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Facilitating prelithiation of silicon carbon anode by localized high-concentration electrolyte for high-rate and long-cycle lithium storage

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Carbon energy 2024年第6期6卷 216-233页

作者： Yuanxing Zhang Borong Wu Jiaying Bi Xinyu Zhang Daobin Mu Xin-Yu Zhang Ling Zhang Yao Xiao Feng Wu School of Materials Science and Engineering Beijing Institute of TechnologyBeijingChina Chongqing Innovation Center Beijing Institute of TechnologyChongqingChina College of New energy Xi′an Shiyou UniversityXi′anChina institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhouChina Key Laboratory of Advanced energy Materials chemistry(Ministry of Education) Nankai UniversityTianjinChina

The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)***,a feasible and cost-effective prelithiation method under a localized highconcentration electrolyte system(LHCE)for the silicon-silica/graphite(Si-SiO_(2)/C@G)anode is designed for stabilizing the SEI layer and enhancing the *** thin SiO_(2)/C layers with-NH_(2) groups covered on nano-Si surfaces are demonstrated to be beneficial to the prelithiation process by density functional theory calculations and electrochemical *** SEI formed under LHCE is proven to be rich in ionic conductivity,inorganic substances,and flexible organic ***,faster Li+transportation across the SEI further enhances the prelithiation effect and the rate performance of Si-SiO_(2)/C@G *** also leads to uniform decomposition and high stability of the SEI with abundant organic *** a result,the prepared anode shows a high reversible specific capacity of 937.5 mAh g^(-1)after 400 cycles at a current density of 1 *** 811‖Li-SSGLHCE full cell achieves a high-capacity retention of 126.15 mAh g^(-1)at 1 C over 750 cycles with 84.82%ICE,indicating the great value of this strategy for Si-based anodes in large-scale applications.

关键词： localized high-concentration electrolytes prelithiation SEI layer silicon anode

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Introducing hydroxyl groups to tailor the d-band center of Ir atom through side anchoring for boosted ORR and HER

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Journal of energy chemistry 2024年第3期90卷 144-151,I0005页

作者： Qing Lv Meiping Li Xiaodong Li Xingru Yan Zhufeng Hou Changshui Huang Science Center for Material Creation and energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan 250100ShandongChina institute of chemistry Chinese Academy of ScienceBeijing 100191China State Key Laboratory of Structural chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina

Tuning the coordination atoms of central metal is an effective means to improve the electrocatalytic activity of atomic ***,iridium(Ir) is proposed to be asymmetrically anchored by sp-N and pyridinic N of hydrogen-substituted graphdiyne(HsGDY),and coordinated with OH as an Ir atomic catalyst(Ir_(1)-N-HsGDY).The electron structures,especially the d-band center of Ir atom,are optimized by these specific coordination ***,the as-synthesized Ir_(1)-N-HsGDY exhibits excellent electrocatalytic performances for oxygen reduction and hydrogen evolution reactions in both acidic and alkaline *** from the unique structure of HsGDY,IrN_(2)(OH)_(3) has been developed and demonstrated to act as the active site in these electrochemical *** those indicate the fresh role of the sp-N in graphdiyne in producing a new anchor way and contributing to promote the electrocatalytic activity,showing a new strategy to design novel electrochemical catalysts.

关键词： Oxygen reduction reaction D-band center Graphdiyne Hydroxyl group Electrocatalysis

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High donor-number and low content electrolyte additive for stabilizing zinc metal anode

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Journal of energy chemistry 2024年第8期95卷 626-635,I0014页

作者： Yuxin Gong Ruifan Lin Bo Wang Huaizheng Ren Lei Wang Han Zhang Jianxin Wang Deyu Li Yueping Xiong Dianlong Wang Huakun Liu Shixue Dou MIIT Key Laboratory of Critical Materials Technology for New energy Conversion and Storage State Key Laboratory of Urban Water Resource and EnvironmentSchool of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina Key Laboratory of Advanced energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China institute of energy Material Science University of Shanghai for Science and TechnologyShanghai 200093China

