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能源与环境材料（英文）
能源与环境材料（英文）
能源与环境材料（英文）/Journal Energy & Environmental MaterialsSCI
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    3D-Printed Monolith Metallic Ni-Mo Electrodes for Ultrahigh Current Hydrogen Evolution

    Yanran XunHongmei JinYuemeng LiShixiang Zhou...
    224-233页
    查看更多>>摘要：In this work,we reported a series of monolithic 3D-printed Ni-Mo alloy electrodes for highly efficient water splitting at high current density(1500 mA cm-2)with excellent stability,which provides a solution to scale up Ni-Mo catalysts for HER to industry use.All possible Ni-Mo metal/alloy phases were achieved by tuning the atomic composition and heat treatment procedure,and they were investigated through both experiment and simulation,and the optimal NiMo phase shows the best performance.Density functional theory(DFT)calculations elucidate that the NiMo phase has the lowest H2O dissociation energy,which further explains the exceptional performance of NiMo.In addition,the microporosity was modulated via controlled thermal treatment,indicating that the 1100 ℃ sintered sample has the best catalytic performance,which is attributed to the high electrochemically active surface area(ECSA).Finally,the four different macrostructures were achieved by 3D printing,and they further improved the catalytic performance.The gyroid structure exhibits the best catalytic performance of driving 500 mA cm-2 at a low overpotential of 228 mV and 1500 mA cm-2 at 325 mV,as it maximizes the efficient bubble removal from the electrode surface,which offers the great potential for high current density water splitting.
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    Insights into the Origins of Solar-Assisted Electrochemical Water Oxidation in Allotropic Co5.47N/CON Heterojunctions

    Sirui LiuQiong GaoBo GengLili Wu...
    234-243页
    查看更多>>摘要：Solar irradiation can efficiently promote the kinetics of the oxygen evolution reaction(OER)during water splitting,where heterojunction catalysts exhibit excellent photoresponsive properties.However,insights into the origins of photoassisted OER catalysis remain unclear,especially the interfaced promotion under convergent solar irradiation(CSI).Herein,novel allotropic Co5.47N/CoN heterojunctions were synthesized,and corresponding OER mechanisms under CSI were comprehensively uncovered from physical and chemical aspects using the in situ Raman technique and electrochemical cyclic voltammetry method.Our results provide a unique mechanism where high-energy UV light promotes the Co3+/4+conversion process in addition to the ordinary photoelectric effect excitation of the Co2+material.Importantly,visible light under CSI can produce a photothermal effect for Co2+excitation and Co3+/4+conversion,which promotes the OER significantly more than the usual photoelectric effect.As a result,Co5.47N/CoN(containing 28％CoN)obtained 317.9％OER enhancement,which provides a pathway for constructing excellent OER catalysts.
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    Optimizing Electrocatalytic Hydrogen Evolution Stability via Minimal Bubble Adhesion at Electrodeposited Crack-Structured NiPx Catalysts

    Qian SunXiaoyu HaoDina ZhangTianyi Zhang...
    244-254页
    查看更多>>摘要：In response to the ongoing energy crisis,advancing the field of electrocatalytic water splitting is of utmost significance,necessitating the urgent development of high-performance,cost-effective,and durable hydrogen evolution reaction catalysts.But the generated gas bubble adherence to the electrode surface and sluggish separation contribute to significant energy loss,primarily due to the insufficient exposure of active sites,thus substantially hindering electrochemical performance.Here,we successfully developed a superaerophobic catalytic electrode by loading phosphorus-doped nickel metal(NiPx)onto various conductive substrates via an electrodeposition method.The electrode exhibits a unique surface structure,characterized by prominent surface fissures,which not only exposes additional active sites but also endows the electrode with superaerophobic properties.The NiPx/Ti electrode demonstrates superior electrocatalytic activity for hydrogen evolution reaction,significantly outperforming a platinum plate,displaying an overpotential of mere 216 mV to achieve a current density of-500 mA cm-2 in 1 M KOH.Furthermore,the NiPx/Ti electrode manifests outstanding durability and robustness during continuous electrolysis,maintaining stability at a current density of-10 mA cm-2 over a duration of 2000 h.Owing to the straightforward and scalable preparation methods,this highly efficient and stable NiPx/Ti electrocatalyst offers a novel strategy for the development of industrial water electrolysis.
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    CuO/Co3O4 Bifunctional Catalysts for Electrocatalytic 5-Hydroxymethylfurfural Oxidation Coupled Cathodic Ammonia Production

