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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Preparation of silicon oxycarbide (SiOC) anodes for high performance Li-ion batteries using competitive relationship between crosslinking and polymerization

Pengfei Wu,Xiaoxin Guo,Zhiming Su,Chao Liu,Shaohong Chen,Zhicheng Zheng,Anhua Liu

SiOC anode is considered as a candidate for the next generation of lithium ion batteries, because of its appealing specific capacity and relative small volume expansion. However, the inherent inferior electron conductivity blocks its development. Recently, controlling the amount of free carbon domains is adopted to modify the performance, ignoring the influence of free C on the SiOC phases change and their synergistic effect on the performance. The crosslinking and polymerization competition between divinylbenzene and polymethylsilsesquioxane was coordinated to regulate the free carbon and phase composition of SiOC ceramics, and a durable SiOC anode with high ceramic yield was prepared. The result is that, keeping the proportion of free C about 10% and increasing the SiO 3 C and SiO 2 C 2 phases ratios can obtain good anode within limited cycle life (440 cycle in this work), and increasing free C amount further is necessary for durable long cycle life. Herein, S-DVB-2 anode with 12% free C delivers 698.7 mAh g −1 at a current density of 100 mA g −1 after 100 cycles, and S-DVB-1 anode with 20.6% free C shows excellent stable long cycle performance at the current density of 0.5 A g −1 , the remaining capacity is 476 mAh g −1 after 500 cycles.

CAS / MDL: 78-67-1 1321-74-0
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Interlayer-expanded VS2 nanosheet: Fast ion transport, dynamic mechanism and application in Zn2+ and Mg2+/Li+ hybrid batteries systems

Jing Xu,Yinbing Liu,Peilong Chen,Ao Wang,Ke-jing Huang,Linxia Fang,Xu Wu

Currently, the development of polyvalent ions battery systems are still restricted by lacking suitable cathode materials with high energy density and long cycle life attributing to sluggish kinetic mechanism and of polyvalent ions. Herein, an effective inter-layer scaling strategy is proposed by using a simple hydrothermal method . The super layer spacing VS 2 (∼1 nm) cathode dramatically improves electrochemical performance of zinc-ion batteries (ZIBs) and magnesium/lithium hybrid ion batteries (MLIBs). The specific discharge capacities of ZIBs and MLIBs are 450.7 and 488.8 mA h g −1 at current density of 0.1 A g −1 which are much higher than the same type of battery systems. Finally, the diffusion mechanism and the corresponding theoretical model is established by adopting first principles . In brief, the work provides an effective strategy for the large scale application of multivalent and hybrid batteries systems.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Porous structure engineering of N-doped carbons for enhanced mass transfer towards High-Performance supercapacitors and Li-Ion batteries

Xueying Fan,Wen Zhang,Yongsheng Xu,Jie Zheng,Yang Li,Xiaobin Fan,Fengbao Zhang,Junyi Ji,Wenchao Peng

Tailoring the porous structure of carbon materials is one essential approach to improve the energy storage performance of carbon-based electrode materials . Herein, hierarchical porous carbons (HPCs) with different meso -structure are synthesized via a one-pot pyrolysis process with SiO 2 and ZnCl 2 as template and activator, respectively. The energy storage capacities of the obtained HPC samples are investigated as bi-functional electrode both for supercapacitor and LIBs . The results show that different meso -structure of HPCs can effectively affect the energy storage performance. In the range of 15 ∼ 50 nm, smaller size of mesopore can result better electrochemical performance of HPCs. And the optimized HPC sample (HPC-15) manifests high specific capacitance of 432F g −1 and good cyclic stability in the supercapacitor application. When used as anode of LIBs, the HPC-15 presents a high capacity of 820 mAh g −1 . In addition, COMSOL simulation is employed to study the effect of pore structure on mass transfer during electrochemical process. The HPC-15 is calculated to have the highest total porosity (ε p ) and effective diffusivity of K + (D e  = 6.776 × 10 -10 m 2 s −1 ), thus leading to its best electrochemical performance.

