The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic ...The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.展开更多
The~790 ka Australasian(micro)tektite strewn field is one of the most recent and best-known examples of impact ejecta emplacement as the result of a large-scale cratering event across a considerable part of Earth'...The~790 ka Australasian(micro)tektite strewn field is one of the most recent and best-known examples of impact ejecta emplacement as the result of a large-scale cratering event across a considerable part of Earth's surface(>10%in area).The Australasian strewn field is characterized by a tri-lobe pattern consisting of a large central distribution lobe,and two smaller side lobes extending to the west and east.Here,we report on the discovery of microtektite-like particles in sedimentary traps,containing abundant micrometeorite material,in the Sør Rondane Mountain(SRM)range of East Antarctica.The thirty-three glassy particles display a characteristic pale yellowcolor and are predominantly spherical in shape,except for a single dumbbell-shaped particle.The vitreous spherules range in size from220 to 570μm,with an average diameter of~370μm.This compares relatively well with the size distribution(75–778μm)of Australasian microtektites previously recovered from the TransantarcticMountains(TAM)and located ca.2500–3000 km fromthe SRM.In addition,the chemical composition of the SRM particles exhibits limited variation and is nearly identical to the‘normal-type’(i.e.,<6%MgO)TAM microtektites.The Sr and Nd isotope systematics for a single batch of SRM particles(n=26)strongly support their affiliation with TAMmicrotektites and the Australasian tektite strewn field in general.Furthermore,Sr isotope ratios and Nd model ages suggest that the target material of the SRM particles was composed of a plagioclase-or carbonate-rich lithology derived from a Paleo-or Mesoproterozoic crustal unit.The affiliation to the Australasian strewn field requires long-range transportation,with estimated great circle distances of ca.11,600 km from the hypothetical source crater,provided transportation occurred along the central distribution lobe.This is in agreement with the observations made for the Australasian microtektites recovered from Victoria Land(ca.11,000 km)and Larkman Nunatak(ca.12,000 km),which,on average,decrease in size and alkali concentrations(e.g.,Na and K)as their distance from the source crater increases.The values for the SRMparticles are intermediate to those of the Victoria Land and Larkman Nunatak microtektites for both parameters,thus supporting this observation.We therefore interpret the SRM particles as‘normal-type’Australasian microtektites,which significantly extend the central distribution lobe of the Australasian strewn field westward.Australasian microtektite distribution thus occurred on a continent-wide scale across Antarctica and allows for the identification of new,potential recovery sites on the Antarctic continent as well as the southeastern part of the Indian Ocean.Similar to volcanic ash layers,the~790 ka distal Australasian impact ejecta are thus a record of an instantaneous event that can be used for time-stratigraphic correlation across Antarctica.展开更多
This study investigated the deterioration of a lubricant-infused anodic aluminium oxide surface in a 1M NaCl solution for~200 days.Direct observation by cryo-SEM and quantitative analyses by UV spectroscopy and EIS re...This study investigated the deterioration of a lubricant-infused anodic aluminium oxide surface in a 1M NaCl solution for~200 days.Direct observation by cryo-SEM and quantitative analyses by UV spectroscopy and EIS revealed that the long-term deterioration of the lubricant-infused surface was divided into two stages:the surface-adhered lubricant layer gradually dissolved at a constant rate until the substrate was exposed;afterwards the lubricant infused in the nanochannels began to diffuse and was depleted after~200 days.The EIS results also revealed that the defects reduced the corrosion resistance of the lubricant-infused surface considerably.展开更多
