Conventional lithium-ion batteries(LIBs)with liquid electrolytes are challenged by their big safety concerns,particularly used in electric vehicles.All-solid-state batteries using solid-state electrolytes have been pr...Conventional lithium-ion batteries(LIBs)with liquid electrolytes are challenged by their big safety concerns,particularly used in electric vehicles.All-solid-state batteries using solid-state electrolytes have been proposed to significantly improve safety yet are impeded by poor interfacial solid–solid contact and fast interface degradation.As a compromising strategy,in situ solidification has been proposed in recent years to fabricate quasi-solid-state batteries,which have great advantages in constructing intimate interfaces and cost-effective mass manufacturing.In this work,quasi-solid-state pouch cells with high loading electrodes(≥3 m Ah cm^(-2))were fabricated via in situ solidification of poly(ethylene glycol)diacrylate-based polymer electrolytes(PEGDA-PEs).Both single-layer and multilayer quasi-solid-state pouch cells(2.0 Ah)have demonstrated stable electrochemical performance over500 cycles.The superb electrochemical stability is closely related to the formation of robust and compatible interphase,which successfully inhibits interfacial side reactions and prevents interfacial structural degradation.This work demonstrates that in situ solidification is a facile and cost-effective approach to fabricate quasi-solid-state pouch cells with both excellent electrochemical performance and safety.展开更多
Li metal batteries are supposed to reach real application in order to fulfill the high-energy density requirement of energy storage system.Unfortunately,the commonly used carbonate electrolyte react with pristine Li,w...Li metal batteries are supposed to reach real application in order to fulfill the high-energy density requirement of energy storage system.Unfortunately,the commonly used carbonate electrolyte react with pristine Li,which result in short lifetime of lithium metal battery.To alleviate the side reactions of Li metal with liquid electrolyte,here we propose a phosphate rich polymer-inorganic layer as an interphase.Due to the inert properties of lithium phosphate derived from LiPO_(2)F_(2)and poly-ether,the side-reaction of carbonate solvent are prevented.As a result,lithium metal anode sustains for 800 cycles in symmetrical cell test under 1 m A cm^(-2).Even under strict condition(20μm Li,capacity ratio N/P=2.3,electrolyte/active material=3μL mg^(-1)),coin cell test still runs stable for 150 cycles with high Coulombic efficiency.Furthermore,both LiFePO_(4)and LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)pouch cell under 5μL m A^(-1)h^(-1)condition also exhibit good stability at 0.5 C and 2 C rate.With this approach,high-energy and high-power Li metal batteries are approaching to real application in the near future.展开更多
The past decade has witnessed a rapid surge of interest in the research and development of non-precious metal-based electrocatalysts for the oxygen reduction reaction (ORR). Until now, the best catalysts in acidic e...The past decade has witnessed a rapid surge of interest in the research and development of non-precious metal-based electrocatalysts for the oxygen reduction reaction (ORR). Until now, the best catalysts in acidic electrolytes have exclusively been Fe-N-C-type materials from high-temperature pyrolysis. Despite the ORR activities of metal phthalocyanine or porphyrin macrocydes having long been known, their durability remains poor. In this work, we use these macrocycles as a basis to develop a novel organic-carbon hybrid material from in-situ polymerization of iron phthalocyanine on conductive multiwalled carbon nanotube scaffolds using a low-temperature microwave heating method. At an optimal polymer- to-carbon ratio, the hybrid electrocatalyst exhibits excellent ORR activity with a positive half-wave potential (0.80 V), large mass activity (up to 18.0 A/g at 0.80 V), and a low peroxide yield (〈3%). In addition, strong electronic coupling between the polymer and carbon nanotubes is believed to suppress demetallization of the macrocycles, significantly improving cycling stability in acids. Our study represents a rare example of non-precious metal-based electrocatalysts prepared without high-temperature pyrolysis, while having ORR activity in acidic media with potential for practical applications.展开更多
Nanostructured metal sulfides are potential electrode materials for sodium-ion batteries; however, they typically suffer from very poor cycling stability due to large volume changes and dissolution of discharge produc...Nanostructured metal sulfides are potential electrode materials for sodium-ion batteries; however, they typically suffer from very poor cycling stability due to large volume changes and dissolution of discharge products. Herein we propose a rational material design strategy for sulfide-based materials to address these problems. Taking nickel sulfide (NiSx) as an example, we demonstrated that its electrochemical performance can be dramatically improved by confining the NiSx nanoparticles in a percolating conductive carbon nanotube network, and stabilizing them with an ultrathin carbon coating layer. The carbon layer serves as a physical barrier to alleviate the effects of both the volume change and dissolution of active materials. The hybrid material exhibited a large reversible specific capacity of 〉500 mAh/g and excellent cycling stability over 200 cycles. Given the traditionally problematic nature of NiSx as a battery anode material, we believe that the observed high performance reported here reflects the effectiveness of our material design strategy.展开更多
基金supported by the Natural Sciences and Engineering Research Council of Canada(NSERC),Canada Research Chair Program(CRC),Canada Foundation for Innovation(CFI),Ontario Research Fund(ORF),China Automotive Battery Research Institute Co.,Ltd.,Glabat Solid-State Battery Inc.,Canada Light Source(CLS)at the University of Saskatchewan,Interdisciplinary Development Initiatives(IDI)by Western University,and University of Western Ontariothe support from Mitacs Accelerate Program(IT13735)the funding support from Banting Postdoctoral Fel owship(BPF—180162)
文摘Conventional lithium-ion batteries(LIBs)with liquid electrolytes are challenged by their big safety concerns,particularly used in electric vehicles.All-solid-state batteries using solid-state electrolytes have been proposed to significantly improve safety yet are impeded by poor interfacial solid–solid contact and fast interface degradation.As a compromising strategy,in situ solidification has been proposed in recent years to fabricate quasi-solid-state batteries,which have great advantages in constructing intimate interfaces and cost-effective mass manufacturing.In this work,quasi-solid-state pouch cells with high loading electrodes(≥3 m Ah cm^(-2))were fabricated via in situ solidification of poly(ethylene glycol)diacrylate-based polymer electrolytes(PEGDA-PEs).Both single-layer and multilayer quasi-solid-state pouch cells(2.0 Ah)have demonstrated stable electrochemical performance over500 cycles.The superb electrochemical stability is closely related to the formation of robust and compatible interphase,which successfully inhibits interfacial side reactions and prevents interfacial structural degradation.This work demonstrates that in situ solidification is a facile and cost-effective approach to fabricate quasi-solid-state pouch cells with both excellent electrochemical performance and safety.
