JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Junfang Cheng,Ziling Wang,Lu Zou,Ming Zhang,Guozhu Zhang,Yabin Dong,Yuexing Jiang,Yizhen Huang,Naotoshi Nakashima,Bo Chi
Perovskite oxides with low cost and high catalytic activity are reported as suitable cathode catalysts for the Li–O 2 batteries (LOBs), while their catalytic mechanism is not yet fully clarified. Herein, La 0.8 Sr 0.2 Co 0.8 Ni 0.2 O 3-δ (LSCN8282) perovskite oxide is used as a cathode catalyst for the LOBs and further improved by adjusting the Co/Ni ratio in the B-site. Thus, La 0.8 Sr 0.2 Co 0.6 Ni 0.4 O 3-δ (LSCN8264) and La 0.8 Sr 0.2 Co 0.4 Ni 0.6 O 3-δ (LSCN8246) are also synthesized and used as cathode catalysts for the LOBs. Among the obtained perovskite catalysts in this study, LSCN8264 shows the highest electrochemical activity in 1 M KOH and best catalytic effectivity when used in the LOBs. The catalytic mechanism and doping optimization are clarified by analyzing the morphology of the discharge products and the X-ray photoelectron spectroscopy (XPS) of the perovskite oxides.
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GREEN CHEMISTRY
·
2020
·Vol. 22
·期 14
·4473-4482
·
IF 9.48
Shubin Wang,Zuotai Zhang,Zhouguang Lu,Zhenghe Xu
Deep eutectic solvents (DESs), as a green alternative technology, exhibit great potential to recycle valuable elements from spent lithium-ion batteries (LIBs). However, due to the weak reducing power of DESs, raising the temperature and extending the duration of processing are not efficient for screening suitable DESs for the recycling of LIBs. Here, we propose a novel, simple and robust experimental method to identify suitable DESs for recycling spent LIBs. Based on electrochemical principles, the method proposed in this study can be used to quickly determine the reducing power of DESs. As an example, a choline chloride (ChCl) and urea mixture as a DES was found to possess strong reducing power, with a Li and Co extraction efficiency of 95% from spent LIBs obtained at a reduced reaction temperature of 180 °C and reaction time of 12 h. The results are in good agreement with the results from Fukui functions calculations. The kinetic experiments revealed that the Li and Co extraction is controlled by solution and electron diffusion through the DES. Furthermore, a cubic cobalt oxide spinel (Co3O4) was obtained from the loaded DES using H2C2O4 and NaOH in the dilution–precipitation–calcination process. The current strategy demonstrates great potential for rapid and reliable screening of suitable DESs for the effective recycling of spent LIBs.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jiaming Xu,Chao Ma,Chengyue Chang,Xiaofeng Lei,Yinwei Fu,Jian Wang,Xizheng Liu,Yi Ding
Hybrid solid/gel electrolytes (SGEs) have generated much research attentions because of their capability to suppress Li dendrite growth and improve battery safety. However, the interfacial compatibility of the electrode/electrolyte or polymer/inorganic ceramics within hybrid electrolytes remains challenging for practical applications. Herein, an SGE is fabricated by confining ceramic particles (Li7La3Zr2O12; LLZO) into in situ formed tetraethylene glycol dimethyl ether (G4)-based gel electrolytes within assembled cells. A hierarchical layered structure is formed when LLZO settles near the Li anode within the liquid electrolyte during the gradual gelatinization process. Good interfacial compatibility is obtained from good contact with the liquid G4 component. The LLZO layer also serves as an ionic sieve to redistribute the Li deposition. This SGE endows stable Li stripping/plating cycling over 800 h at 0.5 mA/cm2 (60 °C). Moreover, Li-metal batteries with an SGE coupled with LiFePO4 and an air cathode both exhibit superior cycling performance. This work presents a promising strategy for hierarchically layered SGEs for high-performance Li-metal batteries.
