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Nature Energy · 2024 · IF 49.7

Oscillatory solvation chemistry for a 500 Wh kg−1 Li-metal pouch cell

Zhang Shuoqing,Li Ruhong,Deng Tao,Ma Qiang,Hong Xiang,Zhang Hao,Zhang Ruixin,Ding Shouhong,Wu Yongjian,Zhu Haotian,Li Menglu,Zhang Haikuo,Lu Di,Ma Baochen,Lv Ling,Li Yong,Chen Lixin,Shen Yanbin,Guo Rui,Fan Xiulin

Cation solvation is well understood in the bulk solution phase, but knowledge is limited regarding the electrode–electrolyte interface. The process by which cation solvation conforms to the interfacial field to form interphases remains unclear. Here we examine the synergistic effects of external and intramolecular fields on accommodating Li + solvates to the Li-metal anode, leading to dielectric-mediated transfer dynamics on the interface. At charged interfaces, cation–anion pairs arrange in a periodic oscillatory distribution. A low-oscillation amplitude exacerbates the electrolyte decomposition and increases surface impedance. We propose a dielectric protocol that maintains cation–anion coordination with a high oscillation amplitude at the interfaces, addressing these issues. Accordingly, we demonstrate a Li-metal pouch cell with an energy density of 500 Wh kg −1 at the Ah level using an ultra-lean electrolyte (1 g Ah −1 ). Our study offers insights into solid/liquid interfaces that are crucial in advancing battery technologies.

CAS / MDL: 141-78-6
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Journal of Materials Chemistry A · 2024 · IF 10.7

Metal-ion exsolution effect to accelerate the reaction kinetics in Li–S batteries

Hongxu Zhou,Weichen Han,Hongquan Chai,Hao Huang,Jingang Zheng,Han Zhang,Lixiang Li,Weimin Zhou,Baigang An,Chengguo Sun

Sluggish reaction kinetics in lithium–sulfur (Li–S) batteries has seriously hindered their practical application. Herein, a three-dimensional (3D) granular carbon skeleton decorated with nickel-rich NCM materials (NCM@3D-SP) is prepared as a cathode host for Li–S batteries, where the carbon matrix is rich in pore channels, can provide good conductivity and electrolyte diffusion, and NCM811 particles contribute abundant metal sulfides active sites through metal-ion exsolution. The different metal sulfides (NiS, Ni3S2, Ni7S6, and CoS) in heterogeneous structures exhibit outstanding catalytic and adsorption effects on polysulfides during cycling, where the ion diffusion coefficient is increased by approximately 2.5 times compared to the cathode without catalytic active sites (3D-SP). A Li metal battery using NCM@3D-SP/S as the cathode exhibits a capacity decay of only 0.051% per cycle at 2C after 500 cycles. Even at an ultra-high current density of 10C and a sulfur-loading of 6 mg cm−2, the cells maintain a stable reversible discharge capacity of 453.1 mA h g−1 after 500 cycles and 4 mA h cm−2. The incorporation of nickel-rich cathode materials and 3D sulfur host structure presents a novel strategy for high-catalytic activity cathodes of Li–S batteries.

CAS / MDL: 7704-34-9
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Chemical Engineering and Processing-Process Intensification · 2024 · IF 3.8

Performance study of lithium ion sieve composite in high gravity for Li+ adsorption

Ying Ma,Youzhi Liu,Jiayu Li,Chengqian Zhang,Shufei Wang

The demand for lithium-ion batteries in new energy vehicles and energy storage technologies is rapidly increasing, making the efficient extraction of lithium resources from salt lakes, which are rich in lithium reserves, crucial. To address the issues of slow adsorption rate and low adsorption capacity of lithium ion sieves in the adsorption column, In this paper, the high-gravity rotating packed bed (RPB) is utilized for the first time to enhance the adsorption process of Li + on lithium ion sieve composite material(CTS/L-HMO), thereby investigating its adsorption mechanism. Specifically, CTS/L-HMO was prepared by combining manganese-based lithium ion sieves with chitosan, and used as the filler for the RPB to adsorb lithium containing solution. The research showed that chitosan successfully coated the manganese-based lithium ion sieves and the distribution of various elements was uniform. In the RPB, the adsorption capacity of CTS/L-HMO increased first and then decreased with the increase of liquid flow rate and high gravity factor. Compared to a fixed bed, the adsorption capacity and adsorption rate in the RPB increased by 43.30 % and 33.33 %, respectively. After 10 cycles of regeneration experiments, the adsorption capacity of CTS/L-HMO remained as high as 30.19 mg/g, and it exhibited high selective adsorption for Li + .