The aqueous zinc ion batteries(AZIBs)are thought as promising competitors for electrochemical energy storage,though their wide application is curbed by the uncontrollable dendrite growth and gas evolution side ***,to stabilize both zinc anodes and water molecules,we developed a modified electrolyte by adding a trace amount of N,N-diethylformanmide(DEF)into the ZnSO_(4)electrolyte for the first time in zinc ion *** effectiveness of DEF is predicted by the comparison of donor number and its preferential adsorption behavior on the zinc anode is further demonstrated by several spectroscopy characterizations,electrochemical methods,and molecular dynamics *** modified electrolyte with 5%*** content can ensure a stable cycling life longer than 3400 h of Zn‖Zn symmetric cells and an ultra-reversible Zn stripping/plating process with a high coulombic efficiency of 99.7%.The Zn‖VO_(2)full cell maintains a capacity retention of 83.5%and a 104 mA h g^(-1)mass capacity after *** work provides insights into the role of interfacial adsorption behavior and the donor number of additive molecules in designing low-content and effective aqueous electrolytes.

关键词： Aqueous zinc ion batteries Zinc anode Electrolyte additives Donor number Zinc dendrites

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Self assembled electron blocking and lithiophilic interface towards dendrite-free solid-state lithium battery

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Chinese Chemical Letters 2024年第4期35卷 220-225页

作者： Caixia Li Yi Qiu Yufeng Zhao Wuliang Feng institute for Sustainable energy&College of Sciences Shanghai UniversityShanghai 200444China Key Laboratory of Advanced energy Materials chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

The poor interfacial contact is one of the biggest challenges that solid-state lithium batteries suffer *** the solid-state electrolyte surface energy by transforming the interface from lithiophobic to lithiophilic is effective to promote the interfacial contact, but electronic conductive interphases usually increase the risk of electron attack, thus leading to uncontrollable Li dendrite growth. Herein, we propose a self-assembled thermodynamic stable Li I interphase to simultaneously improve the interfacial contact between the garnet electrolyte Li_7La_(3)Zr_(2)O_(12)(LLZO) and Li anode, and prohibit the electron attack. The direct contact between LLZO and Li and the high temperature Li melting process was ascribed to Zr4+reduction, which facilitated Li dendrite formation and propagation. With the modification of the high lithiophilic I_(2) thin film, the area specific interfacial resistance of LLZO/Li was reduced from 1525 Ω/cm^(2) to 57 Ω/cm^(2). More importantly, LLZO was protected from being reduced due to the outstanding electronic insulativity of the Li I interphase, which leaded to a high critical current density of 1.2/7.0 m A/cm^(2) in the time/capacity-constant modes, respectively.

关键词： Li_7La_(3)Zr_(2)O_(12) LiI interphase Interfacial contact Li dendrite Thermodynamic stable

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Unsaturated bi-heterometal clusters in metal-vacancy sites of 2D MoS2 for efficient hydrogen evolution

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Carbon energy 2024年第3期6卷 264-275页

作者： Gonglei Shao Jie Xu Shasha Gao Zhang Zhang Song Liu Xu Zhang Zhen Zhou Interdisciplinary Research Center for Sustainable energy Science and Engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityZhengzhouHenanChina College of chemistry and Materials Engineering Wenzhou UniversityWenzhouZhejiangChina Key Laboratory of Advanced energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjinChina State Key Laboratory of Chemo/Biosensing and Chemometrics Institute of Chemical Biology and Nanomedicine(ICBN)College of Chemistry and Chemical EngineeringHunan UniversityChangshaHunanChina institute of New energy Material chemistry School of Materials Science and EngineeringNankai UniversityTianjinChina

The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation ***,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum *** unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active *** them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical ***,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.

