Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Chen Ze,Wang Tairan,Wu Zhuoxi,Hou Yue,Chen Ao,Wang Yanbo,Huang Zhaodong,Schmidt Oliver G.,Zhu Minshen,Fan Jun,Zhi Chunyi
The high redox potential of Zn 0/2+ leads to low voltage of Zn batteries and therefore low energy density, plaguing deployment of Zn batteries in many energy-demanding applications. Though employing high-voltage cathode like spinel LiNi 0.5 Mn 1.5 O 4 can increase the voltages of Zn batteries, Zn 2+ ions will be immobilized in LiNi 0.5 Mn 1.5 O 4 once intercalated, resulting in irreversibility. Here, we design a polymer hetero-electrolyte consisting of an anode layer with Zn 2+ ions as charge carriers and a cathode layer that blocks the Zn 2+ ion shuttle, which allows separated Zn and Li reversibility. As such, the Zn ‖ LNMO cell exhibits up to 2.4 V discharge voltage and 450 stable cycles with high reversible capacity, which are also attained in a scale-up pouch cell. The pouch cell shows a low self-discharge after resting for 28 days. The designed electrolyte paves the way to develop high-voltage Zn batteries based on reversible lithiated cathodes.
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高影响因子
Science China-Chemistry
·
2025
·
IF 9.7
Huang Wenhuan,Wang Shun,Hou Xuehan,Zhang Yanan,Zhang Xingxing,Zhao Yaoxiao,Jin Xilang,Zhang Huabin,Wang Fei,Zhang Jian
Lithium-sulfur (Li-S) battery, as a promising next-generation high-energy-density battery, suffers from lithium polysulfides (LPSs) shuttle and Li dendrites issues. Porous crystalline framework-based membranes as separator can effectively absorb and restrain LPSs but without precise structural design principal exploration and mechanism studies. Herein, bio-inspired 1D oriented lithium-ion transport channels with molecular negatively charged PO 3 (−1) have been developed in hybrid tetrazole frameworks for promoting the transmission of Li + ions. The theoretical calculations and in situ spectroscopy demonstrated the higher binding energy and inhibited diffusion of LPSs in PO 3 . The assembled PP@PO 3 Janus separator in Li-S coin cell delivered a high initial capacity of 1410.9 mAh g −1 at 0.1 C and a low attenuation rate of 0.038% per cycle over 500 cycles at 5 C. Besides, the high capacities of 862, 542 and 409 mAh g −1 based on high-sulfur-loading cathodes of 2.6, 3.8 and 5.0 mg cm −2 at 0.5 C were achieved, respectively. Moreover, the punch battery of PO 3 @PP separator with S-cathode of 1.2 mg cm −2 has been developed for demonstrating its potentials commercial application, which displays impressive capacity of 873.4 mAh g −1 with the retention of ∼78.9% over 50 cycles.
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ACS Omega
·
2025
·
IF 4.3
Zhihua Xu,Yu Wu,Yangyang Zheng,Yucheng Chen,De Li,Wenting Ji,Yong Chen
As a well-known graphite-like material in superconductivity, lithium borocarbide (LiBC) can also be utilized as an electrode material in Li-ion batteries with a high specific capacity, which is assigned to the B–B bond produced through the aqueous reaction or the initial charge process. In this work, a rod-like LiBC sample (Ti-LiBC) is synthesized with the precursors of LiH + B + graphite in a sealed Ti tube through high-temperature sintering. Compared with the normal SUS-LiBC sintered in a sealed SUS304 tube, the Ti-LiBC possesses a lot of B–B bonds and a strong EPR signal, and it delivers a higher specific capacity (ca. 500 mAh g–1 at a mean discharge and charge potentials of 0.85 and 1.89 V, respectively) with excellent rate and cycle performances. Actually, the Ti metal can react with the H2 gas to produce the TiH2 phase at a high temperature, of which the extent determines the morphology of LiBC product, and the substitution of Li metal for LiH as the precursor can also result in the rod-like structure and the high specific capacity. Therefore, a hydrogen-free atmosphere is the key to synthesizing rodlike LiBC with excellent electrochemical properties, and this strategy might be extended to other graphite-like materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jian Lu,Chenye Dai,Shilong Li,Dong Zou,Yuqing Sun,Wenheng Jing
Similar physicochemical properties render the separation of Li + /Mg 2+ from salt lake brine difficult for two-dimensional (2D) membranes. Herein, ultraefficient Li + /Mg 2+ separation was achieved under the influence of an electric field using MXene/carbon nanotube (CNT) membranes developed on tubular ceramic substrates via thermal crosslinking. Crosslinking reactions between CNTs and MXene yielded well–intercalated CNTs between MXene nanosheets, forming antiswelling MXene/CNT membranes (MCMs) (interlayer spacing: 8.04 Å) suitable for Li + /Mg 2+ separation. At 2.8 V applied voltage, the MCMs exhibited Li + flux of 0.0491 mol m −2 h −1 and high Li + /Mg 2+ selectivity of 54.5, which outperform existing state–of–the–art 2D membranes. Specifically, under a positive electric field, Li + with a small hydration diameter and low hydration energy permeated through the membrane nanochannels more easily than Mg 2+ , increasing and decreasing Li + and Mg 2+ flux, respectively. Additionally, Mg 2+ retention was enhanced via the complexation of enriched Mg 2+ with –OH and –COOH on the membrane surface. The MXene membrane surface was thus reconfigured to be positively charged, inducing effective Mg 2+ rejection. This study offers a novel and practical approach for efficiently separating Li + /Mg 2+ as well as monovalent/multivalent ions.