CAS / MDL: 2224-15-9 7758-29-4
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Coatings · 2024 ·Vol. 14 ·期 11 ·1473 · IF 2.9

TiO2 Coated with Carbon via Chemical Vapor Deposition as Li-Ion Batteries Anode

Bin Zhu,Wenjun Li,Wu Tang,Hui Tang

With the increasing demand for renewable energy and sustainable technologies, lithium-ion batteries (LIBs) have become crucial energy storage components. Despite the promising properties of the high capacity and stability of TiO2, its large-scale application as an anode for LIBs is hindered by challenges like poor conductivity and volumetric changes during cycling. Here, a rutile TiO2composite material with a thinned carbon coating (TiO2@TC) was synthesized through chemical vapor deposition (CVD) and a subsequent annealing process, which significantly improved the reversibility, cycling stability, and rate performance of the TiO2anode materials. The thickness of the carbon layer on TiO2was precisely controlled and thinned from 4.2 nm to 1.9 nm after secondary annealing treatment, leading to a smaller steric hindrance and an improved conductivity while serving as protective coatings by preventing the electrochemical degradation of the TiO2surface and hindering volumetric changes during cycling. The resulting TiO2@TC with the thin carbon layer demonstrated a high specific capacity of 167 mAh g−1at 0.5 C in Li-based half cells, which could stably run for 200 cycles with nearly 100% capacity retention. The thin carbon layer also contributes to an improved rate performance of 90 mAh g−1at even 20 C. This work provides an innovational strategy for improving the conductivity and volumetric changes during the cycling of TiO2anodes.

CAS / MDL: 13463-67-7
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Using hydrogen bond to promote the ionization of benzene sulfonamide for extracting Li+

Ruzhen Zhao,Manxing Huo,Qifeng Wei,Xiulian Ren

Ensuring a continuous and sustainable supply of lithium requires the development of green and efficient separation processes, such as liquid-liquid extraction for primary sources. In this work, a green method of extracting Li + from Qinghai old brine by using benzene sulfonamides is proposed. The method forms a green extraction system by hydrogen bonding between long-chain alcohol and benzene sulfonamide substance N221. It is proved that the formation of hydrogen bond promotes the ionization of N221 by means of conductivity measurement, equilibrium constant calculation, molecular dynamics simulation . This system has an obvious attraction to Li + , and the highest extraction efficiency of Li + can reach 95 %, and amine substances are added to maintain the pH of the system. The extraction effect is comparable to TBP (tributyl phosphate) and functional ionic liquid . After stripping, Li + enters the aqueous phase, and the separation effect is desirable. Therefore, a new green extractant is proposed in this study, which provides a new idea for green and environmentally friendly lithium extraction .

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ACS Nano · 2025 · IF 16

Intermolecular Interaction Adjustment for LiNO3 Solubility Promotion toward High-Performance Li||NCM811 Batteries

Chong Xu,Shuang Liu,Sai Che,Guang Ma,Gong Cheng,Dongyuan Zhang,Junjie Fu,Ye Wang,Jiahao Yang,Yuci Tian,Yongpeng Cui,Weihua Chen,Yongfeng Li

Incorporating lithium nitrate (LiNO3) as a film-forming additive into carbonate-based electrolytes presents a promising strategy to enhance the stability of high-energy-density Li||NCM811 batteries. However, the small size of Li+ and the high donor number (DN) of NO3– hinder the dissociation of LiNO3, and its limited solubility (<800 ppm) in carbonate-based electrolytes poses significant challenges for practical application. To address this issue, we propose a “Small-Sized Carrier” strategy that enhances the solubility of LiNO3 in carbonate solvents by modulating the intermolecular interactions within the solvent system. This approach employs vinylene carbonate (VC), a small molecule with moderate polarity, to enhance the dissolution of LiNO3 without compromising the compatibility of the electrolyte with the lithium metal anode. The introduction of the “Small-Sized Carrier” additive system simultaneously enhances the stability of the electrode–electrolyte interfaces and optimizes the solvation structure of the electrolyte. As a result, the electrolyte developed through this strategy demonstrates outstanding electrochemical performance, with Li||NCM811 batteries achieving a capacity retention of 83.8% after 600 cycles. This work provides an insightful approach to designing advanced electrolytes tailored to high-energy-density lithium metal batteries (LMBs).

