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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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    Potential-dependent insights into the origin of high ammonia yield rate on copper surface via nitrate reduction:A computational and experimental study

    Yangge GuoNannan SunLiuxuan LuoXiaojing Cheng...
    272-281页
    查看更多>>摘要：Focusing on revealing the origin of high ammonia yield rate on Cu via nitrate reduction(NO3RR),we herein applied constant potential method via grand-canonical density functional theory(GC-DFT)with implicit continuum solvation model to predict the reaction energetics of NO3RR on pure copper surface in alkaline media.The potential-dependent mechanism on the most prevailing Cu(111)and the minor(100)and(110)facets were established,in consideration of NO2,NO,NH3,NH2OH,N2,and N2O as the main products.The computational results show that the major Cu(111)is the ideal surface to produce ammonia with the highest onset potential at 0.06 V(until-0.37 V)and the highest optimal potential at-0.31 V for ammonia production without kinetic obstacles in activation energies at critical steps.For other minor facets,the secondary Cu(100)shows activity to ammonia from-0.03 to-0.54 V with the ideal potential at-0.50 V,which requires larger overpotential to overcome kinetic activation energy barriers.The least Cu(110)possesses the longest potential range for ammonia yield from-0.27 to-1.12 V due to the higher adsorption coverage of nitrate,but also with higher tendency to generate di-nitrogen species.Experimental evaluations on commercial Cu/C electrocatalyst validated the accuracy of our proposed mechanism.The most influential(111)surface with highest percentage in electrocata-lyst determined the trend of ammonia production.In specific,the onset potential of ammonia production at 0.1 V and emergence of yield rate peak at-0.3 V in experiments precisely located in the predicted potentials on Cu(111).Four critical factors for the high ammonia yield and selectivity on Cu surface via NO3RR are summarized,including high NO3RR activity towards ammonia on the dominant Cu(111)facet,more possibilities to produce ammonia along different pathways on each facet,excellent ability for HER inhibition and suitable surface size to suppress di-nitrogen species formation at high nitrate coverage.Overall,our work provides comprehensive potential-dependent insights into the reac-tion details of NO3RR to ammonia,which can serve as references for the future development of NO3RR electrocatalysts,achieving higher activity and selectivity by maximizing these characteristics of copper-based materials.
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    Coordination structure regulation in non-flammable electrolyte enabling high voltage lithium electrochemistry

    Zhiwen DengYe JiaYan DengChanghaoyue Xu...
    282-290页
    查看更多>>摘要：High-voltage battery systems bring significant increases in energy density but are also accompanied by fast degradation of electrochemical performance and serious safety issues.Herein,Li+coordination struc-ture regulation was conducted to formulate a non-flammable electrolyte,which consists of 1.5 M lithium bis(fluor sulfonyl)imide(LiFSI)in triethyl phosphate and methyl 2,2,2-trifluoromethyl carbonate(FEMC).The renamed TEP-FEMC-FEC(TFF)electrolyte exhibits an FSI--dominated solvation structure contributed by the weakly-solvating ability of FEMC.The generated inorganic-rich interfacial layers are conducive to stabilizing the phase transition of high-voltage cathodes while suppressing the dendritic growth on lithium metal or co-intercalation behavior in graphite anode.This TFF electrolyte enables LiCoO2||Li batteries to achieve capacity maintenance over 79％after 400 cycles with high-rate of 5 C at an ultra-high voltage of 4.6 V,and an outstanding capacity exceeding 100 mA h g-1 even at a super-high current density of 20 C.Additionally,the Ah-level LiCoO2||graphite pouch cells also exhibit high capacity retention and satisfactory safety performance even under fast charging.This work provides a novel research direction for the pursuit of high energy density non-flammable electrolytes.
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    Strategic regulation of nitrogen-containing intermediates for enhanced nitrate reduction over Co3O4/SiC catalyst having multiple active centers

