The preparation method of H_4MoO_(26)-polyaniline film modified electrode and its voltammetric behaviour are described. The modified electrode has high electrocatalytic activity on chlorate ions.
Strong metal–support interaction(SMSI),namely the strong electronic and structural interaction between metal nanoparticles and supports,one of the most typical synergetic catalytic effects in composite catalysts,has ...Strong metal–support interaction(SMSI),namely the strong electronic and structural interaction between metal nanoparticles and supports,one of the most typical synergetic catalytic effects in composite catalysts,has been found critically important in the design of catalyst for thermocatalysis in the past.Recently,however,important and great progress of SMSI-based synergetic effects has been made in electrocatalysis,such as electrocatalyst design and electrocatalytic mechanism investigations.To better understand the nature of the synergetic effect assisting the further development of electrocatalysts,a comprehensive and in-depth overview highlighting and discussing the recent advances of SMSI in electrocatalysis is necessary and highly desirable but still absent.Herein,this review firstly presents various strategies of designing and constructing composite catalysts featuring SMSI.Further from the perspectives of electrocatalysis,the characterization techniques towards the electron structure,local interfacial and morphological features and active sites for SMSI-based electrocatalysts,have been summarized in detail.Importantly,the recent advances in the design of single-and bi-functional electrocatalysts featuring SMSI-based synergetic catalytic effects,and the key roles of SMSI during the electrocatalytic reactions are emphasized.Finally,the challenges and prospects are discussed to highlight the key remaining issues in the future development of SMSI-based electrocatalysts.展开更多
Transforming industrial heritage will have internal economic and cultural effects and will also catalyse changes in surrounding urban areas.Transforming industrial heritage is therefore an essential part of strategies...Transforming industrial heritage will have internal economic and cultural effects and will also catalyse changes in surrounding urban areas.Transforming industrial heritage is therefore an essential part of strategies to regenerate decayed industrial districts.The aim of this study was to attempt to answer three questions.Can all transformed industrial heritage give catalytic effects?How should the potential for catalytic effects be assessed?What factors prevent catalytic effects?The Sanbao Street Industrial Heritage Historic District in Changzhou,China,was used as an example,and three effects catalysed by transforming industrial heritage were assessed.These were(1)reuse of industrial and non-industrial buildings in and near the historic district,(2)new construction in and near the historic district,and(3)revitalisation of the whole historic district.Failure of the catalytic effect caused by a lack of a conversion mechanism,failure to communicate the value of industrial heritage,and limited cultural industrial capacity was assessed.Formal transformation strategies focused on the connotative value of industrial heritage are proposed,and are expected to support future research and planning practices.展开更多
The effects of peptides,amino acids and organic bases as an axial ligand on reaction ac- tivities in the electrocarboxylation of benzyl chloride with CO_2 catalyzed by CoTPP are reported. The imidazole organic base,pe...The effects of peptides,amino acids and organic bases as an axial ligand on reaction ac- tivities in the electrocarboxylation of benzyl chloride with CO_2 catalyzed by CoTPP are reported. The imidazole organic base,peptide containing —SH and amino acid containing imidazolyl en- hance the catalytic activity.The effect of imidazole amounts on the catalytic activity of CoTPP is studied.展开更多
The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste g...The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste gas but also recover clean energy H_(2),which has significant socio-economic and ecological advantages.However,the highly effective decomposition of H_(2)S at low temperatures is still a great challenge,because of the stringent thermodynamic equilibrium constraints(only 20% even at high temperature of 1010℃).Conventional microwave catalysts exhibit unsatisfactory performance at low temperatures(below 600℃).Herein,Mo_(2)C@CeO_(2) catalysts with a core-shell structure were successfully developed for robust microwave catalytic decomposition of H_(2)S at low temperatures.Two carbon precursors,para-phenylenediamine(Mo_(2)C-p)and meta-phenylenediamine(Mo_(2)C-m),were employed to tailor Mo_(2)C configurations.Remarkably,the H_(2)S conversion of Mo_(2)C-p@CeO_(2) catalyst at a low temperature of 550℃ is as high as 92.1%,which is much higher than the H_(2)S equilibrium conversion under the conventional thermal conditions(2.6% at 550℃).To our knowledge,this represents the most active catalyst for microwave catalytic decomposition of H_(2)S at low temperature of 550℃.Notably,Mo_(2)C-p demonstrated superior intrinsic activity(84%)compared to Mo_(2)C-m(6.4%),with XPS analysis revealing that its enhanced performance stems from a higher concentration of Mo_(2+)active sites.This work presents a substitute approach for the efficient utilization of H_(2)S waste gas and opens up a novel avenue for the rational design of microwave catalysts for microwave catalytic reaction at low-temperature.展开更多
Ag-based nanocatalysts exhibit good catalytic activity for the electrochemical reduction of organic halides. Ag-Ni alloy nanoparticles（NPs） were facilely prepared by chemical reduction, and the as-prepared nanocatal...Ag-based nanocatalysts exhibit good catalytic activity for the electrochemical reduction of organic halides. Ag-Ni alloy nanoparticles（NPs） were facilely prepared by chemical reduction, and the as-prepared nanocatalysts were characterized by X-ray diffraction, ultraviolet-visible spectroscopy, transmission electron microscopy and energy-dispersive X-ray spectroscopy. The electrocatalytic activity of Ag-Ni NPs for benzyl chloride reduction was studied in organic medium using cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy. The results show that the addition of Ni element can obviously decrease the size of Ag-Ni NPs, shift the reduction peak potential（φp） of benzyl chloride positively, and increase the catalytic activity of Ag-Ni NPs. However, when the Ni content reaches a certain value, the catalytic activity of Ag-Ni NPs decreases. Meanwhile, the synergistic catalytic effect of Ag-Ni NPs was also discussed.展开更多
