Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,par...Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,particularly the presence of aggressive Cl^(-),has been proven to be prone to parasitic chloride ion oxidation and corrosion reactions,thus restricting seawater electrolyzer lifetime.Herein,hierarchical structure(Ni,Fe)O(OH)@NiCoS nanorod arrays(NAs)catalysts with heterointerfaces and localized oxygen vacancies were synthesized at nickel foam substrates via the combination of hydrothermal and annealing methods to boost seawater dissociation.The hiera rchical nanostructure of NiCoS NAs enhanced electrode charge transfer rate and active surface area to accelerate oxygen evolution reaction(OER)and generated sulfate gradient layers to repulsive aggressive Cl^(-).The fabricated heterostructure and vacancies of(Ni,Fe)O(OH)tuned catalyst electronic structure into an electrophilic state to enhance the binding affinity of hydroxyl intermediates and facilitate the structural transformation into amorphousγ-NiFeOOH for promoting OER.Furthermore,through operando electrochemistry techniques,we found that theγ-NiFeOOH possessing an unsaturated coordination environment and lattice-oxygen-participated OER mechanism can minimize electrode Cl^(-)corrosion enabled by stabilizing the adsorption of OH*intermediates,making it one of the best OER catalysts in the seawater medium reported to date.Consequently,these catalysts can deliver current densities of 100 and 500 mA cm-2for boosting OER at minimal overpotentials of 245and 316 mV,respectively,and thus prevent chloride ion oxidation simultaneously.Impressively,a highly stable anion exchange membrane(AEM)seawater electrolyzer based on the non-noble metal heterostructure electrodes reached a record low degradation rate under 100μV h-1at constant industrial current densities of 400 and 600 mA cm-2over 300 h,which exhibits a promising future for the nonprecious and stable AEMWE in the direct seawater electrolysis industry.展开更多
Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts f...Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis reactions.Herein,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen generation.Experimental and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol electrolysis.Moreover,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping technique.The high catalytic kinetics and stability,as well as the promotion effect,were also carefully discussed.Specifically,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.展开更多
Green hydrogen produced by water electrolysis combined with renewable energy is a promising alternative to fossil fuels due to its high energy density with zero-carbon emissions.Among water electrolysis technologies,t...Green hydrogen produced by water electrolysis combined with renewable energy is a promising alternative to fossil fuels due to its high energy density with zero-carbon emissions.Among water electrolysis technologies,the anion exchange membrane(AEM) water electrolysis has gained intensive attention and is considered as the next-generation emerging technology due to its potential advantages,such as the use of low-cost non-noble metal catalysts,the relatively mature stack assembly process,etc.However,the AEM water electrolyzer is still in the early development stage of the kW-level stack,which is mainly attributed to severe performance decay caused by the core component,i.e.,AEM.Here,the review comprehensively presents the recent progress of advanced AEM from the view of the performance of water electrolysis cells.Herein,fundamental principles and critical components of AEM water electrolyzers are introduced,and work conditions of AEM water electrolyzers and AEM performance improvement strategies are discussed.The challenges and perspectives are also analyzed.展开更多
The metal-lightweighted electrocatalysts for water splitting are highly desired for sustainable and economic hydrogen energy deployments,but challengeable.In this work,a low-content Ni-functionalized approach triggers...The metal-lightweighted electrocatalysts for water splitting are highly desired for sustainable and economic hydrogen energy deployments,but challengeable.In this work,a low-content Ni-functionalized approach triggers the high capability of black phosphorene(BP)with hydrogen and oxygen evolution reaction(HER/OER)bifunctionality.Through a facile in situ electro-exfoliation route,the ionized Ni sites are covalently functionalized in BP nanosheets with electron redistribution and controllable metal contents.It is found that the as-fabricated Ni-BP electrocatalysts can drive the water splitting with much enhanced HER and OER activities.In 1.0 M KOH electrolyte,the optimized 1.5 wt%Nifunctionalized BP nanosheets have readily achieved low overpotentials of 136 mV for HER and 230 mV for OER at 10 mA cm^(−2).Moreover,the covalently bonding between Ni and P has also strengthened the catalytic stability of the Ni-functionalized BP electrocatalyst,stably delivering the overall water splitting for 50 h at 20 mA cm^(−2).Theoretical calculations have revealed that Ni–P covalent binding can regulate the electronic structure and optimize the reaction energy barrier to improve the catalytic activity effectively.This work confirms that Ni-functionalized BP is a suitable candidate for electrocatalytic overall water splitting,and provides effective strategies for constructing metal-lightweighted economic electrocatalysts.展开更多
Seawater splitting into hydrogen,a promising technology,is seriously limited by the durability and tolerance of electrocatalysts for chlorine ions in seawater at large current densities due to chloride oxidation and c...Seawater splitting into hydrogen,a promising technology,is seriously limited by the durability and tolerance of electrocatalysts for chlorine ions in seawater at large current densities due to chloride oxidation and corrosion.Here,we present a robust and weak-nucleophilicity nickel-iron hydroxide electrocatalyst with excellent selectivity for oxygen evolution and an inert response for chlorine ion oxidation which are key and highly desired for efficient seawater electrolysis.Such a weak-nucleophilicity electrocatalyst can well match with strong-nucleophilicity OH-compared with the weak-nucleophilicity Cl^(-),resultantly,the oxidation of OH-in electrolyte can be more easily achieved relative to chlorine ion oxidation,confirmed by ethylenediaminetetraacetic acid disodium probing test.Further,no strongly corrosive hypochlorite is produced when the operating voltage reaches about 2.1 V vs.RHE,a potential that is far beyond the thermodynamic potential of chlorine ion oxidatio n.This concept and approach to reasonably designing weaknucleophilicity electrocatalysts that can greatly avoid chlorine ion oxidation under alkaline seawater environments can push forward the seawater electrolysis technology and also accelerate the development of green hydrogen technique.展开更多
