Nanoscale
·
2022
·Vol. 15
·期 2
·588-598
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IF 8.307
Zhenbo Wang,Yanfeng Yin,Guanjie He,Huiling Zhao,Ying Bai
With large specific capacity, wide voltage window, and high energy density, Li-rich layered oxides have been considered as a promising cathode candidate for advanced lithium-ion batteries (LIBs). However, their commercial application is challenging due to severe capacity degradation and voltage fading caused by irreversible oxygen evolution and phase transition upon repeated cycling. This work proposes an effective strategy to improve the long-term electrochemical performances of Li1.2Mn0.56Ni0.17Co0.07O2 (LMNCO) by constructing multifunctional nanolayers composed of element-doping, layered-spinel heterostructural connection, and fast ion conductor shell via a facile method. The Li0.09B0.97PO4 (LBPO) coating shell acts as a fast ion carrier and physical screen to promote Li+ diffusion and isolate side reactions at the cathode-electrolyte interface; moreover, two-phase transitional region provides three-dimensional channel to facilitate Li+ transport and inhibit phase transition. Besides, B3+ and PO43−-doping collaborates with oxygen vacancies to stabilize lattice oxygen and restrain oxygen evolution from the bulk active cathode. The optimized LMNCO@LBPO material exhibits a superior capacity retention of 78.6%, higher than that of the pristine sample (49.3%), with the mitigated voltage fading of 0.73 mV per cycle after 500 cycles at 1 C. This study opens up an avenue for the surface modification to the electrochemical properties and perspective application of Li-rich cathodes in high-performance LIBs.
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高影响因子
Sustainable Materials and Technologies
·
2023
·
IF 9.6
Yunchun Zha,Zitong Fei,Zelong Yang,Qi Meng,Peng Dong,Yingjie Zhang,Yong Li
Recycling of spent lithium-ion batteries is an urgent task in view of the resource shortage and environmental concerns. Pretreatment as the first step in recycling of spent lithium-ion batteries has become urgent issue for efficient separation of spent cathode materials from aluminum foil . Herein, a facile ternary molten salts approach is presented for efficient separation of cathode material and aluminum foil synchronous implementation of regeneration of spent cathode material. The separation efficiency reaches 99.98% at molar ratio of LiNO 3 : LiOH·H 2 O: Li 2 CO 3 (LNOC) of 3:2:0.5 with mass ratio of spent cathode pieces to the ternary molten salts of 1:2 holding at 300 °C for 15 min. The regenerated materials show discharging capacity of 122.2 mAhg −1 at 1C with retention rate of 99.97% after 100 cycles. The ternary molten salts are also made available for separation of other spent cathode materials with achieving high separation efficiency.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Huanhuan Wu,Haoyue Zhao,Yakai Lin,Xin Liu,Lin Wang,Hong Yao,Yuanhui Tang,Lixin Yu,Haihui Wang,Xiaolin Wang
Positively charged nanofiltration membrane has gained significant interest in magnesium and lithium separation due to its separation mechanism, especially in salt lake-based lithium industry. To obtain a high-density positive charged surface and high Li + /Mg 2+ selectivity, a novel thin-film nanocomposite (TFN) nanofiltration (NF) membrane for recovery of Li + from Mg/Li mixtures with Mg 2+ /Li + ratios of 20 was successfully prepared by using polymeric amine polyethyleneimine (PEI) and monomeric amine silane coupling agent (3-diamino-methyl-cyclohexyl triethoxysilane, DTES). Then the effect of DTES on the surface properties and performance of the prepared DTES/PEI/TMC TFN membranes were investigated. Chemical composition analysis revealed that DTES not only hydrolyzed to Si–OH and then self-polymerized to Si–O–Si, but also reacted with the self-carrying acyl chloride of 1,3,5-benzene trichloromethane (TMC). Moreover, SiO 2 nanoparticles were in-situ generated from DTES inside the PA layer with high compatibility. Due to the compatible properties with the positively charged PEI polymer, the reacted DTES was distributed uniformly in the formed TFN selective layer with no noticeable aggregation. The doping of SiO 2 into the polyamide network gave rise to the enlargement of the membrane pore size, enhanced the surface hydrophilicity, and reinforced the surface positive charges. The water flux of the DTES/PEI/TMC membrane improved from 36.9 L m −2 h −1 to 49.58 L m −2 h −1 compared to the PEI/TMC membrane. Additionally, the Mg 2+ and Li + rejection of the optimized membranes was 91.46% and −10.5%, respectively, with permeability and selectivity (S Li, Mg = 12.95) superior to that of the commercial NF membranes. Considering the commercial availability of DTES, this study not only offers a high-performance nanofiltration membrane for recovering lithium from brines but also provides a feasible strategy for industrial separation of other monovalent and divalent ions.