The monodispersed Co nanoparticles were successfully prepared by means of hydrogen plasma method in inert atmosphere. The particle size, specific surface area, crystal structure and morphology of the samples were char...The monodispersed Co nanoparticles were successfully prepared by means of hydrogen plasma method in inert atmosphere. The particle size, specific surface area, crystal structure and morphology of the samples were characterized by transmission electron microscopy （TEM）, BET equation, X-ray diffraction （XRD）, and the corresponding selected area electron diffraction （SAED）. The catalytic effect of Co nanoparticles on the decomposition of ammonium perchlorate （AP） was investigated by differential thermal analyzer （DTA）. Compared with the thermal decomposition of pure AP, the addition of Co nanoparticles （2%-10%, by mass） decreases the decomposition temperature of AP by 145.01-155.72℃. Compared with Co3O4 nano-particles and microsized Co particles, the catalytic effect of Co nanoparticles for AP is stronger. Such effect is attributed to the large specific surface area and its interaction of Co with decomposition intermediate gases. The present work provides useful information for the application of Co nanoparficles in the AP-based propellant.展开更多
By transition metals （Fe, Ni, Mn, Co） and their alloys as catalysts during the diamond synthesis, some transition phases will be formed, such as FeaC type carbides and y solid solutions. Based on the empirical elect...By transition metals （Fe, Ni, Mn, Co） and their alloys as catalysts during the diamond synthesis, some transition phases will be formed, such as FeaC type carbides and y solid solutions. Based on the empirical electron theory of the solid and molecules, the valence electron structures of different kinds of carbides and y solid solutions and the relative electron density differences of various diamond/carbide and y solid solution/carbide interfaces were calculated and analyzed in this paper. The electron structure conditions of the ideal catalyst were presented by analyzing the different catalytic effects of the catalysts, which provide a new theoretical path to the optimal design of the catalyst composition展开更多
A new kinetic spectrophotometric method is developed for the measurement of manganese(Ⅱ) in water. The method is based on the catalytic effect of manganese(Ⅱ) with the oxidation of weak acid brilliant blue dye(RAWL)...A new kinetic spectrophotometric method is developed for the measurement of manganese(Ⅱ) in water. The method is based on the catalytic effect of manganese(Ⅱ) with the oxidation of weak acid brilliant blue dye(RAWL) by KIO4 using the Nitrilo triacetic acid(NTA) as an activation reagent. The optimum conditions obtained are 40 mgL-1 RAWL,1×10-4molL-1 KIO4,2×10-4 molL-1 Nitrilo triacetic acid(NTA),pH = 5.8,the reaction time of 3.00 min and the temperature of 20.0 ℃. Under the optimum conditions,the proposed method allows the measurement of manganese(Ⅱ) in a range of 0-50.0 ng mL-1 and with a detection limit of down to 0.158 ng mL-1. The recovery efficiency in measuring the standard manganese(Ⅱ) solution is in a range of 98.5%-102%,and the RSD is in a range of 0.76%-1.25%. The new method has been successfully applied to the measurement of manganese(Ⅱ) in both fresh water and seawater samples with satisfying results. Moreover,few cations and anions interfere with the measurement of manganese(Ⅱ). Compared with other kinetic catalytic methods and instrumental methods,the proposed method shows fairly good selectivity and sensitivity,low cost,cheapness,low detection limit and rapidity. It can be applied on boats easily.展开更多
Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-elec...Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.展开更多
As alkali additive,KC1 catalyzes effectively the carbothermic reduction of pre-oxidized ilmenite,and the catalytic effect becomes more remarkable as the amount of KC1 increases.During the carbothermic reduction,the ga...As alkali additive,KC1 catalyzes effectively the carbothermic reduction of pre-oxidized ilmenite,and the catalytic effect becomes more remarkable as the amount of KC1 increases.During the carbothermic reduction,the gaseous product consists mainly of CO,and the partial pressure of which increases with reaction temperature.The EPMA and XPS of the partially reduced ilmenite ore and that of the used graphite as reductant showed that the potassium ions enter both ilmenite particles and graphite powders during reduction.The above-mentioned phenomena result in the distortion of ilmenite and carbon structure by potassium ions and reaction activity of carbon and ilmenite was enhanced.As a result,the overall carbothermic reduction was catalyzed by KC1.展开更多
Catalysis and regeneration efficiency of granular activated carbon （GAC） and activated carbon fiber （ACF） were investigated in a non-equilibrium plasma water treatment reactor with a combination of pulsed streamer...Catalysis and regeneration efficiency of granular activated carbon （GAC） and activated carbon fiber （ACF） were investigated in a non-equilibrium plasma water treatment reactor with a combination of pulsed streamer discharge and GAC or ACF. The experimental results show that the degradation efficiency of methyl orange （MO） by the combined treatment can increase 22% （for GAC） and 24% （for ACF） respectively compared to pulsed discharge treatment alone, indicating that the combined treatment has a synergetic effect. The MO degradation efficiency by the combined treatment with pulsed discharge and saturated GAC or ACF can increase 12% and 17% respectively compared to pulsed discharge treatment alone. Both GAC and ACF show catalysis and the catalysis of ACF is prominent. Meanwhile, the regeneration of GAC and ACF are realized in this process. When H202 is introduced into the system, the utilization efficiency of ozone and ultraviolet light is improved and the regeneration efficiency of GAC and ACF is also increased.展开更多