CAS / MDL: 27860-83-9 7790-69-4
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ChemSusChem · 2024 · IF 7.5

Tri-anion solvation structure electrolyte improves the electrochemical performance of Li||LiNi0.8Co0.1Mn0.1O2 batteries

Ling Huang,Miaolan Sun,Yuxiang Xie,Huayu Huang,Yixin Huang,Hui Chen,Shishi Liu,Peng Dai,Rui Huang,Shigang Sun

Li||LiNi0.8Co0.1Mn0.1O2 batteries,which consist of lithium  metal anode (LMA) matched with NCM811 cathode, have an energy density more than twice that of lithium ion battery (LIB). However, the unstable electrode/electrolyte interface still hinders its practical application.Ether electrolytes show promise in improving the stability of LMA and NCM811 cathodes.However, a robust and stable electrode/electrolyte interface in Li||NCM811 batteries cannot be easily and efficiently achieved with most of the ether electrolytes reported in present studies. Herein, we present a straightforward and efficient tri-anion synergistic strategy to overcome this bottleneck. The addition of ClO4− and NO3− anions to LiFSI-based ether electrolytes forms a unique solvation structure with tri-anion (FSI−/ClO4−/NO3−) participation (LB511).This structure not only enhances the electrochemical window of the ether electrolytes but also achieves a stable Li||NCM811 batteries interface.The interaction between electrode and electrolyte is suppressed and an inorganic-rich (LiF/Li3N/LiCl) SEI/CEI layer is formed. Meanwhile, the coordination structure in the LB511 electrolyte increases the overpotential for Li deposition, resulting in a uniform and dense layer of deposition.Therefore, the Li||Cu cells using the LB511 electrolyte have an average CE of 99.6%.The Li||NCM811 batteries was cycled stably for 250 cycles with a capacity retention of 81% in the LB511 electrolyte (N/P = 2.5, 0.5 C).

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Energy Storage Materials · 2025 · IF 20.2

Lithiophilic Cu-Ag Architectures with Li-Si Alloys for Stable Lithium Metal Batteries

Siyu Fang,Tiansheng Bai,Jialin Liao,Shuai Zhang,Jiaxian Wang,Funian Mo,Wei Zhai,Zhenglin Hu,Jingyu Lu,Kwun Nam Hui,Lijie Ci,Deping Li

Lithium metal anodes hold the potential for high-energy-density batteries due to their substantial theoretical capacity, but their practical application is hindered by issues such as dendrite growth, poor cycling stability, and safety concerns. This study presents the development of a three-dimensional Li-Si composite alloy anode (Ag@Cu@Li-Si), combining a porous copper scaffold with a lithiophilic silver (Ag) layer and a lithium-silicon (Li-Si) alloy. The Ag@Cu@Li-Si composite demonstrates significant improvements in dendrite suppression, cycling stability, and electrochemical performance. The composite anode exhibits a critical current density of 15 mA cm −2 and over 900 hours of stable operation at 1.0 mA cm −2 in symmetric cells. When integrated into a full cell with a commercial LiFePO 4 cathode, it maintains excellent cycling stability, delivering over 600 cycles with a rate capability of 1.0 C. This study provides valuable insights into the design of lithium metal anodes, highlighting the importance of lithiophilic materials and 3D frameworks for high-performance lithium-metal batteries.

CAS / MDL: 7761-88-8
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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Sustainable and exceptional Li+ /Mg2+selectivity through electrocoagulation enhanced triamino guanidine modified membrane

Bin Liu,Xinyue Cui,Xiaozhen Lu,Xuewu Zhu,Lin Wang,Junyong Zhu

Positively charged polyamide (PA) nanofiltration (NF) membranes with sub-nanopores show promise for lithium extraction from salt-lake brines with high Mg 2+ /Li + ratios. This study introduces the use of triamino guanidine (TG), a highly positively charged molecule, to regulate grafting on monolayer PA membranes, resulting in dual-layer (PEI-TMC-TG) NF membranes. The monolayer PA membranes were created via spin-coating assisted interfacial polymerization between polyethyleneimine (PEI) and tricarbonyl chloride (TMC). The PEI/TMC-TG NF membranes exhibited several advantages over unmodified PEI-TMC NF membranes, including higher positive charge density, narrower pore size distribution, excellent hydrophilicity, and a more porous separation layer microstructure. Experimental results indicated that enhanced Donnan effect, size sieving, and dielectric repulsion within the sub-nanopores contributed to exceptional Li + /Mg 2+ selectivity during filtration of East Taijiner brine (S Li + /Mg 2+  = 64.5). Furthermore, the TG hydrophilic layer significantly improved water permeability (15.4 LMH/bar) and long-term stability. To reduce membrane fouling in the charge-positive NF process by removing organic matter from complex salt lake brine, we explored electrocoagulation as a pre-treatment method and identified optimal conditions for the EC-NF process. This strategy maximizes sustainable lithium recovery from brine in an economically viable green manner while enhancing the efficiency of NF membranes for lithium extraction from salt lakes.