Iron-rich electrolytic manganese residue(IREMR)is an industrial waste produced during the processing of electrolytic metal manganese,and it contains certain amounts of Fe and Mn resources and other heavy metals.In thi...Iron-rich electrolytic manganese residue(IREMR)is an industrial waste produced during the processing of electrolytic metal manganese,and it contains certain amounts of Fe and Mn resources and other heavy metals.In this study,the slurry electrolysis technique was used to recover high-purity Fe powder from IREMR.The effects of IREMR and H2SO4 mass ratio,current density,reaction temper-ature,and electrolytic time on the leaching and current efficiencies of Fe were studied.According to the results,high-purity Fe powder can be recovered from the cathode plate,and the slurry electrolyte can be recycled.The leaching efficiency,current efficiency,and purity of Fe reached 92.58%,80.65%,and 98.72wt%,respectively,at a 1:2.5 mass ratio of H2SO4 and IREMR,reaction temperature of 60℃,electric current density of 30 mA/cm^(2),and reaction time of 8 h.In addition,vibrating sample magnetometer(VSM)analysis showed that the coercivity of electrolytic iron powder was 54.5 A/m,which reached the advanced magnetic grade of electrical pure-iron powder(DT4A coercivity standard).The slurry electrolytic method provides fundamental support for the industrial application of Fe resource recovery in IRMER.展开更多
The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)R...The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)RRs)in solid oxide elec-trolysis cells(SOECs).However,practical appli-cation of nanofiber-based electrodes faces chal-lenges in establishing sufficient interfacial contact and adhesion with the dense electrolyte.To tackle this challenge,a novel hybrid nanofiber electrode,La_(0.6)Sr_(0.4)Co_(0.15)Fe_(0.8)Pd_(0.05)O_(3-δ)(H-LSCFP),is developed by strategically incorporating low aspect ratio crushed LSCFP nanofibers into the excess porous interspace of a high aspect ratio LSCFP nanofiber framework synthesized via electrospinning technique.After consecutive treatment in 100% H_(2) and CO_(2) at 700°C,LSCFP nanofibers form a perovskite phase with in situ exsolved Co metal nanocatalysts and a high concentration of oxygen species on the surface,enhancing CO_(2) adsorption.The SOEC with the H-LSCFP electrode yielded an outstanding current density of 2.2 A cm^(-2) in CO_(2) at 800°C and 1.5 V,setting a new benchmark among reported nanofiber-based electrodes.Digital twinning of the H-LSCFP reveals improved contact adhesion and increased reaction sites for CO_(2)RR.The present work demonstrates a highly catalytically active and robust nanofiber-based fuel electrode with a hybrid structure,paving the way for further advancements and nanofiber applications in CO_(2)-SOECs.展开更多
Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we r...Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.展开更多
The epitaxial heterostructure can be rationally designed based on the in situ growth of two compatible phases with lattice similarity,in which the modulated electronic states and tuned adsorption behaviors are conduci...The epitaxial heterostructure can be rationally designed based on the in situ growth of two compatible phases with lattice similarity,in which the modulated electronic states and tuned adsorption behaviors are conducive to the enhancement of electrocatalytic activity.Herein,theoretical simulations first disclose the charge transfer trend and reinforced inherent electron conduction around the epitaxial heterointerface between Ru clusters and Ni_(3)N substrate(cRu-Ni_(3)N),thus leading to the optimized adsorption behaviors and reduced activation energy barriers.Subsequently,the defectrich nanosheets with the epitaxially grown cRu-Ni_(3)N heterointerface are successfully constructed.Impressively,by virtue of the superiority of intrinsic activity and reaction kinetics,such unique epitaxial heterostructure exhibits remarkable bifunctional catalytic activity toward electrocatalytic OER(226 mV@20 mA cm^(−2))and HER(32 mV@10 mA cm^(−2))in alkaline media.Furthermore,it also shows great application prospect in alkaline freshwater and seawater splitting,as well as solar-to-hydrogen integrated system.This work could provide beneficial enlightenment for the establishment of advanced electrocatalysts with epitaxial heterointerfaces.展开更多
Stro ntium-doped lanthanum ferrite(LSF)is a potential ceramic cathode for direct CO_(2) electrolysis in solid oxide electrolysis cells(SOECs),but its application is limited by insufficient catalytic activity and stabi...Stro ntium-doped lanthanum ferrite(LSF)is a potential ceramic cathode for direct CO_(2) electrolysis in solid oxide electrolysis cells(SOECs),but its application is limited by insufficient catalytic activity and stability in CO_(2)-containing atmospheres.Herein,a novel strategy is proposed to enhance the electrolytic performance as well as chemical stability,achieved by doping F into the O-site of the perovskite LSF.Doping F does not change the phase structure but reduces the cell volume and improves the chemical stability in a CO_(2)-rich atmosphere.Importantly,F doping favors oxygen vacancy formation,increases oxygen vacancy concentration,and enhances the CO_(2) adsorption capability.Meanwhile,doping with F greatly improves the kinetics of the CO_(2) reduction reaction.For example,kchem increases by 78%from3.49×10^(-4) cm s^(-1) to 6.24×10^(-4) cm s^(-1),and Dchem doubles from 4.68×10^(-5) cm^(2) s^(-1) to 9.45×10^(-5)cm^(2) s^(-1).Consequently,doping F significantly increases the electrochemical performance,such as reducing R_(p) by 52.2%from 0.226Ωcm^(2) to 0.108Ωcm^(2) at 800℃.As a result,the single cell with the Fcontaining cathode exhibits an extremely high current density of 2.58 A cm^(-2) at 800℃and 1.5 V,as well as excellent durability over 200 h for direct CO_(2) electrolysis in SOECs.展开更多