CAS / MDL: 9002-84-0
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RARE METALS · 2021 ·Vol. 41 ·期 4 ·1265-1275 · IF 4.003

High-entropy chemistry stabilizing spinel oxide (CoNiZnXMnLi)3O4 (X = Fe, Cr) for high-performance anode of Li-ion batteries

Tian Kang-Hui,Duan Chan-Qin,Ma Qun,Li Xing-Long,Wang Zhi-Yuan,Sun Hong-Yu,Luo Shao-Hua,Wang Dan,Liu Yan-Guo

High entropy oxides (HEOs), as a new type of single-phase multielement solid solution materials, have shown many attractive features and promising application prospect in the energy storage field. Herein, six-element HEOs (CoNiZnFeMnLi) 3 O 4 and (CoNiZnCrMnLi) 3 O 4 with spinel structure are successfully prepared by conventional solid-phase method and present outstanding lithium storage performances due to the synergy effect of various electrochemically active elements and the entropy stabilization. By contrast, (CoNiZnFeMnLi) 3 O 4 delivers higher initial discharge specific capacity of 1104.3 mAh·g −1 , better cycle stability (84% capacity retention after 100 cycles at 100 mA·g −1 ) and rate performance (293 mAh·g −1 at 2000 mA·g −1 ) in the half-cell. Moreover, the full-cell assembled with (CoNiZnFeMnLi) 3 O 4 and LiCoO 2 provides a reversible specific capacity of 260.2 mAh·g −1 after 100 cycles at 500 mA·g −1 . Ex situ X-ray diffraction reveals the electrochemical reaction mechanism of HEOs (CoNiZnFeMnLi) 3 O 4 , and the amorphous phase and the large amount of oxygen vacancies were obtained after the initial discharge process, which are responsible for the excellent cycle and rate performance. This research puts forward fresh insights for the development of advanced energy storage materials for high-performance batteries. Graphical Abstract

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CARBON · 2021 · IF 9.594

Bioderived carbon fiber conductive networks with inlaid electrocatalysts as an ultralight freestanding interlayer for working Li–SeS2 pouch cells

Yin Zhang,Boya Wang,Peng Jing,Yi Guo,Yueying Zhang,Yunhong Wei,Qian Wang,Yun Zhang,Hao Wu

Introducing a freestanding functional interlayer has been a conventional tactic to immobilize the soluble polysulfide intermediate in Li–S batteries . However, most of the designed interlayers possess extra heavy weight, casting additional technical challenges toward practical high-specific-energy batteries. Herein, an ultralight self-standing interlayer with an extremely low mass loading (∼0.14 mg cm −2 ), composed of porous curly carbon fibers derived from natural biomass with inlaid cobalt electrocatalysts (CF–Co), was engineered via a convenient way. After replacing the poor conductivity sulfur (∼10 −28  S m −1 ) by higher conductivity selenium disulfide (SeS 2 , ∼10 −6  S m −1 ) as active cathode materials , the hierarchically porous-structured, conductive CF-Co interlayer with outstanding adsorptive and electrocatalytic effects is introduced into the resulted Li–SeS 2 batteries to capture dual-intermediate polysulfides/polyselenides, boost their conversion kinetics, and ensure favorable running of Li–SeS 2 cells with high SeS 2 loading and lean electrolyte. Consequently, the coin cells deliver outstanding high-rate capability (404 mAh g −1  at 8 A g −1 ) and superior cycling stability (∼81.5% areal capacity retention in 125 cycles) under high SeS 2 loading (5.0 mg cm −2 ). Significantly, practical high-areal-capacity (>5.5 mAh cm −2 ) Li–SeS 2 pouch cells can be realized by assembling this interlayer with double-side SeS 2 -loading cathodes (132 mg), working stably at relatively lower electrolyte condition (6.0 μL mg −1 ).

