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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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    Flexible planar micro supercapacitor diode

    Yihui MaPei TangZhenyuan MiaoWuyang Tan...
    429-435页
    查看更多>>摘要：Supercapacitor diode is a novel ion device that performs both supercapacitor energy storage and ion diode rectification functions.However,previously reported devices are limited by their large size and complex processes.In this work,we demonstrate a screen-printed micro supercapacitor diode(MCAPode)that based on the insertion of a finger mode with spinel ZnCo2O4 as cathode and activated carbon as anode for the first time,and featuring an excellent area specific capacitance(1.21 mF cm-2 at 10 mV s-1)and high rectification characteristics(rectification ratio I of 11.99 at 40 mV s-1).Taking advantage of the ionic gel electrolyte,which provides excellent stability during repeated flexing and at high temperatures.In addition,MCAPode exhibits excellent electrochemical performance and rectifica-tion capability in"AND"and"OR"logic gates.These findings provide practical solutions for future expan-sion of micro supercapacitor diode applications.
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    A-site assisted perovskite crystallization via ion-exchange MOFs for high efficient and stable perovskite solar cells

    Xingrui ZhangJian ZhangWei WangBoyuan Hu...
    436-442页
    查看更多>>摘要：Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrange-ment of perovskite grains through employing Cs+contained metal-organic frameworks In-aip(Cs)obtained by ion-exchange and crystalline transform.Interatomic forces between Cs-O atoms split the pore channels of the pristine In-aip,endowing In-aip(Cs)with multidimensional charge transport chan-nels.In addition,the partially freed Cs+in the interlayer compensates for the vacancy of A-site cations during the perovskite preparation process.The In-aip(Cs)modified perovskite films have a flat morphol-ogy,large grains and excellent optoelectronic properties.Benefiting from the high-quality perovskite films and faster charge extraction,the In-aip(Cs)-modified PSCs achieved a champion PCE of 23.03％,superior to the In-aip-modified(22.29％)and control device(21.13％).More importantly,the unencapsu-lated PSCs modified with In-aip(Cs)exhibited outstanding humidity and thermal stability.Over a period of almost 1000 h,the unencapsulated In-aip(Cs)-modified device retained 85％of its initial PCE after stor-ing in a glove box at 85 ℃,and retained 87％of the primary PCE upon storage in ambient condition at 25 ℃ under a humidity of 40％.
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    Construction of MnS/MoS2 heterostructure on two-dimensional MoS2 surface to regulate the reaction pathways for high-performance Li-O2 batteries

    Guoliang ZhangHan YuXia LiXiuqi Zhang...
    443-452页
    查看更多>>摘要：The inherent catalytic anisotropy of two-dimensional(2D)materials has limited the enhancement of Li-O2 batteries(LOBs)performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuning the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance LOBs.Herein,a MnS/MoS2 heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the surface.Different from the toroidal-like discharge products on the MoS2 cathode,the MnS/MoS2 surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge products.MnS can disturb the layer growth of MoS2,in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge products.Experimental and theoretical results confirm that the MnS/MoS2 heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li2O2.In conse-quence,the MnS/MoS2 heterostructure exhibits a high specific capacity of 11696.0 mA h g-1 and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g-1 at current density of 100 mA g-1.This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.
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    Viologen-based flexible electrochromic devices