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高影响因子
Energy Storage Materials
·
2021
·
IF 17.789
Xiaowei Mu,Chao Xia,Bin Gao,Shuyi Guo,Xueping Zhang,Jianping He,Yonggang Wang,Hao Dong,Ping He,Haoshen Zhou
Rechargeable Li-O 2 batteries have captured increasing attention owing to their ultra-high theoretical specific energy. However, this promising system is confronted with the large overpotential, limited discharge capacity and low cyclic life. Herein, three two-dimensional (2D) molybdenum-based compounds of MoN, MoO 3 and MoS 2 are used as cathode catalysts in Li-O 2 batteries . The catalytic performance and electronic structures of these catalysts are compared comprehensively. Electrochemical test results reveal the superior battery performance of MoN cathodes, which deliver the highest specific discharge capacity of approximately 7400 mAh g − 1 and the lowest discharge/charge overpotential of 0.19/0.72 V. Density functional theory (DFT) calculations demonstrate the metallic property of MoN whereas MoO 3 and MoS 2 are poor conductive. Besides, interface properties between MoN and Li 2 O 2 products as well as reaction pathways of the Li-O 2 battery with MoN cathode are also investigated detailedly by DFT calculations, explaining the excellent catalytic properties of MoN at the atomic level. The present work provides intrinsic insights into designing high-performance cathode catalysts for Li-O 2 batteries with fine-tuned morphology and electronic characteristics.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 9
·090545
·
IF 4.316
Jia Wen,Zhenying Chen,Sheng Han,Jinhui Zhu,Changchun Ke,Emmanuel Kymakis,Xiaodong Zhuang
Poly(ethylene oxide) (PEO) is regarded as an attractive solid-state electrolyte in lithium-ion batteries (LIBs). However, relatively low ionic conductivity of pristine PEO is a critical bottleneck to boost high-performance solid-state LIBs. Herein, poly(2-aminoazulene) (PAAz) was synthesized using the oxidation polymerization strategy and acted as a polymeric filler in the fabrication of PEO−PAAz composite electrolyte. Compared with PEO electrolyte, the composite electrolyte had a better ionic conductivity (9.27 × 10−6 vs 6.47 × 10−5 S cm−1 at 30 °C), Li+ transference number (0.21 vs 0.51), and suppression of Li dendrites. Consequently, the PEO−PAAz electrolyte paired Li/LiFePO4 cell had a high capacity (156 mAh g−1 at 0.5 C, 1 C = 170 mA g−1) and stability (only 8% capacity loss after 300 cycles); these are better than those of the PEO-based cell (132 mAh g−1, 45% capacity loss). In addition, the PEO−PAAz-based cell could run for 1200 cycles with 60% capacity retention at 1 C. This study provides both a new organic filler for PEO-based solid-state LIBs and a method of improving the performance of solid-state LIBs, especially in terms of a long lifetime.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Peng Hei,Chaozhu Shu,Zhiqian Hou,Ruixin Zheng,Tingshuai Yang,Minglu Li,Zhiqun Ran,Yue Wang,Dexin Mei,Jianping Long
In this work, we fabricated a novel free-standing Fe doped CoP nanowire on carbon cloth (Fe–CoP/CC) electrode with high catalytic activity for Li–O 2 batteries. It is unexpected that the Li–O 2 battery with Fe–CoP/CC electrode demonstrated a low potential of 0.8 V and exceptional cycle stability of more than 500 cycles with no significant voltage attenuation compared with previously reported counterparts. Such excellent performance can be partly attributed to its fine nanowire structure and its large specific surface area (419.14 m 2 g −1 ). Furthermore, iron doping plays a crucial role in improvement of battery performance because the doped Fe can modulate the internal electronic structure and optimize the absorption of intermediate products, which have been proved to be the determinant for optimizing the catalytic activity. Thus, it is believed that heterogeneous element doping in binary or ternary metal compounds is a promising strategy to fabricate high performance oxygen electrode materials for Li–O 2 batteries in the next few years.