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ADVANCED MATERIALS
·
2023
·Vol. 35
·期 12
·2208951
·
IF 29.4
Jie Biao,Bing Han,Yidan Cao,Qidong Li,Guiming Zhong,Jiabin Ma,Likun Chen,Ke Yang,Jinshuo Mi,Yonghong Deng,Ming Liu,Wei Lv,Feiyu Kang,Yan-Bing He
Poor ion and high electron transport at the grain boundaries (GBs) of ceramic electrolytes are the primary reasons for lithium filament infiltration and short-circuiting of all-solid-state lithium metal batteries (ASLMBs). Herein, it is discovered that Li 2 CO 3 at the GBs of Li 7 La 3 Zr 2 O 12 (LLZO) sheets is reduced to highly electron-conductive LiC x during cycling, resulting in lithium penetration of LLZO. The ionic and electronic conductivity of the GBs within LLZO can be simultaneously tuned using sintered Li 3 AlF 6 . The generated LiAlO 2 (LAO) infusion and F-doping at the GBs of LLZO (LAO-LLZOF) significantly reduce the Li 2 CO 3 content and broaden the energy bandgap of LLZO, which decreases the electronic conductivity of LAO-LLZOF. LAO forms a 3D continuous ion transport network at the GB that significantly improves the total ionic conductivity. Lithium penetration within LLZO is suppressed and an all-solid-state LiFePO 4 /LAO-LLZOF/Li battery stably cycled for 5500 cycles at 3 C. This work reveals the chemistry of Li 2 CO 3 at the LLZO GBs during cycling, presents a novel lithium penetration mechanism within garnet electrolytes, and provides an innovative method to simultaneously regulate the ion and electron transport at the GBs in garnet electrodes for advanced ASLMBs.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yaru Li,Xiaoyan Liu,Jiwei Zhang,Haitao Yu,Jingwei Zhang
In order to more effectively alleviate the volume extension and shrinkage of the Si anode during Li intercalation/deintercalation processes, and also to improve the electron and ion transport dynamics, carbon coated Si-porous carbon composite fibres with a sandwich structure were prepared using a sacrificial template (ZIF-8) to construct mesoporous carbon, combined with electrospinning technology and subsequent hydrothermal carbon coating. The carbon fibre skeleton and carbon-coated sandwich structure provide support for the volume extension and shrinkage of Si, avoiding Si from directly contacting with the electrolyte, and forming a stable solid electrolyte interphase film. Furthermore, the polyvinylpyrrolidone spinning solution assists ZIF-8 to obtain a mesoporous structure inside the carbon fibre, which improves the specific surface area and pore volume of the composite material. In this case, the mesoporous structure also helps to alleviate the volume extension and shrinkage of Si during the charging /discharging processes and improves the transmission dynamics of lithium ions and electrons. Benefit from the unique structural features, this anode composite material exhibits enhanced electrochemical properties for Li-ion batteries, with a reversible specific capacity of 1114 mAh g −1 at 1 A g −1 , and demonstrates a capacity retention rate of 66% with a specific capacity of 740 mAh g −1 after 400 cycles.