关键词： clusters hydrogen evolution reaction metal vacancy MoS2 unsaturated heterometal

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Design,preparation,application of advanced array structured materials and their action mechanism analyses for high performance lithium-sulfur batteries

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Journal of energy chemistry 2024年第2期89卷 266-303,I0007页

作者： Nanping Deng Xiaofan Feng Yongbing Jin Zhaozhao Peng Yang Feng Ying Tian Yong Liu Lu Gao Weimin Kang Bowen Cheng State Key Laboratory of Separation Membranes and Membrane processes/National Center for International Joint Research on Separation Membranes School of Textile Science and EngineeringTiangong UniversityTianjin 300387China Key Laboratory of Advanced energy Materials chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

Lithium-sulfur battery(LSB)has brought much attention and concern because of high theoretical specific capacity and energy density as one of main competitors for next-generation energy storage *** widely commercial application and development of LSB is mainly hindered by serious“shuttle effect”of lithium polysulfides(Li PSs),slow reaction kinetics,notorious lithium dendrites,*** various structures of LSB materials,array structured materials,possessing the composition of ordered micro units with the same or similar characteristics of each unit,present excellent application potential for various secondary cells due to some merits such as immobilization of active substances,high specific surface area,appropriate pore sizes,easy modification of functional material surface,accommodated huge volume change,enough facilitated transportation for electrons/lithium ions,and special functional groups strongly adsorbing Li *** many novel array structured materials are applied to battery for tackling thorny problems mentioned *** this review,recent progresses and developments on array structured materials applied in LSBs including preparation ways,collaborative structural designs based on array structures,and action mechanism analyses in improving electrochemical performance and safety are ***,we also have detailed discussion for array structured materials in LSBs and constructed the structure-function relationships between array structured materials and battery ***,some directions and prospects about preparation ways,functional modifications,and practical applications of array structured materials in LSBs are *** hope the review can attract more researchers'attention and bring more studying on array structured materials for other secondary batteries including LSB.

关键词： Array structured materials Preparation methods and structural designs Action mechanism analyses Advanced Li-S batteries Excellent electrochemical performances and safety

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Revisiting the sodium-ion storage capability of hard carbon in carbonate-based electrolytes via a sodium-metal-free protocol

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Science China chemistry 2024年第7期67卷 2240-2247页

作者： Gaopan Liu Yanbing Mo Jiawei Chen Yu Peng Xiao Zhu Fei Wang Xiaoli Dong Yongyao Xia Department of chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Institute of New EnergyLaboratory of Advanced MaterialsFudan UniversityShanghai 200438China

Common evaluation methodology of sodium(Na)-containing two-electrode or three-electrode configurations overlooks the interference from highly reactive Na metal,leading to the underestimation or inconsistent performance of low-potential hard carbon(HC)***,the trap of Na metal was systematically investigated with or without applied current,uncovering its inadequacy as the reference or counter electrode in different configurations.A Na-metal-free three-electrode protocol is proposed for evaluating the actual Na^(+)-storage capability of the typical low-potential HC *** avoiding Na crosstalk and precisely controlling the working electrode's potential,the actual electrochemical performance of HC in the carbonate esterbased electrolyte can be recognized with high capacity of 222 mAh g^(-1)at 2 C and 113 mAh g^(-1)at 5 C,correcting the misunderstanding of the inferior performance of HC in coin-type half cells(68%and 50%undervaluation at 2 C and 5 C,respectively).The advanced protocol is expected to reduce misunderstandings or underestimation due to evaluation methods and to guide the development of high-performance battery materials.

关键词： highly reactive sodium potential drift carbonate ester sodium-metal-free protocol sodium storage capability

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Solar Driven 15.7% Hydrogen Conversion by Harmony of Light Harvesting,Electron Transporting Bridge,and S-Defection in a Self-Assembled Microscale CuS/rGO/CP Photoanode

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energy & Environmental Materials 2024年第3期7卷 194-205页

作者： Sujeong Kim Boseok Seo Hyerim Park Younghwan Im Jeong Yeon Do Byung Sub Kwak Namgyu Son Minkyu Kim Misook Kang Department of chemistry College of Natural SciencesYeungnam University School of Chemical Engineering Yeungnam University Department of energy and Hydrocarbon chemistry Graduate School of EngineeringKyoto University Korea Evaluation institute of Industrial Technology (Keit) Electric Power Research institute (KEPRI) 105 Munji-ro

