This work proposed a strategy of indirectly inducing uniform microarc discharge by controlling the content and distribution ofβ-Mg_(17)Al_(12)phase in AZ91D Mg alloy.Two kinds of nano-particles(ZrO_(2)and TiO_(2))wer...This work proposed a strategy of indirectly inducing uniform microarc discharge by controlling the content and distribution ofβ-Mg_(17)Al_(12)phase in AZ91D Mg alloy.Two kinds of nano-particles(ZrO_(2)and TiO_(2))were designed to be added into the substrate of Mg alloy by friction stir processing(FSP).Then,Mg alloy sample designed with different precipitated morphology ofβ-Mg_(17)Al_(12)phase was treated by microarc oxidation(MAO)in Na_(3)PO_(4)/Na2SiO3electrolyte.The characteristics and performance of the MAO coating was analyzed using scanning electron microscopy(SEM),energy dispersive spectrometer(EDS),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),contact angle meter,and potentiodynamic polarization.It was found that the coarseα-Mg grains in extruded AZ91D Mg alloy were refined by FSP,and theβ-Mg_(17)Al_(12)phase with reticular structure was broken and dispersed.The nano-ZrO_(2)particles were pinned at the grain boundary by FSP,which refined theα-Mg grain and promoted the precipitation ofβ-Mg_(17)Al_(12)phase in grains.It effectively inhibited the“cascade”phenomenon of microarcs,which induced the uniform distribution of discharge pores.The MAO coating on Zr-FSP sample had good wettability and corrosion resistance.However,TiO_(2)particles were hardly detected in the coating on TiFSP sample.展开更多
Electroreduction of carbon dioxide(CO_(2)) into value-added chemicals offers an entrancing approach to main-taining the global carbon cycle and eliminating environmental threats.A key obstacle to achieving long-term a...Electroreduction of carbon dioxide(CO_(2)) into value-added chemicals offers an entrancing approach to main-taining the global carbon cycle and eliminating environmental threats.A key obstacle to achieving long-term and large-scale implementation of electrochemical CO_(2) reduction technology is the lack of active and selective cat-alysts.Copper(Cu)is one of the few candidates that can facilitate C–C coupling to obtain high-energy oxygenates and hydrocarbons beyond carbon monoxide(CO),but it suffers from poor selectivity for products of interest and high overpotentials.Alloying is an effective way to break the linear scaling relations and uniquely manipulate the reactivity and selectivity,which is hard to achieve by using monometallic compositions alone.By alloying Cu with other metals,one could change the catalytic properties of the catalyst by tuning the local electronic structure and modulating the adsorption strength of the reaction intermediates,thus improving the catalytic activity and selectivity.In this review,we focus on the recently developed Cu-based alloy catalysts(including conventional alloys,high-entropy alloys and single-atom alloys)that have been applied in electrocatalytic CO_(2) reduction(ECR).Theoretical calculations and experimental advances in understanding the key rate-limiting and selectivity-determining steps in those alloys are summarized,with a particular focus on identifying binding energy de-scriptors and the dynamic product formation mechanisms.In addition,we outline the opportunities and chal-lenges in the fundamental understanding of ECR by recommending advanced in-situ characterization techniques and standardized electrochemical methods and offer atomic-level design principles for steering the reaction pathways to the desired products.展开更多
CO_(2)地质利用与封存(CO_(2) geological utilization and storage,CGUS)是实现“碳中和”目标的重要技术手段,解决CGUS过程中的钢材腐蚀问题对于降低CGUS技术风险、实现CGUS技术规模化推广应用至关重要。综述了目前已经提出的CO_(2)...CO_(2)地质利用与封存(CO_(2) geological utilization and storage,CGUS)是实现“碳中和”目标的重要技术手段,解决CGUS过程中的钢材腐蚀问题对于降低CGUS技术风险、实现CGUS技术规模化推广应用至关重要。综述了目前已经提出的CO_(2)腐蚀钢材反应机制,总结了CO_(2)腐蚀钢材的主要影响因素,阐明了CO_(2)分压、温度、矿化度及pH值、CO_(2)封存环境中含有杂质、流体流动等因素对钢材腐蚀行为的影响,归纳了适用于CO_(2)腐蚀钢材防护的主要措施。基于此,提出了CGUS环境下钢材遭受CO_(2)腐蚀问题的重点研究方向。主要包括:CO_(2)腐蚀钢材反应机制的进一步探究;各项环境因素耦合作用影响CO_(2)腐蚀规律和腐蚀程度的量化研究;高浓度CO_(2)条件下腐蚀防护技术的开发与应用。展开更多
基金funded by China Postdoctoral Science Foundation(No.2021M700569)Chongqing Postdoctoral Science Foundation(No.7 cstc2021jcyj-bshX0087)。
