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
At present,there is limited research on the application of fuel cell power generation system technology using solid hydrogen storage materials,especially in hydrogen-assisted two-wheelers.Considering the disadvantages...At present,there is limited research on the application of fuel cell power generation system technology using solid hydrogen storage materials,especially in hydrogen-assisted two-wheelers.Considering the disadvantages of low hydrogen storage capacity and poor kinetics of hydrogen storage materials,our primary focus is to achieve smooth hydrogen ab-/desorption over a wide temperature range to meet the requirements of fuel cells and their integrated power generation systems.In this paper,the Ti_(0.9)Zr_(0.1)Mn_(1.45)V_(0.4)Fe_(0.15) hydrogen storage alloy was successfully prepared by arc melting.The maximum hydrogen storage capacity reaches 1.89 wt% at 318 K.The alloy has the capability to absorb 90% of hydrogen storage capacity within 50 s at 7 MPa and release 90% of hydrogen within 220 s.Comsol Multiphysics 6.0 software was used to simulate the hydrogen ab-/desorption processes of the tank.The flow rate of cooling water during hydrogen absorption varied in a gradient of(0.02 t x)m s^(-1)(x=0,0.02,0.04,0.06,0.08,0.1,0.12).Cooling water flow rate is positively correlated with the hydrogen absorption rate but negatively correlated with the cost.When the cooling rate is 0.06 m s^(-1),both simulation and experimentation have shown that the hydrogen storage tank is capable of steady hydrogen desorption for over 6 h at a flow rate of 2 L min^(-1).Based on the above conclusions,we have successfully developed a hydrogen-assisted two-wheeler with a range of 80 km and achieved regional demonstration operations in Changzhou and Shaoguan.This paper highlights the achievements of our team in the technological development of fuel cell power generation systems using solid hydrogen storage materials as hydrogen storage carriers and their application in twowheelers in recent years.展开更多
2A14-T62 butt joint was successfully welded by stationary shoulder friction stir welding(SSFSW)method.The results showed that using a pin with small shoulder could broaden the process window,and under a rotation speed...2A14-T62 butt joint was successfully welded by stationary shoulder friction stir welding(SSFSW)method.The results showed that using a pin with small shoulder could broaden the process window,and under a rotation speed of 2000 r/min and welding speed of 30 mm/min,joint with smooth surface,small reduction in thickness and little inner defects was obtained.The weld nugget zone was approx-imately circular,which was a unique morphology for SSFSW.The heat-affected zone(HAZ)and thermo-mechanically affected zone(TMAZ)were both quite narrow due to the lower heat input and slight mechanical action of the stationary shoulder.The fraction of high angle grain boundaries(HAGBs)exhibited a“W”shape along horizontal direction(from advancing side to retreating side),and the minim-um value located at HAZ.The average ultimate tensile strength and elongation of the joint were 325 MPa and 4.5%,respectively,with the joint efficiency of 68.3%.The joint was ductile fractured and the fracture surface contained two types of dimples morphology in different re-gions of the joint.Microhardness distribution in the joint exhibited a“W”shape,and the difference along the thickness direction was negli-gible.The joint had strong stress corrosion cracking susceptibility,and the slow stain rate tensile strength was 139 MPa.Microcrack and Al2O3 particulates were observed at the fracture surface.展开更多
The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high c...The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR.展开更多
The effect of Ce content(0–1.6 wt.%)on the modification of Mg_(2)Si phase in the as-cast Mg-5Al-2Si alloy was investigated.The original Chinese script type Mg_(2)Si phase was refined distinctly and transformed to dis...The effect of Ce content(0–1.6 wt.%)on the modification of Mg_(2)Si phase in the as-cast Mg-5Al-2Si alloy was investigated.The original Chinese script type Mg_(2)Si phase was refined distinctly and transformed to dispersive block shape gradually by adding Ce element.The length of Chinese script type Mg_(2)Si phase was reduced from 110 to 50μm with increasing Ce content to 1.6 wt.%.The results calculated by Pandat software indicated that the added Ce element first combined with Si to form CeSi_(2)phase,which could serve as the heterogeneous nucleation of Mg_(2)Si phase due to the small lattice mismatch of 7.97%.The modification of Mg_(2)Si phase was mainly attributed to the facts that Ce changed the growth steps of Mg_(2)Si phase and CeSi_(2)promoted the nucleation of Mg_(2)Si phase.With increasing Ce content from 0 wt.%to 1.6 wt.%,the YS,UTS and EL at 150℃were improved from 67.7 MPa,91.2 MPa and 1.6%to 84.2 MPa,128 MPa and 7.5%,respectively.展开更多