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Advanced Energy Materials
·
2019
·Vol. 9
·期 14
·1803935
·
IF 24.884
Yanyan Liu,Miaomiao Han,Qizhong Xiong,Shengbo Zhang,Cuijiao Zhao,Wanbing Gong,Guozhong Wang,Haimin Zhang,Huijun Zhao
The Haber-Bosch process can be replaced by the ambient electrocatalytic N 2 reduction reaction (NRR) to produce NH 3 if suitable electrocatalysts can be developed. However, to develop high performance N 2 fixation electrocatalysts, a key issue to be resolved is to achieve efficient hydrogenation of N 2 without interference by the thermodynamically favored hydrogen evolution reaction (HER). Herein, in-operando created strong Li–S interactions are reported to empower the S-rich MoS 2 nanosheets with superior NRR catalytic activity and HER suppression ability. The Li + interactions with S-edge sites of MoS 2 can effectively suppress hydrogen evolution reaction by reducing H* adsorption free energy from 0.03 to 0.47 eV, facilitate N 2 adsorption by increasing N 2 adsorption free energy from –0.32 to –0.70 eV and enhance electrocatalytic N 2 reduction activity by decreasing the activation energy barrier of the reaction control step (*N 2 → *N 2 H) from 0.84 to 0.42 eV. A NH 3 yield rate of 43.4 μg h −1 mg −1 MoS 2 with a faradaic efficiency (FE) of 9.81% can be achieved in presence of strong Li–S interactions, more than 8 and 18 times by the same electrocatalyst in the absence of Li–S interactions. This report opens a new way to design and develop catalysts and catalysis systems.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Yang Hai,Wei Cui,Yemao Lin,Pei Han,Huaican Chen,Zhiyong Zhu,Cuihua Li,Bo Yang,Caizhen Zhu,Jian Xu
Nowadays, graphite is still the commercial anode material for Li-ion batteries although many kinds of anode materials have been reported. A great deal of efforts has been devoting to improving the specific gravimetric capacity of graphite by doping or preparing hierarchical structure. However, the volumetric capacity of graphite is not taken seriously compared to the specific gravimetric capacity. In this paper, a surface modification method, ion implantation , has been put forward to improve the volumetric capacity of graphite with high coulombic efficiency. After modification with 50 keV N + ions at 1 × 10 12 ions/cm 2 , the volumetric capacity of implanted graphite increases 29.6% (696 mAh/cm 3 ) compared to that of pure graphite electrode (537 mAh/cm 3 ) with a super-high initial coulombic efficiency of ~95.9%. Moreover, the influence of nitrogen doping and vacancies induced by N + ions implantation on the improving of volumetric capacity is discussed. The implanted effects of graphite are also observed by HRTEM , GIXRD , Raman and XPS .
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 10
·5712-5718
·
IF 10.733
Ying Zhou,Kai Zhao,Yu Han,Zhenhe Sun,Hongtao Zhang,Lingqun Xu,Yanfeng Ma,Yongsheng Chen
The two most challenging issues for Li metal anodes are large volume change during the plating/stripping process and the growth of Li dendrites induced by uneven Li deposition. They lead to low coulombic efficiency, short cycling lifespan and serious safety issues of Li metal batteries. Here we developed a facile strategy to prepare a nitrogen-doped-carbon/ZnO (NDC/ZnO) modified Cu foam (MCuF) current collector for Li metal anodes. The MCuF shows stable Li plating/stripping behavior with the Li dendrite-mitigation feature. The resultant half cells achieve a super long lifespan of over 600 cycles at 1 mA cm−2 and over 200 cycles at a high current density 10 mA cm−2. Moreover, the full cell paired with LiFePO4 also exhibits a long lifespan of over 150 cycles at a high rate of 5C. Such high performance can be attributed to the characteristics of MCuF, including its 3D porous structure with high conductivity, enlarged surface area and uniform lithophilic NDC/ZnO sites. We believed that our work can provide a facile strategy for fabricating high-performance 3D current collectors for Li metal storage and stable Li metal batteries.
