Small
·
2025
·
IF 12.1
Wentao Wang,Aili Jia,Yiping Wang,Yuanxiao Qu,Junfeng Huang,Wen Zhang,Haitao Zhang
A novel polymer electrolyte based on CsPbI 3 quantum dots (QDs) reinforced polyacrylonitrile (PAN), named as PIL, is exploited to address the low room-temperature (RT) ion conductivity and poor interfacial compatibility of polymer solid-state electrolytes. After optimizing the content of CsPbI 3 QDs, RT ion conductivity of PIL largely increased from 0.077 to 0.56 mS cm −1 , and its Li-ion transference number ( τ L i + ${{\tau }_{{\mathrm{L}}{{{\mathrm{i}}}^ + }}}$ ) from 0.20 to 0.63. It is revealed that the synergistic enhancement of Li-ion transport and interface stability is realized by CsPbI 3 QDs through Lewis acid–base interaction, ordered polarization of PAN, and interface chemical regulation. These two effects guarantee the robust solid-electrolyte interface (SEI) in PIL-based solid-state batteries. Consequently, PIL electrolyte enables solid-state Li-metal batteries to deliver extraordinary RT cycling performance as verified by excellent cycling stability (>2000 h at 0.1 mA cm −2 ) of Li|PIL|Li symmetric batteries. Moreover, Li|PIL|LFP (LFP is LiFePO 4 ) and Li|PIL|NCM811 (NCM811 is Li(Ni 0.8 Co 0.1 Mn 0.1 )O 2 ) batteries maintain capacity retention of 81.2% and 77.9%, respectively, after 600 cycles at 0.5 C, as well as good rate-capability and very high Coulombic efficiency at RT.
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高影响因子
ACS Nano
·
2024
·
IF 15.8
Xue Tian,Huan Liu,Bin Cao,Peng Zhang,Yanze Li,Yanchao Ou,Haonan Cui,Mengyao Xu,Bin Xu
MXenes are promising cathodes for Li–CO2 batteries owing to their high electrical conductivity and efficient CO2 activation function. However, the effects of adsorption and electronic structures of MXene on the full life cycle of Li–CO2 batteries have been rarely investigated. Here, we employ a coregulation approach to enhance the adsorption–decomposition of lithium carbonate (Li2CO3) by introducing Zn and Cl surface groups onto the Ti3C2 MXene (Zn–Ti3C2Cl2) catalyst. The incorporation of Cl surface groups enhances Li2CO3 adsorption on the MXene catalyst surface, resulting in the formation of small-sized and uniform Li2CO3. Additionally, the introduction of Zn shifts the d-band centers of titanium and promotes CO2 evolution reaction (CO2ER) activity, thereby facilitating the decomposition of discharge products. As a result, the Li–CO2 battery based on the Zn–Ti3C2Cl2 catalyst exhibits an ultralow overpotential (0.72 V) at 200 mA g–1 and stable cycling for up to 1500 h. This work validates the efficacy of promoting reversibility in Li–CO2 batteries by adjusting the adsorption-decomposition process.
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高影响因子
ACS Energy Letters
·
2022
·
IF 23.991
Furong Sun,Yubo Yang,Shu Zhao,Yongtao Wang,Mingxue Tang,Qingzhen Huang,Yang Ren,Heng Su,Boya Wang,Ning Zhao,Xiangxin Guo,Haijun Yu
Garnet-type solid-state electrolytes Li7La3Zr2O12 (LLZO) for high-energy-density batteries have attracted extensive attention. However, stabilizing the high-conductive cubic phase and improving its ionic conductivity remain challenges of current research. Here, a Ca–W dual-substitution strategy has been designed, and the effect of doping on cubic phase formation and Li+ mobility has been investigated thoroughly. The results indicated that the partial substitution of Ca2+ at the La3+ site and W6+ at the Zr4+ site can effectively stabilize the cubic phase while reducing the endothermic enthalpy during the synthesis. Moreover, Ca–W dual substitution regulates the local Li+ framework by increasing Li+ occupancy at the 96h site, which can significantly lower the Li+ migration barrier and thus improve the ionic conductivity by two orders of magnitude. This work addresses the challenge of stabilizing a highly conductive cubic phase with low-energy consumption and represents a major breakthrough in understanding how to improve the ionic conductivity by regulating local structures.
