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Reaction视频中用户弹幕信息交互行为的情感反应生成机理研究
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作者 叶许婕 赵宇翔 +2 位作者 张妍 李金昊 Preben Hansen 《信息资源管理学报》 2024年第2期104-120,共17页
深入挖掘Reaction视频中弹幕信息交互行为的情感反应机理有助于理解用户弹幕创作背后的情感生成原因及情感变化过程。本文基于情感反应模型,利用定向内容分析法对哔哩哔哩网站中11个热门视频的弹幕信息资源、视频内容以及reactor反应情... 深入挖掘Reaction视频中弹幕信息交互行为的情感反应机理有助于理解用户弹幕创作背后的情感生成原因及情感变化过程。本文基于情感反应模型,利用定向内容分析法对哔哩哔哩网站中11个热门视频的弹幕信息资源、视频内容以及reactor反应情况展开编码研究,构建了Reaction视频中用户弹幕信息交互行为的情感反应生成机理模型。研究发现,Reaction视频弹幕信息交互行为中的情感反应生成机理总体上遵循“信息刺激-情感反应”的路径,信息刺激有时会独立唤醒情绪或特定情感态度,有时也会通过唤醒特定情感态度进而影响情绪或内化情感态度的生成。该模型有助于提升情感反应理论在计算机协助交流中的情境化探索,也将为社交媒体中用户与信息交互提供优化建议。 展开更多
关键词 reaction视频 弹幕 用户信息交互 情感反应模型 定向内容分析
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Tuning electronic structure of RuO_(2)by single atom Zn and oxygen vacancies to boost oxygen evolution reaction in acidic medium 被引量:1
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作者 Qing Qin Tiantian Wang +7 位作者 Zijian Li Guolin Zhang Haeseong Jang Liqiang Hou Yu Wang Min Gyu Kim Shangguo Liu Xien Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期94-102,I0003,共10页
The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct ... The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER. 展开更多
关键词 ELECTROCATALYST Acidic oxygen evolution reaction Electronic structure engineering DURABILITY reaction barrier
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Exciting lattice oxygen of nickel–iron bi-metal alkoxide for efficient electrochemical oxygen evolution reaction 被引量:1
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作者 Saihang Zhang Senchuan Huang +8 位作者 Fengzhan Sun Yinghui Li Li Ren Hao Xu Zhao Li Yifei Liu Wei Li Lina Chong Jianxin Zou 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期194-201,I0005,共9页
High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion te... High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts. 展开更多
关键词 Oxygen evolution reaction Nickel-iron bi-metal alkoxide Lattice oxygen-mediated reaction mechanism Alkaline electrolysis ELECTROCATALYSTS
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Deformable Catalytic Material Derived from Mechanical Flexibility for Hydrogen Evolution Reaction 被引量:2
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作者 Fengshun Wang Lingbin Xie +7 位作者 Ning Sun Ting Zhi Mengyang Zhang Yang Liu Zhongzhong Luo Lanhua Yi Qiang Zhao Longlu Wang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第2期287-311,共25页
Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent year... Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst. 展开更多
关键词 Deformable catalytic material Micro-nanostructures evolution Mechanical flexibility Hydrogen evolution reaction
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Precisely Control Relationship between Sulfur Vacancy and H Absorption for Boosting Hydrogen Evolution Reaction 被引量:1
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作者 Jing Jin Xinyao Wang +4 位作者 Yang Hu Zhuang Zhang Hongbo Liu Jie Yin Pinxian Xi 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第4期14-24,共11页
Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performan... Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy. 展开更多
关键词 Hydrogen evolution reaction S vacancies NANOSHEET H Adsorption
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Particle agglomeration and inhibition method in the fluidized pyrolysis reaction of waste resin 被引量:1
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作者 Congjing Ren Peng Zhang +3 位作者 Qi Song Zhengliang Huang Yao Yang Yongrong Yang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第3期135-147,共13页
This work investigated the pyrolysis reaction of waste resin in a fluidized bed reactor.It was found that the pyrolysis-generated ash would adhere to the surface of ceramic particles,causing particle agglomeration and... This work investigated the pyrolysis reaction of waste resin in a fluidized bed reactor.It was found that the pyrolysis-generated ash would adhere to the surface of ceramic particles,causing particle agglomeration and defluidization.Adding kaolin could effectively inhibit the particle agglomeration during the fluidized pyrolysis reaction through physical isolation and chemical reaction.On the one hand,kaolin could form a coating layer on the surface of ceramic particles to prevent the adhesion of organic ash generated by the pyrolysis of resin.On the other hand,when a sufficient amount of kaolin(-0.2%(mass))was added,the activated kaolin could fully contact with the Na+ ions generated by the pyrolysis of resin and react to form a high-melting aluminosilicate mineral(nepheline),which could reduce the formation of low-melting-point sodium sulfate and thereby avoid the agglomeration of ceramic particles. 展开更多