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Zhen Wang,Li Deng,Xue-Rui Yang,Jin-Xia Lin,De-Quan Cao,Jun-Ke Liu,Zhen Tong,Jing Zhang,Gao-Yang Bai,Yu-Xi Luo,Zu-Wei Yin,Yao Zhou,Juntao Li
The production of Li 2 CO 3 /C through CO 2 reduction reaction in nonaqueous systems is a complex four-electron, multi-step process, and the short existence time of intermediate monomers is not conducive to observation, which causes great difficulties in clarifying and regulating the CO 2 reduction path. Herein, ferrocene (Fc) as a functional additive into the electrolyte can stabilize the discharge intermediates and favor the occurrence of the two-electron reaction path during CO 2 RR, which leads to more stable operation of the Li-CO 2 battery; with the assistance of Fc, the CO 2 reduction pathway in Li-CO 2 battery is also clarified. Theoretical calculation analysis combined with experimental characterization observation confirms that Fc can shorten the CO 2 reduction distance through interaction with CO 2 and affecting the solvent environment around Li + , stabilize intermediate products to clarify the discharge path. The existence time of intermediates and discharge depth of the battery are key factors affecting the CO 2 reduction pathway. The Li 2 C 2 O 4 formed by CO 2 reduction through the 2-electron pathway is more favorable for the reversible operation of the Li-CO 2 battery than Li 2 CO 3 /C through the 4-electron pathway. This work provides inspiration for clarifying the reaction mechanism and regulating the CO 2 reduction pathway to improve the electrochemical performance of Li-CO 2 battery in the future.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
·
IF 4.1
Hu Fu,Weigang Zhu,Wenhua Xu,Zhongwei Zhao
Lithium-ion detection is necessary for extraction of lithium. Electrochemical sensors based on spinel LiMn 2 O 4 /λ-MnO 2 are expected to enable low-cost detection of lithium ions. Many studies demonstrate preferential intercalation of lithium ions, but little research has been done on how the differences in intercalation between lithium and other ions arise. Here, the differences in intercalation were identified by electrochemical impedance spectroscopy. Lithium ions were preferentially intercalated into λ-MnO 2 because of low charge transfer impedance. The apparent diffusion coefficient of sodium or potassium ions was one order of magnitude lower than that of lithium ions, while that of magnesium or calcium ions was two orders of magnitude lower. Therefore, insignificant intercalation of sodium, magnesium, potassium, and calcium ions slowed down diffusion of lithium ions through the channel and obstructed lithium-ion intercalation. The concentration of lithium ions was detected in brine of Baqiancuo Salt Lake by stripping voltammetry using λ-MnO 2 and an average recovery of 95.0 % was achieved. This study gives insights into ion intercalation of LiMn 2 O 4 in brine, which favors improvement of lithium-ion sensor based on LiMn 2 O 4 . In addition, the investigation facilitates understanding of the selectivity of similar materials (e.g., LiFePO 4 and Prussian blue analogous) in intercalation process.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2025
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IF 4.9
Huan Huan,Wei Wu,Qingyi Feng,Yongliang Tang,Sean Li,Hongxiang Deng,Xia Xiang,Xiaotao Zu,Yangfang Li
Wrinkled graphene prepared by the bubbling chemical vapor deposition method was ball milled to produce active materials for lithium-ion battery anode. By controlling milling parameters, the graphene with optimum electrode performance was obtained. After 2000 cycles at a current of 2000 mA g −1 , the reversible specific capacity can be maintained at 213.04 mAh g −1 , with a retention rate of 150.61 %. It was found that two lithium storage mechanisms coexist in this graphene material, and their capacitive control plays a major role, for example, accounting for 75.87 % contribution at a voltage scan rate of 0.8 mV s −1 . To further improve the electrode performance, B and N co-doped graphene was also prepared through ball milling. The results showed that, at the current of 2000 mA g −1 , the reversible specific capacity after 2000 cycles could reach 225.59 mAh g −1 , which was 5.9 % higher than that of the undoped one.
