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期刊信息/Journal information
能源化学
能源化学

包信和 ALEXIS T.BELL

双月刊

2095-4956

jngc@dicp.ac.cn

0411-84379237

116023

大连市中山路457号

能源化学/Journal Journal of Energy ChemistryCSCDCSTPCD北大核心EISCI
查看更多>>本刊旨在报道世界范围内天然气化学及其相关领域的最新发展动态和科技信息,增进国际交流,促进科技发展。以天然气及其相关领域从事化学和化学工程方面研究的科研人员及工程技术人员、大专院校的本科生、研究生和教师等为读者对象。
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    Lattice strain induced by trace Pt single atoms in nickel for accelerating industrial hydrogen evolution

    Rui YaoYun WuKaiyang ZhangShuhui Fan...
    503-511页
    查看更多>>摘要:Strategically designing the electrocatalytic system and cleverly inducing strain is an effective approach to balance the cost and activity of Pt-based electrocatalysts for industrial-scale hydrogen production.Herein,we present a unipolar pulsed electrodeposition(UPED)strategy to induce strain in the Ni lattice by introducing trace amounts of Pt single atoms(SAs)(0.22 wt%).The overpotential decreased by 183 mV at 10 mA cm-2 in 1.0 M KOH after introducing trace amounts of PtsAs.The industrial electrolyzer,assem-bled with PtsAsNi cathode and a commercial NiFeOx anode,requires a cell voltage of 1.90 V to attain 1 A cm-2 of current density and remains stable for 280 h,demonstrating significant potential for practical applications.Spherical aberration corrected scanning transmission electron microscopy(AC-STEM),X-ray absorption(XAS),and geometric phase analysis(GPA)indicate that the introduction of trace amounts of Pt SAs induces tensile strain in the Ni lattice,thereby altering the local electronic structure and coordi-nation environment around cubic Ni for enhancing the water decomposition kinetics and fundamentally changing the reaction pathway.The doping-strain strategy showcases conformational relationships that could offer new ideas to construct efficient hydrogen evolution reaction(HER)electrocatalysts for indus-trial hydrogen production in the future.

    High-performance imidazole-containing polymers for applications in high temperature polymer electrolyte membrane fuel cells

    Tong MuLele WangQian WangYang Wu...
    512-523页
    查看更多>>摘要:This work focuses on the development of high temperature polymer electrolyte membranes(HT-PEMs)as key materials for HT-PEM fuel cells(HT-PEMFCs).Recognizing the challenges associated with the phosphoric acid(PA)doped polybenzimidazole(PBI)membranes,including the use of carcinogenic monomers and complex synthesis procedures,this study aims to develop more cost-effective,readily synthesized,and high-performance alternatives.A series of superacid-catalyzed polyhydroxyalkylation reactions have been carefully designed between p-terphenyl and aldehydes bearing imidazole moieties,resulting in a new class of HT-PEMs.It is found that the chemical structure of aldehyde-substituted N-heterocycles significantly impacts the polymerization reaction.Specifically,the use of 1-methyl-2-imidazole-formaldehyde and 1 H-imidazole-4-formaldehyde monomers leads to the formation of high-viscosity,rigid,and ether-free polymers,denoted as PTIm-a and PTIm-b.Membranes fabricated from these polymers,due to their pendent imidazole groups,exhibit an exceptional capacity for PA absorption.Notably,PTIm-a,carrying methylimidazole moieties,demonstrates a superior chemical stability by maintaining morphology and structural stability during 350 h of Fenton testing.After being immersed in 75 wt%PA at 40 ℃,the PTlm-a membrane reaches a PA content of 152%,maintains a good tensile strength of 13.6 MPa,and exhibits a moderate conductivity of 50.2 mS cm-1 at 180 ℃.Under H2/O2 operational conditions,a single cell based on the PTIm-a membrane attains a peak power density of 732 mW cm-2 at 180 ℃ without backpressure.Furthermore,the membrane demonstrates stable cycle stability over 173 h within 18 days at a current density of 200 mA cm-2,indicating its potential for prac-tical application in HT-PEMFCs.This work highlights innovative strategies for the synthesis of advanced HT-PEMs,offering significant improvements in membrane properties and fuel cell performance,thus expanding the horizons of HT-PEMFC technology.