关键词 Pyrolysis reaction of waste resin FLUIDIZATION Particle agglomeration KAOLIN
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“Buckets effect”in the kinetics of electrocatalytic reactions 被引量:1
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作者 Haowen Cui Yan-Xia Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第2期388-396,I0010,共10页
In this study,we systematically investigated the effect of proton concentration on the kinetics of the oxygen reduction reaction(ORR)on Pt(111)in acidic solutions.Experimental results demonstrate a rectangular hyperbo... In this study,we systematically investigated the effect of proton concentration on the kinetics of the oxygen reduction reaction(ORR)on Pt(111)in acidic solutions.Experimental results demonstrate a rectangular hyperbolic relationship,i.e.,the ORR current excluding the effect of other variables increases with proton concentration and then tends to a constant value.We consider that this is caused by the limitation of ORR kinetics by the trace oxygen concentration in the solution,which determines the upper limit of ORR kinetics.A model of effective concentration is further proposed for rectangular hyperbolic relationships:when the reactant concentration is high enough to reach a critical saturation concentration,the effective reactant concentration will become a constant value.This could be due to the limited concentration of a certain reactant for reactions involving more than one reactant or the limited number of active sites available on the catalyst.Our study provides new insights into the kinetics of electrocatalytic reactions,and it is important for the proper evaluation of catalyst activity and the study of structureperformance relationships. 展开更多
关键词 Oxygen reduction reaction KINETICS Zero order Rectangular hyperbolic relationship pH effect
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Possibilities for the synthesis of superheavy element Z=121 in fusion reactions 被引量:1
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作者 Ming-Hao Zhang Yu-Hai Zhang +3 位作者 Ying Zou Xiu-Xiu Yang Gen Zhang Feng-Shou Zhang 《Nuclear Science and Techniques》 SCIE EI CAS CSCD 2024年第6期90-100,共11页
Based on the dinuclear system model,the calculated evaporation residue cross sections matched well with the current experimental results.The synthesis of superheavy elements Z=121 was systematically studied through co... Based on the dinuclear system model,the calculated evaporation residue cross sections matched well with the current experimental results.The synthesis of superheavy elements Z=121 was systematically studied through combinations of stable projectiles with Z=21-30 and targets with half-lives exceeding 50 d.The influence of mass asymmetry and isotopic dependence on the projectile and target nuclei was investigated in detail.The reactions^(254)Es(^(46)Ti,3n)^(297)121 and^(252)Es(^(46)Ti,3n)^(295)121 were found to be experimentally feasible for synthesizing superheavy element Z=121,with maximal evaporation residue cross sections of 6.619 and 4.123 fb at 219.9 and 223.9 MeV,respectively. 展开更多
关键词 Superheavy nuclei Dinuclear system model Fusion reaction Evaporation residue cross section
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Effects of Maillard reaction and its product AGEs on aging and age-related diseases 被引量:1
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作者 Huan Peng Yuqi Gao +4 位作者 Chenye Zeng Rui Hua Yannan Guo Yida Wang Zhao Wang 《Food Science and Human Wellness》 SCIE CSCD 2024年第3期1118-1134,共17页
Maillard reaction(MR)is a non-enzymatic browning reaction commonly seen in food processing,which occurs between reducing sugars and compounds with amino groups.Despite certain advantages based on Maillard reaction pro... Maillard reaction(MR)is a non-enzymatic browning reaction commonly seen in food processing,which occurs between reducing sugars and compounds with amino groups.Despite certain advantages based on Maillard reaction products(MRPs)found in some food for health and storage application have appeared,however,the MR occurring in human physiological environment can produce advanced glycation end products(AGEs)by non-enzymatic modification of macromolecules such as proteins,lipids and nucleic acid,which could change the structure and functional activity of the molecules themselves.In this