ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 20
·2112113
·
IF 19.924
Zhonghui Gao,Yang Bai,Haoyu Fu,Jiayi Yang,Thimo Ferber,Junrun Feng,Wolfram Jaegermann,Yunhui Huang
Garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTaO) is considered a promising solid-state electrolyte (SSE) for all-solid-state batteries (SSBs), but LLZTaO/Li interfacial issues limit their power density. The key question of whether LLZTaO does or does not form an interphase layer before and at the initial stage of electrochemical cycling remains debatable. An XPS interface approach, electrochemical cycling, and an electrochemically coupled phase field model to study the dynamic changes of interfacial resistance during cycling are utilized, and it is found that the generation rate of the interphase via electrochemical reaction processes at the LLZTaO/Li interface depends on the applied current density. For a Li/LLZTaO/Li cell, the impedance and overpotential increase gradually at the initial stage of electrochemical cycling at a current density of 0.1 mA cm –2 due to the formation of a passivating reaction zone (interphase) at LLZTaO/Li interface, which can protect the LLZTaO from being continuously reacted. With increasing the current density to 0.5 mA cm –2 , the electrochemical reaction is suppressed and tied to uneven Li ion transport across the LLZTaO/Li interface on plating, leading to a short circuit of the cell. Understanding how interface dynamic transformations influence electrochemical degradation is helpful to stabilize these interfaces in SSBs.
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Advanced Energy Materials
·
2022
·Vol. 12
·期 14
·2103932
·
IF 29.698
Xing Zhou,Yu Zhang,Ming Shen,Zhong Fang,Taoyi Kong,Wuliang Feng,Yihua Xie,Fei Wang,Bingwen Hu,Yonggang Wang
Sulfide solid electrolytes with high conductivity that is close to that of liquid electrolyte have been considered to be one of the most promising electrolytes for all-solid-state lithium batteries (ASSLBs). Unfortunately, the narrow electrochemical windows of sulfide electrolyte and contact loss at the interface upon cycles much limits the application of sulfide-based ASSLBs. In this work, an organic quinone cathode, 5,7,12,14-pentacenetetrone (PT), is used to fabricate an ASSLB with a sulfide electrolyte of glass ceramic 70Li 2 S-30P 2 S 5 (LPS). Based on the various in situ/ex situ analyses, it is successfully demonstrated that the decomposition of LPS is negligible and the corresponding effects on interfacial impedance are reversible with optimized carbon additives. In addition, the inherent low Young's modulus of the PT electrode efficiently prevents the contact loss at the interface. As a result, the PT-based ASSLBs deliver a high specific capacity (312 mAh g −1 ) and an excellent capacity retention (90.6%) over 500 cycles which is superior to previous reports. Moreover, a carbon-free ASSLB is constructed by employing Mo 6 S 8 as conductive additives in a PT-based cathode, which shows an improved rate performance and a long life.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Shenyang Xu,Zhihai Gao,Hao Chen,Liang Chang,Nian Zhang,Dong Zhou,Tianyi Li,Tony Wang,Cong Lin,Haoyu Xue,Qinghao Lai,Weiyuan Huang,Luyi Yang,Jiajie Liu,Tongchao Liu,Lunhua He,Mingjian Zhang,Zhengyan Lun,Feng Pan
Li-rich Mn-based layered (LMR) cathodes with anionic redox chemistry show great potential for next-generation sustainable Li-ion battery (LIB) applications due to the low cost and high energy density. However, the asynchronous structural evolutions with cycling in the heterogeneous composite structure of LMR lead to serious lattice strain and thus fast electrochemical decay, which hinders the commercialization of LMR cathodes. Here, an order–disorder coherent LMR cathode is demonstrated that exhibits a higher average voltage (by 0.25 V), negligible voltage decay (97.6% voltage retention after 100 cycles at 100 mA g −1 ), and enhanced cycling stability (98% capacity retention after 200 cycles at 100 mA g −1 ) compared to its layered oxide counterparts. It is proposed that this order–disorder coherent structure design can promote a more synchronous and homogeneous structure evolution during charge and discharge, thus minimizing lattice strain, which significantly prevents layer collapse and collective degradation at high voltage, improving the electrochemical stability. The study displays the feasibility of optimizing the performance of Li-rich cathode materials through a dedicated order–disorder structure control for sustainable energy storage.
