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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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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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Cation effects in electrocatalytic reduction reactions:Recent advances
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作者 Qinghui Ren Liang Xu +4 位作者 Mengyu Lv Zhiyuan Zhang Zhenhua Li Mingfei Shao Xue Duan 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第8期16-32,共17页
Electrocatalytic reduction reactions,powered by clean energy sources such as solar energy and wind,offer a sustainable method for converting inexpensive feedstocks(e.g.,CO_(2),N_(2)/NO_(x),organics,and O_(2))into high... Electrocatalytic reduction reactions,powered by clean energy sources such as solar energy and wind,offer a sustainable method for converting inexpensive feedstocks(e.g.,CO_(2),N_(2)/NO_(x),organics,and O_(2))into high-value-added chemicals or fuels.The design and modification of electrocatalysts have been widely implemented to improve their performance in these reactions.However,bottle-necks are encountered,making it challenging to further improve performance through catalyst development alone.Recently,cations in the electrolyte have emerged as critical factors for tuning both the activity and product selectivity of reduction reactions.This review summarizes recent advances in understanding the role of cation effects in electrocatalytic reduction reactions.First,we introduce the mechanisms underlying cation effects.We then provide a comprehensive overview of their application in electroreduction reactions.Characterization techniques and theoretical calcula-tion methods for studying cation effects are also discussed.Finally,we address remaining challeng-es and future perspectives in this field.We hope that this review offers fundamental insights and design guidance for utilizing cation effects,thereby advancing their development. 展开更多
关键词 ELECTROCATALYSIS Reduction reaction Cation effect MECHANISM APPLICATION
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Study on synergistic leaching of potassium and phosphorus from potassium feldspar and solid waste phosphogypsum via coupling reactions
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作者 Chao Li Shizhao Wang +3 位作者 Yunshan Wang Xuebin An Gang Yang Yong Sun 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第1期117-129,共13页
To achieve the resource utilization of solid waste phosphogypsum(PG)and tackle the problem of utilizing potassium feldspar(PF),a coupled synergistic process between PG and PF is proposed in this paper.The study invest... To achieve the resource utilization of solid waste phosphogypsum(PG)and tackle the problem of utilizing potassium feldspar(PF),a coupled synergistic process between PG and PF is proposed in this paper.The study investigates the features of P and F in PG,and explores the decomposition of PF using hydrofluoric acid(HF)in the sulfuric acid system for K leaching and leaching of P and F in PG.The impact factors such as sulfuric acid concentration,reaction temperature,reaction time,material ratio(PG/PF),liquid–solid ratio,PF particle size,and PF calcination temperature on the leaching of P and K is systematically investigated in this paper.The results show that under optimal conditions,the leaching rate of K and P reach more than 93%and 96%,respectively.Kinetics study using shrinking core model(SCM)indicates two significant stages with internal diffusion predominantly controlling the leaching of K.The apparent activation energies of these two stages are 11.92 kJ·mol^(-1)and 11.55 kJ·mol^(-1),respectively. 展开更多
关键词 PHOSPHOGYPSUM Potassium feldspar Coupling reaction LEACHING Waste treatment Kinetics
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Why Don’t We Adequately Identify and Manage Adverse Drug Reactions despite Having the Needed Information?