基金supported by the Jilin Province Science and Technology Department Program(Nos.YDZJ202201ZYTS304)the Science and Technology Project of Jilin Provincial Education Department(JJKH20220428KJ)+3 种基金the R&D Program of Power Batteries with Low Temperature and High Energy,Science and Technology Bureau of Changchun(19SS013)the Key Subject Construction of Physical Chemistry of Northeast Normal Universitythe Fundamental Research Funds for the Central Universities(2412020FZ007,2412020FZ008)the National Natural Science Foundation of China(22102020)。
文摘Li metal batteries are supposed to reach real application in order to fulfill the high-energy density requirement of energy storage system.Unfortunately,the commonly used carbonate electrolyte react with pristine Li,which result in short lifetime of lithium metal battery.To alleviate the side reactions of Li metal with liquid electrolyte,here we propose a phosphate rich polymer-inorganic layer as an interphase.Due to the inert properties of lithium phosphate derived from LiPO_(2)F_(2)and poly-ether,the side-reaction of carbonate solvent are prevented.As a result,lithium metal anode sustains for 800 cycles in symmetrical cell test under 1 m A cm^(-2).Even under strict condition(20μm Li,capacity ratio N/P=2.3,electrolyte/active material=3μL mg^(-1)),coin cell test still runs stable for 150 cycles with high Coulombic efficiency.Furthermore,both LiFePO_(4)and LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)pouch cell under 5μL m A^(-1)h^(-1)condition also exhibit good stability at 0.5 C and 2 C rate.With this approach,high-energy and high-power Li metal batteries are approaching to real application in the near future.
基金Acknowledgements We acknowledge supports from the National Natural Science Foundation of China (Nos. 51472173, 51522208 and 21472135), the Natural Science Foundation of Jiangsu Province (Nos. BK20140302 and SBK2015010320), the Priority Academic Program Development of Jiangsu Higher Education Institutions and Collaborative Innovation Center of Suzhou Nano Science and Technology
文摘The past decade has witnessed a rapid surge of interest in the research and development of non-precious metal-based electrocatalysts for the oxygen reduction reaction (ORR). Until now, the best catalysts in acidic electrolytes have exclusively been Fe-N-C-type materials from high-temperature pyrolysis. Despite the ORR activities of metal phthalocyanine or porphyrin macrocydes having long been known, their durability remains poor. In this work, we use these macrocycles as a basis to develop a novel organic-carbon hybrid material from in-situ polymerization of iron phthalocyanine on conductive multiwalled carbon nanotube scaffolds using a low-temperature microwave heating method. At an optimal polymer- to-carbon ratio, the hybrid electrocatalyst exhibits excellent ORR activity with a positive half-wave potential (0.80 V), large mass activity (up to 18.0 A/g at 0.80 V), and a low peroxide yield (〈3%). In addition, strong electronic coupling between the polymer and carbon nanotubes is believed to suppress demetallization of the macrocycles, significantly improving cycling stability in acids. Our study represents a rare example of non-precious metal-based electrocatalysts prepared without high-temperature pyrolysis, while having ORR activity in acidic media with potential for practical applications.
基金The authors greatly acknowledge the financial support from the National Natural Science Foundation of China (Nos. 51472173 and 51522208), the Natural Science Foundation of Jiangsu Province (Nos. BK20140302 and SBK2015010320), the Priority Academic Program Development of Jiangsu Higher Education Institutions and Collaborative Innovation Center of Suzhou Nano Science and Technology.
文摘Nanostructured metal sulfides are potential electrode materials for sodium-ion batteries; however, they typically suffer from very poor cycling stability due to large volume changes and dissolution of discharge products. Herein we propose a rational material design strategy for sulfide-based materials to address these problems. Taking nickel sulfide (NiSx) as an example, we demonstrated that its electrochemical performance can be dramatically improved by confining the NiSx nanoparticles in a percolating conductive carbon nanotube network, and stabilizing them with an ultrathin carbon coating layer. The carbon layer serves as a physical barrier to alleviate the effects of both the volume change and dissolution of active materials. The hybrid material exhibited a large reversible specific capacity of 〉500 mAh/g and excellent cycling stability over 200 cycles. Given the traditionally problematic nature of NiSx as a battery anode material, we believe that the observed high performance reported here reflects the effectiveness of our material design strategy.