Energy & Environmental Materials
·
2021
·Vol. 5
·期 2
·524-532
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IF 15.122
Jun Zhao,Yongfu Tang,Qiushi Dai,Congcong Du,Yin Zhang,Dingchuan Xue,Tianwu Chen,Jingzhao Chen,Bo Wang,Jingming Yao,Ning Zhao,Yanshuai Li,Shuman Xia,Xiangxin Guo,Stephen J. Harris,Liqiang Zhang,Sulin Zhang,Ting Zhu,Jianyu Huang
Lithium (Li) penetration through solid electrolytes (SEs) induces short circuits in Li solid-state batteries (SSBs), which is a critical issue that hinders the development of high energy density SSBs. While cracking in ceramic SEs has been often shown to accompany Li penetration, the interplay between Li deposition and cracking remains elusive. Here, we constructed a mesoscale SSB inside a focused ion beam-scanning electron microscope (FIB-SEM) for in situ observation of Li deposition-induced cracking in SEs at nanometer resolution. Our results revealed that Li propagated predominantly along transgranular cracks in a garnet Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO). Cracks appeared to initiate from the interior of LLZTO beneath the electrode surface and then propagated by curving toward the LLZTO surface. The resulting bowl-shaped cracks resemble those from hydraulic fracture caused by high fluid pressure on the surface of internal cracks, suggesting that the Li deposition-induced pressure is the major driving force of crack initiation and propagation. The high pressure generated by Li deposition is further supported by in situ observation of the flow of filled Li between the crack flanks, causing crack widening and propagation. This work unveils the dynamic interplay between Li deposition and cracking in SEs and provides insight into the mitigation of Li dendrite penetration in SSBs.
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NATURE
·
2021
·Vol. 592
·期 7855
·551-557
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IF 49.962
Chi Xiwen,Li Malin,Di Jiancheng,Bai Pu,Song Lina,Wang Xiaoxue,Li Fei,Liang Shuang,Xu Jijing,Yu Jihong
Solid-state lithium (Li)–air batteries are recognized as a next-generation solution for energy storage to address the safety and electrochemical stability issues that are encountered in liquid battery systems 1 , 2 , 3 , 4 . However, conventional solid electrolytes are unsuitable for use in solid-state Li–air systems owing to their instability towards lithium metal and/or air, as well as the difficulty in constructing low-resistance interfaces 5 . Here we present an integrated solid-state Li–air battery that contains an ultrathin, high-ion-conductive lithium-ion-exchanged zeolite X (LiX) membrane as the sole solid electrolyte. This electrolyte is integrated with cast lithium as the anode and carbon nanotubes as the cathode using an in situ assembly strategy. Owing to the intrinsic chemical stability of the zeolite, degeneration of the electrolyte from the effects of lithium or air is effectively suppressed. The battery has a capacity of 12,020 milliamp hours per gram of carbon nanotubes, and has a cycle life of 149 cycles at a current density of 500 milliamps per gram and at a capacity of 1,000 milliamp hours per gram. This cycle life is greater than those of batteries based on lithium aluminium germanium phosphate (12 cycles) and organic electrolytes (102 cycles) under the same conditions. The electrochemical performance, flexibility and stability of zeolite-based Li–air batteries confer practical applicability that could extend to other energy-storage systems, such as Li–ion, Na–air and Na–ion batteries.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 167
·期 16
·160557
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IF 4.316
Guange Wang,Tong Wu,Borui Liu,Shanshan Gong,Qing Huang,Yuefeng Su,Feng Wu,Ryan M. Kelly
Considering that lithium-ion battery (LIB) is still an indispensable and important component of energy storage materials, the sustainable post-processing of spent LIBs in labs or enterprises becomes a tricky problem. Herein, a novel scheme is proposed to dissert the recycling of the spent LIBs. The LIB is recycled into Li(Ni0.9Co0.05Mn0.05)O2 (NCM90) cathode material with high specific capacity by introducing an innovative hydrometallurgy-coprecipitation treatment method. The spent LiCoO2 (LCO) cathode material is firstly leached by sulfuric acid, and the leachate is gradient used as the raw materials to resynthesize high-nickel NCM material by adjusting the leachate dosage to about 50%. Interestingly, when the dosage exceeds 50%, the crystal structure aggravates, and Li+/Ni2+ mixing improves. The specific capacity of regenerated battery is 181.4 mAh g−1 at 0.5 C (1 C = 200 mAh g−1) and the capacity retention achieves 93.2% after 100 cycles. The reasons can be attributed to the cation mixing and crystal strucure and the small amount of Al doping. In conclusion, this combined method recycling of LIBs has huge potential value for environment protection and production.