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作者 Mark J. Kupersmith Karl Kieburtz 《Health》 2024年第2期148-159,共12页
Importance/Objective: Adverse Drug Reactions (ADRs) are unavoidable, but recognizing and addressing ADRs early can improve wellness and prevent permanent injury. We suggest that available medical information and digit... Importance/Objective: Adverse Drug Reactions (ADRs) are unavoidable, but recognizing and addressing ADRs early can improve wellness and prevent permanent injury. We suggest that available medical information and digital/electronic methods could be used to manage this major healthcare problem for individual patients in real time. Methods: We searched the available digital applications and three literature databases using the medical subject heading terms, adverse drug reaction reporting systems or management, filtered by clinical trial or systemic reviews, to detect publications with data about ADR identification and management approaches. We reviewed the reports that had abstract or summary data or proposed or implemented methods or systems with potential to identify or manage ADRs in clinical settings. Results: The vast majority of the 481 reports used retrospectively collected data for groups of patients or were limited to surveying one population group or class of medication. The reports showed potential and definite associations of ADRs for specific drugs and problems, mostly, but not exclusively, for patients in hospitals and nursing homes. No reports described complete methods to collect comprehensive data on ADRs for individual patients in a healthcare system. The digital applications have ADR information, but all are too cumbersome or incomplete for use in active clinical settings. Several studies suggested that providing information about potential ADRs to clinicians can reduce these problems. Conclusion and Relevance: Although investigators and government agencies agree with the need, there is no comprehensive ADR management program in current use. Informing the patient’s healthcare practitioners of potential ADRs at the point of service has the potential for reduction of these complications, which should improve healthcare and reduce unneeded costs. 展开更多
关键词 Adverse Drug reaction Medication Side Effect Identification Medication Complication Medication Safety
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Selective photosynthesis of Z-olefins through crystalline metal-organic cage-initiated expeditious cascade reactions
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作者 Jia-Ni Lu Yunze Huang +6 位作者 Yuan-Sheng Xia Long-Zhang Dong Lei Zhang Jing-Jing Liu Lan-Gui Xie Jiang Liu Ya-Qian Lan 《Carbon Energy》 SCIE EI CAS CSCD 2024年第3期118-131,共14页
The semi-hydrogenation of alkyne to form Z-olefins with high conversion and high selectivity is still a huge challenge in the chemical industry.Moreover,flammable and explosive hydrogen as the common hydrogen source o... The semi-hydrogenation of alkyne to form Z-olefins with high conversion and high selectivity is still a huge challenge in the chemical industry.Moreover,flammable and explosive hydrogen as the common hydrogen source of this reaction increases the cost and danger of industrial production.Herein,we connect the photocatalytic hydrogen evolution reaction and the semihydrogenation reaction of alkynes in series and successfully realize the high selective production of Z-alkenes using low-cost,safe,and green water as the proton source.Before the cascade reaction,a series of isomorphic metal–organic cage catalysts(Co_(x)Zn_(8−x)L_(6),x=0,3,4,5,and 8)are designed and synthesized to improve the yield of the photocatalytic hydrogen production.Among them,Co_(5)Zn_(3)L_(6) shows the highest photocatalytic activity,with a H_(2) generation rate of 8.81 mmol g^(−1) h^(−1).Then,Co_(5)Zn_(3)L_(6) is further applied in the above tandem reaction to efficiently reduce alkynes to Z-alkenes under ambient conditions,which can reach high conversion of>98%and high selectivity of>99%,and maintain original catalytic activity after multiple cycles.This“one-pot”tandem reaction can achieve a highly selective and safe stepwise conversion from water into hydrogen into Z-olefins under mild reaction conditions. 展开更多
关键词 alkyne semi-hydrogenation hydrogen evolution reaction metal-organic cages photocatalysis Z-olefins
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Energetic and Entropic Changes in Volume Work and Chemical Reactions
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作者 Frank Diederichs 《Advances in Chemical Engineering and Science》 CAS 2024年第1期8-47,共40页
