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ACS Applied Nano Materials · 2024 · IF 5.3

SiOx@ZrO2@C Nanospheres as a High-Capacity and Stable Anode Material for Lithium-Ion Batteries

Wenwen Deng,Shaocong Ni,Naiqi Hu,Ying Zhou,Zhong Jin

Silicon oxide (SiOx) has been widely studied due to its ultrahigh theoretical specific capacity for lithium storage. However, its inherent low electronic conductivity and large volume change before and after lithium insertion have limited its commercialization. To address this issue, we report the synthesis of SiOx@ZrO2@C ternary composite nanospheres by convenient and scalable wet chemistry and sintering processes. In the unique structure of 3D porous SiOx@ZrO2@C nanospheres, zirconium oxide (ZrO2) supplies high structural stability, while the amorphous carbon (C) layer helps to form a stable solid–electrolyte interface, suppress volume expansion, and greatly improve the conductivity. Electrochemical measurements demonstrate that the SiOx@ZrO2@C nanospheres exhibit a capacity retention of 72.2% after 500 cycles at 500 mA g–1. At a high current density of 800 mA g–1, the SiOx@ZrO2@C nanospheres can still deliver a capacity of 529.1 mAh g–1. This work provides a promising mass-scale synthesis method for producing SiOx composites and introduces a high-performance anode material for lithium-ion batteries.

CAS / MDL: 1071-76-7
研究领域: 材料科学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Cathode-electrolyte interface modification by electrolyte engineering for vanadium-based zinc-ion batteries

Zhiqiang Dai,Chengwu Yang,Jin Cao,Xueqing Zhang,Yinghao Zhao,Dongdong Zhang,Xinyu Zhang,Jiaqian Qin

The vanadium (V)-based cathode of aqueous zinc-ion batteries (ZIBs) faces the problem of rapid capacity decay due to material dissolution and structural collapse during the continuous cycling process. Here, we present a strategy to convert the irreversible cathode-electrolyte interphase (CEI) layer of the NH 4 V 4 O 10 (NVO) cathode into a protective layer by incorporating alkali metal sulfate as an additive. After the introduction of Na + , the dynamic consumption and replenishment of OH – during the conversion of Zn 3 (OH) 2 V 2 O 7 ·2H 2 O and Na 2 ZnV 2 O 7 regulates the pH value on the surface of the NVO cathode and inhibits the occurrence of side reactions. The NVO cathode exhibits a higher specific capacity (from 371.8 to 407.8mAh g −1 at 0.1 A g −1 ), better capacity retention (from 30.5 % to 65.9 % after 150 cycles), and superior rate capability after Na + introduction. Additionally, the Na + additives could be also applied for other V-based materials (e.g., V 2 O 5 and VO 2 ) to significantly improve the capacity retention rate. This strategy of incorporating alkali metal sulfate electrolyte additives to fortify cathode cycling stability serves to expedite the transition of aqueous ZIBs from the realm of academia to the industrial sector.

研究领域: 材料科学 · 电化学
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ACS Nano · 2024 · IF 15.8

Generality Rules and Synergistic Effect of Mitigating the Jahn–Teller Effect by Multisites Compositionally Complex Doping

Shuyu Zhou,Junhong Liao,Chenglong Yu,Pengpeng Dai,Tong Gao,Tingzheng Hou,Guozhong Cao,Shixi Zhao

The Jahn–Teller (JT) deformation triggers severe structural distortion and large capacity fading in the cathode materials of alkali-ion batteries. Although conventional doping containing over 20 dopant species has been demonstrated to suppress the JT effect, how the short-range and cooperative JT effect are regulated remains an open question. Recently, the new compositionally complex (high entropy) doping has been validated in various oxide cathodes and achieved “zero strain”, but the reported “synergistic effect” is largely factual reporting with a limited fundamental understanding of the link between multicomponents and the JT effect. By comparing a group of spinel LiMn2O4 (LMO) cathodes with tridoping sites containing one, three, or five dopants’ species, the present work shows that MnO6 octahedral distortion systematically decreases, whereas capacity retention and structure stability systematically increase as the number of dopants’ species increases. We propose the generality rules that Mn-site doping breaks the linear continuous short-range JT distortion while 16c-sites doping disturbs the dz2-orbital collinear ordering and mitigates the cooperative JT effect. Moreover, our complex doping strategy further buffers and rotates the JT strain, resulting in isotropic moderate volume distortion. Based on this synergic effect, both the short-range and cooperative JT effect are significantly suppressed in our synthesized multisites multicomponent doped LMO.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