    Promoting electroreduction of nitrite to ammonia over electron-deficient Pd modulated by rectifying Schottky contacts

    Shaobo ZhangYabo GuoLu-Hua ZhangZhihao Feng...
    524-530页
    查看更多>>摘要:Electrochemical nitrite reduction reaction(NO2RR)is a potential sustainable route for regulating the nitrogen cycle and ambient ammonia(NH3)synthesis.However,it remains a challenge to precisely reg-ulate the reaction pathways and inhibit competing reactions(e.g.hydrogenolysis)for efficient and selec-tive NH3 production in an aqueous solution environment.Here,we utilize the Schottky barrier-induced surface electric field to construct high-density electron-deficient Pd nanoparticles by modulating the N content in the carbon carrier to promote the enrichment and immobilization of NO2 on the electrode sur-face,which ensures the ultimate selectivity for NH3.With these properties,Pd@N0.14C with the highest N content achieved excellent catalytic performance for the reduction of NO2 to NH3 with the 100%Faraday efficiency at-0.5 and-0.6 V vs.reversible hydrogen electrode(RHE)for NH3 production,which was sig-nificantly better than Pd/C and Pd@NxC samples with lower N content.This study opens new avenues for rational construction of efficient electrocatalysts for nitrite removal and NH3 electrosynthesis.

    Transforming Cu into Cu2O/RuAl intermetallic heterojunction for lowering the thermodynamic energy barrier of the CO2 reduction and evolution reactions in Li-CO2 battery

    Wenqing MaJiagang HouSiyu LiuTianzhen Jian...
    531-540页
    查看更多>>摘要:The Li-CO2 battery has been under the spotlight of future battery technologies since it can achieve CO2 utilization and energy conversion simultaneously.However,its advancement is hampered by poor energy efficiency and limited reversibility due to the sluggish kinetics of the CO2 reduction and evolution reactions.Herein,a multiscale nanoporous interpenetrating phase nanohybrid of RuAl intermetallic and Cu2O(MP-Cu2O/RuAl)was carved by driving synchronous phase and microstructure evolutions through dealloying of one RuCuAl master alloy.The built-in RuAl intermetallic and Cu2O closely stack to form abundant nano-interfaces with revolutionized electronic structure.The theoretical simulations reveal that the Cu2O/RuAl interface can distinctly reduce the energy barrier of the Li2CO3 decomposition reac-tion.The interconnected pore channels with large surface area can enhance catalytic site accessibility,mass transfer,and uniform deposition of the discharge products.In situ differential electrochemical mass spectrometry discloses that the CO2-to-electron ratio during charging coincides with the theoretical value of 3/4,demonstrating the high efficacy of MP-Cu2O/RuAl in achieving the recycling of CO2.The deal-loying protocol provides an affordable platform to empower transition metal oxides into high-efficiency electrocatalysts by hybridizing with metallic nano-sponge for advancing the application of Li-CO2 batteries.

    Optimized electrochemical ammonia production:From metal-N2/NOx batteries to aqueous metal-NOx-batteries

    Feng-Xiao YanHao-Yu WangYi FengHao Wang...
    541-555页
    查看更多>>摘要:Ammonia plays a crucial role in contemporary society,impacting medicine,agriculture,and the chemical industry.The conventional industrial synthesis of NH3 through the Haber-Bosch technique,carried out under severe reaction conditions,leads to substantial energy consumption and environmental pollution.It is thus imperative for NH3 synthesis methods to be investigated under more favorable conditions.Synthesis of ammonia by electrocatalysis can effectively reduce the environmental damage and other urgent problems,which is a promising solution.Metal-nitrogen series batteries(M-N batteries),such as metal-nitrogen gas batteries,metal-nitrogen oxide batteries and metal-oxynitride batteries have been regarded recently as an exemplar of concurrent NH3 synthesis and energy production.Nonetheless,the large-scale application of these batteries is still limited by numerous challenges are currently existing in building high-efficiency M-N batteries,including poor Faradic efficiency and low NH3 yield.Therefore,a comprehensive overview of M-N batteries is offered,specifically focusing on advanced strategies for designing highly efficient cathode catalysts in anticipation of future developments.The metal anodes,cathodic electro-reduction reactions,and design principles are encompassed in the discus-sion,offering detailed insights to enhance understanding.Mechanisms,feasibility analyses,technoeco-nomic assessments,device combinations,and comparative evaluations are delved into in the review,contributing to a thorough comprehension of diverse systems and their application potential.Perspectives and opportunities for future research directions are also delineated.