A novel catalytic kinetic method is proposed for the determination of Se（Ⅳ）, Se（Ⅵ）, and total inorganic selenium in water based on the catalytic effect of Se（Ⅳ） on the reduction of Celestine blue by sodium su...A novel catalytic kinetic method is proposed for the determination of Se（Ⅳ）, Se（Ⅵ）, and total inorganic selenium in water based on the catalytic effect of Se（Ⅳ） on the reduction of Celestine blue by sodium sulfide at pH 7.0 phosphate buffer. The fixed-time method was adopted for the determination and speciation of inorganic selenium. Under the optimum conditions, the two calibration graphs are linear with a good correlation coefficient in the range 2-20 and 20-200 μg·L-1 of Se（Ⅳ） for the fixed-time method at 30℃. The experimental and theo- retical detection limits of the developed kinetic method were found to be 0.21 and 2.50 μg·L-1 for the fixed-time method （3 min）. All of the variables that affect the sensitivity at 645 nm were investigated, and the optimum conditions were established. The interference effect of various cations and anions on the Se（Ⅳ） determination was also studied. The selectivity of the selenium determination was greatly improved with the use of the strongly cation exchange resin such as Amberlite IR120 plus as long as chelating agents of thiourea and thiosulphate. The proposed kinetic method was validated statistically and through recovery studies in natural water samples. The relative standard deviations （RSDs） for ten replicate measurements of 2, 10, and 20 μg·L-1 of Se（Ⅳ） change between 0.35% and 5.58%, while the RSDs for ten replicate measurements of 3, 6, and 12 μg·L-1 of Se（Ⅵ） change between 0.49% and 1.61%. Analyses of a certified standard reference material （NIST SRM 1643e） for selenium using the fixed-time method showed that the proposed kinetic method has good accuracy. The Se（Ⅳ）, Se（Ⅵ）, and total inorganic selenium in lake and river water samples have been successfully determined by this method after selective reduction of Se（Ⅵ） to Se（Ⅳ）.展开更多
A novel photoenzyme-coupled artificial catalytic system is fabricated by immobilizing horseradish peroxidase(HRP)on the Bi_(2)WO_(6)hollow nanospheres via a facile electrostatic self-assembly process.The obtained Bi_(...A novel photoenzyme-coupled artificial catalytic system is fabricated by immobilizing horseradish peroxidase(HRP)on the Bi_(2)WO_(6)hollow nanospheres via a facile electrostatic self-assembly process.The obtained Bi_(2)WO_(6)/HRP sample not only improves the visible light harvest ability but also promotes the high-efficiency separation of charge carriers.More importantly,the photogenerated electrons and produced H2O2 on Bi_(2)WO_(6)directly take part in redox cycle reactions of HRP to induce photoenzyme synergic catalytic effect.In consequence,the degradation activity of Bi_(2)WO_(6)/HRP is significantly improved relative to Bi_(2)WO_(6)and HRP for removing bisphenol A(BPA)under the visible light irradiation.This work launches a feasible design strategy for exploiting photoenzyme-coupled artificial catalytic system with special structure to degrade organic pollutants in water efficiently.展开更多
A novel sensitive and relatively selective kinetic method is presented for the determination of V（V） based on its catalytic effect on the oxidation reaction of Celestine blue by potassium bromate in the presence of ...A novel sensitive and relatively selective kinetic method is presented for the determination of V（V） based on its catalytic effect on the oxidation reaction of Celestine blue by potassium bromate in the presence of citric acid as an activator. The reaction was monitored spectropho- tometrically by measuring the decrease in absorbance of Celestine blue at a maximum absorption wavelength of 540 nm between 0.5 and 9 min （the fixed-time method） in an H3PO4 medium at 45℃. The effect of various parameters such as concentrations of H3PO4, citric acid, potassium bromate and Celestine blue, ionic strength, reaction temperature and time on the rate of V（V） catalyzed reaction was studied. The method is free from the most interferences, especially from large amounts of V（IV）. The decrease in absorbance is proportional to the concentration of V（V） over the entire concentration range tested （0.025-1.25 lag.mL^-1） with a detection limit of 6.80 tag.L^-1 （according to statistical 3Sblank/k criterion） and a coefficient of variation （CV） of 1.78% （for ten replicate measurements at 95% confidence level）. The proposed method suffers from a few interferences such as Cr（VI） and Hg（Ⅱ） ions. The method was successfully applied to the determination of V（V） in river water, lake water, tap water, natural drinking water samples and a certified standard reference material such as SRM-1640 with satis- factory results. The vanadium contents of natural water samples were detected by using both linear calibration curve and standard addition curve methods. The recoveries of spiked vanadium （V） into the certified standard water sample were found to be quantitative, and the reproducibility was satisfactory. It was observed that the results of the SRM 1640 were in good agreement with the certified value.展开更多
A new kinetic spectrophotometric method has been developed for the determination of trace Ni （Ⅱ in natural water. The method is based on the catalytic effect of Ni （Ⅱ） on the oxidation of weak acid brilliant blue...A new kinetic spectrophotometric method has been developed for the determination of trace Ni （Ⅱ in natural water. The method is based on the catalytic effect of Ni （Ⅱ） on the oxidation of weak acid brilliant blue dye （RAWL） by KIO4 in acid medium. The concentration of nickel （Ⅱ） can be determined spectrophotometrically by measuring the decrease of absorbance of RAWL at λ = 626 nm using the fix-time method. The influencing factors are investigated by the orthogonal experimental design. The obtained optimum analytical conditions are： pH = 2.00, CRAWL = 5.00×10^-5 mol·L^-1, c KlO4 = 2.00× 10^-5 mol·L^-1, the reaction time t= 10min and the temperature T = 25 ℃. Under the optimum conditions, the developed method allows the measurement of Ni （Ⅱ） in a range of 0 - 40.0ngmL1. The standard deviation of eleven independent measurements of blank reaction is S = 3.08× 10^-3 and the limit of detection is 2.20ng·mL^-1. The relative standard deviations （RSDs） in six replicate determinations of 5 ngmL-1 and 8 ngmL1 Ni （Ⅱ） are 2.87% and 1.11%, respectively. Moreover, the experiments show few cations and anions can interfere with the measurement of Ni （Ⅱ）. The recovery efficiencies of this method are in a range of 97.0%-102.5% in freshwater samples. But there is a decreasing effect, which is about 0.2 times the added Ni （Ⅱ） in seawater medium. After reasonable calibration this processing method is used for the determination of Ni （Ⅱ） in seawater samples successfully. The results show this developed method has high accuracy and precision, high sensitivity, large range of linearity and high speed. The method can, therefore, be employed at room temperature.展开更多
