JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Tianbiao Zeng,Lichen Zhang,Xingtong Wang,Yihong Ding,Huile Jin
The LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode is susceptible to degradation due to the presence of trace amounts of HF generated from H 2 O interacting with the electrolyte salt LiPF 6 . In this work, Al 2 O 3 -decorated carbon nanotubes was introduced as a conductive additive to safeguard the LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode, resulting in a significant enhancement of its reversible capacity and cycling stability. The electrode incorporated of Al 2 O 3 /CNTs delivered an initial discharge capacity of 184.1 mAh g −1 at 200 mA g −1 under 1.0 C, and retained 65.6 % of its capacity at 100th cycle, outperforming traditional electrodes. The synthesis of Al 2 O 3 /CNTs involves only two straightforward steps: precipitation and heat treatment. Additionally, the amount of this additive occupies a mere 2.0 wt% of the overall electrode material, making it suitable for large-scale applications.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Cheng Ouyang,Hongpeng Zheng,Qiwen Chen,Hezhou Liu,Huanan Duan
Solid-state lithium batteries hold great promise for next-generation energy storage systems. However, the formation of lithium filaments within the solid electrolyte remains a critical challenge. In this study, we investigate the crucial role of morphology in determining the resistance of garnet-type electrolytes to lithium filaments. By proposing a new test method, namely, cyclic linear sweep voltammetry, we can effectively evaluate the electrolyte resistance against lithium filaments. Our findings reveal a strong correlation between the microscopic morphology of the solid electrolyte and its resistance to lithium filaments. Samples with reduced pores and multiple grain boundaries demonstrate remarkable performance, achieving a critical current density of up to 3.2 mA cm–2 and excellent long-term cycling stability. Kelvin probe force microscopy and finite element method simulation results shed light on the impact of grain boundaries and electrolyte pores on lithium-ion transport and filament propagation. To inhibit lithium penetration, minimizing pores and achieving a uniform morphology with small grains and plenty of grain boundaries are essential.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 51
·2305815
·
IF 19
Huawen Peng,Yafei Su,Xufei Liu,Jiapeng Li,Qiang Zhao
High performance polyamide nanofiltration membranes play important roles in Mg 2+ /Li + separation and Li + extraction, but they are prepared via multiple time-/labor demanding steps. Both the scalability of these membranes and the engineering of membrane modules remain an elusive challenge. Here the design of a Gemini-electrolyte monomer (GEM) featuring bidentate amine groups, quaternary ammonia, and endocyclic contorted conformation is reported. The monomer's low interfacial diffusivity is balanced by high condensational reactivity during its interfacial polymerization with trimesoyl chloride (TMC), leading to the straightforward formation of defect-free, ≈14 nm thick membranes. The membrane shows the highest permeance (≈19.2 L m −2 h −1 bar −1 ) among Mg 2+ /Li + nanofiltration membranes prepared via straightforward interfacial polymerization without post-modification, combined with good Mg 2+ /Li + selectivity (≈15.4) and stability. The validity of GEM design is verified by control monomers. Large-area (1 × 2 m 2 ) GEM-TMC membranes and spiral-wound modules (effective area: 0.5 m 2 ) are prepared, both of which show reproducible and high performance.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2023
·Vol. 39
·期 4
·636-641
·
IF 3.1
Fu Zerui,Wang Shu,Yu Haohan,Nie Meilin,Feng Xilan,Zuo Xintao,Fu Lichao,Liu Dapeng,Zhang Yu
Li-O 2 battery(LOB) has an ultrahigh specific capacity(3500 W·h/kg), however, its slow kinetics of oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) at cathode often leads to a high overpotential, a limited discharge capacity, and a poor cycling performance. Therefore, it is important to design and prepare cathode materials with a excellent catalytic activity. In this study, CeO 2 nanoparticles(NPs) supported on reduced graphene oxide(rGO) have been prepared and employed as cathode. Compared with either CeO 2 NPs or rGO, CeO 2 /rGO cathode greatly improves the discharge capacity(10644 mA·h/g at a current density of 100 mA/g) and the cycling performance(95 cycles at 200 mA/g with a limited capacity of 500 mA·h/g) by virtue of the good conductivity of rGO and the oxygen storage/release capability of CeO 2 .