In the present study, energetic and entropic changes are investigated on a comparative basis, as they occur in the volume changes of an ideal gas in the Carnot cycle and in the course of the chemical reaction in a lea... In the present study, energetic and entropic changes are investigated on a comparative basis, as they occur in the volume changes of an ideal gas in the Carnot cycle and in the course of the chemical reaction in a lead-acid battery. Differences between reversible and irreversible processes have been worked out, in particular between reversibly exchanged entropy (∆<sub>e</sub>S) and irreversibly produced entropy (∆<sub>i</sub>S). In the partially irreversible case, ∆<sub>e</sub>S and ∆<sub>i</sub>S add up to the sum ∆S for the volume changes of a gas, and only this function has an exact differential. In a chemical reaction, however, ∆<sub>e</sub>S is independent on reversibility. It arises from the different intramolecular energy contents between products and reactants. Entropy production in a partially irreversible Carnot cycle is brought about through work-free expansions, whereas in the irreversible battery reaction entropy is produced via activated complexes, whereby a certain, variable fraction of the available chemical energy becomes transformed into electrical energy and the remaining fraction dissipated into heat. The irreversible reaction process via activated complexes has been explained phenomenologically. For a sufficiently high power output of coupled reactions, it is essential that the input energy is not completely reversibly transformed, but rather partially dissipated, because this can increase the process velocity and consequently its power output. A reduction of the counter potential is necessary for this purpose. This is not only important for man-made machines, but also for the viability of cells. 展开更多
关键词 Exchanged Entropy Entropy Production Coupled reactions Activated Complexes Power Output
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Adverse drug reactions of first-line antitubercular drugs:A retrospective study on characteristics,management,factors,and impacts
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作者 Ai Ling Oh Mohd Makmor-Bakry +3 位作者 Farida Islahudin Chuo Yew Ting Swee Kim Chan Siew Teck Tie 《Asian Pacific Journal of Tropical Medicine》 SCIE CAS 2024年第10期456-464,共9页
Objective:To elucidate the characteristics,management strategies,risk factors,and clinical impacts associated with adverse drug reactions(ADRs)induced by first-line antitubercular drugs to enhance tuberculosis(TB)mana... Objective:To elucidate the characteristics,management strategies,risk factors,and clinical impacts associated with adverse drug reactions(ADRs)induced by first-line antitubercular drugs to enhance tuberculosis(TB)management.Methods:A retrospective cohort study was conducted by retrieving drug-susceptible TB records among adult patients who received TB treatment from 2018 to 2021 at 10 public health clinics in Sarawak,Malaysia.Only the initial TB treatment and occurrence of specific ADRs within the study period were considered.Regression analysis was performed to identify the risk factors associated with both overall ADRs and individual types of ADRs.Results:Among 2953 cases,705(23.9%)developed ADRs.Cutaneous reactions were the most prevalent(47.1%),followed by hepatotoxicity(32.8%)and gastrointestinal disturbances(29.8%).Six out of seven types of ADRs investigated occurred within the intensive phase,mostly manifesting at approximately 2 weeks of initiation.Hepatotoxicity resulted in the majority(85.3%)of treatment discontinuations,while vision problems led to treatment modifications in half of the cases.Risk factors for all ADRs included age≥60 years,females,illicit drug use,and comorbidities such as HIV-positive,diabetes,and chronic liver disease.Alcohol consumption was independently associated with hepatotoxicity.ADRs caused around one-third of interruptions exceeding 2 weeks(33.0%)and subsequently necessitated treatment restarts(34.5%).Conclusions:Understanding these various aspects contributes to improving the overall management of ADRs in TB treatment.Close ADR monitoring and reporting are essential to strengthen ADR management. 展开更多
关键词 Adverse events Cutaneous reactions HEPATOTOXICITY Gastrointestinal disturbances Risk factors TUBERCULOSIS
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Possibility of reaching the predicted center of the“island of stability”via the radioactive beam-induced fusion reactions