    Li ZhangPeiyue JinZe WuBo Zhou...
    255-262页
    查看更多>>摘要：The electrochemical coupling of biomass oxidation and nitrogen conversion presents a potential strategy for high value-added chemicals and nitrogen cycling.Herein,in this work,CuO/Co3O4 with heterogeneous interface is successfully constructed as a bifunctional catalyst for the electrooxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid and the electroreduction of nitrate to ammonia(NH3).The open-circuit potential spontaneous experiment shows that more 5-hydroxymethylfurfural molecules are adsorbed in the Helmholtz layer of the CuO/Co3O4 composite,which certifies that the CuO/Co3O4 heterostructure is conducive to the kinetic adsorption of 5-hydroxymethylfurfural.In situ electrochemical impedance spectroscopy further shows that CuO/Co3O4 has faster reaction kinetics and lower reaction potential in oxygen evolution reaction and 5-hydroxymethylfurfural electrocatalytic oxidation.Moreover,CuO/Co3O4 also has a good reduction effect on NO3.The ex-situ Raman spectroscopy shows that under the reduction potential,the metal oxide is reduced,and the generated Cu2O can be used as a new active site for the reaction to promote the electrocatalytic conversion of NO3 to NH3 synthesis.This work provides valuable guidance for the synthesis of value-added chemicals by 5-hydroxymethylfurfural electrocatalytic oxidation coupled with NO3 while efficiently producing NH3.
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    Interpretable Machine Learning-Assisted High-Throughput Screening for Understanding NRR Electrocatalyst Performance Modulation between Active Center and C-N Coordination

    Jinxin SunAnjie ChenJunming GuanYing Han...
    263-271页
    查看更多>>摘要：Understanding the correlation between the fundamental descriptors and catalytic performance is meaningful to guide the design of high-performance electrochemical catalysts.However,exploring key factors that affect catalytic performance in the vast catalyst space remains challenging for people.Herein,to accurately identify the factors that affect the performance of N2 reduction,we apply interpretable machine learning(ML)to analyze high-throughput screening results,which is also suited to other surface reactions in catalysis.To expound on the paradigm,33 promising catalysts are screened from 168 carbon-supported candidates,specifically single-atom catalysts(SACs)supported by a BC3 monolayer(TM@VB/C-Nn=0-3-BC3)via high-throughput screening.Subsequently,the hybrid sampling method and XGBoost model are selected to classify eligible and non-eligible catalysts.Through feature interpretation using Shapley Additive Explanations(SHAP)analysis,two crucial features,that is,the number of valence electrons(Nv)and nitrogen substitution(Nn),are screened out.Combining SHAP analysis and electronic structure calculations,the synergistic effect between an active center with low valence electron numbers and reasonable C-N coordination(a medium fraction of nitrogen substitution)can exhibit high catalytic performance.Finally,six superior catalysts with a limiting potential lower than-0.4 V are predicted.Our workflow offers a rational approach to obtaining key information on catalytic performance from high-throughput screening results to design efficient catalysts that can be applied to other materials and reactions.
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    Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support