CAS / MDL: 7791-13-1
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JOURNAL OF POWER SOURCES · 2023 · IF 9.2

Effects of strontium oxide on synthesis and performance of monocrystalline ultrahigh-Ni layered cathode materials for Li-ion batteries

Tingmin Lai,Ao Sheng,Zifang Zhang,Wei Li,Jianwen Yang,Shengkui Zhong,Yanwei Li,Yi Pei,Bin Huang

Monocrystalline layered cathode is of particular interest owing to the satisfactory mechanical integrity against long-term cycling. However, the high-temperature calcination , which is perceived as the indispensable reaction condition, favors the formation of Ni 2+ that triggers the Li + /Ni 2+ disorder and the formation of electrochemically inactive NiO. Herein, we develop a SrO-assistant method to synthesize a monocrystalline ultrahigh-Ni LiNi 0.95 Co 0.04 Mn 0.01 O 2 under a moderate calcination temperature. The addition of an appropriate amount of SrO (0.3 wt%, SCN95–Sr-3) facilitates the formation of monocrystalline LiNi 0.95 Co 0.04 Mn 0.01 O 2 (grain size: 2–4 μm) under 790 °C. The obtained LiNi 0.95 Co 0.04 Mn 0.01 O 2 represents excellent electrochemical properties with an initial discharge capacity of 240.5 mAh g −1 and a Coulombic efficiency of 90.1 % at 0.1C (1C = 220 mA g −1 ) in a Li-metal half cell. Upon long-term cycling, the monocrystalline feature with less crystallographic defect effectively enhances the structural stability and inhibits the formation of intergranular cracks, resulting in an enhanced cyclic stability (discharge capacity of 151.0 mAh g −1 maintained after 300 cycles at 1C in a Li-metal half cell). Coupled with a graphite anode, the LiNi 0.95 Co 0.04 Mn 0.01 O 2 || graphite full cell represents a stable cycling at 1C, with a capacity retention of 99.0 % after 100 cycles.

CAS / MDL: 1310-66-3 1314-11-0
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Small · 2023 · IF 13.3

Coupling MoSe2 with Non-Stoichiometry Ni0.85Se in Carbon Hollow Nanoflowers for Efficient Electrocatalytic Synergistic Effect on Li-O2 Batteries

Yuxin Long,Qiang Li,Zidong Zhang,Qingxi Zeng,Dong Liu,Lanling Zhao,Yao Liu,Yebing Li,Yiming Zhang,Kunqian Ji,Zhaorui Zhou,Xue Han,Jun Wang

Li-O 2 batteries could deliver ultra-high theoretical energy density compared to current Li-ion batteries counterpart. The slow cathode reaction kinetics in Li-O 2 batteries, however, limits their electrocatalytic performance. To this end, MoSe 2 and Ni 0.85 Se nanoflakes were decorated in carbon hollow nanoflowers, which were served as the cathode catalysts for Li-O 2 batteries. The hexagonal Ni 0.85 Se and MoSe 2 show good structural compatibility with the same space group, resulting in a stable heterogeneous structure. The synergistic interaction of the unsaturated atoms and the built-in electric fields on the heterogeneous structure exposes abundant catalytically active sites, accelerating ion and charge transport and imparting superior electrochemical activity, including high specific capacities and stable cycling performance. More importantly, the lattice distances of the Ni 0.85 Se (101) plane and MoSe 2 (100) plane at the heterogeneous interfaces are highly matched to that of Li 2 O 2 (100) plane, facilitating epitaxial growth of Li 2 O 2 , as well as the formation and decomposition of discharge products during the cycles. This strategy of employing nonstoichiometric compounds to build heterojunctions and improve Li-O 2 battery performance is expected to be applied to other energy storage or conversion systems.

