Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sust...Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sustainable development.Despite significant progress in various electrochemical systems,the regulatory mechanisms of PDE in energy and mass transfer and the lifespan extension of electrolysis systems,particularly in water electrolysis(WE)for hydrogen production,remain insufficiently explored.Therefore,there is an urgent need for a deeper understanding of the unique contributions of PDE in mass transfer enhancement,microenvironment regulation,and hydrogen production optimization,aiming to achieve low-energy consumption,high catalytic activity,and long-term stability in the generation of target products.Here,this review critically examines the microenvironmental effects of PDE on energy and mass transfer,the electrode degradation mechanisms in the lifespan extension of electrolysis systems,and the key factors in enhancing WE for hydrogen production,providing a comprehensive summary of current research progress.The review focuses on the complex regulatory mechanisms of frequency,duty cycle,amplitude,and other factors in hydrogen evolution reaction(HER)performance within PDE strategies,revealing the interrelationships among them.Finally,the potential future directions and challenges for transitioning from laboratory studies to industrial applications are proposed.展开更多
Ion-solvaing membranes(ISMs)have received extensive attention in recent years as a key component in electrochemical energy conversion and storage devices.This article provides an overview of structural composition,per...Ion-solvaing membranes(ISMs)have received extensive attention in recent years as a key component in electrochemical energy conversion and storage devices.This article provides an overview of structural composition,performance advan-tages,research progress,ion conduction mechanism and existing issues of ISMs,primarily classifying them according to the matrix structure.A detailed analysis of performance enhancement methods,key performance indicators of ISMs and performance influencing factors is also presented.The article contributes to further optimizing the design and application of ion-solvation membranes,providing theoretical support for the development of fields such as hydrogen production through electrolysis of water and electrochemical energy in the future.展开更多
Alkaline water electrolysis(AWE)represents a promising approach for green hydrogen production,yet the development of high-performance separators with gas impermeability,high ion conductivity,and stability under alkali...Alkaline water electrolysis(AWE)represents a promising approach for green hydrogen production,yet the development of high-performance separators with gas impermeability,high ion conductivity,and stability under alkaline operating conditions has proven challenging.To address this challenge,we develop a pre-concentration regulated phase separation strategy for scalable fabrication of asymmetric hierarchical porous membranes(AHPMs)for AWE.The resulting AHPMs demonstrate a hierarchical structure composed of an ultrathin dense skin layer and highly interconnected porous support.Benefitting from the structural advantages,the AHPMs exhibit outstanding characteristics,including a high bubble point pressure up to 12.4 bar,extremely low area resistance of 0.03Ωcm^(2) in 30 wt%KOH at 80℃,and excellent hydrophilicity and long-term alkaline stability.When applied in AWE with commercial catalysts,the AHPMs achieved an impressive current density of 1.9 A cm^(-2) at 2.0 V in 30 wt%KOH and the anodic hydrogen contents(AHCs)below 0.5 vol.%at a low current density of 0.1 A cm^(-2),differential pressure of 2 bar,and temperature of 80℃.Moreover,AHPMs demonstrate exceptional stability over 2,400 h of continuous operation and maintain superior performance in a 1 Nm^(3) h^(-1) industrialscale electrolyzer stack.This work advances the development of efficient separators for highperformance AWE systems,contributing to the advancement of hydrogen technologies in sustainable energy applications.展开更多
Seawater electrolysis is an appealing route toward sustainable hydrogen production,yet its practical deployment is hindered by severe chloride-induced corrosion and parasitic chlorine oxidation.Here,we report noble me...Seawater electrolysis is an appealing route toward sustainable hydrogen production,yet its practical deployment is hindered by severe chloride-induced corrosion and parasitic chlorine oxidation.Here,we report noble metal-doped NiV layered double hydroxides(LDHs)that integrate electronic modulation with a dual chloride confinement mechanism.Ir incorporation simultaneously establishes strong Ir-Cl coordination and dynamically regenerated VO_(4)^(3-)layers,producing an adaptive electrostatic shield that effectively suppresses chloride penetration.As a result,Ir-NiV LDH delivers nearly 100%oxygen evolution reaction selectivity and outstanding stability over2750 h at 500 mA cm^(-2).Meanwhile,Ru doping optimizes the hydrogen evolution pathway,enabling a low overpotential of 195 mV and>2350 h durability.When paired in a twso-electrode electrolyzer,the Ru-NiVLDH‖Ir-NiVLDH system exhibits industrial-level performance and unprecedented robustness in alkaline seawater.This dual chloride confinement concept provides a general framework for catalyst design in corrosive ionic environments,extending beyond seawater splitting toward other electrochemical energy conversion processes.展开更多
Seawater electrolysis has been explored as a viable and sustainable method for green hydrogen production in regions characterized by freshwater scarcity but abundant renewable energy resources.However,the high concent...Seawater electrolysis has been explored as a viable and sustainable method for green hydrogen production in regions characterized by freshwater scarcity but abundant renewable energy resources.However,the high concentration of chlorine ions(Cl^(-))in seawater leads to severe corrosion of metallic electrodes,which significantly challenges the stability of electrode catalysts in seawater electrolysis.Owing to the Cl^(-)corrosion and the competitive oxygen/chlorine evolution reactions,the design of durable and active anode catalysts is key to achieving practical seawater electrolysis.To address this challenge,this review systematically analyzes the chlorine-induced corrosion mechanisms of anode catalysts,evaluates various anticorrosion strategies,and explores future prospects for enhancing anode durability.Three mainstream anticorrosion strategies are summarized and assessed for their effectiveness in mitigating the chlorineinduced damage to anode catalysts:the physical surface coatings,electrostatic repulsion,and Cl^(-)adsorption regulation.In addition,some emerging strategies are further introduced to highlight the future trends of state-of-the-art techniques for seawater electrolysis.This review aims to provide novel insights and practical guidance for developing more stable and efficient anode catalysts for hydrogen production via seawater electrolvsis.展开更多