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作者 Ming-Hao Zhang Ying Zou +3 位作者 Mei-Chen Wang Gen Zhang Qing-Lin Niu Feng-Shou Zhang 《Nuclear Science and Techniques》 SCIE EI CAS CSCD 2024年第9期186-195,共10页
Based on the dinuclear system model,the synthesis of the predicted double-magic nuclei^(298)Fl and 304120 was investigated via neutron-rich radioactive beam-induced fusion reactions.The reaction^(58)Ca+^(244)Pu is pre... Based on the dinuclear system model,the synthesis of the predicted double-magic nuclei^(298)Fl and 304120 was investigated via neutron-rich radioactive beam-induced fusion reactions.The reaction^(58)Ca+^(244)Pu is predicted to be favorable for producing^(298)Fl with a maximal ER cross section of 0.301 pb.Investigations of the entrance channel effect reveal that the^(244)Pu target is more promising for synthesizing^(298)Fl than the neutron-rich targets^(248)Cm and^(249)Bk,because of the influence of the Coulomb barrier.For the synthesis of 304120,the maximal ER cross section of 0.046 fb emerges in the reaction^(58)V+^(249)Bk,indicating the need for further advancements in both experimental facilities and reaction mechanisms. 展开更多
关键词 Superheavy nuclei Dinuclear system model Fusion reaction Double-magic nucleus Radioactive beam
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Decouple charge transfer reactions in the Li-ion battery
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作者 Yuxuan Bai Qiu-An Huang +1 位作者 Kai Wu Jiujun Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期759-798,共40页
In the development of Li-ion batteries(LIBs)with high energy/power density,long cycle-life,fast charging,and high safety,an insight into charge transfer reactions is required.Although electrochemical impedance spectro... In the development of Li-ion batteries(LIBs)with high energy/power density,long cycle-life,fast charging,and high safety,an insight into charge transfer reactions is required.Although electrochemical impedance spectroscopy(EIS)is regarded as a powerful diagnosis tool,it is not a direct but an indirect measurement.With respect to this,some critical questions need to be answered:(i)why EIS can reflect the kinetics of charge transfer reactions;(ii)what the inherent logical relationship between impedance models under different physical scenes is;(iii)how charge transfer reactions compete with each other at multiple scales.This work aims at answering these questions via developing a theory framework so as to mitigate the blindness and uncertainty in unveiling charge transfer reactions in LIBs.To systematically answer the above questions,this article is organized into a three-in-one(review,tutorial,and research)type and the following contributions are made:(i)a brief review is given for impedance model development of the LIBs over the past half century;(ii)an open source code toolbox is developed based on the unified impedance model;(iii)the competive mechanisms of charge transfer reactions are unveiled based on the developed EIS-Toolbox@LIB.This work not only clarifies theoretical fundamentals,but also provides an easy-to-use open source code for EIS-Toolbox@LIB to optimize fast charge/discharge,mitigate cycle aging,and improve energy/power density. 展开更多
关键词 Electrochemical impedance spectroscopy Unified impedance model Charge transfer reactions Solid/electrolyte diffusion Porous electrode EIS-Toolbox@LIB
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Experimental study on reactions between alkaline basaltic melt and orthopyroxenes: constraints on the evolution of lithospheric mantle in the North China Craton
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作者 Hanqi He Mingliang Wang Hongfeng Tang 《Acta Geochimica》 EI CAS CSCD 2024年第2期354-365,共12页
The experimental results of the reactions between an alkaline basaltic melt and mantle orthopyroxenes under high-temperature and high-pressure conditions of 1300–1400℃ and 2.0–3.0 GPa using a six-anvil apparatus ar... The experimental results of the reactions between an alkaline basaltic melt and mantle orthopyroxenes under high-temperature and high-pressure conditions of 1300–1400℃ and 2.0–3.0 GPa using a six-anvil apparatus are reported in this paper.The reactions are proposed to simulate the interactions between melts from the asthenospheric mantle and the lithospheric mantle.The starting melt in the experiments was made from the alkaline basalt occurring in Fuxin,Liaoning Province,and the orthopyroxenes were separated from the mantle xenoliths