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ADVANCED MATERIALS
·
2023
·Vol. 35
·期 33
·2302325
·
IF 29.4
Chang Guo,Fuli Zhang,Xiao Han,Lipeng Zhang,Qian Hou,Lele Gong,Jincheng Wang,Zhenhai Xia,Jianhua Hao,Keyu Xie
To date, the effect of noble metal (NM) electronic structures on CO 2 reaction activity remains unknown, and explicit screening criteria are still lacking for designing highly efficient catalysts in CO 2 -breathing batteries. Herein, by preferentially considering the decomposition of key intermediate Li 2 CO 3 , an intrinsic descriptor constituted of the d x 2 − y 2 ${{\rm{d}}}_{{x}^2 - {y}^2}$ orbital states and the electronegativity for predicting high-performance cathode material are discovered. As a demonstration, a series of graphene-supported noble metals (NM@G) as cathodes are fabricated via a fast laser scribing technique. Consistent with the preliminary prediction, Pd@G exhibits an ultralow overpotential (0.41 V), along with superior cycling performance up to 1400 h. Moreover, the overall thermodynamic reaction pathways on NM@G confirm the reliability of the established intrinsic descriptor. This basic finding of the relationship between the electronic properties of noble metal cathodes and the performance of Li-CO 2 batteries provides a novel avenue for designing remarkably efficient cathode materials for metal-CO 2 batteries.
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Nano Research
·
2023
·Vol. 16
·期 7
·9344-9351
·
IF 9.9
Zeng Zhichao,Shi Xiaomeng,Sun Mingzi,Zhang Hongtu,Luo Wei,Huang Yunhui,Huang Bolong,Du Yaping,Yan Chun-Hua
Rare-earth (RE) halide solid electrolytes (HSEs) have been an emerging research area due to their good electrochemical and mechanical properties for all-solid-state lithium batteries (ASSBs). However, only very limited types of HSEs have been reported with high performance. In this work, tens of grams of RE-HSE Li 3 TbBr 6 (LTbB) was synthesized by a vacuum evaporation-assisted method. The as-prepared LTbB displays a high ionic conductivity of 1.7 mS·cm −1 , a wide electrochemical window, and good formability. Accordingly, the assembled solid lithium-tellurium (Li-Te) battery based on the LTbB HSE exhibits excellent cycling stability up to 600 cycles, which is superior to most previous reports. The processes and the chemicals during the discharge/charge of Li-Te batteries have been studied by various in situ and ex situ characterizations. Theoretical calculations have demonstrated the dominant conductivity contributions of the direct [octahedral]-[octahedral] ([Oct]–[Oct]) pathway for Li ion migrations in the electrolyte. The Tb sites guarantee efficient electron transfer while the Li 2s orbitals are not affected during migration, leading to a low activation barrier. Therefore, this successful fabrication and application of LTbB have offered a highly competitive solution for solid electrolytes in ASSBs, indicating the great potential of RE-based HSEs in energy devices.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 19
·10425-10434
·
IF 11.9
Ke Yang,Chan Li,Haoyuan Qi,Yunfei Dai,Yuhong Cui,Yibo He