The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-ass...The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-assembly method is used to fabricate controllable MOF-on-MOF multiscale heterostructures,where triangular host MOF(ZIF-67)nanosheets undergo in situ epitaxial growth to form uniform orthogonal vip MOF(CoFe PBA)nanosheets.Phosphorus(P)is further introduced in situ to fabricate CoP and Fe_(2)P heterostructured nanosheets(CoFe-P-NS),which exhibit excellent bifunctional electrocatalytic performance due to the enhancement of intrinsic electrocatalytic activity by p-d orbital hybridization.Specifically,the CoFe-P-NS requires low overpotential of 259 and 307 mV to reach 500 mA cm−2 for HER and OER,respectively.Remarkably,the assembled electrolysis cell maintained a large current density of 300 mA cm−2 for over 360 h with negligible voltage increase during alkaline seawater electrolysis.Experiments and theoretical calculations show that the synergistic catalytic activity of bimetallic phosphides arises from p-d orbital hybridization,where the CoP-P sites enhance HER by optimizing H*adsorption in the Volmer-Heyrovsky steps,while the Fe_(2)P-Fe sites accelerate OER by lowering the energy barrier of the rate-determining step from O*to OOH*.This study provides valuable insights into the design of a controllable MOF-on-MOF-based electrocatalyst toward alkaline seawater splitting.展开更多
Water-cooled system have significantly enhanced the power generation efficiency of offshore wind turbines.However,these innovative systems are susceptible to substantial biological fouling,maintenance challenges,and h...Water-cooled system have significantly enhanced the power generation efficiency of offshore wind turbines.However,these innovative systems are susceptible to substantial biological fouling,maintenance challenges,and high upkeep costs.Therefore,the development of a specialized front-end filter tailored for direct current water-cooled system is importance.This involves the integration of dimensionally stable anode(DSA)and nickel alloy cathode,valued for their corrosion resistance in seawater,into a novel front-end filter system for Water-cooled applications.This system has the dual capability of generating hydrogen and chlorine for self-cleaning purposes.Implementing a flushing pulse electrolysis mode,it effectively mitigates electrode failure induced by cathodic calcium and magnesium deposition,thereby significantly prolonging electrode lifespan.Laboratory tests comprising system assembly and performance evaluations were conducted,with the system programmed to operate for 5 minutes every 24 hours under continuous flushing by natural seawater to simulate real-world conditions.After more than 11 months of continuous flushing,observations reveal that the DSA mesh and nickel alloy mesh maintain intact structural integrity and normal functioning.Subsequent 1꞉1 physical prototype Sea trial further validated the soundness of the system design and electrolytic control parameters.展开更多
Membra ne electrode assemblies(MEAs)are pivotal to advancing proton exchange membra ne water electrolysis(PEMWE),yet conventional designs suffer from limited triple-phase boundaries(TPBs),inefficient mass/charge trans...Membra ne electrode assemblies(MEAs)are pivotal to advancing proton exchange membra ne water electrolysis(PEMWE),yet conventional designs suffer from limited triple-phase boundaries(TPBs),inefficient mass/charge transport,and insufficient durability.This study introduces a three-dimensional ordered pattern-array(3D OPA)architecture fabricated via a scalable laser-machined mask and hot-pressing strategy.The 3D OPA MEA achieves a current density of 3.73 A cm^(-2) at 2 V,demonstrating a 50%performance improvement over the conventional MEA(2.48 A cm^(-2)),alongside a degradation rate of 26.6μV h^(-1) in a highly dynamic accelerated stress test(AST).Additionally,numerical simulations corroborate that the OPA architecture optimizes localized oxygen diffusion and liquid water replenishment,enhancing reaction kinetics.The 3D OPA architecture enhances TPBs and establishes optimized gas-liquid tra nsport pathways,significantly improving catalyst utilization while minimizing mass transfer overpotential and bubble-induced losses.Furthermore,its interlocking design reinforces mechanical interactions,reducing ohmic resistance a nd ensuring sustained mecha nical integrity and electrochemical durability.This work provides a simple,cost-effective,and scalable approach for patterned MEAs,addressing critical barriers to PEMWE commercialization through rational TPB engineering and transport pathway optimization.展开更多
Developing practical anion exchange membrane water electrolysis(AEMWE)technology encounters great challenges in not only cell efficiency but also long-term durability due to mechanical electrocatalyst detachment and e...Developing practical anion exchange membrane water electrolysis(AEMWE)technology encounters great challenges in not only cell efficiency but also long-term durability due to mechanical electrocatalyst detachment and electrochemical dissolution of active species,especially for the anodic oxygen evolution reaction(OER).Herein,a"two-pronged"approach is proposed to construct organophosphorus-protected NiFe layered double hydroxide catalysts on plasma-modified substrate,serving as an efficient and robust anode for practical AEMWE.Mechanical tests combined with operando spectroscopies and theoretical calculations demonstrate that the plasma modification strengthens the catalyst-substrate adhesion,while the organophosphorus protection prevents Fe leaching and promotes reaction kinetics during OER.The resultant electrode delivers an ultralow overpotential of 276 mV at 1 A cm^(-2),together with a remarkable stability at 0.5 A cm^(-2)over 500 h.Furthermore,assembling the optimized anode into an AEMWE device contributes to a minimized cell voltage of 1.70 V at 1 A cm^(-2),which sustains durable green hydrogen production with an economical energy consumption of 4.16 kW h Nm^(-3)H_(2).展开更多
Titanium exhibits outstanding properties,particularly,high specific strength and resistance to both high and low temperatures,earning it a reputation as the metal of the future.However,because of the highly reactive n...Titanium exhibits outstanding properties,particularly,high specific strength and resistance to both high and low temperatures,earning it a reputation as the metal of the future.However,because of the highly reactive nature of titanium,metallic titanium production involves extensive procedures and high costs.Considering its advantages and limitations,the European Union has classified titanium metal as a critical raw material(CRM)of low category.The Kroll process is predominantly used to produce titanium;however,molten salt electrolysis(MSE)is currently being explored for producing metallic titanium at a low cost.Since 2000,electrolytic titanium production has undergone a wave of technological advancements.However,because of the intermediate and disproportionation reactions in the electrolytic titanium production process,the process efficiency and titanium purity according to industrial standards could not be achieved.Consequently,metallic titanium production has gradually diversified into employing technologies such as thermal reduction,MSE,and titanium alloy preparation.This study provides a comprehensive review of research advances in titanium metal preparation technologies over the past two decades,highlighting the challenges faced by the existing methods and proposing potential solutions.It offers useful insights into the development of low-cost titanium preparation technologies.展开更多
With the in-depth implementation of sustainable development strategies,hydrogen energy as a clean energy source is receiving increasing attention[1,2].Among the various methods of hydrogen production,the electrocataly...With the in-depth implementation of sustainable development strategies,hydrogen energy as a clean energy source is receiving increasing attention[1,2].Among the various methods of hydrogen production,the electrocatalytic decomposition of abundant seawater into hydrogen utilizing renewable energy has emerged as a green and promising approach.However,natural seawater contains complex components,such as halide ions,which lead to the corrosion of catalysts or the occurrence of competitive side reactions during the electrolysis process[3].展开更多