in Damaping,Hebei Province.The results show that clinopyroxenes were formed in all the reactions between the alkaline basaltic melt and orthopyroxenes under the studied P–T conditions.The formation of clinopyroxene in the reaction zone is mainly controlled by dissolution–crystallization,and the chemical compositions of the reacted melt are primarily infl uenced by the diff usion eff ect.Temperature is the most important parameter controlling the reactions between the melt and orthopyroxenes,which has a direct impact on the melting of orthopyroxenes and the diff usion of chemical components in the melt.Temperature also directly controls the chemical compositions of the newly formed clinopyroxenes in the reaction zone and the reacted melt.The formation of clinopyroxenes from the reactions between the alkaline basaltic melt and orthopyroxenes can result in an increase of CaO and Al_(2)O_(3) contents in the rocks containing this mineral.Therefore,the reactions between the alkaline basaltic melt from the asthenospheric mantle and orthopyroxenes from the lithospheric mantle can lead to the evolution of lithospheric mantle in the North China Craton from refractory to fertile with relatively high CaO and Al 2 O 3 contents.In addition,the reacted melts in some runs were transformed from the starting alkaline basaltic into tholeiitic after reactions,indicating that tholeiitic magma could be generated from alkaline basaltic one via reactions between the latter and orthopyroxene. 展开更多
关键词 Alkaline basaltic melt ORTHOPYROXENE Melt–mineral reaction High-temperature and high-pressure experiment Genesis of basalt Evolution of lithospheric mantle in the North China Craton
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Prevention and Nursing of Adverse Reactions of Novel Coronavirus Inactivated Vaccine (Vero Cells)
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作者 Jingyu He Muyang Bian +1 位作者 Jianan Du Liping Wang 《Journal of Clinical and Nursing Research》 2024年第5期100-107,共8页
Objective:To discuss and analyze the causes of adverse reactions caused by the inactivated novel coronavirus vaccine(Vero cells),and to propose methods of prevention and care.Methods:A questionnaire was used to random... Objective:To discuss and analyze the causes of adverse reactions caused by the inactivated novel coronavirus vaccine(Vero cells),and to propose methods of prevention and care.Methods:A questionnaire was used to randomly select 229 adults who were vaccinated with the inactivated novel coronavirus vaccine(Vero cells)at Xi’an People’s Hospital(Xi’an Fourth Hospital).The adverse reactions were statistically analyzed.Results:Among the 229 adults vaccinated with the inactivated novel coronavirus vaccine(Vero cells),30 experienced vaccination reactions.The main reaction was local induration at the inoculation site,and dizziness was the primary systemic symptom.Conclusion:To reduce the incidence of adverse reactions to the inactivated novel coronavirus vaccine(Vero cells),it is necessary to effectively evaluate the health status of adults before vaccination,select the correct vaccination site,and strictly implement the rules of 3-inspections,7-checks,and 1-verification.Standardizing the operation process and providing thorough health education after vaccination can effectively reduce the occurrence of adverse reactions. 展开更多
关键词 Novel coronavirus inactivated vaccine(Vero cells) VACCINATION Adverse reactions nursing
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Facet Engineering of Advanced Electrocatalysts Toward Hydrogen/Oxygen Evolution Reactions 被引量:10
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作者 Changshui Wang Qian Zhang +7 位作者 Bing Yan Bo You Jiaojiao Zheng Li Feng Chunmei Zhang Shaohua Jiang Wei Chen Shuijian He 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第4期97-137,共41页
The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality... The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality.Electrocatalysts can effectively reduce the reaction energy barrier and increase the reaction efficiency.Facet engineering is considered as a promising strategy in controlling the ratio of desired crystal planes on the surface.Owing to the anisotropy,crystal planes with different orientations usually feature facet-dependent physical and chemical properties,leading to differences in the adsorption energies of oxygen or hydrogen intermediates,and thus exhibit varied electrocatalytic activity toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this review,a brief introduction