    Enhancing lead-free photovoltaic performance:Minimizing buried surface voids in tin perovskite films through weakly polar solvent pre-treatment strategy

    Dongdong YanHan ZhangChensi GongHailong Wang...
    556-561页
    查看更多>>摘要:Buried interfacial voids have always been a notorious phenomenon observed in the fabrication of lead perovskite films.The existence of interfacial voids at the buried interface will capture the carrier,sup-press carrier transport efficiencies,and affect the stability of photovoltaic devices.However,the impact of these buried interfacial voids on tin perovskites,a promising avenue for advancing lead-free photo-voltaics,has been largely overlooked.Here,we utilize an innovative weakly polar solvent pre-treatment strategy(WPSPS)to mitigate buried interfacial voids of tin perovskites.Our investigation reveals the presence of numerous voids in tin perovskites during annealing,attributed to trapped dimethyl sulfoxide(DMSO)used in film formation.The WPSPS method facilitates accelerated DMSO evaporation,effectively reducing residual DMSO.Interestingly,the WPSPS shifts the energy level of PEDOT:PSS downward,making it more aligned with the perovskite.This alignment enhances the effi-ciency of charge carrier transport.As the result,tin perovskite film quality is significantly improved,achieving a maximum power conversion efficiency approaching 12%with only an 8.3%efficiency loss after 1700 h of stability tests,which compares well with the state-of-the-art stability of tin-based per-ovskite solar cells.

    Wearable flexible zinc-ion batteries based on electrospinning technology

    Tiantian ZhangJingge JuZehao ZhangDongyue Su...
    562-587页
    查看更多>>摘要:Flexible wearable batteries are widely used in smartwatches,foldable phones,and fitness trackers due to their thinness and small size.Zinc-based batteries have the advantages of low cost,high safety,and eco-friendliness,which are considered to be the best alternative to flexible lithium-ion batteries(LIBs).Therefore,wearable flexible zinc-ion batteries(FZIBs)have attracted considerable interest as a promising energy storage device.Electrospun nanofibers(ESNFs)have great potential for application in wearable FZIBs due to their low density,high porosity,large specific surface area,and flexibility.Moreover,elec-trospinning technology can achieve the versatility of nanofibers through structural design and incorpo-ration of other multifunctional materials.This paper reviews a wide range of applications of electrospinning in FZIBs,mainly in terms of cathode,anode,separator,polymer electrolyte,and all-in-one flexible batteries.Firstly,the electrospinning device,principles,and influencing parameters are briefly described,showing its positive impact on FZIBs.Subsequently,the energy storage principles and electrode configurations of FZIBs are described,and some of the common problems of the batteries are illustrated,including zinc anode dendrite growth,corrosion,cathode structure collapse,and poor electrical conductivity.This is followed by a comprehensive overview of research progress on the individ-ual components of FZIBs(cathode,anode,separator,and polymer electrolyte)from the perspective of electrostatically spun fiber materials and an in-depth study of all-in-one flexible batteries.Finally,the challenges and future development of FZIBs are individually concluded and look forward.We hope that this work will provide new ideas and avenues for the development of advanced energy technologies and smart wearable systems.