Seawater electrolysis has attracted considerable attention in hydrogen production.However,the chloride ions(Cl^(-))in seawater can corrode metal sites and decrease the lifespans of the oxygen evolution reaction(OER).H...Seawater electrolysis has attracted considerable attention in hydrogen production.However,the chloride ions(Cl^(-))in seawater can corrode metal sites and decrease the lifespans of the oxygen evolution reaction(OER).Herein,we report a reversed-active sites strategy,converting Cl^(-)-affinitive metal sites to Cl^(-)-repellent oxygen sites,for OER in alkaline seawater electrolysis.First,ex/in situ experiments confirm the effectiveness of such a strategy using typical perovskites following the adsorbate evolution mechanism(AEM)or lattice oxygen-mediated mechanism(LOM).Furthermore,the origins of the superior activity and durability of as-prepared La_(0.3)SrCo_(0.5)Fe_(0.5)Ox(La_(0.3))can be ascribed to higher participation of lattice oxygen in OER,rapid bulk oxygen diffusion,and excellent OH-adsorption kinetics.Hence,an alkaline seawater electrolytic cell with La_(0.3)as the anode produces 10 mA cm^(-2)at just 1.57 V and maintains near-constant activity over 150 hours.This work introduces novel concepts for the production of superactive and steady electrocatalysts for the electrolysis of seawater.展开更多
Valence state engineering has emerged as a powerful strategy to optimize catalytic performance by modulating the electronic structure of metal active sites.However,the valence state regulation in high-entropy compound...Valence state engineering has emerged as a powerful strategy to optimize catalytic performance by modulating the electronic structure of metal active sites.However,the valence state regulation in high-entropy compounds(HECs)remains elusive due to their complex multi-element components and electronic interactions.Here,the valence states of different metals in twodimensional(2D)high entropy oxide(HEO)(FeNiMoRuV)O_(2-x)are precisely modulated through controlled pyrolysis of corresponding 2D high entropy hydroxide(HEHO)(FeNiMoRuV)(OH)_(2)under varying temperatures.Temperature-controlled pyrolysis selectively reduces the oxidation state of Ru,while simultaneously increasing the valence state of other constituent metals(Fe,Ni,Mo,and V),suggesting a competitive redox equilibrium.Notably,these low-valence Ru sites with oxygen vacancy in 2D HEO significantly reduce Ru-O bond energy and promote the generation of O-^(O)intermediates,thereby enabling oxygen evolution with a lattice oxygen mediated-oxygen vacancy site mechanism.2D HEO with low-valence Ru exhibits superior electrolytic water performance(HER/OER)compared to HEHO and other HEO with high-valence Ru,achieving a current density of 1000 mA cm^(-2)at 1.923 V,which exceeds the commercial Pt/C‖RuO_(2)system.Therefore,this study reveals the valence state regulatory mechanism of HECs and provides a solid hammer for the catalytic mechanism of valence state engineering.展开更多
Large-scale hydrogen production via water electrolysis faces a freshwater shortage.Direct seawater electrolysis offers a solution but encounters new challenges.Herein,we report a feasible strategy to both prevent meta...Large-scale hydrogen production via water electrolysis faces a freshwater shortage.Direct seawater electrolysis offers a solution but encounters new challenges.Herein,we report a feasible strategy to both prevent metal hydroxides deposition and boost the hydrogen evolution reaction by adding a chelating agent,EDTA-Na_(4),that chelates with Mg^(2+)/Ca^(2+),thus inhibiting their deposition and gathering them near the cathode surface,resulting in breaking the ordered hydrogen bond networks of interfacial water and reducing the activation energy of water dissociation.Furthermore,hydrolysis of–COO^(-) also promoted water dissociation to produce more active*H and*OH near the electrode surface that in turn serves as a diffusion medium for*OH,accelerating mass transfer and enabling seawater electrolysis to exhibit a stable performance,which operates continuously at 100 mA cm^(-2)@2.20 V and 200 mA cm^(-2)@2.58 V for 400 h in the symmetric electrolyzer and 500 mA cm^(-2)@2.29 V for over 500 h in the asymmetric electrolyzer.This study provides a new perspective to address the issues of stable and scalable direct seawater electrolysis for practical green hydrogen production.展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR),powered by advanced technologies such as solid oxide electrolysis cells(SOEC),is a promising method to convert CO_(2) into valuable carbon-based products usi...Electrochemical carbon dioxide reduction reaction(CO_(2)RR),powered by advanced technologies such as solid oxide electrolysis cells(SOEC),is a promising method to convert CO_(2) into valuable carbon-based products using renewable electricity.The high chemical stability of CO_(2) requires catalysts to exhibit both high activity and stable electrocatalytic performance.However,catalysts that deliver high performance in CO_(2)RR are rare and still require further improvement.Here,we report a strategy that can efficiently enhance catalyst activity through Zn doping,which introduces active frustrated Lewis pairs(FLP)to improve the catalyst's ability to activate small molecules.A high current density of-1.85 A cm^(-2)at 800℃under a bias voltage of 1.5 V was achieved using the Sr_(2)Fe_(0.8)Zn_(0.2)MoO_(6-δ)(SFZn_(0.2)M)cathode with pure CO_(2) feeding gas,surpassing previously reported results for perovskite oxide cathodes.This SOEC device also demonstrates excellent stability,with negligible degradation over tests lasting up to 110 h.展开更多
The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for...The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for hydrogen production.Despite remarkable advancements in this field,confronting the sluggish electrochemical kinetics and inherent high-energy consumption arising from deteriorated mass transport within PEMWE systems remains a formidable obstacle.This impediment stems primarily from the hindered protons mass transfer and the untimely hydrogen bubbles detachment.To address these challenges,we harness the inherent variability of electrical energy and introduce an innovative pulsed dynamic water electrolysis system.Compared to constant voltage electrolysis(hydrogen production rate:51.6 m L h^(-1),energy consumption:5.37 kWh Nm-^(3)H_(2)),this strategy(hydrogen production rate:66 m L h^(-1),energy consumption:3.83 kWh Nm-^(3)H_(2))increases the hydrogen production rate by approximately 27%and reduces the energy consumption by about 28%.Furthermore,we demonstrate the practicality of this system by integrating it with an off-grid photovoltaic(PV)system designed for outdoor operation,successfully driving a hydrogen production current of up to 500 mA under an average voltage of approximately 2 V.The combined results of in-situ characterization and finite element analysis reveal the performance enhancement mechanism:pulsed dynamic electrolysis(PDE)dramatically accelerates the enrichment of protons at the electrode/solution interface and facilitates the release of bubbles on the electrode surface.As such,PDE-enhanced PEMWE represents a synergistic advancement,concurrently enhancing both the hydrogen generation reaction and associated transport processes.This promising technology not only redefines the landscape of electrolysis-based hydrogen production but also holds immense potential for broadening its application across a diverse spectrum of electrocatalytic endeavors.展开更多