Water electrolysis is a promising technology to produce hydrogen but it was severely restricted by the slow oxygen evolution reaction(OER).Herein,we firstly reported an advanced electrocatalyst of MOF-derived hollow Z...Water electrolysis is a promising technology to produce hydrogen but it was severely restricted by the slow oxygen evolution reaction(OER).Herein,we firstly reported an advanced electrocatalyst of MOF-derived hollow Zn-Co-Ni sulfides(ZnS@Co_(9)S_(8)@Ni_(3)S_(2)-1/2,abbreviated as ZCNS-1/2)nanosword arrays(NSAs)with remarkable hydrogen evolution reaction(HER),OER and corresponding water electrolysis performance.To reach a current density of 10 mA cm^(-2),the cell voltage of assembled ZCNS-1/2//ZCNS-1/2 for urea electrolysis(1.314 V)is 208 mV lower than that for water electrolysis(1.522 V)and stably catalyzed for over 15 h,substantially outperforming the most reported water and urea electrolysis electrocatalysts.Density functional theory calculations and experimental result clearly reveal that the properties of large electrochemical active surface area(ECSA)caused by hollow NSAs and fast charge transfer resulted from the Co_(9)S_(8)@Ni_(3)S_(2) heterostructure endow the ZCNS-1/2 electrode with an enhanced electrocatalytic performance.展开更多
Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the ...Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis.展开更多
CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy...CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy is used to replicate intermittent energy availability,and the stability and conversion rate of the cyclic operation by a large-scale flat-tube SOEC are studied.One hundred cycles under pulsed current ranging from -100 to -300 mA/cm^(2) with a total operating time of about 800 h were carried out.The results show that after 100 cycles,the cell voltage attenuates by 0.041%/cycle in the high current stage of−300 mA/cm^(2),indicating that the lifetime of the cell can reach up to about 500 cycles.The total CO_(2) conversion rate reached 52%,which is close to the theoretical value of 54.3% at -300 mA/cm^(2),and the calculated efficiency approached 98.2%,assuming heat recycling.This study illustrates the significant advantages of SOEC in efficient electrochemical energy conversion,carbon emission mitigation,and seasonal energy storage.展开更多
Developing high-efficiency electrocatalysts for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) is required to enhance the sluggish kinetics of water dissociation and optimize the adsorption free e...Developing high-efficiency electrocatalysts for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) is required to enhance the sluggish kinetics of water dissociation and optimize the adsorption free energy of reaction intermediates.Herein,we tackle this challenge by incorporating high-valence Zr into CoP(ZrxCo_(1-x)P),which significantly accelerates the elementary steps of water electrolysis.Theoretical calculations indicate that the appropriate Zr incorporation effectively expedites the sluggish H2O dissociation kinetics and optimizes the adsorption energy of reaction intermediates for boosting the alkaline water electrolysis.These are confirmed by the experimental results of Zr_(0.06)Co_(0.94)P catalyst that delivers exceptional electrochemical activity.The overpotentials at the current density of 10 mA cm^(-2)(j10) are only 62(HER) and 240 mV(OER) in alkaline media.Furthermore,the Zr_(0.06)Co_(0.94)P/CC‖Zr_(0.06)Co_(0.94)P/CC system exhibits superior overall water splitting activity(1.53 V/j10),surpassing most of the reported bifunctional catalysts.This high-valence Zr incorporation and material design methods explore new avenues for realizing high-performance non-noble metal electrocatalysts.展开更多
Electrochemical reduction of CO_(2)into valuable fuels and chemicals has become a contemporary research area,where the heterogeneous catalyst plays a critical role.Metal nanoparticles supported on oxides performing as...Electrochemical reduction of CO_(2)into valuable fuels and chemicals has become a contemporary research area,where the heterogeneous catalyst plays a critical role.Metal nanoparticles supported on oxides performing as active sites of electrochemical reactions have been the focus of intensive investigation.Here,we review the CO_(2)reduction with active materials prepared by exsolution.The fundamental of exsolution was summarized in terms of mechanism and models,materials,and driven forces.The advances in the exsolved materials used in hightemperature CO_(2)electrolysis were catalogued into tailored interfaces,synergistic effects on alloy particles,phase transition,reversibility and electrochemical switching.展开更多
Small-molecule electrooxidation-boosted water electrolysis(WE)is an energy-saving method for hydrogen(H2)production.Herein,PdPt bimetallenes(PdPt BMLs)are obtained through the simple galvanic replacement reaction.PdPt...Small-molecule electrooxidation-boosted water electrolysis(WE)is an energy-saving method for hydrogen(H2)production.Herein,PdPt bimetallenes(PdPt BMLs)are obtained through the simple galvanic replacement reaction.PdPt BMLs reveal 2.93-fold enhancement in intrinsic electroactivity and 4.53-fold enhancement in mass electroactivity for the formate oxidation reaction(FOR)with respect to Pd metallenes(Pd MLs)at 0.50 V potential due to the synergistic effect.Meanwhile,the introduction of Pt atoms also considerably increases the electroactivity of PdPt BMLs for hydrogen evolution reaction(HER)with respect to Pd MLs in an alkaline medium,which even exceeds that with the use of commercial Pt nanocrystals.Inspired by the outstanding FOR and HER electroactivity of bifunctional PdPt BMLs,a two-electrode FOR-boosted WE system(FOR-WE)is constructed by using PdPt BMLs as the cathode and the anode.The FOR-WE system only requires an operational voltage of 0.31 V to achieve H2 production,which is 1.48 V lower than that(ca.1.79 V)with the use of the traditional WE system.展开更多
Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)holds great promise in green energy conversion and storage.However,for current CO_(2) electrolyzers that rely on the oxygen evolution reaction,a large portion of the...Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)holds great promise in green energy conversion and storage.However,for current CO_(2) electrolyzers that rely on the oxygen evolution reaction,a large portion of the input energy is"wasted"at the anode due to the high overpotential requirement and the recovery of low-value oxygen.To make efficient use of the electricity during electrolysis,coupling CO_(2)RR with anodic alternatives that have low energy demands and/or profitable returns with high-value products is then promising.Herein,we review the latest advances in paired systems for simultaneous CO_(2) reduction and anode valorization.We start with the cases integrating CO_(2)RR with concurrent alternative oxidation,such as inorganic oxidation using chloride,sulfide,ammonia and urea,and organic oxidation using alcohols,aldehydes and primary amines.The paired systems that couple CO_(2)RR with on-site oxidative upgrading of CO_(2)-reduced chemicals are also introduced.The coupling mechanism,electrochemical performance and economic viability of these co-electrolysis systems are discussed.Thereby,we then point out the mismatch issues between the cathodic and anodic reactions regrading catalyst ability,electrolyte solution and reactant supply that will challenge the applications of these paired electrolysis systems.Opportunities to address these issues are further proposed,providing some guidance for future research.展开更多