review,we take AGEs as our main object,on the one hand,discuss physiologic aging,that is,age-dependent covalent cross-linking and modification of proteins such as collagen that occur in eyes and skin containing connective tissue.On the other hand,pathological aging associated with autoimmune and inflammatory diseases,neurodegenerative diseases,diabetes and diabetic nephropathy,cardiovascular diseases and bone degenerative diseases have been mainly proposed.Based on the series of adverse effects of accelerated aging and disease pathologies caused by MRPs,the possible harm caused by some MR can be slowed down or inhibited by artificial drug intervention,dietary pattern and lifestyle control.It also stimulates people's curiosity to continue to explore the potential link between the MR and human aging and health,which should be paid more attention to for the development of life sciences. 展开更多
关键词 Maillard reaction Advanced glycation end products Physiologic aging Pathological aging Drug intervention
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Metal-organic-framework-derived copper-based catalyst for multicomponent C-S coupling reaction
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作者 Lixin Chen Hui Zhang +1 位作者 Linxi Hou Xin Ge 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第6期1-8,共8页
Copper-based metal-organic frameworks(Cu-MOFs)are a promising multiphase catalyst for catalyzing C-S coupling reactions by virtue of their diverse structures and functions.However,the unpleasant odor and instability o... Copper-based metal-organic frameworks(Cu-MOFs)are a promising multiphase catalyst for catalyzing C-S coupling reactions by virtue of their diverse structures and functions.However,the unpleasant odor and instability of the organosulfur,as well as the mass-transfer resistance that exists in multiphase catalysis,have often limited the catalytic application of Cu-MOFs in C-S coupling reactions.In this paper,a Cu-MOFs catalyst modified by cetyltrimethylammonium bromide(CTAB)was designed to enhance mass transfer by increasing the adsorption of organic substrates using the long alkanes of CTAB.Concurrently,elemental sulfur was used to replace organosulfur to achieve a highly efficient and atom-economical multicomponent C-S coupling reaction. 展开更多
关键词 Design Copper-based metal-organic frameworks (Cu-MOFs) Adsorption C-S coupling reaction Multiphase reaction
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The reaction mechanism and interfacial crystallization of Al nanoparticle-embedded Ni under shock loading
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作者 Yifan Xie Jian-Li Shao +1 位作者 Rui Liu Pengwan Chen 《Defence Technology(防务技术)》 SCIE EI CAS CSCD 2024年第3期114-124,共11页
The shock-induced reaction mechanism and characteristics of Ni/Al system,considering an Al nanoparticle-embedded Ni single crystal,are investigated through molecular dynamics simulation.For the shock melting of Al nan... The shock-induced reaction mechanism and characteristics of Ni/Al system,considering an Al nanoparticle-embedded Ni single crystal,are investigated through molecular dynamics simulation.For the shock melting of Al nanoparticle,interfacial crystallization and dissolution are the main characteristics.The reaction degree of Al particle first increases linearly and then logarithmically with time driven by rapid mechanical mixing and following dissolution.The reaction rate increases with the decrease of particle diameter,however,the reaction is seriously hindered by interfacial crystallization when the diameter is lower than 9 nm in our simulations.Meanwhile,we found a negative exponential growth in the fraction of crystallized Al atoms,and the crystallinity of B2-NiAl(up to 20%)is positively correlated with the specific surface area of Al particle.This can be attributed to the formation mechanism of B2-NiAl by structural evolution of finite mixing layer near the collapsed interface.For shock melting of both Al particle and Ni matrix,the liquid-liquid phase inter-diffusion is the main reaction mechanism that can be enhanced by the formation of internal jet.In addition,the enhanced diffusion is manifested in the logarithmic growth law of mean square displacement,which results in an almost constant reaction rate similar to the mechanical mixing process. 展开更多
关键词 Shock-induced reaction Molecular dynamics simulations Interfacial crystallization reaction mechanism
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Influence of initial check, information exchange, final accuracy check, reaction information nursing on the psychology of elderly with lung cancer 被引量:1