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Nanomaterials · 2024 ·Vol. 14 ·期 15 ·1269 · IF 4.4

Thermoplastic Polyurethane Derived from CO2 for the Cathode Binder in Li-CO2 Battery

Haobin Wu,Xin Huang,Min Xiao,Shuanjin Wang,Dongmei Han,Sheng Huang

High-energy-density Li-CO2batteries are promising candidates for large-capacity energy storage systems. However, the development of Li-CO2batteries has been hindered by low cycle life and high overpotential. In this study, we propose a CO2-based thermoplastic polyurethane (CO2-based TPU) with CO2adsorption properties and excellent self-healing performance to replace traditional polyvinylidene fluoride (PVDF) as the cathode binder. The CO2-based TPU enhances the interfacial concentration of CO2at the cathode/electrolyte interfaces, effectively increasing the discharge voltage and lowering the charge voltage of Li-CO2batteries. Moreover, the CO2fixed by urethane groups (-NH-COO-) in the CO2-based TPU are difficult to shuttle to and corrode the Li anode, minimizing CO2side reactions with lithium metal and improving the cycling performance of Li-CO2batteries. In this work, Li-CO2batteries with CO2-based TPU as the multifunctional binders exhibit stable cycling performance for 52 cycles at a current density of 0.2 A g−1, with a distinctly lower polarization voltage than PVDF bound Li-CO2batteries.

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Advanced Energy Materials · 2024 ·Vol. 14 ·期 18 ·2304407 · IF 24.4

A Highly Stable Practical Li Metal Anode via Interphase Regulation and Nucleation Induction

Shuixin Xia,Zongyan Jiang,Xiaoyu Zhao,Jodie A. Yuwono,Xun Zhang,Xiangfeng Zhang,Guangzhi Yang,Junhe Yang,Yong Jiang,Jianfeng Mao,Kenneth Davey,Zaiping Guo,Shiyou Zheng

The practical utilization of Li metal anodes has been significantly plagued by the challenges of uncontrollable dendritic Li growth and poor interphase instability. Here, the study reports a novel strategy to strengthen interphase and give highly efficient active seeds concurrently to stabilize Li metal via a highly lithiophilic In 2 O 3 decorated porous scaffold. In situ configurated fast-ion-transport Li 2 O-strengthened interphase layer cooperatively with highly efficient Li 13 In 3 nucleation induction can endow the uniform Li nucleation/growth and high Li utilization efficiency. As a result, the achieved modified Li metal manifests high Coulombic efficiency, ultrahigh rate performance (5 mA cm −2 ), and ultra-long lifespan cycling durability (7975 cycles). Importantly, the established Li|LiFePO 4 cells exhibit long-term cycling durability over 600 cycles at 1 C with an ultralow decay rate of ca . 0.017% per cycle. Moreover, the Li|LiCoO 2 pouch cells with ultrahigh areal capacity of ca . 3.89 mAh cm −2 also exhibit extraordinarily prolonged cycling performance with excellent capacity retention despite extremely harsh cycling conditions of low negative-to-positive-capacity (N/P) ratio of ca . 1.7 and lean electrolyte of ca . 4.9 g Ah −1 . This work enlightens a facile and effective avenue toward highly stable Li metal anode toward reliable practicability.

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Advanced Energy Materials · 2018 ·Vol. 8 ·期 16 ·1702374 · IF 21.875

Germanium Thin Film Protected Lithium Aluminum Germanium Phosphate for Solid-State Li Batteries

Yijie Liu,Chao Li,Bojie Li,Hucheng Song,Zhu Cheng,Minrui Chen,Ping He,Haoshen Zhou

Solid-state Li batteries using Na + superionic conductor type solid electrolyte attracts wide interest because of its safety and high theoretical energy density. The NASCION type solid electrolyte LAGP (Li 1. 5 Al 0.5 Ge 0.5 P 3 O 12 ) shows favorable conductivity as well as good mechanical strength to prevent Li dendrite penetration. However, the instability of LAGP with Li metal remains a great challenge. In this work, an amorphous Ge thin film is sputtered on an LAGP surface, which can not only suppress the reduction reaction of Ge 4+ and Li, but also produces intimate contact between the Li metal and the LAGP solid electrolyte. The symmetric cell with the Ge-coated LAGP solid electrolyte shows superior stability and cycle performance for 100 cycles at 0.1 mA cm −2 . A quasi-solid-state Li–air battery has also been assembled to further demonstrate this advantage. A stable cycling performance of 30 cycles in ambient air can be obtained. This work helps to achieve a stable and ionic conducting interface in solid-state Li batteries.

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