The key challenge of industrial water electrolysis is to design catalytic electrodes that can stabilize high current density with low power consumption(i.e.,overpotential),while industrial harsh conditions make the ba...The key challenge of industrial water electrolysis is to design catalytic electrodes that can stabilize high current density with low power consumption(i.e.,overpotential),while industrial harsh conditions make the balance between electrode activity and stability more difficult.Here,we develop an efficient and durable electrode for water oxidation reaction(WOR),which yields a high current density of 1000 mA cm−2 at an overpotential of only 284 mV in 1M KOH at 25°C and shows robust stability even in 6M KOH strong alkali with an elevated temperature up to 80°C.This electrode is fabricated from a cheap nickel foam(NF)substrate through a simple one-step solution etching method,resulting in the growth of ultrafine phosphorus doped nickel-iron(oxy)hydroxide[P-(Ni,Fe)O_(x)H_(y)]nanoparticles embedded into abundant micropores on the surface,featured as a self-stabilized catalyst–substrate fusion electrode.Such self-stabilizing effect fastens highly active P-(Ni,Fe)O_(x)H_(y)species on conductive NF substrates with significant contribution to catalyst fixation and charge transfer,realizing a win–win tactics for WOR activity and durability at high current densities in harsh environments.This work affords a cost-effective WOR electrode that can well work at large current densities,suggestive of the rational design of catalyst electrodes toward industrial-scale water electrolysis.展开更多
Realization of CO_(2) resource utilization is the main development direction of CO_(2) reduction.The CO_(2) methana-tion technology based on microbial electrolysis cell(MEC)has the characteristics of ambient temperatu...Realization of CO_(2) resource utilization is the main development direction of CO_(2) reduction.The CO_(2) methana-tion technology based on microbial electrolysis cell(MEC)has the characteristics of ambient temperature and pressure,green and low-carbon,which meets the need of low-carbon energy transition.However,the lack of the system such as the change of applied voltage and the reactor amplification will affect the methane production efficiency.In this research,the efficiency of methane production with different applied voltages and different types of reactors was carried out.The results were concluded that the maximum methane production rate of the H-type two-chamber microbial electrolysis cells(MECs)at an applied voltage of 0.8 V was obtained to be 1.15 times higher than that of 0.5 V;under the same conditions of inoculated sludge,the reactor was amplified 2.5 times and the cumulative amount of methane production was 1.04 times higher than the original.This research can provide a theoretical basis and technical reference for the early industrial application of CO_(2) methanation tech-nology based on MEC.展开更多
The solid oxide electrolytic cell(SOEC)is one of the most promising energy conversion and storage devices,which could convert CO_(2) to CO with high Faradaic efficiency and production rate.However,the lack of active a...The solid oxide electrolytic cell(SOEC)is one of the most promising energy conversion and storage devices,which could convert CO_(2) to CO with high Faradaic efficiency and production rate.However,the lack of active and stable cathode materials impedes their practical applications.Here we focus on the promising perovskite oxide cathode material Sr_(2)Fe_(1.5)Mo_(0.5)O_(6)-σ,with the aim of understanding how A-atom stoichiometry and catalytic performance are linked.We find that increasing the strontium content in the perovskite improves the chemisorption of CO_(2) on its surface,forming a SrCO_(3) phase.This hinders the charge transfer and oxygen exchange processes.Simulta-neously,strontoium segregation to the cathode surface facilitates coking of the surface during CO_(2) electrolysis,which poisons the electrode.Consequently,a small number of Sr deficiencies are optimal for both electrochemical performance and long-term stability.Our results provide new insights for designing high-performance CO_(2) electrolysis cathode materials.展开更多
基金supported by the National Key Research and Development Program of China(2022YFB4002100)the Key Program of the National Natural Science Foundation of China(22090032,22090030)。
文摘Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,particularly the presence of aggressive Cl^(-),has been proven to be prone to parasitic chloride ion oxidation and corrosion reactions,thus restricting seawater electrolyzer lifetime.Herein,hierarchical structure(Ni,Fe)O(OH)@NiCoS nanorod arrays(NAs)catalysts with heterointerfaces and localized oxygen vacancies were synthesized at nickel foam substrates via the combination of hydrothermal and annealing methods to boost seawater dissociation.The hiera rchical nanostructure of NiCoS NAs enhanced electrode charge transfer rate and active surface area to accelerate oxygen evolution reaction(OER)and generated sulfate gradient layers to repulsive aggressive Cl^(-).The fabricated heterostructure and vacancies of(Ni,Fe)O(OH)tuned catalyst electronic structure into an electrophilic state to enhance the binding affinity of hydroxyl intermediates and facilitate the structural transformation into amorphousγ-NiFeOOH for promoting OER.Furthermore,through operando electrochemistry techniques,we found that theγ-NiFeOOH possessing an unsaturated coordination environment and lattice-oxygen-participated OER mechanism can minimize electrode Cl^(-)corrosion enabled by stabilizing the adsorption of OH*intermediates,making it one of the best OER catalysts in the seawater medium reported to date.Consequently,these catalysts can deliver current densities of 100 and 500 mA cm-2for boosting OER at minimal overpotentials of 245and 316 mV,respectively,and thus prevent chloride ion oxidation simultaneously.Impressively,a highly stable anion exchange membrane(AEM)seawater electrolyzer based on the non-noble metal heterostructure electrodes reached a record low degradation rate under 100μV h-1at constant industrial current densities of 400 and 600 mA cm-2over 300 h,which exhibits a promising future for the nonprecious and stable AEMWE in the direct seawater electrolysis industry.