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作者 Cui Jiang Jing Ma +1 位作者 Wen He Hai-Ying Zhang 《World Journal of Clinical Cases》 SCIE 2024年第4期737-745,共9页
BACKGROUND As one of the fatal diseases with high incidence,lung cancer has seriously endangered public health and safety.Elderly patients usually have poor self-care and are more likely to show a series of psychologi... BACKGROUND As one of the fatal diseases with high incidence,lung cancer has seriously endangered public health and safety.Elderly patients usually have poor self-care and are more likely to show a series of psychological problems.AIM To investigate the effectiveness of the initial check,information exchange,final accuracy check,reaction(IIFAR)information care model on the mental health status of elderly patients with lung cancer.METHODS This study is a single-centre study.We randomly recruited 60 elderly patients with lung cancer who attended our hospital from January 2021 to January 2022.These elderly patients with lung cancer were randomly divided into two groups,with the control group taking the conventional propaganda and education and the observation group taking the IIFAR information care model based on the conventional care protocol.The differences in psychological distress,anxiety and depression,life quality,fatigue,and the locus of control in psychology were compared between these two groups,and the causes of psychological distress were analyzed.RESULTS After the intervention,Distress Thermometer,Hospital Anxiety and Depression Scale(HADS)for anxiety and the HADS for depression,Revised Piper’s Fatigue Scale,and Chance Health Locus of Control scores were lower in the observation group compared to the pre-intervention period in the same group and were significantly lower in the observation group compared to those of the control group(P<0.05).After the intervention,Quality of Life Questionnaire Core 30(QLQ-C30),Internal Health Locus of Control,and Powerful Others Health Locus of Control scores were significantly higher in the observation and the control groups compared to the pre-intervention period in their same group,and QLQ-C30 scores were significantly higher in the observation group compared to those of the control group(P<0.05).CONCLUSION The IIFAR information care model can help elderly patients with lung cancer by reducing their anxiety and depression,psychological distress,and fatigue,improving their tendencies on the locus of control in psychology,and enhancing their life qualities. 展开更多
关键词 Initial check information exchange final accuracy check reaction information care model Lung cancer Mental health
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Solvent effects on Diels-Alder reaction in ionic liquids:A reaction density functional study
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作者 Zijiang Dou Weiqiang Tang +1 位作者 Peng Xie Shuangliang Zhao 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第2期180-188,共9页
Extensive experimental studies have been performed on the Diels-Alder(DA)reactions in ionic liquids(ILs),which demonstrate that the IL environment can significantly influence the reaction rates and selectivity.However... Extensive experimental studies have been performed on the Diels-Alder(DA)reactions in ionic liquids(ILs),which demonstrate that the IL environment can significantly influence the reaction rates and selectivity.However,the underlying microscopic mechanism remains ambiguous.In this work,the multiscale reaction density functional theory is applied to explore the effect of 1-butyl-3-methylimidazolium hexafluorophosphate([BMIM][PF_(6)])solvent on the reaction of cyclopentadiene(CP)with acrolein,methyl acrylate,or acrylonitrile.By analyzing the free energy landscape during the reaction,it is found that the polarization effect has a relatively small influence,while the solvation effect makes both the activation free energy and reaction free energy decrease.In addition,the rearrangement of local solvent structure shows that the cation spatial distribution responds more evidently to the reaction than the anion,and this indicates that the cation plays a dominant role in the solvation effect and so as to affect the reaction rates and selectivity of the DA reactions. 展开更多
关键词 Solvent effect Ionic liquids Diels-Alder reaction reaction density functional theory
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Approaching Ultimate Synthesis Reaction Rate of Ni-Rich Layered Cathodes for Lithium-Ion Batteries
