CoSnO_(3)/C nanocubes with oxygen vacancy as high-capacity cathode materials for rechargeable aluminum batteries

Rechargeable aluminum batteries(RABs)are attractive cadidates for next-generation energy storage and conversion,due to the low cost and high safety of Al resources,and high capacity of metal Al based on the three-electrons reaction mechanism.However,the development of RABs is greatly limited,because of the lack of advanced cathode materials,and their complicated and unclear reaction mechanisms.Exploring the novel nanostructured transition metal and carbon composites is an effective route for obtaining ideal cathode materials.In this work,we synthesize porous CoSnO_(3)/C nanocubes with oxygen vacancies for utilizing as cathodes in RABs for the first time.The intrinsic structure stability of the mixed metal cations and carbon coating can improve the cycling performance of cathodes by regulating the internal strains of the electrodes during volume expansion.The nanocubes with porous structures contribute to fast mass transportation which improves the rate capability.In addition to this,abundant oxygen vacancies promote the adsorption affinity of cathodes,which improves storage capacity.As a result,the CoSnO_(3)/C cathodes display an excellent reversible capacity of 292.1 mAh g^(-1) at 0.1 A g^(-1),a good rate performance with 109 mAh g^(-1) that is maintained even at 1 A g^(-1) and the provided stable cycling behavior for 500 cycles.Besides,a mechanism of intercalation of Al^(3+)within CoSnO_(3)/C cathode is proposed for the electrochemical process.Overall,this work provides a step toward the development of advanced cathode materials for RABs by engineering novel nanostructured mixed transition-metal oxides with carbon composite and proposes novel insights into chemistry for RABs.

Engineering homotype heterojunctions in hard carbon to induce stable solid electrolyte interfaces for sodium-ion batteries

Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis.

分子工程化可持续制备多元素掺杂的分级多孔碳材料用于高性能锌离子存储

具备低价、优异倍率性能、长寿命、高安全性的水系锌离子混合电容器(ZHSCs)是理想的下一代能量存储器件.高比表面积、多级孔、富缺陷的掺杂分级多孔碳(HD-HPCs)是非常有前景的ZHSCs正极材料.但是,可持续且可控原位构筑同时具备多种结构组分优势的HDHPCs仍然面临挑战.本文提出一种新的分子工程化策略,即直接碳化富含多种异质原子的超分子前驱体,便可实现原位构筑多元掺杂HDHPCs.该绿色可持续策略具有多种优势,包括不需要额外的成孔技术、活化剂、模板剂、以及复杂且危险的清洗过程.由于富杂原子超分子前驱体具有较高的活性,高温碳化过程中杂原子以及邻近杂原子的碳原子很容易从碳骨架中脱离,形成丰富的微介孔结构.因此,活性结构与组分优化后的正极材料在水系ZHSCs中0.5和20 A g^(-1)下容量分别达到139.2和88.9 mA h g^(-1),在准固态ZHSCs中0.5 A g^(-1)下容量也能够达到111.5 mA h g^(-1).此外,水系和准固态ZHSCs也具备高能量和功率密度,以及长循环稳定性.理论计算表明多原子掺杂能够协同提升碳材料的导电性,且降低锌离子与碳之间的相互作用能垒,因而提升锌离子的吸附性能.本工作为直接制备HD-HPCs及其电化学储能应用提供了新思路.

High‑Mass‑Loading Electrodes for Advanced Secondary Batteries and Supercapacitors

The growing demand for advanced electrochemical energy storage systems(EESSs)with high energy densities for electric vehicles and portable electronics is driving the electrode revolution,in which the development of high-mass-loading electrodes(HMLEs)is a promising route to improve the energy density of batteries packed in limited spaces through the optimal enlargement of active material loading ratios and reduction of inactive component ratios in overall cell devices.However,HMLEs face significant challenges including inferior charge kinetics,poor electrode structural stability,and complex and expensive production processes.Based on this,this review will provide a comprehensive summary of HMLEs,beginning with a basic presentation of factors influencing HMLE electrochemical properties,the understanding of which can guide optimal HMLE designs.Rational strategies to improve the electrochemical performance of HMLEs accompanied by corresponding advantages and bottlenecks are subsequently discussed in terms of various factors ranging from inactive component modification to active material design to structural engineering at the electrode scale.This review will also present the recent progress and approaches of HMLEs applied in various EESSs,including advanced secondary batteries(lithium-/sodium-/potassium-/aluminum-/calcium-ion batteries,lithium metal anodes,lithium-sulfur batteries,lithium-air batteries,zinc batteries,magnesium batteries)and supercapacitors.Finally,this review will examine the challenges and prospects of HMLE commercialization with a focus on thermal safety,performance evaluation,advanced characterization,and production cost assessment to guide future development.

Nature-inspired porous multichannel carbon monolith:Molecular cooperative enables sustainable production and high-performance capacitive energy storage

The advancement of supercapacitors(SCs)is closely bound up with the breakthrough of rational design of energy materials.Freestanding and thick carbon(FTC)materials with well-organized porous structure is promising SC electrode delivering high areal capacitive performance.However,controllable and sustainable fabrication of such FTC electrode is still of great challenges.Inspired by natural honeycombs with cross-linked multichannel structure,herein,an innovative molecular-cooperative-interaction strategy is elaborately provided to realize honeycomb-like FTC electrodes.The nitrogen-doped porous carbon monolith(N-PCM)is obtained with advantages of interconnect pore structure and abundant nitrogen doping.Such strategy is based on naturally abundant molecular precursors,and free of pore-templates,expensive polymerization catalyst,and dangerous reaction solvent,rendering it a sustainable and cost-effective process.Systematic control experiments reveal that strong interactions among molecular precursors promise the structural stability of N-PCM during carbonization,and rational selection of molecular precursors with chemical blowing features is key step for well-developed honeycomb-like pore structure.Interestingly,the optimized sample exhibits hierarchical pore structure with specific surface area of 626.4 m^(2)g^(-1)and rational N-doping of 7.01 wt%.The derived SC electrode with high mass loading of 40.1 mg cm^(-2)shows an excellent areal capacitance of 3621 mF cm^(-2)at 1 mA cm^(-2)and good rate performance with 2920 mF cm^(-2)at 25 mA cm^(-2).Moreover,the constructed aqueous symmetric SC and quasi-solid-state SC produce high energy densities of 0.32 and 0.27 mWh cm^(-2),respectively.We believe that such a composition/microstructure controllable method can promote the fabrication and development of other thick electrodes for energy storage devices.