The shuttle effect of polysulfides seriously hinders the practical application of lithium–sulfur (Li–S) batteries, and separator modification is supposed to be an effective way to solve this issue. Herein, MXene quantum dots (MQDs) were self-assembled on the surface of g-C3N4 sheets (g-C3N4@MQDs) by electrostatic adsorption principles to construct a functional layer on a Celgard separator. Making MXene into quantum dots was conducive to solving the agglomeration issue of its sheets, providing more active sites to capture the dissolved polysulfides. Moreover, the MQDs could also work as an electrocatalyst to further facilitate the Li2S catalytic conversion, obtaining a high deposition current and capacity (257.4 mA h g−1). Attributed to the regulation effect of MQDs toward the kinetic behavior of polysulfides, the shuttle effect was effectively mitigated. An as-fabricated Li–S battery with a heterostructured g-C3N4@MQD-based separator achieved a high specific capacity of 1433 mA h g−1 at 0.1 C, excellent rate performance (532 mA h g−1 at 4 C), and good cycling performance (0.024% capacity fading per cycle after 1000 cycles at 2 C). The rational design of the g-C3N4@MQD-based separator not only broadens the application of MQDs, but also presents new insights to develop high-performance Li–S batteries.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Qiang Lv,Yajie Song,Bo Wang,Shangjie Wang,Bochen Wu,Yutong Jing,Huaizheng Ren,Shengbo Yang,Lei Wang,Lihui Xiao,Dianlong Wang,Huakun Liu,Shixue Dou
Solid polymer electrolytes (SPEs) are one of the most promising alternatives to flammable liquid electrolytes for building safe Li metal batteries. Nevertheless, the poor ionic conductivity at room temperature (RT) and low resistance to Li dendrites seriously hinder the commercialization of SPEs. Herein, we design a bifunctional flame retardant SPE by combining hydroxyapatite (HAP) nanomaterials with N-methyl pyrrolidone (NMP) in the PVDF-HFP matrix. The addition of HAP generates a hydrogen bond network with the PVDF-HFP matrix and cooperates with NMP to facilitate the dissociation of LiTFSI in the PVDF-HFP matrix. Consequently, the prepared SPE demonstrates superior ionic conductivity at RT, excellent fireproof properties, and strong resistance to Li dendrites. The assembled Li symmetric cell with prepared SPE exhibits a stable cycling performance of over 1200 h at 0.2 mA cm −2 , and the solid-state LiFePO 4 ||Li cell shows excellent capacity retention of 85.3% over 600 cycles at 0.5 C.
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DESALINATION
·
2023
·
IF 9.9
Tingyu Li,Xinzhu Zhang,Yu Zhang,Jixiao Wang,Zhi Wang,Song Zhao
Selective lithium recovery from salt lake brine using emerging nanofiltration membranes is expected to solve the insufficient supply of lithium resources. In this work, 1,4,7,10-tetraazacyclododecane (Cyclen) was employed as a novel structural regulator through interfacial polymerization of polyethyleneimine (PEI) and trimesoyl chloride (TMC) to develop polyamide NF membrane with efficient Li + /Mg 2+ separation performance. After the introduction of Cyclen to aqueous phase , the PEI/Cyclen-TMC selective layer was confirmed to possess a higher crosslinking degree and larger d-spacing than PEI-TMC layer, endowing a dedicated channel for Li + transport. The water permeance of PEI/Cyclen-TMC composite membrane reached 14.0 L·m −2 ·h −1 ·bar −1 , about 3.8 times higher than PEI-TMC composite membrane, and meanwhile the separation factor ( S Li,Mg ) could be stabilized as 8.7 to realize a considerable reduction of Mg 2+ /Li + mass ratio from 20 to 2.3. Additionally, PEI/Cyclen-TMC composite membrane was utilized to operate a three-stage nanofiltration treatment procedure of a simulated salt lake brine (Mg 2+ /Li + mass ratio: 40). The results indicated that Li + could be efficiently retracted to obtain a solution with 19.5 mg·L −1 Li + and Mg 2+ /Li + mass ratio of 0.3. After the subsequent precipitation and filtration, the obtained Li 2 CO 3 purity could reach 93 %, indicating the potential application of nanofiltration for lithium recovery.