文摘This work proposed a strategy of indirectly inducing uniform microarc discharge by controlling the content and distribution ofβ-Mg_(17)Al_(12)phase in AZ91D Mg alloy.Two kinds of nano-particles(ZrO_(2)and TiO_(2))were designed to be added into the substrate of Mg alloy by friction stir processing(FSP).Then,Mg alloy sample designed with different precipitated morphology ofβ-Mg_(17)Al_(12)phase was treated by microarc oxidation(MAO)in Na_(3)PO_(4)/Na2SiO3electrolyte.The characteristics and performance of the MAO coating was analyzed using scanning electron microscopy(SEM),energy dispersive spectrometer(EDS),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),contact angle meter,and potentiodynamic polarization.It was found that the coarseα-Mg grains in extruded AZ91D Mg alloy were refined by FSP,and theβ-Mg_(17)Al_(12)phase with reticular structure was broken and dispersed.The nano-ZrO_(2)particles were pinned at the grain boundary by FSP,which refined theα-Mg grain and promoted the precipitation ofβ-Mg_(17)Al_(12)phase in grains.It effectively inhibited the“cascade”phenomenon of microarcs,which induced the uniform distribution of discharge pores.The MAO coating on Zr-FSP sample had good wettability and corrosion resistance.However,TiO_(2)particles were hardly detected in the coating on TiFSP sample.
基金the National Natural Science Foundation of China(NSFC 22102018 and 52171201)the Natural Science Foundation of Sichuan Province(2022NSFSC0194)+6 种基金the Central Government Funds of Guiding Local Scientific and Technological Development for Sichuan Province(2021ZYD0043)the University of Electronic Science and Technology of China for Startup Funding(A1098531023601264)the Hefei National Research Center for Physical Sciences at the Micro-scale(KF2021005)the China Postdoctoral Science Foundation funded project(2022M710601)the University of Elec-tronic Science and Technology of China for Startup Funding(Y030212059003039)the NSFC(22005291 and 22278067)University of Electronic Science and Technology of China for Startup Funding(A1098531023601356).
文摘Electroreduction of carbon dioxide(CO_(2)) into value-added chemicals offers an entrancing approach to main-taining the global carbon cycle and eliminating environmental threats.A key obstacle to achieving long-term and large-scale implementation of electrochemical CO_(2) reduction technology is the lack of active and selective cat-alysts.Copper(Cu)is one of the few candidates that can facilitate C–C coupling to obtain high-energy oxygenates and hydrocarbons beyond carbon monoxide(CO),but it suffers from poor selectivity for products of interest and high overpotentials.Alloying is an effective way to break the linear scaling relations and uniquely manipulate the reactivity and selectivity,which is hard to achieve by using monometallic compositions alone.By alloying Cu with other metals,one could change the catalytic properties of the catalyst by tuning the local electronic structure and modulating the adsorption strength of the reaction intermediates,thus improving the catalytic activity and selectivity.In this review,we focus on the recently developed Cu-based alloy catalysts(including conventional alloys,high-entropy alloys and single-atom alloys)that have been applied in electrocatalytic CO_(2) reduction(ECR).Theoretical calculations and experimental advances in understanding the key rate-limiting and selectivity-determining steps in those alloys are summarized,with a particular focus on identifying binding energy de-scriptors and the dynamic product formation mechanisms.In addition,we outline the opportunities and chal-lenges in the fundamental understanding of ECR by recommending advanced in-situ characterization techniques and standardized electrochemical methods and offer atomic-level design principles for steering the reaction pathways to the desired products.
文摘CO_(2)地质利用与封存(CO_(2) geological utilization and storage,CGUS)是实现“碳中和”目标的重要技术手段,解决CGUS过程中的钢材腐蚀问题对于降低CGUS技术风险、实现CGUS技术规模化推广应用至关重要。综述了目前已经提出的CO_(2)腐蚀钢材反应机制,总结了CO_(2)腐蚀钢材的主要影响因素,阐明了CO_(2)分压、温度、矿化度及pH值、CO_(2)封存环境中含有杂质、流体流动等因素对钢材腐蚀行为的影响,归纳了适用于CO_(2)腐蚀钢材防护的主要措施。基于此,提出了CGUS环境下钢材遭受CO_(2)腐蚀问题的重点研究方向。主要包括:CO_(2)腐蚀钢材反应机制的进一步探究;各项环境因素耦合作用影响CO_(2)腐蚀规律和腐蚀程度的量化研究;高浓度CO_(2)条件下腐蚀防护技术的开发与应用。