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JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Chen Zheng,Liu Peng,Cao Yu-Long,Xie Yu-Long
The manganese-based ion sieve H 1.6 Mn 1.6 O 4 shows significant advantages in lithium adsorption. Its prominent features include high adsorption capacity and low pollution characteristics of the preparation process. These combined advantages make this material important in the lithium extraction technology in salt lakes. However, problems such as high manganese dissolution loss rate, poor cyclic stability, and difficulty in powder recycling seriously restrict the industrialized application. In this paper, we propose to optimize the structure of spinel-type manganese lithium ion-sieves with a 2% Co 3+ doping strategy, which can effectively inhibit the lattice collapse triggered by Jahn–Teller aberration during the pickling cycle by replacing part of the Mn 3+ active sites with Co 3+ . After doping, the relative Mn 4+ content on the surface of the material increased from 58%–61% according to the XPS test, confirming that the introduction of Co 3+ facilitated the transition of Mn 3+ to the higher valence state Mn 4+ through the charge compensation effect. Reducing the disproportionation activity of Mn 3+ reduces the dissolution loss of Mn 2+ during the pickling process. The experimental results showed that the adsorption of doped HMCO-2 material increased from 28.8–34.9 mg/g. The adsorption capacity retention rate was 77% after five cycles, there was a high selective adsorption of Li + , and the manganese dissolving loss rate was decreased to 2.3%.
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Joule
·
2023
·
IF 39.8
Yatao Liu,Linhan Xu,Yongquan Yu,MengXue He,Han Zhang,Yanqun Tang,Feng Xiong,Song Gao,Aijun Li,Jianhui Wang,Shenzhen Xu,Doron Aurbach,Ruqiang Zou,Quanquan Pang
The transition from dissolution-precipitation to quasi-solid-state sulfur reaction promises restricted polysulfide shuttle and lean electrolyte operation of Li-S batteries but incurs poor reaction kinetics. We here demonstrate that structural reorganization of sparingly solvating electrolytes (SSEs)—which is uniquely afforded by using low-density and low-cost aromatic anti-solvents—is vital for taming the quasi-solid-state sulfur reaction. Aromatic anti-solvents disrupt the interconnected structure of concentrated tetrahydrofuran (THF) electrolyte, uniquely creating subdomains that act to dissolve elemental sulfur, thus accelerating its consumption and re-formation while maintaining ultralow polysulfides solubility. The altered subdomains further result in robust solid electrolyte interphase (SEI) on lithium metal. As a result, the Li-S cell with a 3 mg sulfur cm −2 sulfur cathode can cycle steadily for ∼160 cycles with a lean electrolyte of 5 μL mg sulfur −1 . Our work provides new insights into fine-tuning the electrolyte microstructure through solvent innovations for developing sulfur-based batteries that are high energy, cheap, and durable.