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 15
·8424-8431
·
IF 14.511
Peng Du,Chenbo Yuan,Xiaoyu Cui,Kaifu Zhang,Yu Yu,Xiaodi Ren,Xiaowen Zhan,Shan Gao
The commercialization of Li metal anodes has been long hindered by uncontrolled dendrite growth, infinite volume expansion and poor Li metal utilization. Herein, we achieve a uniform nano-Pb decoration on carbon cloth (Pb@CC) by exploiting the thermal decomposition process of lead acetate trihydrate monitored by in situ Raman spectroscopy. 3D hosted Li anodes are fabricated via a record-fast infusion (1.0 s) of accurate weight-controlled molten Li into the highly lithiophilic Pb@CC host at a considerably low temperature of 250 °C. At an optimal Li loading of 10 mg, the Pb nanoparticles guide the uniform distribution of Li sites over the robust yet porous electron-conducting carbon network, which not only directs and confines Li nucleation and growth, but accommodates volume changes during repeated Li stripping/plating processes. The resulting Li electrodes afford an ultralong cycle life of 4648 h at low overpotentials of <50 mV under 1 mA cm−2/1 mA h cm−2 symmetric-cell cycling, which is among the best records ever reported in the literature. The corresponding LiFePO4 and LiNi0.8Co0.1Mn0.1O2 full cells deliver significantly higher cycling and rate performances than those with Li foils. Furthermore, the effect of Li utilization is explored in Li‖LiFePO4 full cells, with the best cyclability achieved at a low N/P ratio of 63.28. The present findings stretch the practical feasibility of wetting-assisted molten Li infusion in mitigating dendrite growth and improving Li utilization towards long-cycling high-energy-density Li metal batteries.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2022
·
IF 8.91
Liang Chen,Yafei Shen
Waste cathode (BC) from spent lithium-ion battery (LIB) was preliminarily studied for the catalytic pyrolysis of chitin biomass using thermogravimetric and pyrolysis-gas chromatography/mass spectrometry analysis. Compared with the dry-mixing method (BC1), the wet-impregnation method (BC2) significantly increased the decomposition rate of chitin pyrolysis and decreased the apparent activation energy from 85 kJ/mol to 76 kJ/mol. BC2 had a superior catalytic effect on the conversion of heavy components into light fractions. In particular, the selectivities for acetamides and acetonitrile were improved. Furthermore, BC2 enhanced the cleavage of glucosidic, C–O, and C–C bonds, thereby improving the thermolysis of chitin to acetamido acetaldehyde. The production of acetamides, acetonitriles, and other light components (e.g., ketones) was further enhanced via deoxygenation and hydrogenation reactions. Additionally, the selectivity of N-heterocycles (pyridine and pyrrole) and their derivatives (tar-N surrogates) decreased, indicating that tar was significantly reduced during the catalytic pyrolysis and gasification of chitin biomass.
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Materials Advances
·
2022
·Vol. 3
·期 8
·3631-3641
·
IF 0
Jia Luo,Huaiyu Li,Guo Yu,Wenyuan Xu,Hong Yin,Zhaohui Hou
Tin monosulfide (SnS) anodes have attracted much attention for lithium-ion batteries (LIBs) due to their excellent chemical stability, high theoretical specific capacity and outstanding reversibility. However, the slow kinetics and large volume expansion of intrinsic SnS electrodes in the conversion reaction process restrict their application to a certain extent. To address the poor conductivity and volume fluctuation, N-doped double-carbon-layer protective hierarchical structures decorating SnS nanotubes (N-DCSNs) are introduced by in situ polymerization directed using a g-C3N4 soft template. Particularly, N-doped double carbon layers provide fast transport channels for electrons and ions, affording decent conductivity and rapid ionic diffusion rate. Most importantly, the volume expansion of SnS during the charge–discharge cycles can be buffered owing to the confinement effect of the double carbon layer. Synergistic effects of N-DCSNs enhance the mechanical integrity and electrochemical kinetics during the charge–discharge process, leading to high-capacity retention and long-term stability properties. As a remarkable anode for LIBs, the N-DCSN electrode delivers high capacities of 911.5 and 511.3 mA h g−1 at 0.2 and 1.0 A g−1 after 270 and 1000 cycles, respectively. The feasible and versatile structure design can offer new ideas for the preparation and regulation of other transition metal sulfide anode materials, and provide a relevant experimental basis for the further development of lithium/sodium storage equipment.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Rupeng Zhang,Can Cui,Rang Xiao,L. Ruinan,Tiansheng Mu,Hua Huo,Yulin Ma,Geping Yin,Pengjian Zuo
The Mg-metal batteries (MMBs) as a forceful competitor for Li-metal batteries (LMBs) have the advantages of high-safety and high-volume energy density . Whereas, the MMBs still confronts two vital issues to be addressed, including the incompatibility of conventional TFSI-based electrolytes with the Mg electrode and the poor reversibility of the cathode. In this work, to satisfyingly settle the incompatibility, an artificial interphase was first pre-constructed by high-temperature displacement reaction of CuCl 2 and Mg metal, responsible for the faster charge-transfer rate and the lower Mg plating/stripping overpotential (∼0.2 V) in Mg symmetric cells. Regarding the Mg-Mo 6 S 8 full cells, to enhance the reversibility and rate performance, Mg/Li hybrid batteries were designed. Consequently, the Mg-Mo 6 S 8 battery can achieve excellent cycle stability and deliver a desirable capacity. Even as the current density increases to 1C, the battery still shows a desirable capacity of 92 mAh g −1 over 500 cycles.