Various strategies,including controls of morphology,oxidation state,defect,and doping,have been developed to improve the performance of Cu-based catalysts for CO_(2) reduction reaction(CO_(2)RR),generating a large amo...Various strategies,including controls of morphology,oxidation state,defect,and doping,have been developed to improve the performance of Cu-based catalysts for CO_(2) reduction reaction(CO_(2)RR),generating a large amount of data.However,a unified understanding of underlying mechanism for further optimization is still lacking.In this work,combining first-principles calculations and machine learning(ML)techniques,we elucidate critical factors influencing the catalytic properties,taking Cu-based single atom alloys(SAAs)as examples.Our method relies on high-throughput calculations of 2669 CO adsorption configurations on 43 types of Cu-based SAAs with various surfaces.Extensive ML analyses reveal that low generalized coordination numbers and valence electron number are key features to determine catalytic performance.Applying our ML model with cross-group learning scheme,we demonstrate the model generalizes well between Cu-based SAAs with different alloying elements.Further,electronic structure calculations suggest surface negative center could enhance CO adsorption by back donating electrons to antibonding orbitals of CO.Finally,several SAAs,including PCu,AgCu,GaCu,ZnCu,SnCu,GeCu,InCu,and SiCu,are identified as promising CO_(2)RR catalysts.Our work provides a paradigm for the rational design and fast screening of SAAs for various electrocatalytic reactions.展开更多
The high activity of metallic magnesium and alloys limits its potential in biomedical applications;in recent years,extensive efforts have been devoted to modulating this reactivity.In this work,we present Mg(OH)_(2) a...The high activity of metallic magnesium and alloys limits its potential in biomedical applications;in recent years,extensive efforts have been devoted to modulating this reactivity.In this work,we present Mg(OH)_(2) and TiO_(2)barrier coatings to reduce the degradation of magnesium alloy(Mg-Ca-Zn)surfaces.These coatings were deposited by the anodization method and the spin-coating technique,respectively.The anodized layer was coated with TiO_(2)generated from the hydrolysis of 3%weight of TTIP(Ti[OCH(CH_(3))_(2)]_(4),Titanium(IV)isopropoxide)in 2-Propanol deposited by the spin-coating method.Studying the degradation in Ringer’s solution by electrochemical impedance spectroscopy and OCP revealed a 98%reduction in pittings in uncoated samples after 14 days of immersion.The p H measurements revealed that the TiO_(2)coating reduced the alkalization of the physiological environment,keeping the pH at 6.0 values.In vitro studies of two types of bacteria(E.coli and S.aureus)exhibited zones of inhibition in the agar and activity bactericidal(kill time test).The mechanisms behind the improved degradation resistance and enhanced antibacterial activity are presented and discussed here.Surface modification with Mg(OH)_(2)/TiO_(2)coatings is a promising strategy to control the biodegradation of magnesium implants for bone regeneration.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
The electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)into high-value-added chemicals and fuels is a promising strategy to mitigate global warming.However,it remains a significant stumbling block to the rat...The electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)into high-value-added chemicals and fuels is a promising strategy to mitigate global warming.However,it remains a significant stumbling block to the rationally tuning lattice plane of the catalyst with high activity to produce the target product in the eCO_(2)RR process.To attempt to solve this problem,the Culn bimetallic alloy nanocatalyst with specifically exposed lattice planes is modulated and electrodeposited on the nitrogen-doped porous carbon cloth by a simple two-step electrodeposition method,which induces high Faraday efficiency of 80%towards HCOO-(FEHCOO-)with a partial current density of 13.84 mA cm-2at-1.05 V(vs.RHE).Systematic characterizations and theoretical modeling reveal that the specific coexposed Culn(200)and In(101)lattice facets selectively adsorbed the key intermediate of OCHO*,reducing the overpotential of HCOOH and boosting the FEHCOO-in a wide potential window(-0.65--1.25 V).Moreover,a homogeneous distribution of Culn nanoparticles with an average diameter of merely~3.19 nm affords exposure to abundant active sites,meanwhile prohibiting detachment and agglomeration of nanoparticles during eCO_(2)RR for enhanced stability attributing to the self-assembly electrode strategy.This study highlights the synergistic effect between catalytic activity and facet effect,which opens a new route in surface engineering to tune their electrocatalytic performance.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financed by the National Key Research and Development Program of China[grants number 2022YFB3803800]the National Natural Science Foundation of China[grants number 52071141,52271212,52201250,51771056]Interdisciplinary Innovation Program of North China Electric Power University[grants number XM2112355].