This work investigates the transient performance and stability of CO_(2)/H_(2)O co-electrolysis in an air-free environment using a flat-tube solid oxide electrolysis cell(SOEC)stack.The results showed that the transie...This work investigates the transient performance and stability of CO_(2)/H_(2)O co-electrolysis in an air-free environment using a flat-tube solid oxide electrolysis cell(SOEC)stack.The results showed that the transient behavior of the stack with and without blowing gas into the air electrode is almost the same.With a current density of 0.67 A·cm^(-2)@750℃,the stack operated for over 200 h under co-electrolysis conditions without air blowing,and the voltage drop rate of the stack was approximately 0.203%/100 hours.Microstructure analysis revealed a significant loss of nickel particles and an apparent for-mation of an insulating phase strontium chromate(SrCrO4)on the surface of the current collection layer of the air electrode,which are identified as key factors contributing to the performance degradation of the stack.This study provides a reference for development of efficient fuel preparation technology based on SOEC stack in airless environments.展开更多
The rising level of CO_(2) concentration in the atmosphere poses major threats to the global climate and environment.Various technologies have been developed to mitigate its negative effects through nonconversion and ...The rising level of CO_(2) concentration in the atmosphere poses major threats to the global climate and environment.Various technologies have been developed to mitigate its negative effects through nonconversion and conversion routes.Particularly,solid oxide electrolysis cells(SOECs),as a promising technology with the highest energy efficiency,have garnered considerable attention for their effectiveness to electrochemically convert CO_(2) into high-value fuels.However,the insufficient catalytic activity,poor longterm stability,and high costs have significantly hindered the industrial-scale application of SOECs.To this end,substantial efforts,with an emphasis on the smart design of targeting electrode materials for specific applications have been devoted to advancing the electrosynthesis of high-value fuels from CO_(2) in various SOECs,but there still lacks a critical and comprehensive review in-depth discussing the fundamentals,and summarizing the latest advances in various applications and electrode materials for electrochemically converting CO_(2) to high-value fuels in SOECs.This review thus aims to fill this gap by focusing on the fundamentals(i.e.,SOEC working principles,thermodynamics,kinetics and representative evaluation parameters),specific applications(i.e.,pure CO_(2) electrolysis,CO_(2)-H_(2)O co-electrolysis,fuel-assisted CO_(2) conversion),and material selection criteria(i.e.,cathodic materials for CO_(2) conversion,and anodic materials for fuel-assisted CO_(2) conversion).In addition,the challenges that this technology is currently facing,and our perspectives on electrochemical CO_(2) conversion in SOECs are proposed to guide the smart design of high-performance electrocatalysts and future industrial-scale application of SOECs for electrosynthesizing high-value fuels from CO_(2).展开更多
CO_(2)electrolysis using solid oxide electrolysis cells is a promising technology for CO_(2)utilization and conversion,which has attracted more and more attention in recent years because of its extremely high efficien...CO_(2)electrolysis using solid oxide electrolysis cells is a promising technology for CO_(2)utilization and conversion,which has attracted more and more attention in recent years because of its extremely high efficiency.However,traditional Ni-yttria-stabilized zirconia(Ni-YSZ)or Ni-Gd_(0.1)Ce_(0.9)O_(2-δ)(Ni-GDC)metal-ceramic cathode faces many problems such as Ni agglomeration and carbon deposition during long-time operation.Herein,a perovskite oxide La_(0.43-x)Ca_(0.37)Ti_(0.9)Ni_(0.1)O_(3-δ)(LCTN,x=0,0.05,0.1)with nanophase-LaVO_(4)exsolution was investigated as the novel cathode of solid oxide electrolysis cell(SOEC)for efficient CO_(2)electrolysis.The results confirm that the exsolution nanophase on LCTN surface can significantly improve the CO_(2)adsorption and conversion performance.For CO_(2)electrolysis at 1.8 V,an electrolysis current density of 1.24 A/cm2at 800℃can be obtained on SOEC with La_(0.43-x)Ca_(0.37)Ti_(0.9)Ni_(0.1)O_(3-δ)decorated with LaVO_(4)(LCTN-V0.05)cathode.Furthermore,the corresponding cell can maintain stable operation up to 100 h without apparent performance degradation.These results demonstrate that doping-induced second nanophase exsolution is a promising way to design high-performance SOEC cathodes for CO_(2)electrolysis.展开更多
The performance of solid oxide electrolysis cells(SOECs)for CO_(2) electrolysis is significantly impeded by the limited electrochemical activity and insufficient durability of the cathode.This study introduces a novel...The performance of solid oxide electrolysis cells(SOECs)for CO_(2) electrolysis is significantly impeded by the limited electrochemical activity and insufficient durability of the cathode.This study introduces a novel(LaSrPrBaCaGd)_(2)Fe_(1.5)Mo_(0.5)O_(6-δ)(LSPBCGFM)perovskite via A-site entropy engineering,to improve both activity and durability.Experimental results reveal that LSPBCGFM cathode-based SOEC achieves a current density of 1.34 A·cm^(−2) at 1.5 V and 800℃,maintaining stable operation for more than 400 h at 1.2 V with negligible degradation.Theoretical calculations suggest that the high-entropy strategy shifts the transition metal d-band center and O-2p-band center closer to the Fermi energy level simultaneously,thereby initiating more favorable CO_(2) adsorption and activation.In addition,a higher O-2p-band center promotes the formation and diffusion of oxygen vacancies.The findings of this study provide crucial insights into the role of conformational entropy strategies in CO_(2) electrolysis and offer potential pathways for the development of highly efficient and stable catalysts.展开更多
基金financially supported by the Key Research and Development Program of Heilongjiang Province(No.2024ZXJ03C06)National Natural Science Foundation of China(No.52476192,No.52106237)+1 种基金Natural Science Foundation of Heilongjiang Province(No.YQ2022E027)Technology Project of China Datang Technology Innovation Co.,Ltd(No.DTKC-2024-20610).
文摘Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sustainable development.Despite significant progress in various electrochemical systems,the regulatory mechanisms of PDE in energy and mass transfer and the lifespan extension of electrolysis systems,particularly in water electrolysis(WE)for hydrogen production,remain insufficiently explored.Therefore,there is an urgent need for a deeper understanding of the unique contributions of PDE in mass transfer enhancement,microenvironment regulation,and hydrogen production optimization,aiming to achieve low-energy consumption,high catalytic activity,and long-term stability in the generation of target products.Here,this review critically examines the microenvironmental effects of PDE on energy and mass transfer,the electrode degradation mechanisms in the lifespan extension of electrolysis systems,and the key factors in enhancing WE for hydrogen production,providing a comprehensive summary of current research progress.The review focuses on the complex regulatory mechanisms of frequency,duty cycle,amplitude,and other factors in hydrogen evolution reaction(HER)performance within PDE strategies,revealing the interrelationships among them.Finally,the potential future directions and challenges for transitioning from laboratory studies to industrial applications are proposed.