CuS is an encouraging photoelectrode candidate that meets the essential requirements for efficient solar-to-hydrogen production,but it has not been thoroughly studied.A CuS light absorber layer is grown by the self-assembly of copper and sulfur precursors on a carbon paper （CP） ***,rCO is introduced as a buffer layer to control the optical and electrical properties of the *** well-ordered microstructural arrangement suppresses the recombination loss of electrons and holes owing to enhanced charge-carrier generation,separation,and *** potential reaching 10mA cm-2in 1.0 M KOH solution is significantly lowered to 0.87 V,and the photocurrent density at 1.23 V is 94.7 mA *** computational result reveals that the potential-determining step is sensitive to O*stability; the lower stability of O*in the thin layer of CuS/rCO decreases the free-energy gap between the initial and final states of the potential-determining step,resulting in a lowering of the onset *** faradaic efficiency for the photoelectrochemical oxygen evolution reaction in the optimized 2CuS/1rCO/CP photoanode is 98.60%,and the applied bias photon-to-current and the solar-to-hydrogen efficiencies are 11.2%and 15.7%,respectively,and its ultrahigh performance is maintained for 250 *** record-breaking achievement indices may be a trigger for establishing a green hydrogen economy.

关键词： 15.7%-solar to hydrogen density functional theory lower photopotential p-CuS/rGO/CP photoanode photoelectrochemical oxygen evolution

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Regulating the intrinsic electronic structure of carbon nanofibers with high-spin state Ni for sodium storage with high-power density

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Journal of Materials Science & Technology 2024年第4期171卷 16-23页

作者： Zhijia Zhang Gang Xie Yuefang Chen Yanhao Wei Mengmeng Zhang Shulei Chou Yunxiao Wang Yifang Zhang Yong Jiang School of Materials Science and Engineering Institute of Quantum Materials and DevicesState Key Laboratory of Separation Membrane and Membrane ProcessesTiangong UniversityTianjin 300387China institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China institute for Superconducting and Electronic Materials University of WollongongWollongongNSW 2522Australia

Carbon nanofibers(CNFs)with high specific surface area show great potential for sodium storage as a hard carbon ***,CNFs anchored with Ni nanoparticles(CNFs/Ni)were prepared through chemical vapor deposition and impregnation reduction methods,in situ growing on the three-dimensional porous copper current collector(3DP-Cu).The coupling effect of high-spin state Ni nanopar-ticles leads to the increase of defect density and the expansion of lattice spacing of ***,the 3DP-Cu ensures a high loading capacity of CNFs and short ion/electron transport *** an integral binder-free anode,the 3DP-Cu/CNFs/Ni exhibits excellent electrochemical performance,which demon-strates a high specific capacity with 298.5 mAh g^(-1)at 1000 mA g^(-1)after 1500 cycles,and a high power density with 200 mAh g^(-1)over 1000 cycles at 5000 mA g^(-1).Density functional theory calculation re-sults show that the high-spin state Ni regulates the electronic structure of CNFs,which significantly reduces the adsorption energy for Na^(+)(-2.7 Ev)and thus enables high-rate *** regulation of the electronic structure of carbon materials by high-spin state metal provides a new strategy for developing high-power carbonaceous anode materials for sodium-ion batteries.

关键词： Carbon nanofibers Ni nanoparticles High-spin state Sodium-ion batteries Anode materials Density functional theory calculation

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A-site assisted perovskite crystallization via ion-exchange MOFs for high efficient and stable perovskite solar cells

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Journal of energy chemistry 2024年第6期93卷 436-442,I0011页

作者： Xingrui Zhang Jian Zhang Wei Wang Boyuan Hu Yayu Dong Debin Xia Kaifeng Lin Yulin Yang MIIT Key Laboratory of Critical Materials Technology for New energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina

Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrangement of perovskite grains through employing Cs~+contained metal-organic frameworks In-aip(Cs)obtained by ion-exchange and crystalline *** forces between Cs-O atoms split the pore channels of the pristine In-aip,endowing In-aip(Cs)with multidimensional charge transport channels,In addition,the partially freed Cs~+in the interlayer compensates for the vacancy of A-site cations during the perovskite preparation *** In-aip(Cs)modified perovskite films have a flat morphology,large grains and excellent optoelectronic *** 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 unencapsulated PSCs modified with In-aip(Cs)exhibited outstanding humidity and thermal *** a period of almost 1000 h,the unencapsulated In-aip(Cs)-modified device retained 85%of its initial PCE after storing 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%.

关键词： Metal-organic frameworks PSCs Stability Defect passivation

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