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高影响因子
Advanced Energy Materials
·
2024
·Vol. 14
·期 18
·2304407
·
IF 24.4
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
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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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Chi Jiang,Shibo Bai,Jiawang Li,Ming Wang,Yan Zhou,Yingfei Hou
ABSTRACT Extraction of lithium resources from salt lake brines is an effective method to solve the shortage of lithium resources nowadays. However, magnesium-lithium separation has become a critical issue for lithium extraction from salt lakes with high Mg 2+ /Li + ratio, due to the similar ionic characteristics of Li + (0.38 nm), and Mg 2+ (0.43 nm). Herein, a amine monomer containing crown ether group (4'-aminobenzo-15-crown-5-ether (NH 2 -B15C5)) was introduced into the interfacial polymerization (IP) process of piperazine (PIP) and homotrimethylene tricarbonyl chloride (TMC) to prepare polyamide (PA) nanofiltration (NF) membranes with Li + selective transport channels. NH 2 -B15C5 shows good compatibility and selective complexation to Li + , which acts as Li + selective transport channels effectively retaining Mg 2+ and allowing Li + to cross the membrane smoothly, therefore solving the problem of poor lithium-magnesium separation performance of most of the NF membranes currently. Molecular dynamics simulations (MD) also confirmed that NH 2 -B15C5 has a stronger affinity for Li + than for Mg 2+ . The NH 2 -B15C5/PIP-TMC membrane exhibited excellent separation performance and water permeance in simulated salt lake brine (2000 ppm, W Mg/Li =100), where the S Li, Mg and water permeance were 32.2 and 8.22 L·m -2 ·h -1 ·bar -1 . Importantly, the crown ether is introduced into the PA separator layer in the form of covalent bonds, hence showing excellent stability. Overall, an NF membrane with high lithium-magnesium separation performance was designed for the extraction of lithium resources from high Mg 2+ /Li + ratio salt lake brine.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Tao Huang,Xiangzhen Zheng,Ying Pan,Chunfeng Yan,Maoxiang Wu
In this study, we investigate the efficacy of 2,4,6,8-tetramethyl-2,4,6,8-tetravinylcyclotetrasiloxane (ViD 4 ) as an electrolyte additive to enhance the electrochemical stability of Li-rich (LRO)/Li cells. The LRO/Li cell in the 1 vol% ViD4 electrolyte displays a mere 27.9 % capacity loss after 100 cycles at 0.5C (1C = 300 mAh −1 ), in comparison with the 66 % observed in the baseline electrolyte. Theoretical calculations reveal that ViD4 possesses a lower calculated oxidation potential than the electrolyte solution, signifying its preferential oxidation propensity. Physical characterization results demonstrate the formation of a uniform ViD4-derived film spanning 2–3 nm on the LRO cathode surface. This film enhances the stability of the cathode/electrolyte interface and safeguards the structural integrity of LRO. Moreover, ViD4 acts as a scavenger for hydrogen fluoride (HF), which is a decomposition product of LiPF 6 . Theoretical calculations verify the feasibility of ViD4 in effectively eliminating HF.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yongwei Chen,Xiangzhen Zheng,Ying Pan,Tao Huang,Maoxiang Wu
The instability of the electrode–electrolyte interface in high-voltage cathode materials significantly hinders the development of high-energy-density lithium-ion batteries (LIBs). In this study, 1,3-diphenyl-1,1,3,3-tetramethyldisiloxane (DTS) is employed as an electrolyte additive to enhance the cycling stability and capacity retention for Li||LLO (Li-rich layered oxide) batteries operating at 4.8 V. Theoretical calculations show that DTS can preferentially oxidize on the surface of the cathode. The oxidation forms a robust cathode electrolyte interface (CEI) on the LLO surface, significantly mitigating cracking, regeneration, and irreversible phase transitions of the LLO cathode. As anticipated, the Li||LLO batteries with the DTS electrolyte exhibit a capacity retention of 85.4% after 100 cycles at 4.8 V compared to the baseline electrolyte (45.2%). Furthermore, these batteries demonstrate superior capacity retention after 100 cycles at 4.8 V, even with the presence of 1000 ppm of H2O.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 46
·2004302
·
IF 16.836
Jun Chen,Guoqiang Zou,Wentao Deng,Zhaodong Huang,Xu Gao,Cheng Liu,Shouyi Yin,Huanqing Liu,Xinglan Deng,Ye Tian,Jiayang Li,Chiwei Wang,Di Wang,Hanwen Wu,Li Yang,Hongshuai Hou,Xiaobo Ji
The practical application of Li-rich Mn-based oxide cathode is predominately retarded by the capacity decline and voltage fading, associated with the structure distortion and anionic redox reactions. Here, a linkage-functionalized modification approach to tackle these challenges via a synchronous lithium oxidation strategy is reported. The doping of Ce in the bulk phase activates the pseudo-bonding effect, effectively stabilizing the lattice oxygen evolution and suppressing the structure distortion. Interestingly, it also induces the formation of spinel phase Li 4 Mn 5 O 12 in the subsurface, which in turn constructs the phase boundaries, thereby arousing the interior self-built-in electric field to prevent the outward migration of bulk oxygen anions and boost the charge transfer. Moreover, the formed coating layer Li 2 CeO 3 with oxygen vacancies accelerates Li + diffusion and mitigates electrolyte cauterization. The corresponding cathode exhibits superior long-cycle stability after 300 cycles with only a 0.013% capacity drop and 1.76 mV voltage decay per cycle. This work sheds new light on the development of Li-rich Mn-based oxide cathodes toward high energy density applications.