基金supported by the National Natural Science Foundation of China(No.21972124,22102105)a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institution.L.Feng also thanks the support of the Six Talent Peaks Project of Jiangsu Province(XCL-070-2018).
文摘Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis reactions.Herein,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen generation.Experimental and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol electrolysis.Moreover,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping technique.The high catalytic kinetics and stability,as well as the promotion effect,were also carefully discussed.Specifically,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.
基金supported by the National Key Research and Development Program(2022YFB4202200)the Fundamental Research Funds for the Central Universities and sponsored by Shanghai Pujiang Program(22PJ1413100)。
文摘Green hydrogen produced by water electrolysis combined with renewable energy is a promising alternative to fossil fuels due to its high energy density with zero-carbon emissions.Among water electrolysis technologies,the anion exchange membrane(AEM) water electrolysis has gained intensive attention and is considered as the next-generation emerging technology due to its potential advantages,such as the use of low-cost non-noble metal catalysts,the relatively mature stack assembly process,etc.However,the AEM water electrolyzer is still in the early development stage of the kW-level stack,which is mainly attributed to severe performance decay caused by the core component,i.e.,AEM.Here,the review comprehensively presents the recent progress of advanced AEM from the view of the performance of water electrolysis cells.Herein,fundamental principles and critical components of AEM water electrolyzers are introduced,and work conditions of AEM water electrolyzers and AEM performance improvement strategies are discussed.The challenges and perspectives are also analyzed.
基金This work was jointly supported by the National Natural Science Foundation of China(Grant Nos.52371236 and 21872109)Natural Science Foundation of Shaanxi Province(No.2020JQ-165)China Postdoctoral Science Foundation(No.2019M663698).
文摘The metal-lightweighted electrocatalysts for water splitting are highly desired for sustainable and economic hydrogen energy deployments,but challengeable.In this work,a low-content Ni-functionalized approach triggers the high capability of black phosphorene(BP)with hydrogen and oxygen evolution reaction(HER/OER)bifunctionality.Through a facile in situ electro-exfoliation route,the ionized Ni sites are covalently functionalized in BP nanosheets with electron redistribution and controllable metal contents.It is found that the as-fabricated Ni-BP electrocatalysts can drive the water splitting with much enhanced HER and OER activities.In 1.0 M KOH electrolyte,the optimized 1.5 wt%Nifunctionalized BP nanosheets have readily achieved low overpotentials of 136 mV for HER and 230 mV for OER at 10 mA cm^(−2).Moreover,the covalently bonding between Ni and P has also strengthened the catalytic stability of the Ni-functionalized BP electrocatalyst,stably delivering the overall water splitting for 50 h at 20 mA cm^(−2).Theoretical calculations have revealed that Ni–P covalent binding can regulate the electronic structure and optimize the reaction energy barrier to improve the catalytic activity effectively.This work confirms that Ni-functionalized BP is a suitable candidate for electrocatalytic overall water splitting,and provides effective strategies for constructing metal-lightweighted economic electrocatalysts.
基金supported by the National Natural Science Foundation of China(NSFC,No.22078052)the Fundamental Research Funds for the Central Universities(DUT22ZD207,DUT22LAB612)。
文摘Seawater splitting into hydrogen,a promising technology,is seriously limited by the durability and tolerance of electrocatalysts for chlorine ions in seawater at large current densities due to chloride oxidation and corrosion.Here,we present a robust and weak-nucleophilicity nickel-iron hydroxide electrocatalyst with excellent selectivity for oxygen evolution and an inert response for chlorine ion oxidation which are key and highly desired for efficient seawater electrolysis.Such a weak-nucleophilicity electrocatalyst can well match with strong-nucleophilicity OH-compared with the weak-nucleophilicity Cl^(-),resultantly,the oxidation of OH-in electrolyte can be more easily achieved relative to chlorine ion oxidation,confirmed by ethylenediaminetetraacetic acid disodium probing test.Further,no strongly corrosive hypochlorite is produced when the operating voltage reaches about 2.1 V vs.RHE,a potential that is far beyond the thermodynamic potential of chlorine ion oxidatio n.This concept and approach to reasonably designing weaknucleophilicity electrocatalysts that can greatly avoid chlorine ion oxidation under alkaline seawater environments can push forward the seawater electrolysis technology and also accelerate the development of green hydrogen technique.
基金supported by the Key Research and Development Program of Guangxi Province,China (No.AB23075174)the National Natural Science Foundation of China (No.52174386)the Science and Technology Plan Project of Sichuan Province,China (No.2022YFS0459).
