Lithium metal is supposed to be critical material for constructing next-generation batteries due to extremely high capacity and ultralow redox potential. However, the perplexing issue of lithium dendrite growth impede...Lithium metal is supposed to be critical material for constructing next-generation batteries due to extremely high capacity and ultralow redox potential. However, the perplexing issue of lithium dendrite growth impedes the commercial application. The initial nucleation and low Li ions diffusion rate in the electrolyte/electrode interface dominate the deposition behavior. Therefore, a uniform and flexible interface is urgently needed. Here, a facile method is proposed to prepare a thin and porous LiF-rich layer (TPL) by the in-situ reaction of small amount of ammonium hydrogen difluoride (NH4HF2) and Li metal. The deposition morphology on Li metal anode with LiF layer is significantly flat and homogeneous owning to low lateral diffusion barrier on LiF crystals and the porous structure of TPL film. Additionally, the symmetrical cells made with such TPL Li anodes show significantly stable cycling over 100 cycles at high current density of 6 mA/cm^2. The TPL Li|LiFePO4 full cells keep over 99% capacity retention after 100 cycles at 2.0 C. This approach serves as a facile and controllable way of adjusting the protective layer on Li metal.展开更多
To meet the requirements of electronic vehicles(EVs) and hybrid electric vehicles(HEVs),the high energy density Li Ni_(0.8) Co_(0.15) Al_(0.05) O_2(NCA) cathode and Si–C anode have attracted more attention.Here we re...To meet the requirements of electronic vehicles(EVs) and hybrid electric vehicles(HEVs),the high energy density Li Ni_(0.8) Co_(0.15) Al_(0.05) O_2(NCA) cathode and Si–C anode have attracted more attention.Here we report the thermal behaviors of NCA/Si–C pouch cell during the charge/discharge processes at different current densities.The total heat generations are derived from the surface temperature change during electrochemical Li+insertion/extraction in adiabatic surrounding.The reversible heat is determined by the entropic coefficients,which are related with open-circuit voltage at different temperatures; while the irreversible heat is determined by the internal resistance,which can be obtained via V–I characteristic,electrochemical impedance spectroscopy and hybrid pulse power characterization(HPPC).During the electrochemical process,the reversible heat contributes less than 10% to total heat generation; and the heat generated in charge process is less than that in discharge process.The results of thermal behaviors analyses are conducive to understanding the safety management and paving the way for building a reliable thermal model of high energy density lithium ion battery.展开更多
Glycerol is an alternative sustainable fuel for fuel cells,and efficient electrocatalyst is crucial for glycerol oxidation reaction(GOR).The promising Pt catalysts are subject to the inadequate capability of C-C bond ...Glycerol is an alternative sustainable fuel for fuel cells,and efficient electrocatalyst is crucial for glycerol oxidation reaction(GOR).The promising Pt catalysts are subject to the inadequate capability of C-C bond cleavage and the susceptibility to poisoning.Herein,Pt-Sn alloyed nanoparticles are immobilized on hierarchical nitrogen-doped carbon nanocages(hNCNCs)by convenient ethylene glycol reduction and subsequent thermal reduction.The optimal Pt_(3)Sn/hNCNC catalyst exhibits excellent GOR performance with a high mass activity(5.9 A·mg_(Pt)^(-1)),which is 2.7 and 5.4 times higher than that of Pt/hNCNC and commercial Pt/C,respectively.Such an enhancement can be mainly ascribed to the increased anti-poisoning and C-C bond cleavage capability due to the Pt_(3)Sn alloying effect and Sn-enriched surface,the high dispersion of Pt_(3)Sn active species due to N-participation,as well as the high accessibility of Pt_(3)Sn active species due to the three-dimensional(3D)hierarchical architecture of hNCNC.This study provides an effective GOR electrocatalyst and convenient approach for catalyst preparation.展开更多
Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis technology.Herein,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-laye...Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis technology.Herein,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 h.The outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D architecture.Specifically,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both electrodes.This study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.展开更多
基金supported by the National Basic Research Program of China (Grant no. 2015CB251100)Beijing Natural Science Foundation (No. L182023)
文摘Lithium metal is supposed to be critical material for constructing next-generation batteries due to extremely high capacity and ultralow redox potential. However, the perplexing issue of lithium dendrite growth impedes the commercial application. The initial nucleation and low Li ions diffusion rate in the electrolyte/electrode interface dominate the deposition behavior. Therefore, a uniform and flexible interface is urgently needed. Here, a facile method is proposed to prepare a thin and porous LiF-rich layer (TPL) by the in-situ reaction of small amount of ammonium hydrogen difluoride (NH4HF2) and Li metal. The deposition morphology on Li metal anode with LiF layer is significantly flat and homogeneous owning to low lateral diffusion barrier on LiF crystals and the porous structure of TPL film. Additionally, the symmetrical cells made with such TPL Li anodes show significantly stable cycling over 100 cycles at high current density of 6 mA/cm^2. The TPL Li|LiFePO4 full cells keep over 99% capacity retention after 100 cycles at 2.0 C. This approach serves as a facile and controllable way of adjusting the protective layer on Li metal.