For more than six decades, chromic acid anodizing （CAA） has been the central process in the surface pre-treatment of aluminum for adhesively bonded aircraft structures. Unfortunately, this electrolyte contains hexav...For more than six decades, chromic acid anodizing （CAA） has been the central process in the surface pre-treatment of aluminum for adhesively bonded aircraft structures. Unfortunately, this electrolyte contains hexavalent chromium （Cr（VI））, a compound known for its toxicity and carcinogenic properties. To comply with the new strict international regulations, the Cr（VI）-era will soon have to come to an end. Anodizing aluminum in acid electrolytes produces a self-ordered porous oxide layer. Although different acids can be used to create this type of structure, the excellent adhesion and corrosion resistance that is currently achieved by the complete Cr（VI）-based process is not easily matched. This paper provides a critical overview and appraisal of proposed alternatives to CAA, including combinations of multiple anodizing steps, pre- and post anodizing treatments. The work is presented in terms of the modifications to the oxide properties, such as morphological features （e.g., pore size, barrier layer thickness） and surface chemistry, in order to evaluate the link between fundamental principles of adhesion and bond performance.展开更多
Atmospheric corrosion of metals is the most common type of corrosion which has a significant impact on the environment and operational safety in various situations of everyday life.Some of the common examples can be o...Atmospheric corrosion of metals is the most common type of corrosion which has a significant impact on the environment and operational safety in various situations of everyday life.Some of the common examples can be observed in land,water and air transportation systems,electronic circuit boards,urban and offshore infrastructures.The dew drops formed on metal surface due to condensation of atmospheric moisture facilitates corrosion as an electrolyte.The corrosion mechanisms under these droplets are different from classically known bulk electrolyte corrosion.Due to thin and non-uniform geometric thickness of the droplet electrolyte,the atmospheric oxygen requires a shorter diffusion path to reach the metal surface.The corrosion under a droplet is driven by the depletion of oxygen in the center of the droplet compared to the edge,known as differential aeration.In case of a larger droplet,differential aeration leads to preferential cathodic activity at the edge and is controlled by the droplet geometry.Whereas,for a smaller droplet,the oxygen concentration remains uniform and hence cathodic activity is not controlled by droplet geometry.The geometry of condensed droplets varies dynamically with changing environmental parameters,influencing corrosion mechanisms as the droplets evolve in size.In this review,various modelling approaches used to simulate the corrosion under droplet electrolytes are presented.In the efforts of developing a comprehensive model to estimate corrosion rates,it has been noted from this review that the influence of geometric evolution of the droplet due to condensation/evaporation processes on corrosion mechanisms are yet to be modelled.Dynamically varying external factors like environmental temperature,relative humidity,presence of hygroscopic salts and pollutants influence the evolution of droplet electrolyte,making it a complex phenomenon to investigate.Therefore,an overview of available dropwise condensation and evaporation models which describes the formation and the evolution of droplet geometry are also presented from an atmo s pheric corrosion viewpoint.展开更多
This work investigated the chemical and electrochemical mechanisms of localised corrosion triggered by CaS·xMgO·y Al_(2)O_(3)·TiN complex inclusions in high strength low alloy steel(HSLAS)under a simula...This work investigated the chemical and electrochemical mechanisms of localised corrosion triggered by CaS·xMgO·y Al_(2)O_(3)·TiN complex inclusions in high strength low alloy steel(HSLAS)under a simulated marine environment.Special focus was given to the role of the TiN portion of the inclusion on the initiation and growth of the corrosion pits.The thermodynamic process of pitting initiation was investigated by Gibbs free energy,Pourbaix diagram and first principle calculation.Localised corrosion is mainly induced by inclusions and triggered by dissolution of adjacent distorted matrix.Chemical dissolution of CaS portion in CaS·xMgO·y Al_(2)O_(3)·TiN complex inclusion creates an acidic aggressive environment that accelerates the further dissolution of inclusion and matrix.Galvanic coupling effect between TiN inclusion and matrix is directly verified.TiN covered with a TiOfilm acts as the cathodic phase in galvanic corrosion,although it has a lower Volta potential than the matrix.This is an unusual correlation with the scanning Kelvin probe force microscopy result,which has been explained for this special system.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIP)(NRF,2021R1C1C1013953,2022K1A4A7A04094394,2022K1A4A7A04095890)。
文摘The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.