of the basic concepts,fundamental understanding of the reaction mechanisms as well as key evaluating parameters for both HER and OER are provided.The formation mechanisms of the crystal facets are comprehensively overviewed aiming to give scientific theory guides to realize dominant crystal planes.Subsequently,three strategies of selective capping agent,selective etching agent,and coordination modulation to tune crystal planes are comprehensively summarized.Then,we present an overview of significant contributions of facet-engineered catalysts toward HER,OER,and overall water splitting.In particular,we highlight that density functional theory calculations play an indispensable role in unveiling the structure–activity correlation between the crystal plane and catalytic activity.Finally,the remaining challenges in facet-engineered catalysts for HER and OER are provided and future prospects for designing advanced facet-engineered electrocatalysts are discussed. 展开更多
关键词 Crystal facet engineering ANISOTROPY Oxygen evolution reaction Hydrogen evolution reaction Theoretical simulations
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Deciphering engineering principle of three-phase interface for advanced gas-involved electrochemical reactions 被引量:2
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作者 Yanzheng He Sisi Liu +3 位作者 Mengfan Wang Qiyang Cheng Tao Qian Chenglin Yan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第5期302-323,I0008,共23页
As an alternative to conventional energy conversion and storage reactions,gas-involved electrochemical reactions,including the carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and hydrogen e... As an alternative to conventional energy conversion and storage reactions,gas-involved electrochemical reactions,including the carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and hydrogen evolution reaction(HER),have become an emerging research direction and have gained increasing attention due to their advantages of environmental friendliness and sustainability.Various studies have been designed to accelerate sluggish kinetics but with limited results.Most of them promote the reaction by modulating the intrinsic properties of the catalyst,ignoring the synergistic effect of the reaction as a whole.Due to the introduction of gas,traditional liquid-solid two-phase reactions are no longer applicable to future research.Since gas-involved electrochemical reactions mostly occur at the junctions of gaseous reactants,liquid electrolytes and solid catalysts,the focus of future research on reaction kinetics should gradually shift to three-phase reaction interfaces.In this review,we briefly introduce the formation and constraints of the three-phase interface and propose three criteria to judge its merit,namely,the active site,mass diffusion and electron mass transfer.Subsequently,a series of modulation methods and relevant works are discussed in detail from the three improvement directions of‘exposing more active sites,promoting mass diffusion and accelerating electron transfer’.Definitively,we provide farsighted insights into the understanding and research of three-phase interfaces in the future and point out the possible development direction of future regulatory methods,hoping that this review can broaden the future applications of the three-phase interface,including but not limited to gas-involved electrochemical reactions. 展开更多
关键词 Three-phase reaction Surface reactions Mass diffusion Electron transfer Gas-involved electrochemical reactions
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Metal organic polymers with dual catalytic sites for oxygen reduction and oxygen evolution reactions 被引量:3
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作者 Sijia Liu Minghao Liu +4 位作者 Xuewen Li Shuai Yang Qiyang Miao Qing Xu Gaofeng Zeng 《Carbon Energy》 SCIE CSCD 2023年第5期127-137,共11页