    Shamraiz Hussain TalibBeenish BashirMuhammad Ajmal KhanBabar Ali...
    272-282页
    查看更多>>摘要：Single-atom catalysts(SACs)have received significant interest for optimizing metal atom utilization and superior catalytic performance in hydrogen evolution reaction(HER),oxygen evolution reaction(OER),and oxygen reduction reaction(ORR).In this study,we investigate a range of single-transition metal(STM,=Sc1,Ti1,Vi,Cr1,Mni,Fe1,Co1,Ni1,Cu1,Zr1,Nbi,Mo1,Ru1,Rh1,Pd1,Ag1,Wi,Re1,Os1,lr1,Pt1,and Au,)atoms supported on graphyne(GY)surface for HER/OER and ORR using first-principle calculations.Ab initio molecular dynamics(AIMD)simulations and phonon dispersion spectra reveal the dynamic and thermal stabilities of the GY surface.The exceptional stability of all supported STM,atoms within the H1 cavity of the GY surface exists in an isolated form,facilitating the uniform distribution and proper arrangement of single atoms on GY.In particular,Sc1,Co1,Fe1,and Au,/GY demonstrate promising catalytic efficiency in the HER due to idealistic AGH*values via the Volmer-Heyrovsky pathway.Notably,Sc,and Au,/GY exhibit superior HER catalytic activity compared to other studied catalysts.Co,/GY catalyst exhibits higher selectivity and activity for the OER,with an overpotential(0.46 V)comparable to MoC2,lrO2,and RuO2.Also,Rh,and Co,/GY SACs exhibited promising electrocatalysts for the ORR,with an overpotential of 0.36 and 0.46 V,respectively.Therefore,Co,/GY is a versatile electrocatalyst for metal-air batteries and water-splitting.This study further incorporates computational analysis of the kinetic potential energy barriers of Co,and Rh,in the OER and ORR.A strong correlation is found between the estimated kinetic activation barriers for the thermodynamic outcomes and all proton-coupled electron transfer steps.We establish a relation for the Gibbs free energy of intermediates to understand the mechanism of SACs supported on STM,/GY and introduce a key descriptor.This study highlights GY as a favorable single-atom support for designing highly active and cost-effective versatile electrocatalysts for practical applications.
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    Supramolecular Macrocycle Regulated Single-Atom MoS2@Co Catalysts for Enhanced Oxygen Evolution Reaction

    Shuai CaoWenzhuo WuChaozhong LiuLeqian Song...
    283-291页
    查看更多>>摘要：The development of active water oxidation catalysts for water splitting has stimulated considerable interest.Herein,the design and building of single atom Co sites using a supramolecular tailoring strategy are reported,that is,the introduction of pillar[4]arene[1]quinone(P4A1Q)permits mononuclear Co species stereoelectronically assembled on MoS2 matrix to construct an atomically dispersed MoS2@Co catalyst with modulated local electronic structure,definite chemical environment and enhanced oxygen evolution reaction performance.Theoretical calculations indicate that immsobilized single-Co sites exhibit an optimized adsorption capability of oxygen-containing intermediates,endowing the catalyst an excellent electrocatalytic oxygen evolution reaction activity,with a low overpotential of 370 mV at 10 mA cm-2 and a small Tafel slope of 90 mV dec-1.The extendable potential of this strategy to other electrocatalysts such as MoS2@Ni and MoS2@Zn,and other applications such as the hydrogen evolution reaction was also demonstrated.This study affords new insights into the rational design of single metal atom systems with enhanced electrocatalytic performance.
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    Time-Resolved Oxidation State Changes Are Key to Elucidating the Bifunctionality of Perovskite Catalysts for Oxygen Evolution and Reduction