    Wenwen WuShanlu GuoJing BianXingyu He...
    453-470页
    查看更多>>摘要：Electrochromic technology has gained significant attention in various fields such as displays,smart win-dows,biomedical monitoring,military camouflage,human-machine interaction,and electronic skin due to its ability to provide reversible and fast color changes under applied voltage.With the rapid develop-ment and increasing demand for flexible electronics,flexible electrochromic devices(FECDs)that offer smarter and more controllable light modulation hold great promise for practical applications.The elec-trochromic material(ECM)undergoing color changes during the electrochemical reactions is one of the key components in electrochromic devices.Among the ECMs,viologens,a family of organic small molecules with 1,1'-disubstituted-4,4'-dipyridinium salts,have garnered extensive research interest,due to their well-reversible redox reactions,excellent electron acceptance ability,and the ability to pro-duce multiple colors.Notably,viologen-based FECDs demonstrate color changes in the liquid or semi-solid electrolyte layer,eliminating the need for two solid electrodes and thus simplifying the device structure.Consequently,viologens offer significant potential for the development of FECDs with high optical contrast,fast response speed,and excellent stability.This review aims to provide a comprehensive overview of the progress and perspectives of viologen-based FECDs.It begins by summarizing the typical structure and recent exciting developments in viologen-based FECDs,along with their advantages and disadvantages.Furthermore,the review discusses recent advancements in FECDs with additional func-tionalities such as sensing,photochromism,and energy storage.Finally,the remaining challenges and potential research directions for the future of viologen-based FECDs are addressed.
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    Coupling Au with BOx matrix induced by Closo-boron cluster for electrochemical synthesis of ammonia

    Wenjing LiuNan YangYuao WeiYingjie Yu...
    471-477页
    查看更多>>摘要：Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BOx substrates(Au-BOx),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BOx possesses excel-lent NRR activity(NH3 yield of 48.52 μg h-1 mgca1t,Faraday efficiency of 56.18％),and exhibits high sta-bility and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond,which considerably facilitates the hydrogenation of*N2-*NH3.The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utiliz-ing boron clusters as reducing and stabilizing agents.
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    Towards high-performance and robust anion exchange membranes(AEMs)for water electrolysis:Super-acid-catalyzed synthesis of AEMs

    Geun Woong RyooSun Hwa ParkKi Chang KwonJong Hun Kang...
    478-510页
    查看更多>>摘要：The increasing demand for hydrogen energy to address environmental issues and achieve carbon neutral-ity has elevated interest in green hydrogen production,which does not rely on fossil fuels.Among various hydrogen production technologies,anion exchange membrane water electrolyzer(AEMWE)has emerged as a next-generation technology known for its high hydrogen production efficiency and its ability to use non-metal catalysts.However,this technology faces significant challenges,particularly in terms of the membrane durability and low ionic conductivity.To address these challenges,research efforts have focused on developing membranes with a new backbone structure and anion exchange groups to enhance durability and ionic conductivity.Notably,the super-acid-catalyzed condensation(SACC)syn-thesis method stands out due to its user convenience,the ability to create high molecular weight(MW)polymers,and the use of oxygen-tolerant organic catalysts.Although the synthesis of anion exchange membranes(AEMs)using the SACC method began in 2015,and despite growing interest in this synthesis approach,there remains a scarcity of review papers focus-ing on AEMs synthesized using the SACC method.The review covers the basics of SACC synthesis,pre-sents various polymers synthesized using this method,and summarizes the development of these polymers,particularly their building blocks including aryl,ketone,and anion exchange groups.We sys-tematically describe the effects of changes in the molecular structure of each polymer component,con-ducted by various research groups,on the mechanical properties,conductivity,and operational stability of the membrane.This review will provide insights into the development of AEMs with superior perfor-mance and operational stability suitable for water electrolysis applications.
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    A novel multi-channel porous structure facilitating mass transport towards highly efficient alkaline water electrolysis

    Xinge JiangVasileios KyriakouChen SongXianbin Wang...
    511-518页
    查看更多>>摘要：An advantageous porous architecture of electrodes is pivotal in significantly enhancing alkaline water electrolysis(AWE)efficiency by optimizing the mass transport mechanisms.This effect becomes even more pronounced when aiming to achieve elevated current densities.Herein,we employed a rapid and scalable laser texturing process to craft novel multi-channel porous electrodes.Particularly,the obtained electrodes exhibit the lowest Tafel slope of 79 mV dec-1(HER)and 49 mV dec-1(OER).As antic-ipated,the alkaline electrolyzer(AEL)cell incorporating multi-channel porous electrodes(NP-LT30)exhibited a remarkable improvement in cell efficiency,with voltage drops(from 2.28 to 1.97 V)exceed-ing 300 mV under 1 A cm-1,compared to conventional perforated Ni plate electrodes.This enhancement mainly stemmed from the employed multi-channel porous structure,facilitating mass transport and bub-ble dynamics through an innovative convection mode,surpassing the traditional convection mode.Furthermore,the NP-LT30-based AEL cell demonstrated exceptional durability for 300 h under 1.0 A cm-2.This study underscores the capability of the novel multi-channel porous electrodes to expe-dite mass transport in practical AWE applications.
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    Molecule aging induced by electron attacking