    Ming-Hao GuanHao-Nan XuJin LiuTao Wu...
    291-299页
    查看更多>>摘要：Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction(NO3RR)is crucial for the enhancement of reaction efficiency.However,it remains a great challenge to regulate the reaction intermediates through active site manipulation on the surface of the catalyst.Here,a family of n％-Co3O4/SiC(n=5,8,12,20)catalysts with a delicate percentage of Co2+and Co3+were prepared for NO3RR.We found that Co3+primarily acts as the active site for NO-3 reduction to NO-2,while Co2+is responsible for the conversion of NO-2 to NH3.Moreover,the conversion of these intermediates over the active sites is autonomous and separately controllable.Both processes synergistically accomplish the reduction of nitrate ions to synthesize ammonia.Combining the experimental studies and density functional theory(DFT)calculations,it is discovered the pathway(*NHO→*NHOH→*NH2OH→*NH2→*NH3)is more favor-able due to the lower ΔG value(0.25 eV)for the rate-limiting step(*NO→*NHO).The NH3 yield rate of 8％-Co3O4/SiC reached 1.08 mmol/(cm2 h)with a Faradaic efficiency of 96.4％at-0.89 V versus the reversible hydrogen electrode(RHE),surpassing those of most reported non-noble NO3RR catalysts.This strategy not only provides an efficient catalyst for NO3RR but also serves as an illustrative model for the regulation of multi-step reaction intermediates through the design of distinct active sites,thereby presenting a new approach to enhance the efficiency of intricate reactions.
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    Unravelling the ion transport and the interphase properties of a mixed olivine cathode for Na-ion battery

    Luca MinnettiLeonardo SbrasciniAntunes StaffolaniVittorio Marangon...
    300-317页
    查看更多>>摘要：The replacement of Li by Na in an analogue battery to the commercial Li-ion one appears a sustainable strategy to overcome the several concerns triggered by the increased demand for the electrochemical energy storage.However,the apparently simple change of the alkali metal represents a challenging step which requires notable and dedicated studies.Therefore,we investigate herein the features of a NaFe0.6Mn0.4PO4(NFMP)cathode with triphylite structure achieved from the conversion of a LiFe0.6Mn0.4PO4(LFMP)olivine for application in Na-ion battery.The work initially characterizes the structure,morphology and performances in sodium cell of NFMP,achieving a maximum capacity exceed-ing 100 mAh g-1 at a temperature of 55 ℃,adequate rate capability,and suitable retention confirmed by ex-situ measurements.Subsequently,the study compares in parallel key parameters of the NFMP and LFMP such as Na+/Li+ions diffusion,interfacial characteristics,and reaction mechanism in Na/Li cells using various electrochemical techniques.The data reveal that relatively limited modifications of NFMP chemistry,structure and morphology compared to LFMP greatly impact the reaction mechanism,kinetics and electrochemical features.These changes are ascribed to the different physical and chemical features of the two compounds,the slower mobility of Na+with respect to Li+,and a more resistive elec-trode/electrolyte interphase of sodium compared with lithium.Relevantly,the study reveals analogue trends of the charge transfer resistance and the ion diffusion coefficient in NFMP and LFMP during the electrochemical process in half-cell.Hence,the NFMP achieved herein is suggested as a possible candi-date for application in a low-cost,efficient,and environmentally friendly Na-ion battery.
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    Cascade utilization of full spectrum solar energy for achieving simultaneous hydrogen production and all-day thermoelectric conversion