Toward stable lithium-ion batteries: Accelerating the transfer and alloying reactions of Sn-based anodes via coordination atom regulation and carbon hybridization

Junhua Zhou,Yizhou You,Xueyu Lian,Qitao Shi,Yu Liu,Xiaoqin Yang,Alicja Bachmatiuk,Lijun Liu,Jingyu Sun,Ruizhi Yang,Jin-Ho Choi,Mark H. Rümmeli

Although anodes based on Sn alloys (SnX) such as SnO 2 , SnS, and Sn 4 P 3 may be used to increase the gravimetric and volumetric energy densities of existing lithium-ion batteries, the further development of these anodes is hindered by their complex reaction mechanisms , sluggish conversion, and the occurrence of undesired reactions. Herein, we probe the mechanisms of the incompletely reversible reactions of SnO 2 and SnS using analytical and electrochemical techniques and demonstrate that the capacity retention of these species can be further increased using coordination atom regulation and hybridization with carbon. The superior cyclability (sustainable operation for >500 cycles) of the optimized SnS/C composite is attributed to its reinforced conversion and alloying reactions resulting from enhanced bulk structure, higher interface stability, and accelerated kinetics. This work also provides guidance for the development of other alloy-based anode materials , especially regarding the choice of coordination atoms and the understanding of the role of carbon coatings in property optimization.

研究领域: 材料科学 · 电化学
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Applied Sciences-Basel · 2020 ·Vol. 10 ·期 3 ·1021 · IF 2.474

Electrochemical Behavior of NH4F-Pretreated Li1.25Ni0.20Fe0.13Co0.33Mn0.33O2 Cathodes for Lithium-ion Batteries

Yonglei Zheng,Yikai Li,He Wang,Siheng Chen,Xiangxin Guo,Sheng Xu,Zhongyu Cai

We report a novel method to fabricate lithium-ion batteries cathodes with the NH4F pretreatment. In this study, NH4F-pretreated Li1.25Ni0.20Fe0.13Co0.33Mn0.33O2hollow nano-micro hierarchical microspheres were synthesized for use as cathode materials. The X-ray diffraction patterns of NH4F-pretreated Li1.25Ni0.20Co0.33Fe0.13Mn0.33O2were analyzed with the RIETAN-FP software program, and the results showed that the samples possess a layered α-NaFeO2structure. The effects of pretreatment with NH4F on the electrochemical performance of the pristine material were evaluated through charge/discharge cycling, the rate performance, and electrochemical impedance spectroscopy (EIS). Pretreatment with NH4F significantly improved the discharge capacities and coulombic efficiencies of Li1.25Ni0.20Co0.33Fe0.13Mn0.33O2in the first cycle and during subsequent electrochemical cycling. The sample pretreated with an appropriate amount of NH4F (NFCM 90) showed the highest discharge capacity (209.1 mA h g−1) and capacity retention (85.2% for 50 cycles at 0.1 C). The EIS results showed that the resistance of the NFCM 90 sample (76.32 Ω) is lower than that of the pristine one (206.2 Ω).

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Crystalline Sb or Bi in amorphous Ti-based oxides as anode materials for sodium storage

Jun Pan,Kang Yu,Hongzhi Mao,Lili Li,Yuchen Zhang,Yanlu Li,Paulo J. Ferreira,Jian Yang

A simple synthesis has been developed for watermelon-like nanocomposites with Ti-based oxides as the matrix. Using the case of Sb nanocrystals in amorphous TiPO x as an example, in-situ/ex-situ techniques, first-principle calculations and control experiments confirm that the formation of Ti-based oxides promotes the reduction of Sb 3+ to Sb by NH 3 at an elevated temperature. A similar synthesis process also succeeds for Sb nanocrystals in amorphous TiO 2 and for Bi nanocrystals in amorphous TiPO x , confirming the promising potential of this synthesis. More importantly, the nanocomposite composed by crystalline Sb in an amorphous TiPO x matrix, as the anode material for sodium storage, concurrently exhibits a long cycle life (~1000 cycles) and a high capacity retention (~82%), suggesting the advantages of watermelon-like structures.