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Energy Storage Materials
·
2022
·
IF 20.831
Long Chen,Jianhao Lu,Yibo Wang,Pan He,Shaobo Huang,Yan Liu,Yanzhou Wu,Gaoping Cao,Li Wang,Xiangming He,Jingyi Qiu,Hao Zhang
Lithium ion batteries (LIBs) have swept the whole energy storage field. However, the current mainstream lithium batteries are difficult to operate stably at high temperature (>60°C) due to the decomposition of electrolyte and solid electrolyte interphase (SEI), the cathode metal elements dissolution behavior, and potential thermal runaway. Here, We report a double-salt electrolyte with lithium bis(fluorosulfonyl)imide (LiFSI) and lithium difluoro(oxalato)borate (LiDFOB) as electrolyte salt, fluoroethylene carbonate (FEC), and tetra(ethylene glycol) dimethyl ether (TEGDME) as cosolvent, which delivers excellent ionic conductivity, high electrochemical stability and satisfactory ability to impede the dissolution of Fe element under elevated temperature (70°C). In addition, the electrolyte is benefited to form a robust and thermal-resistance solid-electrolyte interface (SEI) layer on the surface of graphite (Gr) anode, which shows improved decomposition temperature (86°C). The assembled thermally stable and high-safety 1300 mAh 18650-type LiFePO 4 |Gr cell shows high Coulombic efficiency (∼99.7%), improved cycling stability with discharge capacity 871.1 mAh after 200 cycles at 0.5 C and 70°C. This work affords a splendid strategy for address the unstable interface at both cathode and anode for safe high-temperature LIBs.
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高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Jingning Lai,Nan Chen,Fengling Zhang,Bohua Li,Yanxin Shang,Liyuan Zhao,Li Li,Feng Wu,Renjie Chen
High energy density lithium-oxygen (Li-O 2 ) batteries require soluble catalysts to accelerate the kinetics of oxygen reduction/evolution reaction (ORR/OER), and require SEI forming additives to protect lithium metal anode from side reaction with solvents, reduced oxygen species and soluble catalysts. In this study, a tri-functional additives 1-methyl, 3-benzyl, 1H imidazolium bromide (IMPBr) is dissolved in the dimethyl sulfoxide (DMSO)-based electrolyte to solve the problems of the slow dynamic process of ORR and OER, and protect the lithium anode by suppressing the dendrite formation in O 2 atmosphere. During discharging, IMP + has a strong binding ability to the intermediate product O 2 − , and Br − is highly associated with Li + , helping drive the solvation mechanism. During charging, Br − mediates the decomposition of battery discharge products and reduces the charge overpotential. Meanwhile, the positively charged IMP + can be attracted to the surface of the anode via electric attraction, in situ forming a stable SEI layer to prevent DMSO, Br 3 – , and Br 2 from attacking the lithium metal and growth of lithium dendrites. The synergy effect of the IMP + and Br – improves the cycle and rate performance of the Li-O 2 battery.
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高影响因子
ADVANCED MATERIALS
·
2022
·Vol. 35
·期 2
·2208974
·
IF 32.086
Wei Zhu,Jingchao Zhang,Jiawei Luo,Cuihua Zeng,Hai Su,Jinfeng Zhang,Rui Liu,Enyuan Hu,Yuansheng Liu,Wei-Di Liu,Yanan Chen,Wenbin Hu,Yunhua Xu
The synthesis of cathode materials plays an important role in determining the production efficiency, cost, and performance of lithium-ion batteries. However, conventional synthesis methods always experience a slow heating rate and involve a complicated multistep reaction process and sluggish reaction dynamics, leading to high energy and long time consumption. Herein, a high-temperature shock (HTS) strategy is reported for the ultrafast synthesis of cathode materials in seconds. The HTS process experiences an ultrahigh heating rate, leading to a non-equilibrium reaction and fast reaction kinetics, and avoids high energy and long time consumption. Mainstream cathode materials (such as LiMn 2 O 4 , LiCoO 2 , LiFePO 4 , and Li-rich layered oxide/NiO heterostructured material) are successfully synthesized with pure phases, oxygen vacancies, ultrasmall particle sizes, and good electrochemical performance. The HTS process not only provides an efficient synthesis approach for cathode materials, but also can be extended beyond lithium-ion batteries.