基金supported by the National Key Research and Development Program of China (2022YFE0138900)the “Scientific and Technical Innovation Action Plan” Basic Research Field of Shanghai Science and Technology Committee (19JC1410500)。
文摘Ion-solvaing membranes(ISMs)have received extensive attention in recent years as a key component in electrochemical energy conversion and storage devices.This article provides an overview of structural composition,performance advan-tages,research progress,ion conduction mechanism and existing issues of ISMs,primarily classifying them according to the matrix structure.A detailed analysis of performance enhancement methods,key performance indicators of ISMs and performance influencing factors is also presented.The article contributes to further optimizing the design and application of ion-solvation membranes,providing theoretical support for the development of fields such as hydrogen production through electrolysis of water and electrochemical energy in the future.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52273059 and 52473219)the Natural Science Foundation of Tianjin(Grant Nos.22JCYBJC01030 and 23JCYBJC00650)provided by Yantai Tayho Advanced Materials Group Co.,Ltd.
文摘Alkaline water electrolysis(AWE)represents a promising approach for green hydrogen production,yet the development of high-performance separators with gas impermeability,high ion conductivity,and stability under alkaline operating conditions has proven challenging.To address this challenge,we develop a pre-concentration regulated phase separation strategy for scalable fabrication of asymmetric hierarchical porous membranes(AHPMs)for AWE.The resulting AHPMs demonstrate a hierarchical structure composed of an ultrathin dense skin layer and highly interconnected porous support.Benefitting from the structural advantages,the AHPMs exhibit outstanding characteristics,including a high bubble point pressure up to 12.4 bar,extremely low area resistance of 0.03Ωcm^(2) in 30 wt%KOH at 80℃,and excellent hydrophilicity and long-term alkaline stability.When applied in AWE with commercial catalysts,the AHPMs achieved an impressive current density of 1.9 A cm^(-2) at 2.0 V in 30 wt%KOH and the anodic hydrogen contents(AHCs)below 0.5 vol.%at a low current density of 0.1 A cm^(-2),differential pressure of 2 bar,and temperature of 80℃.Moreover,AHPMs demonstrate exceptional stability over 2,400 h of continuous operation and maintain superior performance in a 1 Nm^(3) h^(-1) industrialscale electrolyzer stack.This work advances the development of efficient separators for highperformance AWE systems,contributing to the advancement of hydrogen technologies in sustainable energy applications.
基金supported by the National Natural Science Foundation of China(No.22209115,52472226,and U23A20573)the Key Research and Development Program of Shandong Province(No.2022CXGC010305)+2 种基金Guangdong Basic and Applied Basic Research Foundation(No.2025A1515011809,2023B1515120022 and 2022B1515120001)Shenzhen Science and Technology Innovation Program(No.RCBS20231211090522040,KJZD20240903095610014,and KJZD20240903095712017)the High-Level Professional Team in Shenzhen(KQTD20210811090045006)。
文摘Seawater electrolysis is an appealing route toward sustainable hydrogen production,yet its practical deployment is hindered by severe chloride-induced corrosion and parasitic chlorine oxidation.Here,we report noble metal-doped NiV layered double hydroxides(LDHs)that integrate electronic modulation with a dual chloride confinement mechanism.Ir incorporation simultaneously establishes strong Ir-Cl coordination and dynamically regenerated VO_(4)^(3-)layers,producing an adaptive electrostatic shield that effectively suppresses chloride penetration.As a result,Ir-NiV LDH delivers nearly 100%oxygen evolution reaction selectivity and outstanding stability over2750 h at 500 mA cm^(-2).Meanwhile,Ru doping optimizes the hydrogen evolution pathway,enabling a low overpotential of 195 mV and>2350 h durability.When paired in a twso-electrode electrolyzer,the Ru-NiVLDH‖Ir-NiVLDH system exhibits industrial-level performance and unprecedented robustness in alkaline seawater.This dual chloride confinement concept provides a general framework for catalyst design in corrosive ionic environments,extending beyond seawater splitting toward other electrochemical energy conversion processes.
基金sponsored by the National Natural Science Foundation of China(52302039,52301043)the Guangdong Basic and Applied Basic Research Foundation(2024A1515240056)+3 种基金the Shenzhen Science and Technology Program(GXWD20231129113217001)the Shenzhen Key Laboratory of New Materials Technology(SYSPG20241211173609003)the Postdoctoral Research Startup Expenses of Shenzhen(NA25501001)Shenzhen Introduce High-level Talents and Scientific Research Start-up Funds(NA11409005)。
文摘Seawater electrolysis has been explored as a viable and sustainable method for green hydrogen production in regions characterized by freshwater scarcity but abundant renewable energy resources.However,the high concentration of chlorine ions(Cl^(-))in seawater leads to severe corrosion of metallic electrodes,which significantly challenges the stability of electrode catalysts in seawater electrolysis.Owing to the Cl^(-)corrosion and the competitive oxygen/chlorine evolution reactions,the design of durable and active anode catalysts is key to achieving practical seawater electrolysis.To address this challenge,this review systematically analyzes the chlorine-induced corrosion mechanisms of anode catalysts,evaluates various anticorrosion strategies,and explores future prospects for enhancing anode durability.Three mainstream anticorrosion strategies are summarized and assessed for their effectiveness in mitigating the chlorineinduced damage to anode catalysts:the physical surface coatings,electrostatic repulsion,and Cl^(-)adsorption regulation.In addition,some emerging strategies are further introduced to highlight the future trends of state-of-the-art techniques for seawater electrolysis.This review aims to provide novel insights and practical guidance for developing more stable and efficient anode catalysts for hydrogen production via seawater electrolvsis.
基金financial support of the National Natural Science Foundation of China (21875247,21072221, 21172252)the Project of Talent Cultivation for Carbon Peak and Carbon Neutrality of the University of Chinese of Academy of Science
文摘The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-assembly method is used to fabricate controllable MOF-on-MOF multiscale heterostructures,where triangular host MOF(ZIF-67)nanosheets undergo in situ epitaxial growth to form uniform orthogonal vip MOF(CoFe PBA)nanosheets.Phosphorus(P)is further introduced in situ to fabricate CoP and Fe_(2)P heterostructured nanosheets(CoFe-P-NS),which exhibit excellent bifunctional electrocatalytic performance due to the enhancement of intrinsic electrocatalytic activity by p-d orbital hybridization.Specifically,the CoFe-P-NS requires low overpotential of 259 and 307 mV to reach 500 mA cm−2 for HER and OER,respectively.Remarkably,the assembled electrolysis cell maintained a large current density of 300 mA cm−2 for over 360 h with negligible voltage increase during alkaline seawater electrolysis.Experiments and theoretical calculations show that the synergistic catalytic activity of bimetallic phosphides arises from p-d orbital hybridization,where the CoP-P sites enhance HER by optimizing H*adsorption in the Volmer-Heyrovsky steps,while the Fe_(2)P-Fe sites accelerate OER by lowering the energy barrier of the rate-determining step from O*to OOH*.This study provides valuable insights into the design of a controllable MOF-on-MOF-based electrocatalyst toward alkaline seawater splitting.