A new kinetic spectrophotometric method has been developed for the determination of vanadium（V）.The method is based on the catalytic effect of vanadium（V）on the oxidation of weak acid brilliant blue dye（RAWL）by ...A new kinetic spectrophotometric method has been developed for the determination of vanadium（V）.The method is based on the catalytic effect of vanadium（V）on the oxidation of weak acid brilliant blue dye（RAWL）by KBrO3 using the citric acid as activation reagent.The obtained optimum conditions are：c（RAWL）= 1×10-4 molL-1,c（KBrO3）= 3×10-2 molL-1,c（citric acid）=9×10-3 molL-1,pH = 2.50,the reaction time being 7.0min and the temperature being 25.0℃.Under the optimum conditions,the proposed method allows the determination of vanadium（V）in the range of 0-70.0ng mL-1 and the detection limit is down to 0.407 ng mL-1.For standard vanadium（V）solution determination,the recovery efficiency is in the range of 98.5%-102% and the RSD ranges from 0.76%-1.25%.Moreover,it is demonstrated that most cations and anions do not interfere with the determination of vanadium（V）under the analytical condition.The new method was successfully applied in the determination of vanadium（V）in fresh water and seawater samples with satisfactory results.Vanadium（V）in the seawater samples from Qingdao offshore was determined using the method and the distribution of vanadium（V）was mapped.Compared with other instrumental analytical methods,the proposed method shows good selectivity,sensitivity,simplicity,lower cost and rapidity.It can be employed on shipboard easily.展开更多
Ni and carbon materials exhibit remarkable catalysis for the hydriding reaction of Mg.But the underlying mechanism of Ni/C hybrid catalysis is still unclear.In this work,density functional theory(DFT)calculation is ap...Ni and carbon materials exhibit remarkable catalysis for the hydriding reaction of Mg.But the underlying mechanism of Ni/C hybrid catalysis is still unclear.In this work,density functional theory(DFT)calculation is applied to investigate the effect of Ni/C co-incorporation on the hydriding reaction of Mg crystal.The morphology and crystal structure of the Ni/C co-incorporated Mg sample show that the coincorporated structure is credible.The transition state searching calculation suggests that both the incorporations of Ni and C are beneficial for the H_(2) dissociation.But Ni atom has a dramatic improvement for H_(2) dissociation and makes the H diffusion become limiting step of the hyriding reaction.The Ni dz_(2)orbit and H s orbit accept the electrons and combine together compactly,while the Ni d_(xy) orbit is half-occupied.The catalytic effect of Ni on H_(2) dissociation can be ascribed to the bridging effect of Ni d_(xy) orbit.The incorporation of C can weaken the over-strong interaction between Ni and H which hindered the H diffusion on Mg(0001).The Ni/C co-incorporated Mg(0001)shows the best performance during hyriding reaction compared with the clean and single incorporated Mg(0001).展开更多
Lithium-sulfur (Li-S) batteries are considered appealing power sources due to their high theoretical energy density (2600 Wh kg-1), low cost, and environmental friendliness. However, their widespread applicability is ...Lithium-sulfur (Li-S) batteries are considered appealing power sources due to their high theoretical energy density (2600 Wh kg-1), low cost, and environmental friendliness. However, their widespread applicability is restricted by two scientific problems: sluggish sulfur reaction kinetics and severe polysulfide shuttle effects. Multifarious strategies have been developed to overcome these two obstacles and achieve high sulfur utilization and capacity retention. Among these strategies, the introduction of catalytic materials into the Li-S battery system can greatly accelerate sulfur conversion and effectively inhibit the polysulfide shuttle effects. Herein, we have comprehensively reviewed the recent progress of catalytic engineering for polysulfide conversion in high-performance lithium-sulfur batteries. First, various catalytic materials serve as sulfur hosts, functionalized separators, and electrolyte additives;the mechanisms by which these materials promote the conversion of polysulfides in Li-S batteries have been systematically summarized. The relationship of structure, preparation, property, advantages, and limitations of these catalytic materials are comprehensively presented. Subsequently, the advanced characterization techniques of these catalytic processes are discussed, shedding light on the fundamental understanding of catalytic effects for improved electrochemical performance. Furthermore, future design tactics for high-performance Li-S batteries are discussed.展开更多
The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and ...The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and diethylene glycol dinitrate,has been investigated.Extensive characterization of the resulting energetic composites was carried out using scanning electron microscopy(SEM),X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),and differential scanning calorimetry(DSC).Isoconversional kinetic analysis was performed to determine the Arrhenius parameters associated with the thermolysis of the elaborated energetic formulations.It is found that TAG-M complexes have strong catalytic effect on the thermo-kinetic decomposition of NC/DEGDN by decreasing the apparent activation energy and significantly increased the total heat release.The models that govern the decomposition processes are also studied,and it is revealed that different reaction processes are accomplished by introduction metal complexes of triaminoguanidine.Overall,this study serves as a valuable reference for future research focused on the investigation of catalytic combustion features of solid propellants.展开更多
文摘The preparation method of H_4MoO_(26)-polyaniline film modified electrode and its voltammetric behaviour are described. The modified electrode has high electrocatalytic activity on chlorate ions.
