between WFC and burn-out among Chinese doctors.Conclusions WFC was correlated with burn-out, and coping style was a mediator in this relationship among Chinese doctors. Coping style was a positive resource against burn-out.
基金This work was supported by Guangdong Basic and Applied Basic Research Foundation,China(No.2019A1515110980)research project from the National Natural Science Foundation of China(No.21361162004)China Scholarship Council,and CSIRO.We acknowledge Dr Yesim Gozukara,Dr Malisja de Vries,and Dr Yunxia Yang from CSIRO(Clayton)for their help with material characterization training.
文摘As promising anodes for sodium-ion batteries,metal sulfides ubiquitously suffer from low-rate and high-plateau issues,greatly hindering their application in full-cells.Herein,exemplifying carbon nanotubes(CNTs)-stringed metal sulfides superstructure(CSC)assembled by nano-dispersed SnS_(2) and CoS_(2) phases,cocktail mediation effect similar to that of high-entropy materials is initially studied in ether-based electrolyte to solve the challenges.The high nano-dispersity of metal sulfides in CSC anode underlies the cocktail-like mediation effect,enabling the circumvention of intrinsic drawbacks of different metal sulfides.By utilizing ether-based electrolyte,the reversibility of metal sulfides is greatly improved,sustaining a long-life effectivity of cocktail-like mediation.As such,CSC effectively overcomes low-rate flaw of SnS_(2) and highplateau demerit of CoS_(2),simultaneously realizes a high rate and a low plateau.In half-cells,CSC delivers an ultrahigh-rate capability of 327.6 mAh g^(−1) anode at 20 A g^(−1),far outperforming those of monometallic sulfides(SnS_(2),CoS_(2))and their mixtures.Compared with CoS_(2) phase and SnS_(2)/CoS_(2) mixture,CSC shows remarkably lowered average charge voltage up to ca.0.62 V.As-assembled CSC//Na1.5VPO4.8F0.7 full-cell shows a good rate capability(0.05~1.0 A g^(−1),120.3 mAh g^(−1) electrode at 0.05 A g^(−1))and a high average discharge voltage up to 2.57 V,comparable to full-cells with alloy-type anodes.Kinetics analysis verifies that the cocktail-like mediation effect largely boosts the charge transfer and ionic diffusion in CSC,compared with single phase and mixed phases.Further mechanism study reveals that alternative and complementary electrochemical processes between nano-dispersed SnS_(2) and CoS_(2) phases are responsible for the lowered charge voltage of CSC.This electrolyte/structure-dependent cocktail-like mediation effect effectively enhances the practicability of metal sulfide anodes,which will boost the development of high-rate/-voltage sodium-ion full batteries.
基金financially supported by the Tsinghua-Foshan Innovation Special Fund(Grant No.2018THFS0409)the China Postdoctoral Science Foundation(Grant No.2019M650668)the National Key Research and Development Program of China(Grant No.2016YFA0201003)。
文摘Rechargeable lithium-oxygen(Li-O_(2))batteries are the next generation energy storage devices due to their ultrahigh theoretical capacity.Redox mediators(RMs)are widely used as a homogenous electrocatalyst in non-aqueous Li-O_(2)batteries to enhance their discharge capacity and reduce charge overpotential.However,the shuttle effect of RMs in the electrolyte solution usually leads to corrosion of the Li metal anode and uneven Li deposition on the anode surface,resulting in unwanted consumption of electrocatalysts and deterioration of the cells.It is therefore necessary to take some measures to prevent the shuttle effect of RMs and fully utilize the soluble electrocatalysts.Herein,we summarize the strategies to suppress the RM shuttle effect reported in recent years,including electrolyte additives,protective separators and electrode modification.The mechanisms of these strategies are analyzed and their corresponding requirements are discussed.The electrochemical properties of Li-O_(2)batteries with different strategies are summarized and compared.The challenges and perspectives on preventing the shuttle effect of RMs are described for future study.This review provides guidance for achieving shuttle-free redox mediation and for designing Li-O_(2)cells with a long cycle life,high energy efficiency and highly reversible electrochemical reactions.
基金financially supported by the National Natural Science Foundation of China(51702225)the National Key Research and Development Program(2019YFA0708201)+3 种基金the Beijing Municipal Science and Technology Commission(Z161100002116020)the China Postdoctoral Science Foundation funded project(2020 M681704,2021 T140493)the support from Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies,Suzhou,Chinathe support from the Postdoctoral Research Foundation of Jiangsu Province。
文摘The practical applications of lithium-sulfur(Li-S)battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode.One of the effective solutions deals with concurrent management of both electrodes.Nevertheless,this direction remains in a nascent stage due to a lack of material selection and mechanism exploration.Herein,we devise a temperature-mediated direct chemical vapor deposition strategy to realize the controllable synthesis of three-dimensional boron/nitrogen dual-doped graphene(BNG)particulated architectures,which is employed as a light-weighted and multi-functional mediator for both electrodes in Li-S batteries.Benefiting from the“sulfiphilic”and“lithiophilic”features,the BNG modified separator not only enables boosted kinetics of polysulfide transformation to mitigate the shuttle effect but also endows uniform lithium deposition to suppress the dendritic growth.Theoretical calculations in combination with electro-kinetic tests and operando Raman analysis further elucidate the favorable sulfur and lithium electrochemistry of BNG at a molecular level.This work offers direct insight into the mediator design via controllable synthesis of graphene materials to tackle the fundamental challenges of Li-S batteries.
文摘The ever-increasing demand for energy has stimulated the development of economical non-fossil fuels.As representative of clean energy,solar and wind have been identified as the most promising energy sources due to their abundance,cost efficiency,and environmental friendliness.The intrinsic intermittent of the clean energy leads to the urgent requirements large-scale energy storage technique.Redox flow batteries(RFBs)are attractive technology due to their independent control over energy and power.Insoluble redox-active flow battery is a new type of electrochemical energy storage technology that disperses redox-active particles in the electrolyte.Compared with traditional flow batteries,insoluble flow batteries have advantages of large energy density and are very promising in the development of large-scale energy storage systems.At present,three types of insoluble flow batteries have been explored:slurry-based flow batteries,metal/slurry hybrid,and redox-mediator-assisted flow batteries.This Review summarizes the research progress of insoluble flow batteries,and analyzes the key challenges from the fundamental research and practical application perspectives.
基金the Basic Science Research Program of the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(NRF-2019R1A2C1003594 and NRF-2019R1A2C1003551)the Ministry of Education(NRF-2016R1D1A1B03930806).
文摘Lithium-sulfur(Li-S)batteries are promising energy storage devices owing to their high energy density and the low cost of sulfur.However,they are still far from being applied commercially because of the detrimental capacity fade caused by the dissolution of lithium polysulfide(LPS)in liquid electrolyte.In this study,we introduced a new polymer binder having a redox-mediating function that assists in the reduction of soluble LPS to Li2S at the cathode to suppress the shuttle effect as well as enhance sulfur utilization.An amine group containing benzo(ghi)perylene imide(BPI)was synthesized and grafted onto poly(acrylic acid)to produce a redox-mediating polymer binder.An Li-S cell fabricated using the new redox-mediating polymer binder demonstrated a capacity decay retention of 0.036%per cycle up to 500 cycles at 0.5 C with a coulombic efficiency of 98%.