CAS / MDL: 1336-21-6 10025-91-9
研究领域: 材料科学 · 电化学
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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 48 ·期 2 ·621-630 · IF 3.3

Sulfur-containing polymer/carbon nanotube composite cathode materials for high-energy lithium–sulfur batteries

Shuimiao Wang,Yurui Wu,Ming Yang,Li Sun,Yong Tao,Chang-An Yang

Lithium–sulfur (Li–S) batteries have attracted the attention of researchers because of their excellent theoretical capacity and the advantages of cost-saving and environmental friendliness of their cathode materials. However, due to the shuttling of soluble intermediate polysulfides and other issues, the performance of current Li–S batteries is far from satisfactory. Herein, a sulfur-containing polymer (S-TVTCSi4) synthesized by the copolymerization of sulfur with 2,4,6,8-tetravinyl-2,4,6,8-tetramethylcyclotetrasiloxane (TVTCSi), was combined with carbon nanotubes (CNTs) to obtain a sulfur-containing polymer/carbon nanotube composite cathode material for Li–S batteries. S-TVTCSi4 can effectively anchor lithium polysulfide through covalent bonding, and CNTs can improve the electrochemical reaction kinetics inside the battery. As a result, the S-TVTCSi4-CNT-based battery exhibited prominent rate capacity and stable cycling performance at different current densities, the reversible capacity of 980 mA h g−1 can be achieved after 100 cycles at 0.3C, with the capacity retention of 88.3%, and even at a high current density of 1C, 64.6% of the initial capacity can be retained after 1000 cycles, with a capacity decay of only 0.035% per cycle. The impressive cycling performance demonstrated the enormous potential of the S-TVTCSi4-CNT composite cathode in high-energy Li–S batteries.

研究领域: 材料科学 · 能源技术
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Regulating local oxygen covalence and interrupting transition metal migration path by multisite doping to stabilize Li-rich layered cathodes

Ziyang Liang,Wenzhao Huang,Gesong Huang,Xiaola Li,Yuqing Liu,Boyang Zhang,Shuxing Wu,Chenyu Liu,Zhan Lin,Dong Luo

Lithium-rich manganese-based layered oxides (LLOs) are regarded as a kind of ideal cathode materials of the next-generation lithium-ion batteries owing to their exceptionally high theoretical capacity (>300 mAh g −1 ). Nevertheless, these cathode materials are subject to voltage decay and capacity fading due to the irreversible oxygen release and transition metal (TM) migration. Hence, a multisite doping strategy is proposed to interrupt the migration path of TM ions for LLO cathodes with superior structural stability. Moreover, multisite doping also offers pillar effect, and stabilizes lattice oxygen by the establishment of robust covalent P-O bonds to constrain the removal of electrons from the O 2p band. The P-Mg co-doped sample exhibits enhanced dynamic structural reversibility, lattice oxygen stability, and a significantly augmented resistance to electrolyte corrosion. Consequently, the co-doped sample shows outstanding capacity and voltage stability. Its capacity retention ratio is as large as 92.5 % even after 400 cycles, with a corresponding voltage decay rate of merely 0.688 mV/cycle. Multisite doping strategy presents an innovative approach to mitigating voltage decay and capacity fading of Li-rich Mn-based layered cathodes.

研究领域: 材料科学 · 电化学
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Nanomaterials · 2021 ·Vol. 11 ·期 6 ·1429 · IF 5.076

High-Capacity and Long-Lifespan Aqueous LiV3O8/Zn Battery Using Zn/Li Hybrid Electrolyte

Qiang Pang,Xiangyu Yu,Shijing Zhang,Wei He,Siyu Yang,Yao Fu,Ying Tian,Mingming Xing,Xixian Luo