基金supported by National Key R&D Program of China(2022YFB4002700)Shanghai Science and Technology Committee Rising-Star Program(22QA1403400)the Natural Science Foundation of Shanghai(21ZR1418700).
文摘Strong metal–support interaction(SMSI),namely the strong electronic and structural interaction between metal nanoparticles and supports,one of the most typical synergetic catalytic effects in composite catalysts,has been found critically important in the design of catalyst for thermocatalysis in the past.Recently,however,important and great progress of SMSI-based synergetic effects has been made in electrocatalysis,such as electrocatalyst design and electrocatalytic mechanism investigations.To better understand the nature of the synergetic effect assisting the further development of electrocatalysts,a comprehensive and in-depth overview highlighting and discussing the recent advances of SMSI in electrocatalysis is necessary and highly desirable but still absent.Herein,this review firstly presents various strategies of designing and constructing composite catalysts featuring SMSI.Further from the perspectives of electrocatalysis,the characterization techniques towards the electron structure,local interfacial and morphological features and active sites for SMSI-based electrocatalysts,have been summarized in detail.Importantly,the recent advances in the design of single-and bi-functional electrocatalysts featuring SMSI-based synergetic catalytic effects,and the key roles of SMSI during the electrocatalytic reactions are emphasized.Finally,the challenges and prospects are discussed to highlight the key remaining issues in the future development of SMSI-based electrocatalysts.
文摘Transforming industrial heritage will have internal economic and cultural effects and will also catalyse changes in surrounding urban areas.Transforming industrial heritage is therefore an essential part of strategies to regenerate decayed industrial districts.The aim of this study was to attempt to answer three questions.Can all transformed industrial heritage give catalytic effects?How should the potential for catalytic effects be assessed?What factors prevent catalytic effects?The Sanbao Street Industrial Heritage Historic District in Changzhou,China,was used as an example,and three effects catalysed by transforming industrial heritage were assessed.These were(1)reuse of industrial and non-industrial buildings in and near the historic district,(2)new construction in and near the historic district,and(3)revitalisation of the whole historic district.Failure of the catalytic effect caused by a lack of a conversion mechanism,failure to communicate the value of industrial heritage,and limited cultural industrial capacity was assessed.Formal transformation strategies focused on the connotative value of industrial heritage are proposed,and are expected to support future research and planning practices.
文摘The effects of peptides,amino acids and organic bases as an axial ligand on reaction ac- tivities in the electrocarboxylation of benzyl chloride with CO_2 catalyzed by CoTPP are reported. The imidazole organic base,peptide containing —SH and amino acid containing imidazolyl en- hance the catalytic activity.The effect of imidazole amounts on the catalytic activity of CoTPP is studied.
基金supported by the National Natural Science Foundation of China(22178295,21706225)Natural Science Foundation of Hunan Province(2025JJ50085)Hunan Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization.
文摘The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste gas but also recover clean energy H_(2),which has significant socio-economic and ecological advantages.However,the highly effective decomposition of H_(2)S at low temperatures is still a great challenge,because of the stringent thermodynamic equilibrium constraints(only 20% even at high temperature of 1010℃).Conventional microwave catalysts exhibit unsatisfactory performance at low temperatures(below 600℃).Herein,Mo_(2)C@CeO_(2) catalysts with a core-shell structure were successfully developed for robust microwave catalytic decomposition of H_(2)S at low temperatures.Two carbon precursors,para-phenylenediamine(Mo_(2)C-p)and meta-phenylenediamine(Mo_(2)C-m),were employed to tailor Mo_(2)C configurations.Remarkably,the H_(2)S conversion of Mo_(2)C-p@CeO_(2) catalyst at a low temperature of 550℃ is as high as 92.1%,which is much higher than the H_(2)S equilibrium conversion under the conventional thermal conditions(2.6% at 550℃).To our knowledge,this represents the most active catalyst for microwave catalytic decomposition of H_(2)S at low temperature of 550℃.Notably,Mo_(2)C-p demonstrated superior intrinsic activity(84%)compared to Mo_(2)C-m(6.4%),with XPS analysis revealing that its enhanced performance stems from a higher concentration of Mo_(2+)active sites.This work presents a substitute approach for the efficient utilization of H_(2)S waste gas and opens up a novel avenue for the rational design of microwave catalysts for microwave catalytic reaction at low-temperature.
基金Projects(2127106951238002+3 种基金J1210040J1103312)supported by the National Natural Science Foundation of ChinaProject(2013GK3015)supported by the Science and Technology Project of Hunan ProvinceChina
文摘Ag-based nanocatalysts exhibit good catalytic activity for the electrochemical reduction of organic halides. Ag-Ni alloy nanoparticles（NPs） were facilely prepared by chemical reduction, and the as-prepared nanocatalysts were characterized by X-ray diffraction, ultraviolet-visible spectroscopy, transmission electron microscopy and energy-dispersive X-ray spectroscopy. The electrocatalytic activity of Ag-Ni NPs for benzyl chloride reduction was studied in organic medium using cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy. The results show that the addition of Ni element can obviously decrease the size of Ag-Ni NPs, shift the reduction peak potential（φp） of benzyl chloride positively, and increase the catalytic activity of Ag-Ni NPs. However, when the Ni content reaches a certain value, the catalytic activity of Ag-Ni NPs decreases. Meanwhile, the synergistic catalytic effect of Ag-Ni NPs was also discussed.