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JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Mengyuan Song,Changhao Tian,Chunguang Chen,Tao Huang,Aishui Yu
Lithium-oxygen batteries show great energy storage potential due to their high energy density . However, it is difficult for conventional liquid electrolytes to form a stable solid electrolyte interface (SEI) on cathode surface to ensure long-term stable cycling of lithium-oxygen batteries . Herein, LiBOB is added to the LiTFSI-based electrolyte to solve the above-mentioned problems. By introducing LiBOB into LiTFSI single-salt electrolyte system, the electron delocalization of the BOB − anion induces the dissociation equilibrium of the lithium salt to occur positively and the formed electrolyte exhibits good ionic conductivity . Different amounts of LiBOB show different characteristics in electrochemical performance. Trace amounts of LiBOB as an additive increase the solvation of Li + and improve the discharge capacity of the cell. Furthermore, the synergistic effect of the LiTFSI-LiBOB dual-salt electrolyte forms a protective SEI when LiBOB has a larger proportion of lithium salts in the electrolyte, resulting in comparable cycling performance. This work demonstrates a promising approach to design electrolytes for long-term stable cycling of lithium-oxygen batteries.
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Journal of Materials Research and Technology-JMR&T
·
2022
·
IF 6.267
Yun Zhang,Xiaoning Li,Shihua Ding,Tianxiu Song,Zezhen Yin,Jiaying Dan
Ba 1- x Li x Si 2 O 5- x /2 ( x = 0–0.5) ceramics were prepared by solid-state reaction method. The occupation tendency of Li + was well explained based on First-principle calculation and unit cell volume changes. Li + non-equivalent substitution for Ba 2+ considerably reduced the sintering temperature to 975 °C, in comparison with 1225 °C for pure BaSi 2 O 5 . Single phase solid solution with orthorhombic structure was observed with x = 0–0.1. Nevertheless, trace amounts of unexpected secondary phases Li 2 Si 2 O 5 and SiO 2 were detected for higher Li-containing samples. Notably, the Q×f significantly enhanced up to 58.16% from 16,134 GHz ( x = 0) to 25,518 GHz ( x = 0.01), which predominantly depended on the structural characteristics, such as packing fraction and bond covalence. Increase x from 0 to 0.5 led to the reduction of dielectric constant ε r from 7.11 to 5.95. The resonant frequency temperature coefficient τ f was directly dominated by oxygen bond valence ( V O ), rather than V Ba and V Si . Ba 0.99 Li 0.01 Si 2 O 4.995 ceramic sintered at 1050 °C for 4 h exhibited a high Q×f value of 25,518 GHz, and the ε r and τ f values were 6.94 and −29.46 ppm/°C, respectively.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Qiankui Zhang,Kang Wang,Xianshu Wang,Yaotang Zhong,Mingzhu Liu,Xiang Liu,Kang Xu,Weizhen Fan,Le Yu,Weishan Li
Li metal provides an ideal anode for the highest energy density batteries, but its reactivity with electrolytes brings poor cycling stability. Electrolyte additives have been employed to effectively improve the cycling stability, often with the underlying mechanism poorly understood. In this work, applying lithium bis(oxalate)borate (LiBOB) as a chemical source for a dense and protective interphase, we investigate this issue with combined techniques of electrochemical/physical characterizations and theoretical calculations. It was revealed that the solid electrolyte interphase (SEI) formed by Li and the carbonate electrolyte is unstable and responsible for the fast deterioration of the Li anode. When LiBOB is present in the electrolyte, a reinforced SEI was formed, enabling significant improvement in cycling stability due to the preferential reduction of the BOB anion over the carbonate molecules and the strong combination of its reduction products with the species from the electrolyte reduction. The effectiveness of such new SEI chemistry on the Li anode supports excellent performance of a Li/LiFePO4 cell. This approach provides a pathway to rationally design an interphase on the Li anode so that high energy density batteries could be realized.
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