文摘Iron-rich electrolytic manganese residue(IREMR)is an industrial waste produced during the processing of electrolytic metal manganese,and it contains certain amounts of Fe and Mn resources and other heavy metals.In this study,the slurry electrolysis technique was used to recover high-purity Fe powder from IREMR.The effects of IREMR and H2SO4 mass ratio,current density,reaction temper-ature,and electrolytic time on the leaching and current efficiencies of Fe were studied.According to the results,high-purity Fe powder can be recovered from the cathode plate,and the slurry electrolyte can be recycled.The leaching efficiency,current efficiency,and purity of Fe reached 92.58%,80.65%,and 98.72wt%,respectively,at a 1:2.5 mass ratio of H2SO4 and IREMR,reaction temperature of 60℃,electric current density of 30 mA/cm^(2),and reaction time of 8 h.In addition,vibrating sample magnetometer(VSM)analysis showed that the coercivity of electrolytic iron powder was 54.5 A/m,which reached the advanced magnetic grade of electrical pure-iron powder(DT4A coercivity standard).The slurry electrolytic method provides fundamental support for the industrial application of Fe resource recovery in IRMER.
基金This work was supported by the National Research Foundation of Korea(NRF)grant funded by the Korean Government(MSIT)(2019M3E6A1103944,2020R1A2C2010690).
文摘The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)RRs)in solid oxide elec-trolysis cells(SOECs).However,practical appli-cation of nanofiber-based electrodes faces chal-lenges in establishing sufficient interfacial contact and adhesion with the dense electrolyte.To tackle this challenge,a novel hybrid nanofiber electrode,La_(0.6)Sr_(0.4)Co_(0.15)Fe_(0.8)Pd_(0.05)O_(3-δ)(H-LSCFP),is developed by strategically incorporating low aspect ratio crushed LSCFP nanofibers into the excess porous interspace of a high aspect ratio LSCFP nanofiber framework synthesized via electrospinning technique.After consecutive treatment in 100% H_(2) and CO_(2) at 700°C,LSCFP nanofibers form a perovskite phase with in situ exsolved Co metal nanocatalysts and a high concentration of oxygen species on the surface,enhancing CO_(2) adsorption.The SOEC with the H-LSCFP electrode yielded an outstanding current density of 2.2 A cm^(-2) in CO_(2) at 800°C and 1.5 V,setting a new benchmark among reported nanofiber-based electrodes.Digital twinning of the H-LSCFP reveals improved contact adhesion and increased reaction sites for CO_(2)RR.The present work demonstrates a highly catalytically active and robust nanofiber-based fuel electrode with a hybrid structure,paving the way for further advancements and nanofiber applications in CO_(2)-SOECs.
基金This study is supported by the National Key Research and Development Program of China(2017YFB0307500).
文摘Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.
基金financially sponsored by the National Natural Science Foundation of China(Grant No.22075223,22179104)the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology)(2021-ZD-4)the Fundamental Research Funds for the Central Universities(No.2020-YB-012)。
文摘The epitaxial heterostructure can be rationally designed based on the in situ growth of two compatible phases with lattice similarity,in which the modulated electronic states and tuned adsorption behaviors are conducive to the enhancement of electrocatalytic activity.Herein,theoretical simulations first disclose the charge transfer trend and reinforced inherent electron conduction around the epitaxial heterointerface between Ru clusters and Ni_(3)N substrate(cRu-Ni_(3)N),thus leading to the optimized adsorption behaviors and reduced activation energy barriers.Subsequently,the defectrich nanosheets with the epitaxially grown cRu-Ni_(3)N heterointerface are successfully constructed.Impressively,by virtue of the superiority of intrinsic activity and reaction kinetics,such unique epitaxial heterostructure exhibits remarkable bifunctional catalytic activity toward electrocatalytic OER(226 mV@20 mA cm^(−2))and HER(32 mV@10 mA cm^(−2))in alkaline media.Furthermore,it also shows great application prospect in alkaline freshwater and seawater splitting,as well as solar-to-hydrogen integrated system.This work could provide beneficial enlightenment for the establishment of advanced electrocatalysts with epitaxial heterointerfaces.
基金supported by the National Key R&D Program of China(2021YFB4001401)the National Natural Science Foundation of China(51972298)。
文摘Stro ntium-doped lanthanum ferrite(LSF)is a potential ceramic cathode for direct CO_(2) electrolysis in solid oxide electrolysis cells(SOECs),but its application is limited by insufficient catalytic activity and stability in CO_(2)-containing atmospheres.Herein,a novel strategy is proposed to enhance the electrolytic performance as well as chemical stability,achieved by doping F into the O-site of the perovskite LSF.Doping F does not change the phase structure but reduces the cell volume and improves the chemical stability in a CO_(2)-rich atmosphere.Importantly,F doping favors oxygen vacancy formation,increases oxygen vacancy concentration,and enhances the CO_(2) adsorption capability.Meanwhile,doping with F greatly improves the kinetics of the CO_(2) reduction reaction.For example,kchem increases by 78%from3.49×10^(-4) cm s^(-1) to 6.24×10^(-4) cm s^(-1),and Dchem doubles from 4.68×10^(-5) cm^(2) s^(-1) to 9.45×10^(-5)cm^(2) s^(-1).Consequently,doping F significantly increases the electrochemical performance,such as reducing R_(p) by 52.2%from 0.226Ωcm^(2) to 0.108Ωcm^(2) at 800℃.As a result,the single cell with the Fcontaining cathode exhibits an extremely high current density of 2.58 A cm^(-2) at 800℃and 1.5 V,as well as excellent durability over 200 h for direct CO_(2) electrolysis in SOECs.
基金financially supported by the National Science Foundation of China (Grant No.21802126).