基金Supported by the National Natural Science Foundation of China （50306008, 50602024）.
文摘The monodispersed Co nanoparticles were successfully prepared by means of hydrogen plasma method in inert atmosphere. The particle size, specific surface area, crystal structure and morphology of the samples were characterized by transmission electron microscopy （TEM）, BET equation, X-ray diffraction （XRD）, and the corresponding selected area electron diffraction （SAED）. The catalytic effect of Co nanoparticles on the decomposition of ammonium perchlorate （AP） was investigated by differential thermal analyzer （DTA）. Compared with the thermal decomposition of pure AP, the addition of Co nanoparticles （2%-10%, by mass） decreases the decomposition temperature of AP by 145.01-155.72℃. Compared with Co3O4 nano-particles and microsized Co particles, the catalytic effect of Co nanoparticles for AP is stronger. Such effect is attributed to the large specific surface area and its interaction of Co with decomposition intermediate gases. The present work provides useful information for the application of Co nanoparficles in the AP-based propellant.
基金financially supported by the Natural Science Foundation of Hebei Province(No.E2013402004)
文摘By transition metals （Fe, Ni, Mn, Co） and their alloys as catalysts during the diamond synthesis, some transition phases will be formed, such as FeaC type carbides and y solid solutions. Based on the empirical electron theory of the solid and molecules, the valence electron structures of different kinds of carbides and y solid solutions and the relative electron density differences of various diamond/carbide and y solid solution/carbide interfaces were calculated and analyzed in this paper. The electron structure conditions of the ideal catalyst were presented by analyzing the different catalytic effects of the catalysts, which provide a new theoretical path to the optimal design of the catalyst composition
文摘A new kinetic spectrophotometric method is developed for the measurement of manganese(Ⅱ) in water. The method is based on the catalytic effect of manganese(Ⅱ) with the oxidation of weak acid brilliant blue dye(RAWL) by KIO4 using the Nitrilo triacetic acid(NTA) as an activation reagent. The optimum conditions obtained are 40 mgL-1 RAWL,1×10-4molL-1 KIO4,2×10-4 molL-1 Nitrilo triacetic acid(NTA),pH = 5.8,the reaction time of 3.00 min and the temperature of 20.0 ℃. Under the optimum conditions,the proposed method allows the measurement of manganese(Ⅱ) in a range of 0-50.0 ng mL-1 and with a detection limit of down to 0.158 ng mL-1. The recovery efficiency in measuring the standard manganese(Ⅱ) solution is in a range of 98.5%-102%,and the RSD is in a range of 0.76%-1.25%. The new method has been successfully applied to the measurement of manganese(Ⅱ) in both fresh water and seawater samples with satisfying results. Moreover,few cations and anions interfere with the measurement of manganese(Ⅱ). Compared with other kinetic catalytic methods and instrumental methods,the proposed method shows fairly good selectivity and sensitivity,low cost,cheapness,low detection limit and rapidity. It can be applied on boats easily.
基金supported by the National Natural Science Foundation of China(52272194)Liaoning Revitalization Talents Program(XLYC2007155)。
文摘Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.
基金Item Sponsored by National Natural Science Foundation(59774026)
文摘As alkali additive,KC1 catalyzes effectively the carbothermic reduction of pre-oxidized ilmenite,and the catalytic effect becomes more remarkable as the amount of KC1 increases.During the carbothermic reduction,the gaseous product consists mainly of CO,and the partial pressure of which increases with reaction temperature.The EPMA and XPS of the partially reduced ilmenite ore and that of the used graphite as reductant showed that the potassium ions enter both ilmenite particles and graphite powders during reduction.The above-mentioned phenomena result in the distortion of ilmenite and carbon structure by potassium ions and reaction activity of carbon and ilmenite was enhanced.As a result,the overall carbothermic reduction was catalyzed by KC1.
基金National Natural Science Foundation of China(Nos.20576079,20776159)
文摘Catalysis and regeneration efficiency of granular activated carbon （GAC） and activated carbon fiber （ACF） were investigated in a non-equilibrium plasma water treatment reactor with a combination of pulsed streamer discharge and GAC or ACF. The experimental results show that the degradation efficiency of methyl orange （MO） by the combined treatment can increase 22% （for GAC） and 24% （for ACF） respectively compared to pulsed discharge treatment alone, indicating that the combined treatment has a synergetic effect. The MO degradation efficiency by the combined treatment with pulsed discharge and saturated GAC or ACF can increase 12% and 17% respectively compared to pulsed discharge treatment alone. Both GAC and ACF show catalysis and the catalysis of ACF is prominent. Meanwhile, the regeneration of GAC and ACF are realized in this process. When H202 is introduced into the system, the utilization efficiency of ozone and ultraviolet light is improved and the regeneration efficiency of GAC and ACF is also increased.