Aqueous zinc-ion batteries (AZIBs) are promising candidates for large-scale energy storage because of their low cost and high safety. However, their practical applications are impeded by low energy density and short service life. Here, an aqueous Zn2+/Li+hybrid-ion battery is fabricated using the LiV3O8nanorods as the cathode, metallic Zn as the anode, and 3 M Zn(OTf)2+ 0.5 M LiOTf aqueous solution as the electrolyte. Compared with the batteries using pure 3 M Zn(OTf)2electrolyte, the cycle performance of the hybrid-ion battery is significantly improved. After 4000 cycles at 5 A g1, the remaining capacity is 163.9 mA h g−1with impressive capacity retention of 87.0%. Ex-situ XRD, ex-situ XPS, and SEM tests demonstrate that the hybrid electrolyte can inhibit the formation of the irreversible Zn3(OH)2V2O7·2H2O by-product and restrict Zn dendrite growth during cycling, thereby improving the cycle performance of the batteries.

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Pb nanospheres encapsulated in metal–organic frameworks-derived porous carbon as anode for high-performance sodium-ion batteries

Xiaoying Zhao,Ningbo Liu,Chaonan Mu,Bin Qin,Liubin Wang

Alloying-type anode materials are considered promising candidates for sodium-ion batteries (SIBs) due to their high theoretical capacities. However, their application is limited by the severe capacity decay stemming from dramatic volume changes during Na + insertion/extraction processes. Here, Pb nanospheres encapsulated in a carbon skeleton (Pb@C) were successfully synthesized via a facile metal–organic frameworks (MOFs)-derived method and used as anodes for SIBs. The nanosized Pb particles are uniformly incorporated into the porous carbon framework, effectively mitigating volume changes and enhancing Na + ion transport during discharging/charging. Benefiting from this unique architecture, a reversible capacity of 334.2 mAh g −1 at 2 A g −1 is achieved after 6000 cycles corresponding to an impressive 88.2 % capacity retention and a minimal capacity loss of 0.00748 % per cycle. Furthermore, a high-performance full sodium-ion battery of Pb@C//NVPF was constructed, demonstrating a high energy density of 291 Wh kg −1 and power density of 175 W kg −1 . This facile MOFs-derived method offers insights into the design of high-capacity alloy-type anode materials using Pb sources, opening up new possibilities for innovative approaches to Pb recycling and pollution prevention.

研究领域: 材料科学 · 能源存储与转换
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Synthesis of FeS/Fe2O3 hollow fibers derived from Fe-alginate fibers as anodes for high performance sodium-ion batteries

Yan Wang,Ming Liu,Haibing Liu,Junhang Ding,Tian Wang,Jinfeng Dong,Bingbing Wang,Xing Tian,Yanzhi Xia

Search for anode materials for sodium ions batteries (SIBs) attracts researchers around the world because of their high-rate capability and excellent capacity. However, their stability needs to be improved. Thus, this work demonstrates a controllable method for the synthesis of one-dimensional (1D) hollow microfibers using “egg-box-structured” Fe-alginate fibers. The goal was to obtain an SIBs anode material with the optimal number of voids for efficient Na + storage. An optimized micro and pore structures were designed to obtain the shortest Na + -diffusion distance. The novel FeS 2 /Fe 2 O 3 -HF composite was able to withstand volume expansion during charge/discharge processes and showed high specificity and rate capacity (483 mAh/g at 100 mA/g, 241 mAh/g at 2000 mA/g). The capacity retention of this cell was excellent: it maintained 245 mAh/g over four hundred 1000 mA/g cycles. Thus, FeS 2 /Fe 2 O 3 -HF composite is a very promising active anode material for SIBs.

CAS / MDL: 9005-38-3
研究领域: 材料科学 · 能源存储
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ADVANCED MATERIALS · 2017 ·Vol. 29 ·期 12 ·1605160 · IF 19.791

A New Type of Multifunctional Polar Binder: Toward Practical Application of High Energy Lithium Sulfur Batteries

Wei Chen,Tao Qian,Jie Xiong,Na Xu,Xuejun Liu,Jie Liu,Jinqiu Zhou,Xiaowei Shen,Tingzhou Yang,Yu Chen,Chenglin Yan

Graphical A new type of amino polar binder with 3D network flexibility structure for high energy Li–S batteries is synthesized and successfully used with commercial sulfur powder cathodes. The binder shows significant performance improvement in capacity retention and high potential for practical application, which arouse the battery community's interest in the commercial application of high energy Li–S battery.

研究领域: 材料科学 · 能源技术
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