基金the Research Foundation Flanders (FWO)for funding this PhD research to BSthe support by the Belgian Science Policy (BELSPO) through BELAM,Amundsen and BAMM projects+2 种基金the Research Foundation-Flanders (FWO–Vlaanderen) and the VUB strategic researchthe support from the FWO–FNRS “Excellence of Science (EoS)” project ET–Ho ME (ID30442502)the FRS–FNRS for support.
文摘The~790 ka Australasian(micro)tektite strewn field is one of the most recent and best-known examples of impact ejecta emplacement as the result of a large-scale cratering event across a considerable part of Earth's surface(>10%in area).The Australasian strewn field is characterized by a tri-lobe pattern consisting of a large central distribution lobe,and two smaller side lobes extending to the west and east.Here,we report on the discovery of microtektite-like particles in sedimentary traps,containing abundant micrometeorite material,in the Sør Rondane Mountain(SRM)range of East Antarctica.The thirty-three glassy particles display a characteristic pale yellowcolor and are predominantly spherical in shape,except for a single dumbbell-shaped particle.The vitreous spherules range in size from220 to 570μm,with an average diameter of~370μm.This compares relatively well with the size distribution(75–778μm)of Australasian microtektites previously recovered from the TransantarcticMountains(TAM)and located ca.2500–3000 km fromthe SRM.In addition,the chemical composition of the SRM particles exhibits limited variation and is nearly identical to the‘normal-type’(i.e.,<6%MgO)TAM microtektites.The Sr and Nd isotope systematics for a single batch of SRM particles(n=26)strongly support their affiliation with TAMmicrotektites and the Australasian tektite strewn field in general.Furthermore,Sr isotope ratios and Nd model ages suggest that the target material of the SRM particles was composed of a plagioclase-or carbonate-rich lithology derived from a Paleo-or Mesoproterozoic crustal unit.The affiliation to the Australasian strewn field requires long-range transportation,with estimated great circle distances of ca.11,600 km from the hypothetical source crater,provided transportation occurred along the central distribution lobe.This is in agreement with the observations made for the Australasian microtektites recovered from Victoria Land(ca.11,000 km)and Larkman Nunatak(ca.12,000 km),which,on average,decrease in size and alkali concentrations(e.g.,Na and K)as their distance from the source crater increases.The values for the SRMparticles are intermediate to those of the Victoria Land and Larkman Nunatak microtektites for both parameters,thus supporting this observation.We therefore interpret the SRM particles as‘normal-type’Australasian microtektites,which significantly extend the central distribution lobe of the Australasian strewn field westward.Australasian microtektite distribution thus occurred on a continent-wide scale across Antarctica and allows for the identification of new,potential recovery sites on the Antarctic continent as well as the southeastern part of the Indian Ocean.Similar to volcanic ash layers,the~790 ka distal Australasian impact ejecta are thus a record of an instantaneous event that can be used for time-stratigraphic correlation across Antarctica.
基金supported by the National Key Research and Development Program of China(No.2016YFE0203600)the National Natural Science Foundation of China(No.51771029)+1 种基金the Beijing Nova Program(Z171100001117076)the 111 Project(B17003)。
文摘This study investigated the deterioration of a lubricant-infused anodic aluminium oxide surface in a 1M NaCl solution for~200 days.Direct observation by cryo-SEM and quantitative analyses by UV spectroscopy and EIS revealed that the long-term deterioration of the lubricant-infused surface was divided into two stages:the surface-adhered lubricant layer gradually dissolved at a constant rate until the substrate was exposed;afterwards the lubricant infused in the nanochannels began to diffuse and was depleted after~200 days.The EIS results also revealed that the defects reduced the corrosion resistance of the lubricant-infused surface considerably.