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Energy Storage Materials · 2023 · IF 20.4

Engineering cyano groups into hydrogen-bonded organic supramolecules with multi redox centers for high-performance Li-ion battery cathode

Yong Wu,Yifan Wang,Facai Wei,Tingting Zhang,Wenda Li,Lingyan Huang,Ruijuan Qi,Jianwei Fu,Chengbin Jing,Jiangong Cheng,Shaohua Liu

Bottom-up molecular engineering by rational design has emerged as a promising strategy for exploring advanced organic cathodes. However, directly programming organic moieties into high-performance electro-active materials remains a great challenge. Herein, we design and synthesize a hydrogen-bonded supramolecule (hexaazatrinaphthalene hexacarbonitrile, HATN-6CN) anchored with abundant cyano groups, which ensures structural stability, extended π-conjugated system, and multiple redox active centers. As a result, the HATN-6CN cathode delivers a high specific capacity (297.6 mAh g –1 at 0.5 A g –1 , 225.2 mAh g –1 at 5 A g –1 ) and outstanding long-term cycling performance (191.9 mAh g –1 over 1000 cycles at 5 A g –1 with a capacity retention of 85.2 %). Moreover, the charge storage mechanisms, structural evolution, and reversibility during the redox process of HATN-6CN were systematically investigated. This work offers a feasible and promising avenue for bottom-up molecular engineering of organic electrodes by rational design.

CAS / MDL: 872-50-4
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Efficient and ultrafast separation of Li+ and Mg2+ by the porous two-dimensional nanochannel of perm-selective montmorillonite membrane

Tong Wen,Yunliang Zhao,Xingwen Wang,Licai Chen,Renbo Gao,Shutong Wang,Tingting Zhang

Recent innovations have created various two-dimensional membranes to break the Li + /Mg 2+ selectivity limit of traditional separation membranes. However, the simultaneous achievement of ultrafast transport and high selectivity is still below the theoretical prediction. Herein, for overcoming these shortcomings, the two-dimensional montmorillonite membrane (2D MMT membrane) consisting of sulfonated polyvinyl alcohol (SPVA), ethylene glycol (EG), and polyacrylamide (PAM) is proposed based on the design of porous 2D nanochannels. It is found that the SPVA can effectively improve the membrane stability, but will densify the channel, and prevent ion transport. When the appropriate EG is included in the membrane component, the transport rate of Li + can be increased from 0.29 mol h −1  m −2 to 0.56 mol h −1  m −2 . However, because the transport of Mg 2+ needs to overcome the high dehydration energy barrier, the J Mg2+ changes little, hence increases in S Mg 2+ Li + from 4.1 to 7.3. In addition, the selectivity regulation of PAM can be further integrated, and the permselectivity of the membrane is improved to 9.2 due to the strong selective coordination of amide groups to Mg 2+ . This novel strategy provides a valuable reference for developing high-performance 2D MMT membranes, which can also promote the application of 2D membranes in the Li + /Mg 2+ separation.

CAS / MDL: 7447-41-8 7786-30-3
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Hollow Co3O4@N-doped carbon nanocrystals anchored on carbon nanotubes for freestanding anode with superior Li/Na storage performance

Shouji Huang,Liwen Yang,Guobao Xu,Tongye Wei,Jiao Tian,Xiong Liu,Huapeng Li,Ziyuan Xiang,Juexian Cao,Xiaolin Wei

A template-free strategy is developed to construct a composite of hollow Co 3 O 4 nanocrystals with N-doped carbon and carbon nanotubes (CNTs) as freestanding anodes for Li and Na ion batteries (LIBs/NIBs) via a chemical precipitation and subsequent two-step annealing. In this composite, the N-doped carbon coated hollow Co 3 O 4 nanocrystals have a average diameter of 12 nm and are anchored tightly on highly conductive CNT substrates. Such nanocomposite possesses large specific surface area to supply ample active sites, highly conductive carbon networks to enhance electric conductivity, short ion diffusion distance to improve ion transport, and large interior space to accommodate volume expansion during repeatedly electrochemical reaction. Furthermore, kinetic analysis reveal that pseudocapacitive-controlled Li/Na storages plays a vital role. The freestanding composite as a anode for the LIBs exhibits large reversible capacity (1468 mAh g −1 after 130 cycles at 0.2 A g −1 ), superior rate performance (271 mAh g −1 at 12.5 A g −1 ) and good cyclic stability (905 mAh g −1 after 350 cycles at 1.0 A g −1 ). For the NIBs, the freestanding composite delivers attractive rate performance (104 mAh g −1 at 10 A g −1 ) and long cyclic performance (189 mAh g −1 after 400 cycles at 2.0 A g −1 ). Moreover, the assembled Li/Na full cell using the freestanding composite as anodes and LiFePO 4 (for LIBs) and Na 3 V 2 (PO 4 ) 3 (For NIBs) as the cathodes display superior electrochemical performances. Our results suggest the prepared freestanding composite has a highly promising application in high-performance LIBs/NIBs.