    Tuo ZhangLiang DongBaoyuan WangJingkuo Qu...
    318-327页
    查看更多>>摘要：Solar-driven photocatalytic water/seawater splitting holds great potential for green hydrogen produc-tion.However,the practical application is hindered by the relatively low conversion efficiency resulting from the inadequate utilization of solar spectrum with significant waste in the form of heat.Moreover,current equipment struggles to maintain all-day operation subjected to the lack of light during nighttime.Herein,a novel hybrid system integrating photothermal catalytic(PTC)reactor,thermoelectric generator(TEG),and phase change materials(PCM)was proposed and designed(named as PTC-TEG-PCM)to address these challenges and enable simultaneous overall seawater splitting and 24-hour power gener-ation.The PTC system effectively maintains in an optimal temperature range to maximize photothermal-assisted photocatalytic hydrogen production.The TEG component recycles the low-grade waste heat for power generation,complementing the shortcoming of photocatalytic conversion and achieving cascade utilization of full-spectrum solar energy.Furthermore,exceptional thermal storage capability of PCM allow for the conversion of released heat into electricity during nighttime,contributing significantly to the overall power output and enabling PTC-TEG-PCM to operate for more than 12 h under the actual con-dition.Compared to traditional PTC system,the overall energy conversion efficiency of the PTC-TEG-PCM system can be increased by～500％,while maintaining the solar-to-hydrogen efficiency.The advancement of this novel system demonstrated that recycling waste heat from the PTC system and utilizing heat absorption/release capability of PCM for thermoelectric application are effective strategies to improve solar energy conversion.With flexible parameter designing,PTC-TEG-PCM can be applied in various sce-narios,offering high efficiency,stability,and sustainability.
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    Enhanced nitrite electroreduction to ammonia via interfacial dual-site adsorption

    Xiaokang ChenShengliang ZhaiYi TanLe Su...
    328-335页
    查看更多>>摘要：The nitrite(NO2-)to ammonia(NH3)electroreduction reaction(NO2-RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving the NH3 selectivity is to facilitate adsorption and activation of NO2-,which is generally unde-sirable in unitary species.In this work,an efficient NO2-RR catalyst is constructed by cooperating Pd with In2O3,in which NO2 could adsorb on interfacial dual-site through"Pd-N-O-In"linkage,leading to strengthened NO2-adsorption and easier N=O bond cleavage than that on unitary Pd or In2O3.Moreover,the Pd/In2O3 composite exhibits moderate H* adsorption,which may facilitate protonation kinetics while inhibiting competitive HER.As a result,it exhibits a fairly high NH3 yield rate of 622.76 mmol h-1 gca1 with a Faradaic efficiency(FE)of 95.72％,good selectivity of 91.96％,and cycling sta-bility towards the NO2-RR,surpassing unitary In2O3 and Pd/C electrocatalysts.Besides,computed results indicate that NH3 production on Pd/In2O3 follows the deoxidation to hydrogenation pathway.This work highlights the significance of H* and NO2 adsorption modulation and N=O activation in NO2-RR electro-chemistry by creating synergy between a mediocre catalyst with an appropriate cooperator.
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    Cooperation between single atom catalyst and support to promote nitrogen electroreduction to ammonia:A theoretical insight

    Wanying GuoSiyao WangHongxia WangQinghai Cai...
    336-344页
    查看更多>>摘要：The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encom-passing multiple intermediates and pathways.Herein,we utilized defective BC3 monolayer-supported SACs as a prototype to investigate the cooperative effects of SACs and their support on the catalytic per-formance of the nitrogen reduction reaction(NRR)for ammonia(NH3)production.The results showed that these SACs can be firmly stabilized on these defective BC3 supports with high stability against aggre-gation.Furthermore,co-activation of the inert N2 reactant was observed in certain embedded SACs and their neighboring B atoms on certain BC3 sheets due to the noticeable charge transfer and significant N-N bond elongation.Our high-throughput screening revealed that the Mo/DVcc and W/DVCC exhibit superior NRR catalytic performance,characterized by a low limiting potential of-0.33 and-0.43 V,respectively,which can be further increased under acid conditions based on the constant potential method.Moreover,varying NRR catalytic activities can be attributed to the differences in the valence state of active sites.Remarkably,further microkinetic modeling analysis displayed that the turnover frequency of N2-to-NH3 conversion on Mo/DVcc is as large as 1.20 x 10-3 s-1 site-1 at 700 K and 100 bar,thus guaranteeing its ultra-fast reaction rate.Our results not only suggest promising advanced electrocatalysts for NRR but also offer an effective avenue to regulate the electrocatalytic performance via the co-catalytic metal-support interactions.
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    Optimizing the power conversion processes in diluted donor/acceptor heterojunctions towards 19.4％efficiency all-polymer solar cells