    Recent advances in Ni-based catalysts for the electrochemical oxidation of ethanol

    Xing TanShiming ChenDafeng YanRuixing Du...
    588-614页
    查看更多>>摘要:The electrochemical ethanol oxidation reaction(EOR)plays a crucial role in electrochemical hydrogen production and direct ethanol fuel cells,both vital for utilizing renewable energies.Ni-based catalysts are pivotal in enabling efficient EOR,leading to the formation of acetic acid/acetaldehyde or CO2.These can serve as alternative anodic oxidation reactions for oxygen evolution reaction(OER)in water electrol-ysis or the anodic reaction for direct ethanol fuel cells,respectively.This review explores recent advance-ments in EOR over Ni-based catalysts.It begins with an overview of EOR performance across various Ni-based catalysts,followed by an examination of the reaction chemistry,mechanism,and active sites.The review then delves into strategies for designing highly active Ni-based EOR catalysts.These strategies include promotion with transition metals,noble metals,nonmetals,and carbon materials,as well as cre-ating amorphous structures,special morphologies,and single-atom catalysts.Additionally,it discusses the concept of self-supporting catalysts using three-dimensional porous substrates.Finally,the review highlights emerging methodologies that warrant further exploration,along with future directions for designing highly active and stable EOR catalysts.

    Activation mechanism of conventional electrolytes with amine solvents:Species evolution and hydride-containing interphase formation

    Jinlei ZhangNing YuanJing LiuXiaosong Guo...
    615-622页
    查看更多>>摘要:Rechargeable magnesium(Mg)-metal batteries have brought great expect to overcome the safety and energy density concerns of typical lithium-ion batteries.However,interfacial passivation of the Mg-metal anode impairs the reversible Mg plating/stripping chemistries,resulting in low Coulombic effi-ciency and large overpotential.In this work,a facile isobutylamine(IBA)-assisted activation strategy has been proposed and the fundamental mechanism has been unveiled in a specific way of evolving active species and forming MgH2-based solid-electrolyte interphase.After introducing IBA into a typical electrolyte of magnesium bis(trifluoromethanesulfonyl)imide(Mg(TFSI)2)in diglyme(G2)solvents,elec-trolyte species of[Mg2+(IBA)5]2+and protonated amine-based cations of[(IBA)H]+have been detected by nuclear magnetic resonance and mass spectra.This not only indicates direct solvation of IBA toward Mg2+but also suggests its ionization,which is central to mitigating the decomposition of G2 and TFSI anions by forming neutrally charged[(IBAH+)(TFSI-)]0 and other complex ions.A series of experiments,including cryogenic-electron microscopy,D2O titration-mass spectra,and time of flight secondary ion mass spec-trometry results,reveal a thin,non-passivated,and MgH2-containing interphase on the Mg-metal anode.Besides,uniform and dendrite-free Mg electrodeposits have been revealed in composite electrolytes.Benefiting from the activation effects of IBA,the composite electrolyte displays superior electrochemical performance(overpotential is approximately 0.16 V versus 2.00 V for conventional electrolyte;Coulombic efficiency is above 90%versus<10%for conventional electrolyte).This work offers a fresh direction to advanced electrolyte design for next-generation rechargeable batteries.

    In situ synthesis of SnPS3/Ti3C2Tx hybrid anode via molten salt etching method for superior sodium-ion batteries

    Longsheng ZhongMing YueWenhu XieHongxiao He...
    623-633页
    查看更多>>摘要:Recently,SnPS3 has gained attention as an impressive sodium-ion battery anode material because of its significant theoretical specific capacity derived from the conversion-alloying reaction mechanism.Nevertheless,its practical applicability is restricted by insufficient rate ability,and severe capacity loss due to inadequate electrical conductivity and dramatic volume expansion.Inspired by the electrochem-ical enhancement effect of MXene substrates and the innovative Lewis acidic etching for MXene prepa-ration,SnPS3/Ti3C2Tx MXene(T=—Cl and—O)is constructed by synchronously phospho-sulfurizing Sn/Ti3C2Tx precursor.Benefiting from the boosted Na+diffusion and electron transfer rates,as well as the mitigated stress expansion,the synthesized SnPS3/Ti3C2Tx composite demonstrates enhanced rate capa-bility(647 mA h g-1 at 10 A g-1)alongside satisfactory long-term cycling stability(capacity retention of 94.6%after 2000 cycles at 5 A g-1).Importantly,the assembled sodium-ion full cell delivers an impressive capacity retention of 97.7%after undergoing 1500 cycles at 2 A g-1.Moreover,the sodium storage mech-anism of the SnPS3/Ti3C2Tx electrode is elucidated through in-situ and ex-situ characterizations.This work proposes a novel approach to ameliorate the energy storage performance of thiophosphites by facile in-situ construction of composites with MXene.