文摘Water electrolysis is a promising technology to produce hydrogen but it was severely restricted by the slow oxygen evolution reaction(OER).Herein,we firstly reported an advanced electrocatalyst of MOF-derived hollow Zn-Co-Ni sulfides(ZnS@Co_(9)S_(8)@Ni_(3)S_(2)-1/2,abbreviated as ZCNS-1/2)nanosword arrays(NSAs)with remarkable hydrogen evolution reaction(HER),OER and corresponding water electrolysis performance.To reach a current density of 10 mA cm^(-2),the cell voltage of assembled ZCNS-1/2//ZCNS-1/2 for urea electrolysis(1.314 V)is 208 mV lower than that for water electrolysis(1.522 V)and stably catalyzed for over 15 h,substantially outperforming the most reported water and urea electrolysis electrocatalysts.Density functional theory calculations and experimental result clearly reveal that the properties of large electrochemical active surface area(ECSA)caused by hollow NSAs and fast charge transfer resulted from the Co_(9)S_(8)@Ni_(3)S_(2) heterostructure endow the ZCNS-1/2 electrode with an enhanced electrocatalytic performance.
基金supported by the financial support from Natural Science Foundation of China(Nos.21871065,22209129 and 22071038)High-Level Innovation and Entrepreneurship(QCYRCXM-2022-123)+1 种基金support from the“Young Talent Support Plan”of Xi’an Jiaotong University(HG6J024)“Young Talent Lift Plan”of Xi’an city(095920221352).
文摘Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis.
基金National Key Research&Development Project,Grant/Award Number:2017YFE0129300Ningbo Science and Technology Innovation 2025 Major Project,Grant/Award Numbers:2019B10046,2020Z107+2 种基金Zhejiang Provincial Key R&D Program,Grant/Award Number:2021C01101National Natural Science Foundation of China,Grant/Award Numbers:U20A20251,11932005The from 0 to 1 Innovative Program of CAS,Grant/Award Number:ZDBS-LY-JSC021。
文摘CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy is used to replicate intermittent energy availability,and the stability and conversion rate of the cyclic operation by a large-scale flat-tube SOEC are studied.One hundred cycles under pulsed current ranging from -100 to -300 mA/cm^(2) with a total operating time of about 800 h were carried out.The results show that after 100 cycles,the cell voltage attenuates by 0.041%/cycle in the high current stage of−300 mA/cm^(2),indicating that the lifetime of the cell can reach up to about 500 cycles.The total CO_(2) conversion rate reached 52%,which is close to the theoretical value of 54.3% at -300 mA/cm^(2),and the calculated efficiency approached 98.2%,assuming heat recycling.This study illustrates the significant advantages of SOEC in efficient electrochemical energy conversion,carbon emission mitigation,and seasonal energy storage.
基金National Natural Science Foundation of China (22202080,51872116, 12034002)the fellowship of China Postdoctoral Science Foundation (2022 M711296)the Jilin Province Science and Technology Development Program (20210301009GX)。
文摘Developing high-efficiency electrocatalysts for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) is required to enhance the sluggish kinetics of water dissociation and optimize the adsorption free energy of reaction intermediates.Herein,we tackle this challenge by incorporating high-valence Zr into CoP(ZrxCo_(1-x)P),which significantly accelerates the elementary steps of water electrolysis.Theoretical calculations indicate that the appropriate Zr incorporation effectively expedites the sluggish H2O dissociation kinetics and optimizes the adsorption energy of reaction intermediates for boosting the alkaline water electrolysis.These are confirmed by the experimental results of Zr_(0.06)Co_(0.94)P catalyst that delivers exceptional electrochemical activity.The overpotentials at the current density of 10 mA cm^(-2)(j10) are only 62(HER) and 240 mV(OER) in alkaline media.Furthermore,the Zr_(0.06)Co_(0.94)P/CC‖Zr_(0.06)Co_(0.94)P/CC system exhibits superior overall water splitting activity(1.53 V/j10),surpassing most of the reported bifunctional catalysts.This high-valence Zr incorporation and material design methods explore new avenues for realizing high-performance non-noble metal electrocatalysts.
基金This work is supported by the National Key Research and Development Program of China(No.2021YFA0718900)the National Natural Science Foundation of China(No.NSCF52102137)+1 种基金We also appreciate the support from Tsinghua University Initiative Scientific Research Program and Open Funds of the State Key Laboratory of Rare Earth Resource Utilization(RERU2022006EPSRC)the Institute for Guo Qiang,Tsinghua University(2020GQG1003).
文摘Electrochemical reduction of CO_(2)into valuable fuels and chemicals has become a contemporary research area,where the heterogeneous catalyst plays a critical role.Metal nanoparticles supported on oxides performing as active sites of electrochemical reactions have been the focus of intensive investigation.Here,we review the CO_(2)reduction with active materials prepared by exsolution.The fundamental of exsolution was summarized in terms of mechanism and models,materials,and driven forces.The advances in the exsolved materials used in hightemperature CO_(2)electrolysis were catalogued into tailored interfaces,synergistic effects on alloy particles,phase transition,reversibility and electrochemical switching.
基金the National Natural Science Foundation of China(22272103)the Shenzhen Stable Supporting Program(20220716001753001 and SZWD2021015)+3 种基金the University Engineering Research Center of Crystal Growth and Applications of Guangdong Province(2020GCZX005)the Science and Technology Innovation Team of Shaanxi Province(2023-CX-TD-27 and 2022TD-35)the Fundamental Research Funds for the Central Universities(GK202202001)the 111 Project(B14041).