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高影响因子
Energy Storage Materials
·
2021
·
IF 17.789
Lei Zhong,Shuanjin Wang,Min Xiao,Wei Liu,Dongmei Han,Zhifeng Li,Jiaxiang Qin,Yuning Li,Shichao Zhang,Sheng Huang,Yuezhong Meng
Eliminating interfacial incompatibility and creating smooth ions/electrons transport at the interfaces of cathode│electrolyte│anode, are keys for the practical application of all-solid-state lithium-sulfur battery (ASSLSB). Here, we report a fully integrated-ASSLSB ( i -ASSLSB) whose interfacial resistances are suppressed by the segmental motion of polyethylene oxide in hierarchical polymer electrolyte throughout the whole battery system. The mobility of ethylene oxide segments and strength of polyelectrolyte membranes can be controlled by the cross-linking degree of single-ion conductive polyelectrolyte. Such a i -ASSLSB without distinct interface achieves liquid-state-level lithium-ion diffusion coefficient of 2.4 × 10 −12 cm 2 s −1 and demonstrates a remarkable capacity up to 1428 mA h g −1 at 0.05 C and 100-cycle stability at 0.1 C. This work promises a valuable technical approach of interface modulation for high-performance all-solid-state lithium-sulfur batteries.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zheng Lian,Youcai Lu,Shiyu Ma,Liqin Wang,Zhongjun Li,Qingchao Liu
In Li-CO 2 battery, redox mediators (RMs) are considered to have bright prospects due to their advantages of optimizing the mediated reaction pathway and reducing over-potential. However, some inherent defects caused by RMs, such as induced Li anode degradation and electron shuttle, limit its application in Li-CO 2 battery. In this work, ruthenium acetylacetonate (Ru(acac) 3 ) was innovatively applied as an efficient RM to boost the performance of Li-CO 2 battery, and the “shuttle effect” of Ru(acac) 3 to Li anode was also confirmed. To avoid the anode degradation caused by “shuttle effect” of RM, a novel Zn-MOF nanoplate modified glass fiber (M-GF) separator is skillfully prepared and used as a dual-function separator for Li-CO 2 battery. Experiments coupled with density functional theory simulations verifies that M-GF can protect Li anode by preventing Ru(acac) 3 from entering Li anode by physical and chemical interactions. Moreover, the highly ordered micropores in Zn-MOF also induce uniform deposition of Li + on the Li anode to delay the degradation process of anode, and thus prolonged the cycle life of the battery. Thanks to the bidirectional support of Ru(acac) 3 and M-GF strategy, the electrochemical performances of the Li-CO 2 battery, especially the round-trip efficiency and cycle life, has been greatly improved.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yi Yang,Yongbin Wang,Bin Zhou,Qi Tang,Ben Pu,Jin Cui,Yan Liu,Weiqing Yang
Mo 2 Ti 2 C 3 T x , a double transition metals (DTM) MXene, has emerged as a novel promising material for a wide range of applications due to its distinctive physicochemical properties. However, the commonly used method for preparing Mo 2 Ti 2 C 3 T x directly employing hydrofluoric (HF) acid as an etchant, is not only hazardous but also time-consuming. Recognizing the exceptional solubility and ultra-fast mass transfer kinetics of supercritical CO 2 (SC-CO 2 ), we introduced an extremely rapid SC-CO 2 assisted etching method that dramatically reduced the etching duration by a factor of 64, from 96 h to 1.5 h, thereby successfully preparing Mo 2 Ti 2 C 3 T x . When served as an anode in lithium-ion batteries (LIBs), the Mo 2 Ti 2 C 3 T x electrode achieves a high reversible specific capacity of 380 mAh g −1 at a current density of 0.1 A g −1 , significantly outperforming pure DTM-MXene-based anodes in terms of most reported capacities. This work provided a promising and efficient method for the etching of DTM-MXene.
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