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ACS Nano
·
2019
·
IF 13.903
Wei Kou,Xiangcun Li,Yang Liu,Xiaopeng Zhang,Shaoran Yang,Xiaobin Jiang,Gaohong He,Yan Dai,Wenji Zheng,Guihua Yu
Here we report a highly scalable yet flexible triple-layer structured porous C/SiO2 membrane via a facile phase inversion method for advancing Li–sulfur battery technology. As a multifunctional current-collector-free cathode, the conductive dense layer of the C/SiO2 membrane offers hierarchical macropores as an ideal sulfur host to alleviate the volume expansion of sulfur species and facilitate ion/electrolyte transport for fast kinetics, as well as spongelike pores to enable high sulfur loading. The triple-layer structured membrane cathode enables the filling of most sulfur species in the macropores and additional loading of a thin sulfur slurry on the membrane surface, which facilitates ion/electrolyte transport with faster kinetics than the conventional S/C slurry-based cathode. Furthermore, density functional theory simulations and visual adsorption measurements confirm the critical role of the doped SiO2 nanoparticles (∼10 nm) in the asymmetric C membrane in suppressing the shuttle effect of polysulfides via chemisorption and electrocatalysis. The rationally designed C/SiO2 membrane cathodes demonstrate long-term cycling stability of 300 cycles at a high sulfur loading of 2.8 mg cm–2 with a sulfur content of ∼75%. This scalable yet flexible self-supporting cathode design presents a useful strategy for realizing practical applications of high-performance Li–S batteries.
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高影响因子
Nanoscale
·
2019
·Vol. 11
·期 24
·11513-11520
·
IF 6.97
Huan-Feng Wang,Jun-Feng Li,Xue-Xi Sun,Ji-Jing Xu
The design of a nanoporous cathode for Li–O2 batteries that can achieve high chemical stability and superior electrochemical performance remains a formidable challenge. A novel approach for the fabrication of nanoengineered PdNi alloys directly coated onto Ni nonwoven fabric (PdNi/NiNF) obtained through electrospinning has been proposed. On the basis of the contributions of the porous structure, the prepared metal-based cathodes can exhibit high chemical and mechanical stabilities, high catalytic activity, and high conductivity. In this design, the major side reactions were excluded when compared with popularly used carbon cathodes, and excellent cycling stability (266 cycles) could be achieved. The proposed cathode exhibited a high discharge capacity of 15 700 mA h g−1 at 500 mA g−1, which was 5 times higher than those reported for carbon-free cathodes.
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ChemSusChem
·
2018
·Vol. 11
·期 21
·3774-3782
·
IF 7.411
Zhaoshuai Zhang,Long Zhang,Yanyan Liu,Hongqiang Wang,Chuang Yu,Hong Zeng,Li-min Wang,Bo Xu
Graphical The interfacial performance of cubic Li 7 La 3 Zr 2 O 12 (LLZO) as a solid electrolyte for Li-ion batteries is improved by incorporating 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl) imide (BMP-TFSI) ionic liquid. LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)/Li and LiFePO 4 /Li batteries with the hybrid solid electrolyte exhibit superior cycling stability and low polarization. High grain-boundary resistance, Li-dendrite formation, and electrode/Li interfacial resistance are three major issues facing garnet-based solid electrolytes. Herein, interfacial architecture engineering by incorporating 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl) imide (BMP-TFSI) ionic liquid into a garnet oxide is proposed. The “soft” continuous BMP-TFSI coating with no added Li salt generates a conducting network facilitating Li + transport and thus changes the ion conduction mode from point contacts to face contacts. The compacted microstructure suppresses Li-dendrite growth and shows good interfacial compatibility and interfacial wettability toward Li metal. Along with a broad electrochemical window larger than 5.5 V and an Li + transference number that practically reaches unity, LiNi 0.8 Co 0.1 Mn 0.1 O 2 /Li and LiFePO 4 /Li solid-state batteries with the hybrid solid electrolyte exhibit superior cycling stability and low polarization, comparable to those with commercial liquid electrolytes, and excellent rate capability that is better than those of Li-salt-based ionic-liquid electrolytes.
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