文摘For more than six decades, chromic acid anodizing （CAA） has been the central process in the surface pre-treatment of aluminum for adhesively bonded aircraft structures. Unfortunately, this electrolyte contains hexavalent chromium （Cr（VI））, a compound known for its toxicity and carcinogenic properties. To comply with the new strict international regulations, the Cr（VI）-era will soon have to come to an end. Anodizing aluminum in acid electrolytes produces a self-ordered porous oxide layer. Although different acids can be used to create this type of structure, the excellent adhesion and corrosion resistance that is currently achieved by the complete Cr（VI）-based process is not easily matched. This paper provides a critical overview and appraisal of proposed alternatives to CAA, including combinations of multiple anodizing steps, pre- and post anodizing treatments. The work is presented in terms of the modifications to the oxide properties, such as morphological features （e.g., pore size, barrier layer thickness） and surface chemistry, in order to evaluate the link between fundamental principles of adhesion and bond performance.
基金financially supported by the European Union’s Horizon 2020 Research and Innovation Programme under the Marie Sklodowska-Curie grant agreement(No.764977)。
文摘Atmospheric corrosion of metals is the most common type of corrosion which has a significant impact on the environment and operational safety in various situations of everyday life.Some of the common examples can be observed in land,water and air transportation systems,electronic circuit boards,urban and offshore infrastructures.The dew drops formed on metal surface due to condensation of atmospheric moisture facilitates corrosion as an electrolyte.The corrosion mechanisms under these droplets are different from classically known bulk electrolyte corrosion.Due to thin and non-uniform geometric thickness of the droplet electrolyte,the atmospheric oxygen requires a shorter diffusion path to reach the metal surface.The corrosion under a droplet is driven by the depletion of oxygen in the center of the droplet compared to the edge,known as differential aeration.In case of a larger droplet,differential aeration leads to preferential cathodic activity at the edge and is controlled by the droplet geometry.Whereas,for a smaller droplet,the oxygen concentration remains uniform and hence cathodic activity is not controlled by droplet geometry.The geometry of condensed droplets varies dynamically with changing environmental parameters,influencing corrosion mechanisms as the droplets evolve in size.In this review,various modelling approaches used to simulate the corrosion under droplet electrolytes are presented.In the efforts of developing a comprehensive model to estimate corrosion rates,it has been noted from this review that the influence of geometric evolution of the droplet due to condensation/evaporation processes on corrosion mechanisms are yet to be modelled.Dynamically varying external factors like environmental temperature,relative humidity,presence of hygroscopic salts and pollutants influence the evolution of droplet electrolyte,making it a complex phenomenon to investigate.Therefore,an overview of available dropwise condensation and evaporation models which describes the formation and the evolution of droplet geometry are also presented from an atmo s pheric corrosion viewpoint.
基金the National Natural Science Foundation of China(Nos.51871024,51822401 and 52104319)the National Science and Technology Resources Investigation Program of China(No.2019FY101400)。
文摘This work investigated the chemical and electrochemical mechanisms of localised corrosion triggered by CaS·xMgO·y Al_(2)O_(3)·TiN complex inclusions in high strength low alloy steel(HSLAS)under a simulated marine environment.Special focus was given to the role of the TiN portion of the inclusion on the initiation and growth of the corrosion pits.The thermodynamic process of pitting initiation was investigated by Gibbs free energy,Pourbaix diagram and first principle calculation.Localised corrosion is mainly induced by inclusions and triggered by dissolution of adjacent distorted matrix.Chemical dissolution of CaS portion in CaS·xMgO·y Al_(2)O_(3)·TiN complex inclusion creates an acidic aggressive environment that accelerates the further dissolution of inclusion and matrix.Galvanic coupling effect between TiN inclusion and matrix is directly verified.TiN covered with a TiOfilm acts as the cathodic phase in galvanic corrosion,although it has a lower Volta potential than the matrix.This is an unusual correlation with the scanning Kelvin probe force microscopy result,which has been explained for this special system.