基金Cumhuriyet University Scientific Research Council (with F-225 code) for financial support of the present work
文摘A novel catalytic kinetic method is proposed for the determination of Se（Ⅳ）, Se（Ⅵ）, and total inorganic selenium in water based on the catalytic effect of Se（Ⅳ） on the reduction of Celestine blue by sodium sulfide at pH 7.0 phosphate buffer. The fixed-time method was adopted for the determination and speciation of inorganic selenium. Under the optimum conditions, the two calibration graphs are linear with a good correlation coefficient in the range 2-20 and 20-200 μg·L-1 of Se（Ⅳ） for the fixed-time method at 30℃. The experimental and theo- retical detection limits of the developed kinetic method were found to be 0.21 and 2.50 μg·L-1 for the fixed-time method （3 min）. All of the variables that affect the sensitivity at 645 nm were investigated, and the optimum conditions were established. The interference effect of various cations and anions on the Se（Ⅳ） determination was also studied. The selectivity of the selenium determination was greatly improved with the use of the strongly cation exchange resin such as Amberlite IR120 plus as long as chelating agents of thiourea and thiosulphate. The proposed kinetic method was validated statistically and through recovery studies in natural water samples. The relative standard deviations （RSDs） for ten replicate measurements of 2, 10, and 20 μg·L-1 of Se（Ⅳ） change between 0.35% and 5.58%, while the RSDs for ten replicate measurements of 3, 6, and 12 μg·L-1 of Se（Ⅵ） change between 0.49% and 1.61%. Analyses of a certified standard reference material （NIST SRM 1643e） for selenium using the fixed-time method showed that the proposed kinetic method has good accuracy. The Se（Ⅳ）, Se（Ⅵ）, and total inorganic selenium in lake and river water samples have been successfully determined by this method after selective reduction of Se（Ⅵ） to Se（Ⅳ）.
基金supported by the NSFC-Shanxi Coal Based Low Carbon Joint Fund(No.U1810117)the National Natural Science Foundation of China(No.52072153)+3 种基金the Natural Science Foundation of Jiangsu Province(No.BK20190867)the Open Project Program of Key Laboratory of Preparation and Application of Environmental Friendly Materials(Jilin Normal University)(No.2019009)the Open Project Program of Key Laboratory of Groundwater Resources and Environment(Jilin University),Ministry of Education(No.202005001KF)the Young Talent Cultivate Programme of Jiangsu University(No.4111310017)。
文摘A novel photoenzyme-coupled artificial catalytic system is fabricated by immobilizing horseradish peroxidase(HRP)on the Bi_(2)WO_(6)hollow nanospheres via a facile electrostatic self-assembly process.The obtained Bi_(2)WO_(6)/HRP sample not only improves the visible light harvest ability but also promotes the high-efficiency separation of charge carriers.More importantly,the photogenerated electrons and produced H2O2 on Bi_(2)WO_(6)directly take part in redox cycle reactions of HRP to induce photoenzyme synergic catalytic effect.In consequence,the degradation activity of Bi_(2)WO_(6)/HRP is significantly improved relative to Bi_(2)WO_(6)and HRP for removing bisphenol A(BPA)under the visible light irradiation.This work launches a feasible design strategy for exploiting photoenzyme-coupled artificial catalytic system with special structure to degrade organic pollutants in water efficiently.
文摘A novel sensitive and relatively selective kinetic method is presented for the determination of V（V） based on its catalytic effect on the oxidation reaction of Celestine blue by potassium bromate in the presence of citric acid as an activator. The reaction was monitored spectropho- tometrically by measuring the decrease in absorbance of Celestine blue at a maximum absorption wavelength of 540 nm between 0.5 and 9 min （the fixed-time method） in an H3PO4 medium at 45℃. The effect of various parameters such as concentrations of H3PO4, citric acid, potassium bromate and Celestine blue, ionic strength, reaction temperature and time on the rate of V（V） catalyzed reaction was studied. The method is free from the most interferences, especially from large amounts of V（IV）. The decrease in absorbance is proportional to the concentration of V（V） over the entire concentration range tested （0.025-1.25 lag.mL^-1） with a detection limit of 6.80 tag.L^-1 （according to statistical 3Sblank/k criterion） and a coefficient of variation （CV） of 1.78% （for ten replicate measurements at 95% confidence level）. The proposed method suffers from a few interferences such as Cr（VI） and Hg（Ⅱ） ions. The method was successfully applied to the determination of V（V） in river water, lake water, tap water, natural drinking water samples and a certified standard reference material such as SRM-1640 with satis- factory results. The vanadium contents of natural water samples were detected by using both linear calibration curve and standard addition curve methods. The recoveries of spiked vanadium （V） into the certified standard water sample were found to be quantitative, and the reproducibility was satisfactory. It was observed that the results of the SRM 1640 were in good agreement with the certified value.
文摘A new kinetic spectrophotometric method has been developed for the determination of trace Ni （Ⅱ in natural water. The method is based on the catalytic effect of Ni （Ⅱ） on the oxidation of weak acid brilliant blue dye （RAWL） by KIO4 in acid medium. The concentration of nickel （Ⅱ） can be determined spectrophotometrically by measuring the decrease of absorbance of RAWL at λ = 626 nm using the fix-time method. The influencing factors are investigated by the orthogonal experimental design. The obtained optimum analytical conditions are： pH = 2.00, CRAWL = 5.00×10^-5 mol·L^-1, c KlO4 = 2.00× 10^-5 mol·L^-1, the reaction time t= 10min and the temperature T = 25 ℃. Under the optimum conditions, the developed method allows the measurement of Ni （Ⅱ） in a range of 0 - 40.0ngmL1. The standard deviation of eleven independent measurements of blank reaction is S = 3.08× 10^-3 and the limit of detection is 2.20ng·mL^-1. The relative standard deviations （RSDs） in six replicate determinations of 5 ngmL-1 and 8 ngmL1 Ni （Ⅱ） are 2.87% and 1.11%, respectively. Moreover, the experiments show few cations and anions can interfere with the measurement of Ni （Ⅱ）. The recovery efficiencies of this method are in a range of 97.0%-102.5% in freshwater samples. But there is a decreasing effect, which is about 0.2 times the added Ni （Ⅱ） in seawater medium. After reasonable calibration this processing method is used for the determination of Ni （Ⅱ） in seawater samples successfully. The results show this developed method has high accuracy and precision, high sensitivity, large range of linearity and high speed. The method can, therefore, be employed at room temperature.