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Materials
·
2020
·Vol. 13
·期 20
·4611
·
IF 3.057
Wen Ding,Xiaozhong Wu,Yanyan Li,Shuo Wang,Shuping Zhuo
The biomass-based carbons anode materials have drawn significant attention because of admirable electrochemical performance on account of their nontoxicity and abundance resources. Herein, a novel type of nickel-embedded carbon material (nickel@carbon) is prepared by carbonizing the dough which is synthesized by mixing wheat flour and nickel nitrate as anode material in lithium-ion batteries. In the course of the carbonization process, the wheat flour is employed as a carbon precursor, while the nickel nitrate is introduced as both a graphitization catalyst and a pore-forming agent. The in situ formed Ni nanoparticles play a crucial role in catalyzing graphitization and regulating the carbon nanocrystalline structure. Mainly owing to the graphite-like carbon microcrystalline structure and the microporosity structure, the NC-600 sample exhibits a favorable reversible capacity (700.8 mAh g−1at 0.1 A g−1after 200 cycles), good rate performance (51.3 mAh g−1at 20 A g−1), and long-cycling durability (257.25 mAh g−1at 1 A g−1after 800 cycles). Hence, this work proposes a promising inexpensive and highly sustainable biomass-based carbon anode material with superior electrochemical properties in LIBs.Keywords:biomass-based carbon;nickel nanoparticles;lithium-ion batteries;anode material
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Wenhui Zhu,Ali Reza Kamali
A facile and fast molten salt strategy is developed, for the first time, to synthesis sodium dimolybdate (Na 2 Mo 2 O 7 ). The process is based on a thermodynamically favorable reaction between naturally available precursors MoS 2 and NaCl to produce Na 2 Mo 2 O 7 as well as a gas phase that leaves the system. The product is characterized by electron microscopy and energy-dispersive X-ray spectroscopy (EDX) as well as X-ray diffraction (XRD) and Raman spectroscopy . The prepared Na 2 Mo 2 O 7 in combination with molten salt-synthesized graphene nanosheets is examined as anode material for Li-ion batteries, exhibiting an interesting performance, with the first cycle discharge and charge capacities of 1363 and 857 mAh g −1 , respectively, at 100 mA g −1 . A reversible Li storage capacity of 506 mAh g −1 can still be observed after 100 cycles. The results are rather interesting towards the development of low-cost and high-performance Na 2 Mo 2 O 7 anode materials.
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JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Chang Wu,Yuyang Hou,Jicheng Jiang,Haipeng Guo,Hua-Kun Liu,Jun Chen,Jiazhao Wang
Li–O 2 batteries has been widely investigated for its ultra-high capacity as next generation batteries. Nevertheless, some problems like sluggish kinetic reaction and instability hugely impede the practical use of Li–O 2 batteries. In this work, Mo 2 C/MoO 2 @RGO heterostructures was fabricated by in-situ growth of Mo 2 C between MoO 2 and RGO during calcination and being employed as cathode to explore the synergistic effect in Li–O 2 batteries. As a result, Mo 2 C/MoO 2 @RGO exhibits good specific capacity with 2365 mAh g −1 , high round-trip efficiency (89% at first cycle) and improved cycling performance. Density functional theory calculations indicated that the Mo 2 C/MoO 2 @RGO heterostructures have better capability of oxygen adsorption than sole constituent (Mo 2 C@RGO or MoO 2 @RGO), which triggers the formation of film-like amorphous discharge products, leading to lower overpotential and stable performance. Our study reveals the important role of heterostructures in Li–O 2 batteries system and demonstrates a promising design strategy for heterostructured catalyst.