基金supported by the National Key R&D Program of China:Trackling Key Technology for Development and Industrialization of Power Lithium Ion Battery with High Specific Energy (Grant No.2016YFB0100508)
文摘To meet the requirements of electronic vehicles(EVs) and hybrid electric vehicles(HEVs),the high energy density Li Ni_(0.8) Co_(0.15) Al_(0.05) O_2(NCA) cathode and Si–C anode have attracted more attention.Here we report the thermal behaviors of NCA/Si–C pouch cell during the charge/discharge processes at different current densities.The total heat generations are derived from the surface temperature change during electrochemical Li+insertion/extraction in adiabatic surrounding.The reversible heat is determined by the entropic coefficients,which are related with open-circuit voltage at different temperatures; while the irreversible heat is determined by the internal resistance,which can be obtained via V–I characteristic,electrochemical impedance spectroscopy and hybrid pulse power characterization(HPPC).During the electrochemical process,the reversible heat contributes less than 10% to total heat generation; and the heat generated in charge process is less than that in discharge process.The results of thermal behaviors analyses are conducive to understanding the safety management and paving the way for building a reliable thermal model of high energy density lithium ion battery.
基金support from the National Key Research and Development Program of China(No.2021YFA1500900)the National Natural Science Foundation of China(Nos.21832003,21972061,52071174)+2 种基金the Natural Science Foundation of Jiangsu Province,Major Project(No.BK20212005)China Postdoctoral Science Foundation(No.2022M711564)the Fellowship of China National Postdoctoral Program for Innovative Talents(No.BX2021119).
文摘Glycerol is an alternative sustainable fuel for fuel cells,and efficient electrocatalyst is crucial for glycerol oxidation reaction(GOR).The promising Pt catalysts are subject to the inadequate capability of C-C bond cleavage and the susceptibility to poisoning.Herein,Pt-Sn alloyed nanoparticles are immobilized on hierarchical nitrogen-doped carbon nanocages(hNCNCs)by convenient ethylene glycol reduction and subsequent thermal reduction.The optimal Pt_(3)Sn/hNCNC catalyst exhibits excellent GOR performance with a high mass activity(5.9 A·mg_(Pt)^(-1)),which is 2.7 and 5.4 times higher than that of Pt/hNCNC and commercial Pt/C,respectively.Such an enhancement can be mainly ascribed to the increased anti-poisoning and C-C bond cleavage capability due to the Pt_(3)Sn alloying effect and Sn-enriched surface,the high dispersion of Pt_(3)Sn active species due to N-participation,as well as the high accessibility of Pt_(3)Sn active species due to the three-dimensional(3D)hierarchical architecture of hNCNC.This study provides an effective GOR electrocatalyst and convenient approach for catalyst preparation.
基金supported by the National Key Research and Development Program of China(No.2021YFA1500900)the National Natural Science Foundation of China(Nos.52071174,21832003,21972061)+1 种基金the Natural Science Foundation of Jiangsu Province,Major Project(No.BK20212005)the Foundation of Science and Technology of Suzhou(No.SYC2022102).
文摘Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis technology.Herein,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 h.The outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D architecture.Specifically,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both electrodes.This study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.