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作者 Zhedong Liu Jingchao Zhang +9 位作者 Jiawei Luo Zhaoxin Guo Haoran Jiang Zekun Li Yuhang Liu Zijing Song Rui Liu Wei-Di Liu Wenbin Hu Yanan Chen 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第10期392-402,共11页
Nickel-rich layered oxide LiNi_(x)Co_(y)MnzO_(2)(NCM,x+y+z=1)is the most promising cathode material for high-energy lithium-ion batteries.However,conventional synthesis methods are limited by the slow heating rate,slu... Nickel-rich layered oxide LiNi_(x)Co_(y)MnzO_(2)(NCM,x+y+z=1)is the most promising cathode material for high-energy lithium-ion batteries.However,conventional synthesis methods are limited by the slow heating rate,sluggish reaction dynamics,high energy consumption,and long reaction time.To overcome these chal-lenges,we first employed a high-temperature shock(HTS)strategy for fast synthesis of the NCM,and the approaching ultimate reaction rate of solid phase transition is deeply investigated for the first time.In the HTS process,ultrafast average reaction rate of phase transition from Ni_(0.6)Co_(0.2)Mn_(0.2)(OH)_(2) to Li-containing oxides is 66.7(%s^(-1)),that is,taking only 1.5 s.An ultrahigh heating rate leads to fast reaction kinetics,which induces the rapid phase transition of NCM cathodes.The HTS-synthesized nickel-rich layered oxides perform good cycling performances(94%for NCM523,94%for NCM622,and 80%for NCM811 after 200 cycles at 4.3 V).These findings might also assist to pave the way for preparing effectively Ni-rich layered oxides for lithium-ion batteries. 展开更多
关键词 Nickel-rich layered oxides High-temperature shock Solid reaction kinetics Phase transition reaction rate
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In situ infrared, Raman and X-ray spectroscopy for the mechanistic understanding of hydrogen evolution reaction
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作者 Andi Haryanto Kyounghoon Jung +1 位作者 Chan Woo Lee Dong-Wan Kim 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第3期632-651,I0014,共21页
Hydrogen production by water reduction reactions has received considerable attention because hydrogen is considered a clean-energy carrier,key for a sustainable energy future.Computational methods have been widely use... Hydrogen production by water reduction reactions has received considerable attention because hydrogen is considered a clean-energy carrier,key for a sustainable energy future.Computational methods have been widely used to study the reaction mechanism of the hydrogen evolution reaction(HER),but the calculation results need to be supported by experimental results and direct evidence to confirm the mechanistic insights.In this review,we discuss the fundamental principles of the in situ spectroscopic strategy and a theoretical model for a mechanistic understanding of the HER.In addition,we investigate recent studies by in situ Fourier transform infrared(FTIR),Raman spectroscopy,and X-ray absorption spectroscopy(XAS) and cover new findings that occur at the catalyst-electrolyte interface during HER.These spectroscopic strategies provide practical ways to elucidate catalyst phase,reaction intermediate,catalyst-electrolyte interface,intermediate binding energy,metal valency state,and coordination environment during HER. 展开更多
关键词 Hydrogen evolution reaction Infrared spectroscopy Raman spectroscopy X-ray absorption spectroscopy reaction mechanism
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Oxidation Evolution and Activity Origin of N-Doped Carbon in the Oxygen Reduction Reaction
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作者 Jiaqi Wu Chuanqi Cheng +2 位作者 Shanshan Lu Bin Zhang Yanmei Shi 《Transactions of Tianjin University》 EI CAS 2024年第4期369-379,共11页
N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher ... N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production. 展开更多
关键词 Oxygen reduction reaction N-doped carbon reaction path Structural evolution Oxidation in reduction
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Sulfur doped iron-nitrogen-hard carbon nanosheets as efficient and robust noble metal-free catalysts for oxygen reduction reaction in PEMFC
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作者 Bin Liu Jiawang Li +6 位作者 Bowen Yan Qi Wei Xingyu Wen Huarui Xie Huan He Pei Kang Shen Zhi Qun Tian 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第2期422-433,I0010,共13页
Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membr... Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).To tackle the issue,herein,a new type of sulfur-doped ironnitrogen-hard carbon(S-Fe-N-HC)nanosheets with high activity and durability in acid media were developed by using a newly synthesized precursor of amide-based polymer with Fe ions based on copolymerizing two monomers of 2,5-thiophene dicarboxylic acid(TDA)as S source and 1,8-diaminonaphthalene(DAN)as N source via an amination reaction.The as-synthesized S-Fe-N-HC features highly dispersed atomic Fe Nxmoieties embedded into rich thiophene-S doped hard carbon nanosheets filled with highly twisted graphite-like microcrystals,which is distinguished from the majority of M-N-C with soft or graphitic carbon structures.These unique characteristics endow S-Fe-N-HC with high ORR activity and outstanding durability in 0.5 M H_(2)SO_(4).Its initial half-wave potential is 0.80 V and the corresponding loss is only 21 m V after 30,000 cycles.Meanwhile,its practical PEMFC performance is a maximum power output of 628.0 mW cm^(-2)and a slight power density loss is 83.0 m W cm^(-2)after 200-cycle practical operation.Additionally,theoretical calculation shows that the activity of Fe Nxmoieties on ORR can be further enhanced by sulfur doping at meta-site near FeN_(4)C.These results evidently demonstrate that the dual effect of hard carbon substrate and S doping derived from the precursor platform of amid-polymers can effectively enhance the activity and durability of Fe-N-C catalysts,providing a new guidance for developing advanced M-N-C catalysts for ORR. 展开更多
关键词 Transition metal-nitrogen-carbon Oxygen reduction reaction Hard carbon Amide based polymer reaction Proton exchange membrane cells
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Towards a new avenue for rapid synthesis of electrocatalytic electrodes via laser-induced hydrothermal reaction for water splitting
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作者 Yang Sha Menghui Zhu +6 位作者 Kun Huang Yang Zhang Francis Moissinac Zhizhou Zhang Dongxu Cheng Paul Mativenga Zhu Liu 《International Journal of Extreme Manufacturing》 SCIE EI CAS CSCD 2024年第1期340-351,共12页
Electrochemical production of hydrogen from water requires the development ofelectrocatalysts that are active,stable,and low-cost for water splitting.To address these challenges,researchers are increasingly exploring ... Electrochemical production of hydrogen from water requires the development ofelectrocatalysts that are active,stable,and low-cost for water splitting.To address these challenges,researchers are increasingly exploring binder-free electrocatalytic integratedelectrodes (IEs) as an alternative to conventional powder-based electrode preparation methods,for the former is highly desirable to improve the catalytic activity and long-term stability for large-scale applications of electrocatalysts.Herein,we demonstrate a laser-inducedhydrothermal reaction (LIHR) technique to grow NiMoO4nanosheets on nickel foam,which is then calcined under H2/Ar mixed gases to prepare the IE IE-NiMo-LR.This electrode exhibits superior hydrogen evolution reaction performance,requiring overpotentials of 59,116 and143 mV to achieve current densities of 100,500 and 1000 mA·cm-2.During the 350 h chronopotentiometry test at current densities of 100 and 500 m A·cm-2,the overpotentialremains essentially unchanged.In addition,NiFe-layered double hydroxide grown on Ni foam is also fabricated with the same LIHR method and coupled with IE-NiMo-IR to achieve water splitting.This combination exhibits excellent durability under industrial current density.The energy consumption and production efficiency of the LIHR method are systematicallycompared with the conventional hydrothermal method.The LIHR method significantly improves the production rate by over 19 times,while consuming only 27.78%of the total energy required by conventional hydrothermal methods to achieve the same production. 展开更多
关键词 electrocatalytic electrode laser-induced hydrothermal reaction NiFe layered double hydroxides hydrogen evolution reaction water splitting energy consumption production rate
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Direct measurement of the break-out ^(19)F(p,γ)^(20)Ne reaction in the China Jinping underground laboratory(CJPL)
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作者 Yin‑Ji Chen Hao Zhang +28 位作者 Li‑Yong Zhang Jian‑Jun He Richard James deBoer Michael Wiescher Alexander Heger David Kahl Jun Su Daniel Odell Xin‑Yue Li Jian‑Guo Wang Long Zhang Fu‑Qiang Cao Zhi‑Cheng Zhang Xin‑Zhi Jiang Luo‑Huan Wang Zi‑Ming Li Lu‑Yang Song Liang‑Ting Sun Qi Wu Jia‑Qing Li Bao‑Qun Cui Li‑Hua Chen Rui‑Gang Ma Er‑Tao Li Gang Lian Yao‑De Sheng Zhi‑Hong Li Bing Guo Wei‑Ping Liu 《Nuclear Science and Techniques》 SCIE EI CAS CSCD 2024年第8期142-152,共11页