基金Supported by the Project of Design of Anti-corrosion and Anti-fouling Solutions for Offshore Wind Power Water-Cooled Systems(No.E428161)the National Natural Science Foundation of China(No.42176047)。
文摘Water-cooled system have significantly enhanced the power generation efficiency of offshore wind turbines.However,these innovative systems are susceptible to substantial biological fouling,maintenance challenges,and high upkeep costs.Therefore,the development of a specialized front-end filter tailored for direct current water-cooled system is importance.This involves the integration of dimensionally stable anode(DSA)and nickel alloy cathode,valued for their corrosion resistance in seawater,into a novel front-end filter system for Water-cooled applications.This system has the dual capability of generating hydrogen and chlorine for self-cleaning purposes.Implementing a flushing pulse electrolysis mode,it effectively mitigates electrode failure induced by cathodic calcium and magnesium deposition,thereby significantly prolonging electrode lifespan.Laboratory tests comprising system assembly and performance evaluations were conducted,with the system programmed to operate for 5 minutes every 24 hours under continuous flushing by natural seawater to simulate real-world conditions.After more than 11 months of continuous flushing,observations reveal that the DSA mesh and nickel alloy mesh maintain intact structural integrity and normal functioning.Subsequent 1꞉1 physical prototype Sea trial further validated the soundness of the system design and electrolytic control parameters.
基金supported by the National Natural Science Foundation of China(22579043,52461040,22202053,52274297)the Hainan Provincial Department of Science and Technology(G20250218018E)+2 种基金the first batch of“Nanhai New Star”industrial innovation talent platform project(202309006)the Hainan Province Science and Technology Special Fund(ZDYF2025GXJS004)the Start-up Research Foundation of Hainan University(KYQD(ZR)-21124)。
文摘Membra ne electrode assemblies(MEAs)are pivotal to advancing proton exchange membra ne water electrolysis(PEMWE),yet conventional designs suffer from limited triple-phase boundaries(TPBs),inefficient mass/charge transport,and insufficient durability.This study introduces a three-dimensional ordered pattern-array(3D OPA)architecture fabricated via a scalable laser-machined mask and hot-pressing strategy.The 3D OPA MEA achieves a current density of 3.73 A cm^(-2) at 2 V,demonstrating a 50%performance improvement over the conventional MEA(2.48 A cm^(-2)),alongside a degradation rate of 26.6μV h^(-1) in a highly dynamic accelerated stress test(AST).Additionally,numerical simulations corroborate that the OPA architecture optimizes localized oxygen diffusion and liquid water replenishment,enhancing reaction kinetics.The 3D OPA architecture enhances TPBs and establishes optimized gas-liquid tra nsport pathways,significantly improving catalyst utilization while minimizing mass transfer overpotential and bubble-induced losses.Furthermore,its interlocking design reinforces mechanical interactions,reducing ohmic resistance a nd ensuring sustained mecha nical integrity and electrochemical durability.This work provides a simple,cost-effective,and scalable approach for patterned MEAs,addressing critical barriers to PEMWE commercialization through rational TPB engineering and transport pathway optimization.
基金supported by the Natural Science Foundation of Shanghai Municipality(25ZR1401027)the National Natural Science Foundation of China(22572041,11975081,22309037,52274297,and 22402083)+1 种基金Hainan Provincial Natural Science Foundation of China(225YXQN587)Start-up Research Foundation of Hainan University(KYQD(ZR)23035)。
文摘Developing practical anion exchange membrane water electrolysis(AEMWE)technology encounters great challenges in not only cell efficiency but also long-term durability due to mechanical electrocatalyst detachment and electrochemical dissolution of active species,especially for the anodic oxygen evolution reaction(OER).Herein,a"two-pronged"approach is proposed to construct organophosphorus-protected NiFe layered double hydroxide catalysts on plasma-modified substrate,serving as an efficient and robust anode for practical AEMWE.Mechanical tests combined with operando spectroscopies and theoretical calculations demonstrate that the plasma modification strengthens the catalyst-substrate adhesion,while the organophosphorus protection prevents Fe leaching and promotes reaction kinetics during OER.The resultant electrode delivers an ultralow overpotential of 276 mV at 1 A cm^(-2),together with a remarkable stability at 0.5 A cm^(-2)over 500 h.Furthermore,assembling the optimized anode into an AEMWE device contributes to a minimized cell voltage of 1.70 V at 1 A cm^(-2),which sustains durable green hydrogen production with an economical energy consumption of 4.16 kW h Nm^(-3)H_(2).
基金financial support from the Yunnan Province Key Industries Science and Technology Special Project for Colleges and UniversitiesChina(No.FWCY-QYCT2024006)+6 种基金National Natural Science Foundation of China(Nos.52104351 and 52364051)Science and Technology Major Project of Yunnan Province,China(No.202202AG050007)the Yunnan Fundamental Research ProjectsChina(No.202401AT070314)the Key Technology Research and Development Program of Shandong Province,China(No.2023CXGC010903)Central Guidance Local Scientific and Technological Development Funds,China(No.202407AB110022)Yunnan Province Xingdian Talent Support Plan Project,China。
文摘Titanium exhibits outstanding properties,particularly,high specific strength and resistance to both high and low temperatures,earning it a reputation as the metal of the future.However,because of the highly reactive nature of titanium,metallic titanium production involves extensive procedures and high costs.Considering its advantages and limitations,the European Union has classified titanium metal as a critical raw material(CRM)of low category.The Kroll process is predominantly used to produce titanium;however,molten salt electrolysis(MSE)is currently being explored for producing metallic titanium at a low cost.Since 2000,electrolytic titanium production has undergone a wave of technological advancements.However,because of the intermediate and disproportionation reactions in the electrolytic titanium production process,the process efficiency and titanium purity according to industrial standards could not be achieved.Consequently,metallic titanium production has gradually diversified into employing technologies such as thermal reduction,MSE,and titanium alloy preparation.This study provides a comprehensive review of research advances in titanium metal preparation technologies over the past two decades,highlighting the challenges faced by the existing methods and proposing potential solutions.It offers useful insights into the development of low-cost titanium preparation technologies.