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ACS Nano
·
2020
·
IF 14.588
Qingping Wu,Zhenguo Yao,Xuejun Zhou,Jun Xu,Fahai Cao,Chilin Li
A cathode host with strong sulfur/polysulfide confinement and fast redox kinetics is a challenging demand for high-loading lithium–sulfur batteries. Recently, porous carbon hosts derived from metal–organic frameworks (MOFs) have attracted wide attention due to their unique spatial structure and customizable reaction sites. However, the loading and rate performance of Li–S cells are still restricted by the disordered pore distribution and surface catalysis in these hosts. Here, we propose a concept of built-in catalysis to accelerate lithium polysulfide (LiPSs) conversion in confined nanoreactors, i.e., laterally stacked ordered crevice pores encompassed by MoS2-decorated carbon thin layers. The functions of S-fixability and LiPS catalysis in these mesoporous cavity reactors benefit from the 2D interface contact between ultrathin catalytic MoS2 and conductive C pyrolyzed from Al-MOF. The integrated function of adsorption–catalysis–conversion endows the sulfur-infused C@MoS2 electrode with a high initial capacity of 1240 mAh g–1 at 0.2 C, long life cycle stability of at least 1000 cycles at 2 C, and high rate endurance up to 20 C. This electrode also exhibits commercial potential in view of considerable capacity release and reversibility under high sulfur loading (6 mg cm–2 and ∼80 wt %) and lean electrolyte (E/S ratio of 5 μL mg–1). This study provides a promising design solution of a catalysis–conduction 2D interface in a 3D skeleton for high-loading Li–S batteries.
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Materials Today Physics
·
2021
·
IF 9.298
P. Jiang,P. Guo,Y. Shi,S. Li,K. Li,X.Y. Lu,Z. Zhang,D. He,J. Bian,X. Lu
It is still a great challenge to fabricate dense solid electrolyte with high ionic conductivity using a facile and low-cost method for all solid-state rechargeable battery. In this context, a cold sintering process (CSP) is employed to prepare the ceramic solid electrolytes at an extremely low temperature of 120 °C, significantly suppressing the Li loss and impurity formation by traditionally high-temperature sintering. The low temperature prepared Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP)-LiClO 4 (10.0 wt%) composite electrolyte exhibits a high ionic conductivity of 6.35 × 10 −5 S/cm, low activation energy of 0.26 eV and high relative densities of 90%. The Li | CSP LAGP-LiClO 4 (10.0 wt%) | Li symmetric cell delivers a cycling time retention of over 350 h with a stabilized voltage overpotential at a current density of 0.2 mA/cm 2 . Moreover, the high Coulombic efficiency of 99.97% and capacity retention of 150 mAh/g are achieved after 130 cycles at 0.1C in Li | CSP LAGP-LiClO 4 (10.0 wt%) | LiFePO 4 solid cells. These good electrochemical performances are originated from the well-constructed solid electrolyte-electrode interfaces, where the electrochemically active interface demonstrates the powerful self-stabilization function to maintain the tight interface connection as well as the continuous Li ion transport. The CSP method sheds new light on the fabrication of solid electrolytes at a low temperature and inexpensive way, hence provides a rewarding avenue to fabricate better solid-state batteries and other electrochemical devices .
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Jingjing Zhou,Jiahang Chen,Jun Yang,Yanna Nuli,Jiulin Wang
Rechargeable Li-metal anodes have received abundant attention for high-energy-density batteries. A solid electrolyte interphase (SEI) plays a significant role in regulating the Li+ deposition/stripping process. Aimed to solve detrimental Li deposition with a dendritic and mossy morphology, herein, dendrite-free columnar Li deposition in micron size is constructed via creatively adopting a LiNO3-based electrolyte even at a high current density (2 mA cm–2) and areal capacity (4 mAh cm–2). N-rich inorganic SEI (Li3N and LiNxOy) with superior Li+ conductivity is formed on Li deposition, which enables remarkable reversibility and high average Coulombic efficiency (CE) even over 240 cycles. A Li∥LiFePO4 cell delivers excellent cycling stability over 700 cycles with a capacity fading rate of merely 0.022% per cycle. This work provides a way to regulating columnar Li deposition via N-rich SEI coordination and developing electrolyte formulations for secondary Li-metal batteries.