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Nanotechnology Reviews
·
2022
·Vol. 11
·期 1
·824-833
·
IF 6.739
Yu Dou,Jianye Zhang,Xiaoyan Han,Qiming He,Yingkui Yang
An in situ Schiff-base condensation between p -phthalaldehyde (PPD) and 1,3,5-tris(4-aminophenyl)benzene (TAPB) or 1,3,5-tris(4-aminophenyl)triazine (TAPT) was actualized in the presence of carbon nanotubes (CNTs), producing imine-linked hyperbranched poly(PPD-TAPB) and poly(PPD-TAPT)-coated CNTs (abbreviated as CNT@HBP-1 and CNT@HBP-2, respectively). Such quasi-1D core–shell heterostructures are interleaved to build robust 3D networks with porous internal channels, which are favorable for efficient electron transport and ion diffusion, exposing active sites, fast redox kinetics, and high electrochemical utilization. When used as Li-ion anodes, both CNT@HBP-1 and CNT@HBP-2 exhibit larger specific capacity, better rate performance, and higher cycling stability compared to their pure polymers. Furthermore, CNT@HBP-2 delivers higher reversible capacities of 351 mA h g −1 at 0.05 A g −1 , and 81 mA h g −1 at 1.0 A g −1 , respectively, compared to CNT@HBP-1 (335 and 56 mA h g −1 ). Besides, CNT@HBP-2 retains 268 mA h g −1 over 100 cycles at 0.1 A g −1 , and 617 mA h g −1 in the 500th cycles at 0.5 A g −1 , respectively, outperforming CNT@HBP-1 (155 and 256 mA h g −1 ). Further improvements in the electrochemical performance for CNT@HBP-2 relative to CNT@HBP-1 are attributable to the incorporation of additional redox-active triazine units into HBP-2. This work would unlock insights into the rational development of metal-free polymer-based electrodes for rechargeable batteries.
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ChemElectroChem
·
2022
·Vol. 9
·期 9
·e202200301
·
IF 4.782
Shuang Xia,Wen Huang,Wenqi Yan,Xinhai Yuan,Xi Chen,Lili Liu,Lijun Fu,Yusong Zhu,Qinhong Huang,Yuping Wu,Teunis van Ree,Rudolf Holze
Graphical Separators for advanced Li−S batteries were prepared using spherical rutile TiO 2 with oxygen vacancies and three-dimensional interconnected graphene-like carbon. As an advanced energy-storage system, Li−S batteries have attracted much attention, but there is still a series of problems hindering their commercialization, such as the ‘shuttle effect’ and corrosion of lithium anodes. To alleviate these two important problems simultaneously, we modified the separators with spherical rutile TiO 2 with oxygen vacancies (abbreviated OT) and three-dimensional interconnected graphene-like carbon (abbreviated GC) for advanced Li−S batteries to improve the electrochemical performance. The modified separators (abbreviation OTCD) have low charge transfer impedance, a catalytic effect on polysulfides, and a barrier effect on polysulfides, which can suppress the ‘shuttle effect’ and prevents the corrosion of lithium anodes in Li−S batteries. The as-prepared Li−S batteries show good cycling stability for 250 cycles with 0.048 % capacity decay per cycle at 1 C. Moreover, the SEM images of lithium anodes after 50 cycles showed that the lithium anodes were uncorroded. This work provides a practical and effective reference for the advanced Li−S batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yun Zhao,Shuo Chen,Mengxin Guan,Bin Ding,Jianyong Yu,Jianhua Yan
The high reactivity of Li-anodes and the easily separated solid-state interface are two hurdles for constructing stable solid-state Li-metal batteries (SSLBs). Herein, we report a 3D mixed ion–electron conductive (MIEC) Li anode with deformable molten interphase of poly(Ɛ-caprolactone) electrolytes that is highly efficient towards constructing stable SSLBs. The 3D Li anode is fabricated by integrating a Li foil with a MIEC film via a facile hot-rolling process, in which the MIEC frame is composed of Li 0.33 La 0.56 TiO 3 particle attached carbon nanofibers . We propose that the chemical reactions between Li 0.33 La 0.56 TiO 3 and Li facilitates Li-nucleation inside the MIEC frame and thus enables fast stress relaxation and reduces volume fluctuations, while the molten interphase works as a binder to integrate the anodes and electrolytes without delamination during cycling. As a result, the symmetrical batteries run stably for 1200 h at 45 ℃, and the 3D Li/LiFePO 4 full batteries achieve a capacity of 134 mA h g −1 at 1C with a high-capacity retention of 98 % after 250 cycles, showing appealing commercial prospect.
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