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NATURE
·
2025
·Vol. 637
·期 8047
·846-853
·
IF 48.5
Song Huimin,Münch Konrad,Liu Xu,Shen Kaier,Zhang Ruizhuo,Weintraut Timo,Yusim Yuriy,Jiang Dequan,Hong Xufeng,Meng Jiashen,Liu Yatao,He Mengxue,Li Yitao,Henkel Philip,Brezesinski Torsten,Janek Jürgen,Pang Quanquan
With promises for high specific energy, high safety and low cost, the all-solid-state lithium–sulfur battery (ASSLSB) is ideal for next-generation energy storage 1 , 2 , 3 , 4 , 5 . However, the poor rate performance and short cycle life caused by the sluggish solid–solid sulfur redox reaction (SSSRR) at the three-phase boundaries remain to be solved. Here we demonstrate a fast SSSRR enabled by lithium thioborophosphate iodide (LBPSI) glass-phase solid electrolytes (GSEs). On the basis of the reversible redox between I − and I 2 /I 3 − , the solid electrolyte (SE)—as well as serving as a superionic conductor—functions as a surficial redox mediator that facilitates the sluggish reactions at the solid–solid two-phase boundaries, thereby substantially increasing the density of active sites. Through this mechanism, the ASSLSB exhibits ultrafast charging capability, showing a high specific capacity of 1,497 mAh g −1 sulfur on charging at 2C (30 °C), while still maintaining 784 mAh g −1 sulfur at 20C. Notably, a specific capacity of 432 mAh g −1 sulfur is achieved on charging at an extreme rate of 150C at 60 °C. Furthermore, the cell demonstrates superior cycling stability over 25,000 cycles with 80.2% capacity retention at 5C (25 °C). We expect that our work on redox-mediated SSSRR will pave the way for developing advanced ASSLSBs that are high energy and safe.
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Nano Energy
·
2022
·
IF 19.069
Liping Ren,Fanpeng Kong,Xufeng Wang,Yajie Song,Xudong Li,Fang Zhang,Nan Sun,Hanwen An,Zaixing Jiang,Jiajun Wang
The limited stability and the excessive dependence on external heating sources restrict the development of polymer-based solid-state Li-O 2 batteries . Herein, we propose a multifunctional composed cathode with the photo-electro-thermal synergy to achieve a PEO-based solid-state Li-O 2 (PSS Li-O 2 ) battery operating at room temperature. The multifunctional composed cathode consists of the traditional black TiO 2 photocatalyst and carbon cloth (b-TiO 2 /CC). The b-TiO 2 /CC harvests a full spectrum of sunlight, besides the photo-generated electrons and holes enhancing reaction kinetics during discharging and charging processes, though converting solar energy into heat to achieve self-heated replace on external. The photo-electro-thermal synergy-triggered PSS Li-O 2 battery establishes a low overpotential of 0.26 V and long durability of up to 90 cycles, which is a breakthrough for PEO-based Li-O 2 batteries operating at room temperature. A flexible PSS Li-O 2 battery is constructed and exhibits superior flexibility and mechanical stability . The mechanism of the photo-electro-thermal synergy provides a new strategy for PSS Li-O 2 batteries and advances the high-efficiency utilization of solar energy in portable devices.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhen Li,Kailin Luo,Geng Zhang,Lingxuan Qian,Xiaodong Huang
Li metal is promising as the anode for next-generation Li-ion batteries; however, uncontrollable dendrite growth and severe side reactions between the Li metal and electrolyte greatly restrict its commercialization. Here, a 3D porous protective layer constructed by core@shell-Cu@Li 3 N particles is developed to solve the above issues. This protective layer is easily prepared just by one-step dip coating in Cu(NO 3 ) 2 /N-methyl-2-pyrrolidone (NMP) solution. Due to rapid Li + transport and good wettability of the protective layer, it effectively modulates Li + flux and thus homogenizes Li deposition. More importantly, as confirmed by both the experimental results and phase-field simulations, the 3D porous protective layer enforces the Li dendrite to laterally grow to form an interconnected network, which causes that the subsequent Li deposition is constrained and filled in the inner space rather than savage growth. Therefore, both the symmetric battery and full cell constructed by the protected Li electrode displays much longer lifespan than the one with bare Li even in unstable liquid carbonate electrolyte. Also, this protective layer is demonstrated to be compatible with Li 1+x Al x Ti 2−x (PO 4 ) 3 (LATP) solid-state electrolyte by suppressing the side reactions. This work paves a new and facile strategy for developing high-performance Li metal anode.
研究领域:
材料科学
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电化学
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电池技术
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