Metal-organic frameworks and covalent organic frameworks have been widely employed in electrochemical catalysis owing to their designable skeletons,controllable porosities,and well-defined catalytic centers.However,th... Metal-organic frameworks and covalent organic frameworks have been widely employed in electrochemical catalysis owing to their designable skeletons,controllable porosities,and well-defined catalytic centers.However,the poor chemical stability and low electron conductivity limited their activity,and single-functional sites in these frameworks hindered them to show multifunctional roles in catalytic systems.Herein,we have constructed novel metal organic polymers(Co-HAT-CN and Ni-HAT-CN)with dual catalytic centers(metal-N_(4) and metal-N_(2))to catalyze oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).By using different metal centers,the catalytic activity and selectivity were well-tuned.Among them,Co-HAT-CN catalyzed the ORR in a 4e^(-)pathway,with a half-wave potential of 0.8 V versus RHE,while the Ni-HAT-CN catalyze ORR in a 2e^(-)pathway with H_(2)O_(2) selectivity over 90%.Moreover,the Co-HAT-CN delivered an overpotential of 350 mV at 10 mA cm^(-2) with a corresponding Tafel slope of 24 mV dec^(-1) for OER in a 1.0 M KOH aqueous solution.The experimental results revealed that the activities toward ORR were due to the M-N_(4) sites in the frameworks,and both M-N_(4) and M-N_(2) sites contributed to the OER.This work gives us a new platform to construct bifunctional catalysts. 展开更多
关键词 covalent organic frameworks metal organic polymers oxygen evolution reaction oxygen reduction reaction single atom catalysts
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A Review of In‑Situ Techniques for Probing Active Sites and Mechanisms of Electrocatalytic Oxygen Reduction Reactions 被引量:4
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作者 Jinyu Zhao Jie Lian +2 位作者 Zhenxin Zhao Xiaomin Wang Jiujun Zhang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第2期61-113,共53页
Electrocatalytic oxygen reduction reaction(ORR)is one of the most important reactions in electrochemical energy technologies such as fuel cells and metal–O2/air batteries,etc.However,the essential catalysts to overco... Electrocatalytic oxygen reduction reaction(ORR)is one of the most important reactions in electrochemical energy technologies such as fuel cells and metal–O2/air batteries,etc.However,the essential catalysts to overcome its slow reaction kinetic always undergo a complex dynamic evolution in the actual catalytic process,and the concomitant intermediates and catalytic products also occur continuous conversion and reconstruction.This makes them difficult to be accurately captured,making the identification of ORR active sites and the elucidation of ORR mechanisms difficult.Thus,it is necessary to use extensive in-situ characterization techniques to proceed the real-time monitoring of the catalyst structure and the evolution state of intermediates and products during ORR.This work reviews the major advances in the use of various in-situ techniques to characterize the catalytic processes of various catalysts.Specifically,the catalyst structure evolutions revealed directly by in-situ techniques are systematically summarized,such as phase,valence,electronic transfer,coordination,and spin states varies.In-situ revelation of intermediate adsorption/desorption behavior,and the real-time monitoring of the product nucleation,growth,and reconstruction evolution are equally emphasized in the discussion.Other interference factors,as well as in-situ signal assignment with the aid of theoretical calculations,are also covered.Finally,some major challenges and prospects of in-situ techniques for future catalysts research in the ORR process are proposed. 展开更多
关键词 Oxygen reduction reaction CATALYSTS In-situ techniques Active sites MECHANISMS
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Prediction of synthesis cross sections of new moscovium isotopes in fusion‑evaporation reactions 被引量:4
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作者 Peng‑Hui Chen Hao Wu +2 位作者 Zu‑Xing Yang Xiang‑Hua Zeng Zhao‑Qing Feng 《Nuclear Science and Techniques》 SCIE EI CAS CSCD 2023年第1期86-101,共16页
In the framework of the dinuclear system model,the synthesis mechanism of the superheavy nuclides with atomic numbers Z=112,114,115 in the reactions of projectiles 40,^(48)Ca bombarding on targets^(238)U,^(242)Pu,and^... In the framework of the dinuclear system model,the synthesis mechanism of the superheavy nuclides with atomic numbers Z=112,114,115 in the reactions of projectiles 40,^(48)Ca bombarding on targets^(238)U,^(242)Pu,and^(243)Am within a wide interval of incident energy has been investigated systematically.Based on the available experimental excitation functions,the dependence of calculated synthesis cross-sections on collision orientations has been studied thoroughly.The total kinetic energy(TKE)of these collisions with fixed collision orientation shows orientation dependence,which can be used to predict the tendency of kinetic energy diffusion.The TKE is dependent on incident energies,as discussed in this paper.We applied the method based on the Coulomb