文摘Small-molecule electrooxidation-boosted water electrolysis(WE)is an energy-saving method for hydrogen(H2)production.Herein,PdPt bimetallenes(PdPt BMLs)are obtained through the simple galvanic replacement reaction.PdPt BMLs reveal 2.93-fold enhancement in intrinsic electroactivity and 4.53-fold enhancement in mass electroactivity for the formate oxidation reaction(FOR)with respect to Pd metallenes(Pd MLs)at 0.50 V potential due to the synergistic effect.Meanwhile,the introduction of Pt atoms also considerably increases the electroactivity of PdPt BMLs for hydrogen evolution reaction(HER)with respect to Pd MLs in an alkaline medium,which even exceeds that with the use of commercial Pt nanocrystals.Inspired by the outstanding FOR and HER electroactivity of bifunctional PdPt BMLs,a two-electrode FOR-boosted WE system(FOR-WE)is constructed by using PdPt BMLs as the cathode and the anode.The FOR-WE system only requires an operational voltage of 0.31 V to achieve H2 production,which is 1.48 V lower than that(ca.1.79 V)with the use of the traditional WE system.
基金financially supported by the National Natural Science Foundation of China(22002084,22072081)the China Postdoctoral Science Foundation(2020M683420)+1 种基金the Fundamental Research Funds for the Central Universities(GK202103111)the 111 Project(B21005)。
文摘Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)holds great promise in green energy conversion and storage.However,for current CO_(2) electrolyzers that rely on the oxygen evolution reaction,a large portion of the input energy is"wasted"at the anode due to the high overpotential requirement and the recovery of low-value oxygen.To make efficient use of the electricity during electrolysis,coupling CO_(2)RR with anodic alternatives that have low energy demands and/or profitable returns with high-value products is then promising.Herein,we review the latest advances in paired systems for simultaneous CO_(2) reduction and anode valorization.We start with the cases integrating CO_(2)RR with concurrent alternative oxidation,such as inorganic oxidation using chloride,sulfide,ammonia and urea,and organic oxidation using alcohols,aldehydes and primary amines.The paired systems that couple CO_(2)RR with on-site oxidative upgrading of CO_(2)-reduced chemicals are also introduced.The coupling mechanism,electrochemical performance and economic viability of these co-electrolysis systems are discussed.Thereby,we then point out the mismatch issues between the cathodic and anodic reactions regrading catalyst ability,electrolyte solution and reactant supply that will challenge the applications of these paired electrolysis systems.Opportunities to address these issues are further proposed,providing some guidance for future research.
基金National Natural Science Foundation of China,Grant/Award Numbers:11974303,12074332Qinglan Project of Jiangsu Province,Grant/Award Number:137050317the Interdisciplinary Research Project of Chemistry Discipline,Grant/Award Number:yzuxk202014 and High‐End Talent Program of Yangzhou University,Grant/Award Number:137080051。
文摘The key challenge of industrial water electrolysis is to design catalytic electrodes that can stabilize high current density with low power consumption(i.e.,overpotential),while industrial harsh conditions make the balance between electrode activity and stability more difficult.Here,we develop an efficient and durable electrode for water oxidation reaction(WOR),which yields a high current density of 1000 mA cm−2 at an overpotential of only 284 mV in 1M KOH at 25°C and shows robust stability even in 6M KOH strong alkali with an elevated temperature up to 80°C.This electrode is fabricated from a cheap nickel foam(NF)substrate through a simple one-step solution etching method,resulting in the growth of ultrafine phosphorus doped nickel-iron(oxy)hydroxide[P-(Ni,Fe)O_(x)H_(y)]nanoparticles embedded into abundant micropores on the surface,featured as a self-stabilized catalyst–substrate fusion electrode.Such self-stabilizing effect fastens highly active P-(Ni,Fe)O_(x)H_(y)species on conductive NF substrates with significant contribution to catalyst fixation and charge transfer,realizing a win–win tactics for WOR activity and durability at high current densities in harsh environments.This work affords a cost-effective WOR electrode that can well work at large current densities,suggestive of the rational design of catalyst electrodes toward industrial-scale water electrolysis.
基金the Shanghai Science and Technology Development Fund,No.20dz1206300.
文摘Realization of CO_(2) resource utilization is the main development direction of CO_(2) reduction.The CO_(2) methana-tion technology based on microbial electrolysis cell(MEC)has the characteristics of ambient temperature and pressure,green and low-carbon,which meets the need of low-carbon energy transition.However,the lack of the system such as the change of applied voltage and the reactor amplification will affect the methane production efficiency.In this research,the efficiency of methane production with different applied voltages and different types of reactors was carried out.The results were concluded that the maximum methane production rate of the H-type two-chamber microbial electrolysis cells(MECs)at an applied voltage of 0.8 V was obtained to be 1.15 times higher than that of 0.5 V;under the same conditions of inoculated sludge,the reactor was amplified 2.5 times and the cumulative amount of methane production was 1.04 times higher than the original.This research can provide a theoretical basis and technical reference for the early industrial application of CO_(2) methanation tech-nology based on MEC.
基金financially supported by the National Natural Science Foundation of China(No.21975163)Natural Science Foundation of Guangdong Province of China(2020A1515011165)Shenzhen Sci-ence and Technology Program(No.KQTD20190929173914967)and(No.JCYJ20220818100004009)。
文摘The solid oxide electrolytic cell(SOEC)is one of the most promising energy conversion and storage devices,which could convert CO_(2) to CO with high Faradaic efficiency and production rate.However,the lack of active and stable cathode materials impedes their practical applications.Here we focus on the promising perovskite oxide cathode material Sr_(2)Fe_(1.5)Mo_(0.5)O_(6)-σ,with the aim of understanding how A-atom stoichiometry and catalytic performance are linked.We find that increasing the strontium content in the perovskite improves the chemisorption of CO_(2) on its surface,forming a SrCO_(3) phase.This hinders the charge transfer and oxygen exchange processes.Simulta-neously,strontoium segregation to the cathode surface facilitates coking of the surface during CO_(2) electrolysis,which poisons the electrode.Consequently,a small number of Sr deficiencies are optimal for both electrochemical performance and long-term stability.Our results provide new insights for designing high-performance CO_(2) electrolysis cathode materials.