基金financially supported by the Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(No.NY223016)Qinglan Project of Jiangsu Province of China2024 Nanjing Science and Technology Innovation Program(No.NJKCZYZZ2024-06)。
文摘With the in-depth implementation of sustainable development strategies,hydrogen energy as a clean energy source is receiving increasing attention[1,2].Among the various methods of hydrogen production,the electrocatalytic decomposition of abundant seawater into hydrogen utilizing renewable energy has emerged as a green and promising approach.However,natural seawater contains complex components,such as halide ions,which lead to the corrosion of catalysts or the occurrence of competitive side reactions during the electrolysis process[3].
基金supported by the National Natural Science Foundation of China(No.22278203).
文摘Seawater electrolysis has attracted considerable attention in hydrogen production.However,the chloride ions(Cl^(-))in seawater can corrode metal sites and decrease the lifespans of the oxygen evolution reaction(OER).Herein,we report a reversed-active sites strategy,converting Cl^(-)-affinitive metal sites to Cl^(-)-repellent oxygen sites,for OER in alkaline seawater electrolysis.First,ex/in situ experiments confirm the effectiveness of such a strategy using typical perovskites following the adsorbate evolution mechanism(AEM)or lattice oxygen-mediated mechanism(LOM).Furthermore,the origins of the superior activity and durability of as-prepared La_(0.3)SrCo_(0.5)Fe_(0.5)Ox(La_(0.3))can be ascribed to higher participation of lattice oxygen in OER,rapid bulk oxygen diffusion,and excellent OH-adsorption kinetics.Hence,an alkaline seawater electrolytic cell with La_(0.3)as the anode produces 10 mA cm^(-2)at just 1.57 V and maintains near-constant activity over 150 hours.This work introduces novel concepts for the production of superactive and steady electrocatalysts for the electrolysis of seawater.
基金supported by the National Natural Science Foundation of China(22205209)China Postdoctoral Science Foundation(2024T170837 and2022M722867)+2 种基金Joint Fund for Provincial Scientific Research and Development Plan of Henan Province(242301420039)the Key Research Projects of Higher Education Institutions of Henan Province(24A530009)Special Fund for Young Teachers from the Zhengzhou University(JC23257011)。
文摘Valence state engineering has emerged as a powerful strategy to optimize catalytic performance by modulating the electronic structure of metal active sites.However,the valence state regulation in high-entropy compounds(HECs)remains elusive due to their complex multi-element components and electronic interactions.Here,the valence states of different metals in twodimensional(2D)high entropy oxide(HEO)(FeNiMoRuV)O_(2-x)are precisely modulated through controlled pyrolysis of corresponding 2D high entropy hydroxide(HEHO)(FeNiMoRuV)(OH)_(2)under varying temperatures.Temperature-controlled pyrolysis selectively reduces the oxidation state of Ru,while simultaneously increasing the valence state of other constituent metals(Fe,Ni,Mo,and V),suggesting a competitive redox equilibrium.Notably,these low-valence Ru sites with oxygen vacancy in 2D HEO significantly reduce Ru-O bond energy and promote the generation of O-^(O)intermediates,thereby enabling oxygen evolution with a lattice oxygen mediated-oxygen vacancy site mechanism.2D HEO with low-valence Ru exhibits superior electrolytic water performance(HER/OER)compared to HEHO and other HEO with high-valence Ru,achieving a current density of 1000 mA cm^(-2)at 1.923 V,which exceeds the commercial Pt/C‖RuO_(2)system.Therefore,this study reveals the valence state regulatory mechanism of HECs and provides a solid hammer for the catalytic mechanism of valence state engineering.
基金the support from the National Key Research and Development Program of China(2023YFB4005000)the Joint Fund of Liaoning Binhai Laboratory(LBLF-2023-04)+3 种基金Dalian Science and Technology Talent Innovation Support Plan(2022RY09)Innovation Research Fund of Dalian Institute of Chemical Physics(DICP I202318)National Natural Science Foundation of China(22478384)the UK EPSRC(EP/W03784X/1)。
文摘Large-scale hydrogen production via water electrolysis faces a freshwater shortage.Direct seawater electrolysis offers a solution but encounters new challenges.Herein,we report a feasible strategy to both prevent metal hydroxides deposition and boost the hydrogen evolution reaction by adding a chelating agent,EDTA-Na_(4),that chelates with Mg^(2+)/Ca^(2+),thus inhibiting their deposition and gathering them near the cathode surface,resulting in breaking the ordered hydrogen bond networks of interfacial water and reducing the activation energy of water dissociation.Furthermore,hydrolysis of–COO^(-) also promoted water dissociation to produce more active*H and*OH near the electrode surface that in turn serves as a diffusion medium for*OH,accelerating mass transfer and enabling seawater electrolysis to exhibit a stable performance,which operates continuously at 100 mA cm^(-2)@2.20 V and 200 mA cm^(-2)@2.58 V for 400 h in the symmetric electrolyzer and 500 mA cm^(-2)@2.29 V for over 500 h in the asymmetric electrolyzer.This study provides a new perspective to address the issues of stable and scalable direct seawater electrolysis for practical green hydrogen production.
基金support from the National Key Research and Development Program of China(2024YFB4106400)the National Natural Science Foundation of China(22269019,52472202)Hubei Province(2024BCB073,2024EHA045).
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR),powered by advanced technologies such as solid oxide electrolysis cells(SOEC),is a promising method to convert CO_(2) into valuable carbon-based products using renewable electricity.The high chemical stability of CO_(2) requires catalysts to exhibit both high activity and stable electrocatalytic performance.However,catalysts that deliver high performance in CO_(2)RR are rare and still require further improvement.Here,we report a strategy that can efficiently enhance catalyst activity through Zn doping,which introduces active frustrated Lewis pairs(FLP)to improve the catalyst's ability to activate small molecules.A high current density of-1.85 A cm^(-2)at 800℃under a bias voltage of 1.5 V was achieved using the Sr_(2)Fe_(0.8)Zn_(0.2)MoO_(6-δ)(SFZn_(0.2)M)cathode with pure CO_(2) feeding gas,surpassing previously reported results for perovskite oxide cathodes.This SOEC device also demonstrates excellent stability,with negligible degradation over tests lasting up to 110 h.