文摘At present,there is limited research on the application of fuel cell power generation system technology using solid hydrogen storage materials,especially in hydrogen-assisted two-wheelers.Considering the disadvantages of low hydrogen storage capacity and poor kinetics of hydrogen storage materials,our primary focus is to achieve smooth hydrogen ab-/desorption over a wide temperature range to meet the requirements of fuel cells and their integrated power generation systems.In this paper,the Ti_(0.9)Zr_(0.1)Mn_(1.45)V_(0.4)Fe_(0.15) hydrogen storage alloy was successfully prepared by arc melting.The maximum hydrogen storage capacity reaches 1.89 wt% at 318 K.The alloy has the capability to absorb 90% of hydrogen storage capacity within 50 s at 7 MPa and release 90% of hydrogen within 220 s.Comsol Multiphysics 6.0 software was used to simulate the hydrogen ab-/desorption processes of the tank.The flow rate of cooling water during hydrogen absorption varied in a gradient of(0.02 t x)m s^(-1)(x=0,0.02,0.04,0.06,0.08,0.1,0.12).Cooling water flow rate is positively correlated with the hydrogen absorption rate but negatively correlated with the cost.When the cooling rate is 0.06 m s^(-1),both simulation and experimentation have shown that the hydrogen storage tank is capable of steady hydrogen desorption for over 6 h at a flow rate of 2 L min^(-1).Based on the above conclusions,we have successfully developed a hydrogen-assisted two-wheeler with a range of 80 km and achieved regional demonstration operations in Changzhou and Shaoguan.This paper highlights the achievements of our team in the technological development of fuel cell power generation systems using solid hydrogen storage materials as hydrogen storage carriers and their application in twowheelers in recent years.
基金supported by the Research and Development Project of“Jianbing”in Zhejiang Province(2024C01085)Natural Science and Foundation of Ningbo(2022J052).
文摘2A14-T62 butt joint was successfully welded by stationary shoulder friction stir welding(SSFSW)method.The results showed that using a pin with small shoulder could broaden the process window,and under a rotation speed of 2000 r/min and welding speed of 30 mm/min,joint with smooth surface,small reduction in thickness and little inner defects was obtained.The weld nugget zone was approx-imately circular,which was a unique morphology for SSFSW.The heat-affected zone(HAZ)and thermo-mechanically affected zone(TMAZ)were both quite narrow due to the lower heat input and slight mechanical action of the stationary shoulder.The fraction of high angle grain boundaries(HAGBs)exhibited a“W”shape along horizontal direction(from advancing side to retreating side),and the minim-um value located at HAZ.The average ultimate tensile strength and elongation of the joint were 325 MPa and 4.5%,respectively,with the joint efficiency of 68.3%.The joint was ductile fractured and the fracture surface contained two types of dimples morphology in different re-gions of the joint.Microhardness distribution in the joint exhibited a“W”shape,and the difference along the thickness direction was negli-gible.The joint had strong stress corrosion cracking susceptibility,and the slow stain rate tensile strength was 139 MPa.Microcrack and Al2O3 particulates were observed at the fracture surface.
基金supported by the National Natural Science Foundation of China (NSFC)(22075201)the National Key Research and Development Program of China (2022YFB4101800)。
文摘The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR.
基金supported by the Major Science and Technology projects in Qinghai province (2018-GX-A1)Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) of the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT & Future Planning (Grant No. 2013M3A6B1078874)+1 种基金funded by Shanghai Science and Technology Committee (Grant No. 18511109302)the National Natural Science Foundation of China (Grant No. 51825101)
文摘The effect of Ce content(0–1.6 wt.%)on the modification of Mg_(2)Si phase in the as-cast Mg-5Al-2Si alloy was investigated.The original Chinese script type Mg_(2)Si phase was refined distinctly and transformed to dispersive block shape gradually by adding Ce element.The length of Chinese script type Mg_(2)Si phase was reduced from 110 to 50μm with increasing Ce content to 1.6 wt.%.The results calculated by Pandat software indicated that the added Ce element first combined with Si to form CeSi_(2)phase,which could serve as the heterogeneous nucleation of Mg_(2)Si phase due to the small lattice mismatch of 7.97%.The modification of Mg_(2)Si phase was mainly attributed to the facts that Ce changed the growth steps of Mg_(2)Si phase and CeSi_(2)promoted the nucleation of Mg_(2)Si phase.With increasing Ce content from 0 wt.%to 1.6 wt.%,the YS,UTS and EL at 150℃were improved from 67.7 MPa,91.2 MPa and 1.6%to 84.2 MPa,128 MPa and 7.5%,respectively.