文摘A new kinetic spectrophotometric method has been developed for the determination of vanadium（V）.The method is based on the catalytic effect of vanadium（V）on the oxidation of weak acid brilliant blue dye（RAWL）by KBrO3 using the citric acid as activation reagent.The obtained optimum conditions are：c（RAWL）= 1×10-4 molL-1,c（KBrO3）= 3×10-2 molL-1,c（citric acid）=9×10-3 molL-1,pH = 2.50,the reaction time being 7.0min and the temperature being 25.0℃.Under the optimum conditions,the proposed method allows the determination of vanadium（V）in the range of 0-70.0ng mL-1 and the detection limit is down to 0.407 ng mL-1.For standard vanadium（V）solution determination,the recovery efficiency is in the range of 98.5%-102% and the RSD ranges from 0.76%-1.25%.Moreover,it is demonstrated that most cations and anions do not interfere with the determination of vanadium（V）under the analytical condition.The new method was successfully applied in the determination of vanadium（V）in fresh water and seawater samples with satisfactory results.Vanadium（V）in the seawater samples from Qingdao offshore was determined using the method and the distribution of vanadium（V）was mapped.Compared with other instrumental analytical methods,the proposed method shows good selectivity,sensitivity,simplicity,lower cost and rapidity.It can be employed on shipboard easily.
基金This work is supported by the National Key R&D Program of China(Grant No.2017YFB0103002)National Natural Science Foundation of China(Grant Nos.51771056,51371056,51701043 and 52071141)+4 种基金Equipment Preresearch Field Foundation(Grant No.6140721040101)Equipment Preresearch Sharing Technology(No.41421060201)Changzhou Leading Talents Project(Grant No.CQ20183020)333 Project in Jiangsu Province and the Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions,Fundamental Research Funds for the Central Universities(Grant No.2021MS051)Interdisciplinary Innovation Program of North China Electric Power University(grant number XM2112355).
文摘Ni and carbon materials exhibit remarkable catalysis for the hydriding reaction of Mg.But the underlying mechanism of Ni/C hybrid catalysis is still unclear.In this work,density functional theory(DFT)calculation is applied to investigate the effect of Ni/C co-incorporation on the hydriding reaction of Mg crystal.The morphology and crystal structure of the Ni/C co-incorporated Mg sample show that the coincorporated structure is credible.The transition state searching calculation suggests that both the incorporations of Ni and C are beneficial for the H_(2) dissociation.But Ni atom has a dramatic improvement for H_(2) dissociation and makes the H diffusion become limiting step of the hyriding reaction.The Ni dz_(2)orbit and H s orbit accept the electrons and combine together compactly,while the Ni d_(xy) orbit is half-occupied.The catalytic effect of Ni on H_(2) dissociation can be ascribed to the bridging effect of Ni d_(xy) orbit.The incorporation of C can weaken the over-strong interaction between Ni and H which hindered the H diffusion on Mg(0001).The Ni/C co-incorporated Mg(0001)shows the best performance during hyriding reaction compared with the clean and single incorporated Mg(0001).
基金financially supported by National Natural Science Foundation of China(Nos.52164030 and 22179055)Natural Science Foundation of Jiangxi Province(Nos.20202ACBL204007 and 20224BAB204004)Program of Qingjiang Excellent Young Talents of Jiangxi University of Science and Technology(No.JXUSTQJYX2019010).
文摘Lithium-sulfur (Li-S) batteries are considered appealing power sources due to their high theoretical energy density (2600 Wh kg-1), low cost, and environmental friendliness. However, their widespread applicability is restricted by two scientific problems: sluggish sulfur reaction kinetics and severe polysulfide shuttle effects. Multifarious strategies have been developed to overcome these two obstacles and achieve high sulfur utilization and capacity retention. Among these strategies, the introduction of catalytic materials into the Li-S battery system can greatly accelerate sulfur conversion and effectively inhibit the polysulfide shuttle effects. Herein, we have comprehensively reviewed the recent progress of catalytic engineering for polysulfide conversion in high-performance lithium-sulfur batteries. First, various catalytic materials serve as sulfur hosts, functionalized separators, and electrolyte additives;the mechanisms by which these materials promote the conversion of polysulfides in Li-S batteries have been systematically summarized. The relationship of structure, preparation, property, advantages, and limitations of these catalytic materials are comprehensively presented. Subsequently, the advanced characterization techniques of these catalytic processes are discussed, shedding light on the fundamental understanding of catalytic effects for improved electrochemical performance. Furthermore, future design tactics for high-performance Li-S batteries are discussed.
文摘The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and diethylene glycol dinitrate,has been investigated.Extensive characterization of the resulting energetic composites was carried out using scanning electron microscopy(SEM),X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),and differential scanning calorimetry(DSC).Isoconversional kinetic analysis was performed to determine the Arrhenius parameters associated with the thermolysis of the elaborated energetic formulations.It is found that TAG-M complexes have strong catalytic effect on the thermo-kinetic decomposition of NC/DEGDN by decreasing the apparent activation energy and significantly increased the total heat release.The models that govern the decomposition processes are also studied,and it is revealed that different reaction processes are accomplished by introduction metal complexes of triaminoguanidine.Overall,this study serves as a valuable reference for future research focused on the investigation of catalytic combustion features of solid propellants.