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JOURNAL OF MEMBRANE SCIENCE
·
2019
·
IF 7.015
Chengyi Zhang,Yingxin Mu,Wen Zhang,Song Zhao,Yuxin Wang
Developing effective technologies for extraction of Li + from salt-lake brines with high Mg 2+ /Li + ratios is paramount for sustainable utilization of lithium resources in electric vehicle and nuclear energy industries. In this work, hybrid membranes were prepared with polyvinyl chloride matrix and six metal−organic frameworks (MOFs@PVC) to separate Li + from Mg 2+ in solution. The effects of pore size sieving and sulfonation of the MOFs on the Li + /Mg 2+ separation efficiency were evaluated using the current-voltage ( I – V ) method, and the stability of the MOFs@PVC membranes was systematically evaluated. The loading amount of MOFs and the thickness of the membranes were also optimized for Li + transport and selectivity. The results show that the small pore size and sulfonation of MOFs are benefit to separate Li + from Mg 2+ . Specifically, PVC-based hybrid membrane containing HSO 3 -UiO-66 shows the highest selectivity for Li + (Li + /Mg 2+ > 4), with the diffusion coefficient of 2.0×10 -10 cm 2 s -1 for Li + and 4.67×10 -11 cm 2 s -1 for Mg 2+ . This study highlights the stable sulfonated Zr-based MOF with suitable pore sizes for membrane-based Li + /Mg 2+ separation, and provides a potential alternative for recovering lithium from salt-lake brines.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Shiyu Bie,Meili Du,Wenxiang He,Huigang Zhang,Zhentao Yu,Jianguo Liu,Meng Liu,Wuwei Yan,Liang Zhou,Zhigang Zou
Efficient electrocatalysts for Li2CO3 decomposition play an important role in Li–CO2 batteries. In this paper, carbon nanotubes (CNTs) decorated with RuO2 is firstly introduced as cathode materials for Li–CO2 batteries. The CNT@RuO2 composite can not only deliver a high specific capacity but also a lower charge voltage. With the CNT@RuO2 cathodes, the Coulombic efficiency still remains around 100% until the 15th cycle. The charge voltage of early 30 cycles at a current of 50 mA·g–1 with a capacity limit of 500 mAh·g–1 can be fully lowered under 4.0 V. Particularly, the CNT@RuO2 cathode can realize most decomposition of prefilled Li2CO3 and show a platform at around 3.9 V. This catalytic activity toward both in situ formed and preloaded Li2CO3 is more feasible for practical application in complex environment.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2019
·
IF 3.218
Peng Xu,Congdi Chen,Jiajia Zhu,Jian Xie,Pei Zhao,Miao Wang
In this work, we report a novel cathode composed of three-dimensional intersected graphene nanoribbons skeleton decorated with RuO 2 catalyst, where graphene nanoribbons are obtained by unzipping multi-walled carbon nanotubes . The graphene nanoribbons framework exhibits a three-dimensional intersected structure and a large specific surface area, leading to a higher capacity than multi-walled carbon nanotubes. The RuO 2 introduced via a facile dropping method enhances the oxygen evolution reaction kinetics and obviously reduces the charge overpotential. More importantly, the Li–O 2 battery with RuO 2 decorated graphene nanoribbons cathode presents an excellent cycling stability of 424 cycles at a curtailed capacity of 1000 mAh g −1 , which can be attributed to the synergistic effect between the intersected band-like graphene and highly effective RuO 2 particles. The Li 2 O 2 deposited on graphene nanoribbons shows a totally different surface morphology compared with that on multi-walled carbon nanotubes due to the different structures of carbon substrates. This work provides a promising design of highly efficient air electrodes for high-performance Li–O 2 batteries.
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