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ADVANCED FUNCTIONAL MATERIALS · 2021 ·Vol. 31 ·期 24 ·2101181 · IF 18.808

Achieving Desirable Initial Coulombic Efficiencies and Full Capacity Utilization of Li-Ion Batteries by Chemical Prelithiation of Graphite Anode

Yifei Shen,Xiaohui Shen,Mei Yang,Jiangfeng Qian,Yuliang Cao,Hanxi Yang,Yang Luo,Xinping Ai

Chemical prelithiation is an effective approach to elevate the initial Coulombic efficiency (ICE) and energy utilization of Li-ion battery electrodes. However, this approach fails to operate for the most commonly used graphite (Gr) anode, because all the prelithiation reagents reported so far have a much higher redox potential than Gr (≈0.2 V). Based on ionic solvation and coordination chemistry, for the first time, a new design strategy is proposed for prelithiation solution by selecting a strong electron-donating, sterically hindered, and chemically stable solvent to tune the redox potential of prelithiation reagent and also to prevent the solvent co-intercalation during prelithiation process, thus enabling a successful prelithiation of Gr anodes. By theoretical prediction and experimental evaluation, a chemical prelithiation solution, lithium biphenylide/2-methyl tetrahydrofuran, is successfully developed, which can prelithiate Gr anodes accurately to a desired state in few minutes without destroying the lattice structure of Gr. When the prelithiated Gr anodes (pGr) are paired with the conventional cathodes, the full cells demonstrate significantly improved ICEs and higher energy densities than their counterparts using pristine Gr anodes, showing a great prospect for wide Li-ion battery applications.

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JOURNAL OF MATERIALS SCIENCE · 2021 ·Vol. 56 ·期 36 ·20126-20137 · IF 4.22

Cross-linked siloxane-based copolymer binder with combined hardness and softness for stable silicon anodes in Li-ion batteries

Yang Jiyuan,Shi Minghui,Wu Wei,Zhang Qunchao,You Jun,Shi Dean,Jiang Tao

Silicon has become one of the most emerging anode materials in Li-ion batteries due to its excellent specific capacity. The incorporation of binders can significantly reduce the volume expansion of silicon during the cycling process. In this work, a novel type of cross-linked siloxane-based copolymer, poly (tert-butyl acrylate-co-vinyl tri-lactate ethyl silane) (TBA-VTLES) was designed and utilized as the binder for the silicon anode in Li-ion batteries to alleviate the inner stress of adverse volume changes and improve the electrochemical performance. The hard TBA and soft VTLES were interwoven into a 3D network to achieve the adhesive action via free radical polymerization. The soft chains in TBA-VTLES can enhance the cohesion of the copolymer to disperse residual stress, and thus avoid structural damage during lithiation. Meanwhile, the rigid chains can provide sufficient mechanical strength to maintain the integrity of silicon anode during de-lithiation. Moreover, the presence of TBA-VTLES can improve the adhesive strength between the copper collector and the binder. This novel type of siloxane-based copolymer binder with hardness and softness provides a feasible way to improve the silicon anode performance of Li-ion batteries. Graphical abstract The synthesized cross-linked copolymer binder can improve the interfacial interaction and electrochemical performance of Si anode-- present in Graphical abstract figure-- need or not.

CAS / MDL: 78-67-1 1663-39-4
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