barrier distribution function in our calculations.This allowed us to approximately consider all the collision orientations from tip-tip to side-side.The calculations of excitation functions of^(48)Ca+^(238)U,^(48)Ca+242Pu,and^(48)Ca+^(243)Am are in good agreement with the available experimental data.The isospin effect of projectiles on production cross-sections of moscovium isotopes and the influence of the entrance channel effect on the synthesis cross-sections of superheavy nuclei are also discussed in this paper.The synthesis cross-section of new moscovium isotopes 278−286 Mc was predicted to be as large as hundreds of pb in the fusion-evaporation reactions of^(35,37)Cl+^(248)Cf,^(38,40)Ar+^(247)Bk,^(39,41)K+247 Cm,^(40,42,44,46)Ca+^(243)Am,45 Sc+^(244)Pu,and^(46,48,50)Ti+237Np,51 V+^(238)U at some typical excitation energies. 展开更多
关键词 Dinuclear system model Superheavy nuclei Complete fusion reactions Production cross-section
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Production of neutron-rich actinide isotopes in isobaric collisions via multinucleon transfer reactions 被引量:4
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作者 Peng-Hui Chen Chang Geng +2 位作者 Zu-Xing Yang Xiang-Hua Zeng Zhao-Qing Feng 《Nuclear Science and Techniques》 SCIE EI CAS CSCD 2023年第10期166-177,共12页
We systematically calculated the multinucleon transfer reactions of ^(208)Os,^(208)Pt,^(208)Hg,^(208)Pb,^(208)Po,^(208)Rn,^(208)Ra,and ^(132,136) Xe when bombarded on ^(232) Th and ^(248) Cm at Coulomb barrier energie... We systematically calculated the multinucleon transfer reactions of ^(208)Os,^(208)Pt,^(208)Hg,^(208)Pb,^(208)Po,^(208)Rn,^(208)Ra,and ^(132,136) Xe when bombarded on ^(232) Th and ^(248) Cm at Coulomb barrier energies within the dinuclear system model.These results are in good agreement with the available experimental data.The influence of Coulomb and shell effects on actinide production in these reactions has been rigorously studied.We calculated and analyzed the potential energy surface (PES) and total kinetic energy (TKE) mass distributions for the reactions involving ^(208)Hg,^(208)Pb,and ^(208) Po with ^(248) Cm and ^(232)Th.The PES and TKE spectra shed light on the fragment formation mechanisms in multinucleon transfer reactions,with clear indications of isospin and shell effects.The production cross sections for multinucleon transfer products show a strong dependence on isobar projectiles with a mass number A=208.Isobar projectiles with high N/Z ratios are advantageous for generating neutron-rich target-like fragments.Conversely,products induced by isobar projectiles with larger charge numbers tend to shift toward proton-rich regions.The intertwining of the Coulomb potential and shell effect is evident in the production cross sections of actinide isotopes.Drawing from reactions induced by radioactive projectiles,we anticipate the discovery of several new actinide isotopes near the nuclear drip lines,extending our reach into the superheavy nuclei domain. 展开更多
关键词 Dinuclear system model Isobaric collisions Multinucleon transfer reactions Neutron-rich actinides
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Elucidating the Role of Mass Transfer in Electrochemical Redox Reactions on Electrospun Fibers 被引量:1
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作者 Yan Li Ziwang Kan +6 位作者 Lina Jia Dan Zhang Yan Hong Jingjing Liu Haibo Huang Siqi Li Song Liu 《Transactions of Tianjin University》 EI CAS 2023年第5期313-320,共8页
Mass transfer can tune the surface concentration of reactants and products and subsequently infl uence the catalytic perfor-mance.The morphology of nanomaterials plays an important role in the mass transfer of reactio... Mass transfer can tune the surface concentration of reactants and products and subsequently infl uence the catalytic perfor-mance.The morphology of nanomaterials plays an important role in the mass transfer of reaction microdomains,but related studies are lacking.Herein,a facile electrospinning technique utilizing cellulose was employed to fabricate a series of carbon nanofi bers with diff erent diameters,which exhibited excellent electrochemical nitrate reduction reaction and oxygen evolu-tion reaction activities.Furthermore,the microstructure of electrocatalysts could infl uence the gas-liquid-solid interfacial mass transfer,resulting in diff erent electrochemical performances. 展开更多
关键词 Mass transfer ELECTROSPINNING Electrochemical nitrate reduction reaction Oxygen evolution reaction
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