基金supported by the National Natural Science Foundation of China (Grant Nos.62006219 and 62001266)Guangdong Innovative and Entrepre-neurial Research Team Program (grant No.2017ZT07C341)+2 种基金the Bureau of Industry and Information Technology of Shenzhen for the 2017 Graphene Manufacturing Innovation Center Project (No.201901171523)the China Postdoctoral Science Foundation (No.2020M680506)Guangdong Basic and Applied Basic Research Foundation (No.2020A1515110338).
文摘Various strategies,including controls of morphology,oxidation state,defect,and doping,have been developed to improve the performance of Cu-based catalysts for CO_(2) reduction reaction(CO_(2)RR),generating a large amount of data.However,a unified understanding of underlying mechanism for further optimization is still lacking.In this work,combining first-principles calculations and machine learning(ML)techniques,we elucidate critical factors influencing the catalytic properties,taking Cu-based single atom alloys(SAAs)as examples.Our method relies on high-throughput calculations of 2669 CO adsorption configurations on 43 types of Cu-based SAAs with various surfaces.Extensive ML analyses reveal that low generalized coordination numbers and valence electron number are key features to determine catalytic performance.Applying our ML model with cross-group learning scheme,we demonstrate the model generalizes well between Cu-based SAAs with different alloying elements.Further,electronic structure calculations suggest surface negative center could enhance CO adsorption by back donating electrons to antibonding orbitals of CO.Finally,several SAAs,including PCu,AgCu,GaCu,ZnCu,SnCu,GeCu,InCu,and SiCu,are identified as promising CO_(2)RR catalysts.Our work provides a paradigm for the rational design and fast screening of SAAs for various electrocatalytic reactions.
基金financed by the FOMIX-Yucatán 2008-108160,CONACYT LAB-2009-01-123913,292692,294643,188345,and 204822 projectsthe financial support received from CONACYT。
文摘The high activity of metallic magnesium and alloys limits its potential in biomedical applications;in recent years,extensive efforts have been devoted to modulating this reactivity.In this work,we present Mg(OH)_(2) and TiO_(2)barrier coatings to reduce the degradation of magnesium alloy(Mg-Ca-Zn)surfaces.These coatings were deposited by the anodization method and the spin-coating technique,respectively.The anodized layer was coated with TiO_(2)generated from the hydrolysis of 3%weight of TTIP(Ti[OCH(CH_(3))_(2)]_(4),Titanium(IV)isopropoxide)in 2-Propanol deposited by the spin-coating method.Studying the degradation in Ringer’s solution by electrochemical impedance spectroscopy and OCP revealed a 98%reduction in pittings in uncoated samples after 14 days of immersion.The p H measurements revealed that the TiO_(2)coating reduced the alkalization of the physiological environment,keeping the pH at 6.0 values.In vitro studies of two types of bacteria(E.coli and S.aureus)exhibited zones of inhibition in the agar and activity bactericidal(kill time test).The mechanisms behind the improved degradation resistance and enhanced antibacterial activity are presented and discussed here.Surface modification with Mg(OH)_(2)/TiO_(2)coatings is a promising strategy to control the biodegradation of magnesium implants for bone regeneration.
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。
基金supported by the“Scientific and Technical Innovation Action Plan”Basic Research Field of Shanghai Science and Technology Committee(19JC1410500)financial support from the National Natural Science Foundation of China(91645110)。
文摘The electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)into high-value-added chemicals and fuels is a promising strategy to mitigate global warming.However,it remains a significant stumbling block to the rationally tuning lattice plane of the catalyst with high activity to produce the target product in the eCO_(2)RR process.To attempt to solve this problem,the Culn bimetallic alloy nanocatalyst with specifically exposed lattice planes is modulated and electrodeposited on the nitrogen-doped porous carbon cloth by a simple two-step electrodeposition method,which induces high Faraday efficiency of 80%towards HCOO-(FEHCOO-)with a partial current density of 13.84 mA cm-2at-1.05 V(vs.RHE).Systematic characterizations and theoretical modeling reveal that the specific coexposed Culn(200)and In(101)lattice facets selectively adsorbed the key intermediate of OCHO*,reducing the overpotential of HCOOH and boosting the FEHCOO-in a wide potential window(-0.65--1.25 V).Moreover,a homogeneous distribution of Culn nanoparticles with an average diameter of merely~3.19 nm affords exposure to abundant active sites,meanwhile prohibiting detachment and agglomeration of nanoparticles during eCO_(2)RR for enhanced stability attributing to the self-assembly electrode strategy.This study highlights the synergistic effect between catalytic activity and facet effect,which opens a new route in surface engineering to tune their electrocatalytic performance.