    Liang WangChen ChenZirui GanChenhao Liu...
    345-350页
    查看更多>>摘要：All polymer solar cells(all-PSCs)promise mechanically-flexible and morphologically-stable organic pho-tovoltaics and have aroused increased interests very recently.However,due to their disorderly conforma-tion structures within the photoactive film,inefficient charge generation and carrier transport are observed which lead to inferior photovoltaic performance compared to smaller molecular acceptor-based photovoltaics.Here,by diluting PM6 with a cutting-edge polymeric acceptor PY-IT and diluting PY-IT with PM6 or D18,donor-dominating or acceptor-dominating heterojunctions were prepared.Synchrotron X-ray and multiple spectrometer techniques reveal that the diluted heterojunctions receive increased structural order,translating to enhanced carrier mobility,improved exciton diffusion length,and suppressed non-radiative recombination loss during the power conversion.As the results,the corre-sponding PM6+1％PY-IT/PY-IT+1％D18 and PM6+1％PY-IT/PY-IT+1％PM6 devices fabricated by layer-by-layer deposition received superior power conversion efficiency(PCE)of 19.4％and 18.8％respectively,along with enhanced operational lifetimes in air,outperforming the PCE of 17.5％in the PM6/PY-IT refer-ence device.
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    Semitransparent organic photovoltaics enabled by transparent p-type inorganic semiconductor and near-infrared acceptor

    Xue YanJiayu WangWei HeTop Archie Dela Peña...
    351-358页
    查看更多>>摘要：Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating photovoltaics.Organic semi-conductors with high charge carrier mobility usually have planar and conjugated structures,thereby showing strong absorption in visible region.In this work,a new concept of incorporating transparent inorganic semiconductors is proposed for high-performance STOPVs.Copper(Ⅰ) thiocyanate(CuSCN)is a visible-transparent inorganic semiconductor with an ionization potential of 5.45 eV and high hole mobility.The transparency of CuSCN benefits high average visible transmittance(AVT)of STOPVs.The energy levels of CuSCN as donor match those of near-infrared small molecule acceptor BTP-eC9,and the formed heterojunction exhibits an ability of exciton dissociation.High mobility of CuSCN contributes to a more favorable charge transport channel and suppresses charge recombination.The control STOPVs based on PM6/BTP-eC9 exhibit an AVT of 19.0％with a power conversion efficiency(PCE)of 12.7％.Partial replacement of PM6 with CuSCN leads to a 63％increase in transmittance,resulting in a higher AVT of 30.9％and a comparable PCE of 10.8％.
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    Stabilization of cathode electrolyte interphase for aqueous zinc-ion batteries

    Zhenjie YaoWenyao ZhangJunwu Zhu
    359-386页
    查看更多>>摘要：Aqueous zinc-ion battery systems are attractive for next-generation energy storage devices,however,the unstable electrode electrolyte interphase,especially cathode electrolyte interphase(CEI),has induced rapid capacity attenuation,insufficient cycle life,and severe safety issues.Evolving the researching of CEI formation,composition,dynamic structure,and reaction mechanisms would help in understanding the fundamental electrochemistry at CEI such as electron and ion transport processes,further strengthen-ing the specific capacity,rate,and cycle performance of the cathode materials.In this review,we summa-rized the latest progress in understanding interfacial reaction mechanisms and ion dynamic behavior,emphasizing the impact of surface-specific adsorption and solvation behaviors on the interface's ultimate structure and chemical composition.Subsequently,the significant challenges that persist in CEI formation mechanisms,such as cathodic dissolution,by-product formation,electrostatic interactions,constrained electrochemical windows,oxygen evolution reaction,overpotentials,phase transitions,and additional fac-tors,were discussed.These challenges are explored to identify triggers contributing to the depletion of active materials and alterations in the composition or state of the CEI.Ultimately,with a deep comprehen-sion of interfacial behaviors,the review articulates innovative optimization strategies through a detailed categorization of approaches in electrolyte engineering,cathode engineering,and artificial CEI develop-ment.Furthermore,future challenges and development directions of CEI are presented.We hope to offer insights for constructing robust CEI films to achieve high performance aqueous zinc-ion batteries.
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