基金National Natural Science Foundation of China(No.52476192,No.52106237)Natural Science Foundation of Heilongjiang Province(No.YQ2022E027)。
文摘The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for hydrogen production.Despite remarkable advancements in this field,confronting the sluggish electrochemical kinetics and inherent high-energy consumption arising from deteriorated mass transport within PEMWE systems remains a formidable obstacle.This impediment stems primarily from the hindered protons mass transfer and the untimely hydrogen bubbles detachment.To address these challenges,we harness the inherent variability of electrical energy and introduce an innovative pulsed dynamic water electrolysis system.Compared to constant voltage electrolysis(hydrogen production rate:51.6 m L h^(-1),energy consumption:5.37 kWh Nm-^(3)H_(2)),this strategy(hydrogen production rate:66 m L h^(-1),energy consumption:3.83 kWh Nm-^(3)H_(2))increases the hydrogen production rate by approximately 27%and reduces the energy consumption by about 28%.Furthermore,we demonstrate the practicality of this system by integrating it with an off-grid photovoltaic(PV)system designed for outdoor operation,successfully driving a hydrogen production current of up to 500 mA under an average voltage of approximately 2 V.The combined results of in-situ characterization and finite element analysis reveal the performance enhancement mechanism:pulsed dynamic electrolysis(PDE)dramatically accelerates the enrichment of protons at the electrode/solution interface and facilitates the release of bubbles on the electrode surface.As such,PDE-enhanced PEMWE represents a synergistic advancement,concurrently enhancing both the hydrogen generation reaction and associated transport processes.This promising technology not only redefines the landscape of electrolysis-based hydrogen production but also holds immense potential for broadening its application across a diverse spectrum of electrocatalytic endeavors.
基金co-supported by the National Key R&D Program of China(No.2022YFB4002203)Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(No.LBMHY24B060003)Ningbo Key R&D Project(No.2023Z155).
文摘This work investigates the transient performance and stability of CO_(2)/H_(2)O co-electrolysis in an air-free environment using a flat-tube solid oxide electrolysis cell(SOEC)stack.The results showed that the transient behavior of the stack with and without blowing gas into the air electrode is almost the same.With a current density of 0.67 A·cm^(-2)@750℃,the stack operated for over 200 h under co-electrolysis conditions without air blowing,and the voltage drop rate of the stack was approximately 0.203%/100 hours.Microstructure analysis revealed a significant loss of nickel particles and an apparent for-mation of an insulating phase strontium chromate(SrCrO4)on the surface of the current collection layer of the air electrode,which are identified as key factors contributing to the performance degradation of the stack.This study provides a reference for development of efficient fuel preparation technology based on SOEC stack in airless environments.
基金supported by the Pilot Group Program of the Research Fund for International Senior Scientists(No.22350710789)the National Natural Science Foundation of China(NSFC,No.22109182)+2 种基金the Natural Science Foundation of Hunan Province,China(No.2022JJ30684)the Start-up Funding of Central South University(No.206030104)supported in part by the High-Performance Computing Center of Central South University。
文摘The rising level of CO_(2) concentration in the atmosphere poses major threats to the global climate and environment.Various technologies have been developed to mitigate its negative effects through nonconversion and conversion routes.Particularly,solid oxide electrolysis cells(SOECs),as a promising technology with the highest energy efficiency,have garnered considerable attention for their effectiveness to electrochemically convert CO_(2) into high-value fuels.However,the insufficient catalytic activity,poor longterm stability,and high costs have significantly hindered the industrial-scale application of SOECs.To this end,substantial efforts,with an emphasis on the smart design of targeting electrode materials for specific applications have been devoted to advancing the electrosynthesis of high-value fuels from CO_(2) in various SOECs,but there still lacks a critical and comprehensive review in-depth discussing the fundamentals,and summarizing the latest advances in various applications and electrode materials for electrochemically converting CO_(2) to high-value fuels in SOECs.This review thus aims to fill this gap by focusing on the fundamentals(i.e.,SOEC working principles,thermodynamics,kinetics and representative evaluation parameters),specific applications(i.e.,pure CO_(2) electrolysis,CO_(2)-H_(2)O co-electrolysis,fuel-assisted CO_(2) conversion),and material selection criteria(i.e.,cathodic materials for CO_(2) conversion,and anodic materials for fuel-assisted CO_(2) conversion).In addition,the challenges that this technology is currently facing,and our perspectives on electrochemical CO_(2) conversion in SOECs are proposed to guide the smart design of high-performance electrocatalysts and future industrial-scale application of SOECs for electrosynthesizing high-value fuels from CO_(2).
基金Project supported by the National Key Research&Development Project(2023YFB4006001)National Natural Science Foundation of China(52172199)。
文摘CO_(2)electrolysis using solid oxide electrolysis cells is a promising technology for CO_(2)utilization and conversion,which has attracted more and more attention in recent years because of its extremely high efficiency.However,traditional Ni-yttria-stabilized zirconia(Ni-YSZ)or Ni-Gd_(0.1)Ce_(0.9)O_(2-δ)(Ni-GDC)metal-ceramic cathode faces many problems such as Ni agglomeration and carbon deposition during long-time operation.Herein,a perovskite oxide La_(0.43-x)Ca_(0.37)Ti_(0.9)Ni_(0.1)O_(3-δ)(LCTN,x=0,0.05,0.1)with nanophase-LaVO_(4)exsolution was investigated as the novel cathode of solid oxide electrolysis cell(SOEC)for efficient CO_(2)electrolysis.The results confirm that the exsolution nanophase on LCTN surface can significantly improve the CO_(2)adsorption and conversion performance.For CO_(2)electrolysis at 1.8 V,an electrolysis current density of 1.24 A/cm2at 800℃can be obtained on SOEC with La_(0.43-x)Ca_(0.37)Ti_(0.9)Ni_(0.1)O_(3-δ)decorated with LaVO_(4)(LCTN-V0.05)cathode.Furthermore,the corresponding cell can maintain stable operation up to 100 h without apparent performance degradation.These results demonstrate that doping-induced second nanophase exsolution is a promising way to design high-performance SOEC cathodes for CO_(2)electrolysis.
基金supported by the National Natural Science Foundation of China(Nos.22379133,22075256,and 52072350)the Natural Science Foundation of Guangdong Province(No.2024A1515012235).
文摘The performance of solid oxide electrolysis cells(SOECs)for CO_(2) electrolysis is significantly impeded by the limited electrochemical activity and insufficient durability of the cathode.This study introduces a novel(LaSrPrBaCaGd)_(2)Fe_(1.5)Mo_(0.5)O_(6-δ)(LSPBCGFM)perovskite via A-site entropy engineering,to improve both activity and durability.Experimental results reveal that LSPBCGFM cathode-based SOEC achieves a current density of 1.34 A·cm^(−2) at 1.5 V and 800℃,maintaining stable operation for more than 400 h at 1.2 V with negligible degradation.Theoretical calculations suggest that the high-entropy strategy shifts the transition metal d-band center and O-2p-band center closer to the Fermi energy level simultaneously,thereby initiating more favorable CO_(2) adsorption and activation.In addition,a higher O-2p-band center promotes the formation and diffusion of oxygen vacancies.The findings of this study provide crucial insights into the role of conformational entropy strategies in CO_(2) electrolysis and offer potential pathways for the development of highly efficient and stable catalysts.