    Ping SongYining DongXue GongMingbo Ruan...
    519-525页
    查看更多>>摘要：Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule.Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed irreversibly.We further confirm such"molecule aging"via a long-term electron attacking to age water(H2O)molecules.The IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water clusters.Such facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule frame.Further exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water mole-cule is lower than the fresh water on the same Pt/C electrocatalyst.The density functional theory calcu-lations indicate that the shortened O-H bond in H2O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water molecules.Such results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.
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    Influence of O-O formation pathways and charge transfer mediator on lipid bilayer membrane-like photoanodes for water oxidation

    Yingzheng LiShaoqi ZhanZijian DengMeng Chen...
    526-537页
    查看更多>>摘要：Inspired by the function of crucial components in photosystem Ⅱ(PSⅡ),electrochemical and dye-sensitized photoelectrochemical(DSPEC)water oxidation devices were constructed by the self-assembly of well-designed amphipathic Ru(bda)-based catalysts(bda=2,2'-bipyrdine-6,6'-dicarbonoxyl acid)and aliphatic chain decorated electrode surfaces,forming lipid bilayer membrane(LBM)-like struc-tures.The Ru(bda)catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O-O formation mechanisms.However,compared to the slow charge transfer process,the O-O formation pathways did not determine the PEC water oxidation efficiency of the dye-sensitized photoanodes,and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs.Instead,charge transfer plays a decisive role in the PEC water oxidation rate.When an indolo[3,2-b]carbazole derivative was introduced between the Ru(bda)catalysts and aliphatic chain-modified photosensitizer in LBM films,serving as a charge transfer mediator for the tyrosine-histidine pair in PSⅡ,the PEC water oxidation performance of the correspond-ing photoanodes was dramatically enhanced.
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    Fe-N-C core-shell catalysts with single low-spin Fe(Ⅱ)-N4 species for oxygen reduction reaction and high-performance proton exchange membrane fuel cells

    Yan WanLinhui YuBingxin YangCaihong Li...
    538-546页
    查看更多>>摘要：Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(ORR)rel-ative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic con-tributions of Fe-N4 moiety with different chemical/spin states(e.g.D1,D2,D3)to ORR are unclear since various states coexist inevitably.In the present work,Fe-N-C core-shell nanocatalyst with single low-spin Fe(Ⅱ)-N4 species(D1)is synthesized and identified with ex-situ ultralow temperature Mössbauer spectroscopy(T=1.6 K)that could essentially differentiate various Fe-N4 states and invisible Fe-O spe-cies.By quantifying with CO-pulse chemisorption,site density and turnover frequency of Fe-N-C catalysts reach 2.4 × 1019 site g-1 and 23 e site-1 s-1 during the ORR,respectively.Half-wave potential(0.915 VRHE)of the Fe-N-C catalyst is more positive(approximately 54 mV)than that of Pt/C.Moreover,we observe that the performance of PEMFCs on Fe-N-C almost achieves the 2025 target of the US Department of Energy by demonstrating a current density of 1.037 A cm-2 combined with the peak power density of 0.685 W cm-2,suggesting the critical role of Fe(Ⅱ)-N4 site(D1).After 500 h of running,PEMFCs still deliver a power density of 1.26 W cm-2 at 1.0 bar H2-O2.An unexpected rate-determining step is figured out by isotopic labelling experiment and theoretical calculation.This work not only offers valuable insights regarding the intrinsic contribution of Fe-N4 with a single spin state to alkaline/acidic ORR,but also provides great opportunities for developing high-performance stable PEMFCs.
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