    Casey E.BeallEmiliana FabbriAdam H.ClarkVivian Meier...
    292-300页
    查看更多>>摘要：In a unified regenerative fuel cell(URFC)or reversible fuel cell,the oxygen bifunctional catalyst must switch reversibly between the oxygen reduction reaction(ORR),fuel cell mode,and the oxygen evolution reaction(OER),electrolyzer mode.However,it is often unclear what effect alternating between ORR and OER has on the electrochemical behavior and physiochemical properties of the catalyst.Herein,operando X-ray absorption spectroscopy(XAS)is utilized to monitor the continuous and dynamic evolution of the Co,Mn,and Fe oxidation states of perovskite catalysts Ba0.5Sr0.5Co0.8Fe0.2O3-δ(BSCF)and La0.4Sr0.6MnO3-δ(LSM),while the potential is oscillated between reducing and oxidizing potentials with cyclic voltammetry.The results reveal the importance of investigating bifunctional catalysts by alternating between fuel cell and electrolyzer operation and highlight the limitations and challenges of bifunctional catalysts.It is shown that the requirements for ORR and OER performance are divergent and that the oxidative potentials of OER are detrimental to ORR activity.These findings are used to give guidelines for future bifunctional catalyst design.Additionally,it is demonstrated how sunlight can be used to reactivate the ORR activity of LSM after rigorous cycling.
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    Boosting Peroxymonosulfate Activation via Co-Based LDH-Derived Magnetic Catalysts:A Dynamic and Static State Assessment of Efficient Radical-Assisted Electron Transfer Processes

    Wenhan YangJunming XiaFanfan ShangGeGe Yang...
    301-312页
    查看更多>>摘要：Heterogeneous catalysts promoting efficient production of reactive species and dynamically stabilized electron transfer mechanisms for peroxomonosulfates(PMS)still lack systematic investigation.Herein,a more stable magnetic layered double oxides(CFLDO/N-C),was designed using self-polymerization and high temperature carbonization of dopamine.The CFLDO/N-C/PMS system effectively activated PMS to remove 99％(k=0.737 min-1)of tetracycline(TC)within 10 min.The CFLDO/N-C/PMS system exhibited favorable resistance to inorganic anions and natural organics,as well as satisfactory suitability for multiple pollutants.The magnetic properties of the catalyst facilitated the separation of catalysts from the liquid phase,resulting in excellent reproducibility and effectively reducing the leaching of metal ions.An electronic bridge was constructed between cobalt(the active platform of the catalyst)and PMS,inducing PMS to break the O-O bond to generate the active species.The combination of static analysis and dynamic evolution confirmed the effective adsorption of PMS on the catalyst surface as well as the strong radical-assisted electron transfer process.Eventually,we further identified the sites where the reactive species attacked the TC and evaluated the toxicity of the intermediates.These findings offer innovative insights into the rapid degradation of pollutants achieved by transition metals in SR-AOPs and its mechanistic elaboration.
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    Stable Organic Solar Cells Enabled by Simultaneous Hole and Electron Interlayer Engineering

    Wisnu Tantyo HadmojoFurkan H.IsikgorYuanbao LinZhaoheng Ling...
    313-320页
    查看更多>>摘要：The development of high-performance organic solar cells(OSCs)with high operational stability is essential to accelerate their commercialization.Unfortunately,our understanding of the origin of instabilities in state-of-the-art OSCs based on bulk heterojunction(BHJ)featuring non-fullerene acceptors(NFAs)remains limited.Herein,we developed NFA-based OSCs using different charge extraction interlayer materials and studied their storage,thermal,and operational stabilities.Despite the high power conversion efficiency(PCE)of the OSCs(17.54％),we found that cells featuring self-assembled monolayers(SAMs)as hole-extraction interlayers exhibited poor stability.The time required for these OSCs to reach 80％of their initial performance(T80)was only 6h under continuous thermal stress at 85 ℃ in a nitrogen atmosphere and 1 h under maximum power point tracking(MPPT)in a vacuum.Inserting MoOx between ITO and SAM enhanced the T80 to 50 and～15 h after the thermal and operational stability tests,respectively,while maintaining a PCE of 16.9％.Replacing the organic PDINN electron transport layer with ZnO NPs further enhances the cells'thermal and operational stability,boosting the T80 to 1000 and 170 h,respectively.Our work reveals the synergistic roles of charge-selective interlayers and device architecture in developing efficient and stable OSCs.
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