Calcium production and the stellar evolution of first-generation stars remain fascinating mysteries in astrophysics.As one possible nucleosynthesis scenario,break-out from the hot carbon–nitrogen–oxygen(HCNO)cycle w... Calcium production and the stellar evolution of first-generation stars remain fascinating mysteries in astrophysics.As one possible nucleosynthesis scenario,break-out from the hot carbon–nitrogen–oxygen(HCNO)cycle was thought to be the source of the calcium observed in these oldest stars.However,according to the stellar modeling,a nearly tenfold increase in the thermonuclear rate ratio of the break-out ^(19)F(p,γ)^(20) Ne reaction with respect to the competing ^(19)F(p,α)^(16) O back-processing reaction is required to reproduce the observed calcium abundance.We performed a direct measurement of this break-out reaction at the China Jinping underground laboratory.The measurement was performed down to the low-energy limit of E_(c.m.)=186 keV in the center-of-mass frame.The key resonance was observed at 225.2 keV for the first time.At a temperature of approximately 0.1 GK,this new resonance enhanced the thermonuclear ^(19)F(p,γ)^(20) Ne rate by up to a factor of≈7.4,compared with the previously recommended NACRE rate.This is of particular interest to the study of the evolution of the first stars and implies a stronger breakdown in their“warm”CNO cycle through the ^(19)F(p,γ)^(20) Ne reaction than previously envisioned.This break-out resulted in the production of the calcium observed in the oldest stars,enhancing our understanding of the evolution of the first stars. 展开更多
关键词 Nuclear astrophysics First stars Abundance of calcium reaction cross section reaction rate China Jinping underground laboratory(CJPL) JUNA
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Petrology of Spinel-Lherzolite Xenoliths from Mazéléand Others Northen Xenoliths Localities of Cameroon Volcanic Line: Exchange Reactions and Equilibrium State
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作者 Nguihdama Dagwai Kamgang Pierre +2 位作者 Mbowou Gbambié Isaac Bertrand Chazot Gilles Ngounouno Ismaïla 《Open Journal of Geology》 CAS 2024年第5期629-653,共25页
The alkaline volcanism of the Cameroon Volcanic Line in its northern domain has raised many fresh enclaves of peridotites. The samples selected come from five (05) different localities (Liri, in the plateau of Kapsiki... The alkaline volcanism of the Cameroon Volcanic Line in its northern domain has raised many fresh enclaves of peridotites. The samples selected come from five (05) different localities (Liri, in the plateau of Kapsiki, Mazélé in the NE of Ngaoundéré, Tello and Ganguiré in the SE of Ngaoundéré and Likok, locality located in the west of Ngaoundé). The peridotite enclaves of the above localities show restricted mineralogical variation. Most are four-phase spinel-lherzolites, indicating that this is the main lithology that forms the lithospheric mantle below the shallow zone. No traces of garnet or primary plagioclase were detected, which strongly limits the depth range from which the rock fragments were sampled. The textures and the wide equilibrium temperatures (884˚C - 1115˚C) indicate also entrainment of lherzolite xenoliths from shallow depths within the lithosphere and the presence of mantle diapirism. The exchange reactions and equilibrium state established in this work make it possible to characterize the chemical composition of the upper mantle of each region and test the equilibrium state of the phases between them. Variations of major oxides and incompatible elemental concentrations in clinopyroxene indicate a primary control by partial melting. The absence of typical “metasomatic” minerals, low equilibration temperatures and enriched LREE patterns indicate that the upper mantle below septentrional crust of Cameroun underwent an event of cryptic metasomatic enrichment prior to partial melting. The distinctive chemical features, LREE enrichment, strong U, Ce and Pr, depletion relative to Ba, Nb, La, Pb, and T, fractionation of Zr and Hf and therefore ligh high Zr/Hf ratio, low La/Yb, Nb/La and Ti/Eu are all results of interaction of refractory peridotite residues with carbonatite melts. 展开更多
关键词 XENOLITHS Upper Mantle Northern Region Adamawa Cameroon Volcanic Line Exchange reaction
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