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ACS Applied Materials & Interfaces
·
2012
·
IF 4.525
Junfei Liang,Yue Zhao,Lin Guo,Lidong Li
A flexible free-standing graphene/SnO2 nanocomposites paper (GSP) was prepared by coupling a simple filtration method and a thermal reduction together for the first time. Compared with the pure SnO2 nanoparticles, the GSP exhibited a better cycling stability, because the graphene with high mechanical strength and elasticity can work as a buffer to prevent the volume expansion and contraction of SnO2 nanoparticles during the Li+ insertion/extraction process. Meanwhile, compared with single graphene paper, the GSP showed a higher capacity because of the hybridizing with higher capacity SnO2 nanoparticles. The excellent electrochemical performance of the GSP as an anode material in Li-ion battery was obtained. The as-prepared GSP shows a great potential for flexible Li-ion batteries.
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Zhou Yin,Yin Kun,Huang Yingying,Li Jiapei,Zhu Anquan,Lin Dewu,Gan Guoqiang,Zhang Jianfang,Liu Kai,Zhang Tian,Liu Kunlun,Luan Chuhao,Yang Huawei,Chen Hou,Guo Shaojun,Zhang Wenjun,Hong Guo
Charge overpotential for oxygen evolution reaction is a crucial parameter for the energy conversion efficiency of lithium-oxygen (Li-O 2 ) batteries. So far, the realization of low charge overpotential via catalyst design is a grand challenge in this field, which usually exceeds 0.25 V. Herein, we report an orbital reconstruction strategy to significantly decrease the charge overpotential to the low 0.11 V by employing PdCo nanosheet catalyst under a low-loading mass (0.3 mg/cm 2 ) and capacity (0.3 mAh/cm 2 ). Experimental and theoretical calculations demonstrate that the precise d-d orbital coupling ( d xz - d xz , d yz - d yz and d z 2 - d z 2 ) between the low-electronegativity Co and Pd leads to the reconstruction of Pd 4 d orbitals in PdCo nanosheets, thereby resulting in a downward shift of all the three active Pd 4 d orbitals ( d z 2 , d xz and d yz ) relative to that of Pd nanosheets. Furthermore, the highest energy level of the Pd 4 d z 2 orbital in PdCo is lower than the lowest energy levels of the Pd 4 d xz and 4 d yz orbitals in pure Pd, significantly decreasing the charge activation energy and achieving a highest energy conversion efficiency of 91%. This finding provides the orbital-level tuning into rational design of highly efficient electrocatalysts for Li-O 2 batteries.
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高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 8.2
Yunling Tian,Shuang Li,Zhan Wang,Quanchao Zhuang,Zhicheng Ju,Jiangmin Jiang
Silicon monoxide (SiO), with its high specific capacity and low discharge voltage plateau, stands out as a promising anode material for high-energy lithium-ion batteries. However, the application of SiO anodes suffers from an inferior initial Coulombic efficiency (ICE), the instability of the solid electrolyte interface (SEI) layer, and inferior Li+ transport kinetics, leading to unsatisfactory cycling stability and rate capability. Herein, a LiF/Sn–Li hybrid SEI layer is in situ constructed on chemically prelithiated SiO by spontaneous reaction with SnF2 (SnF2–SiO), driven by the redox potential difference between SnF2 and Li, which induces the reductive decomposition of SnF2 and interfacial chemical transformation. Chemical prelithiation compensates for irreversible lithium loss by introducing additional active lithium, thereby enhancing the ICE of the SiO anodes. Notably, the cooperative effect of LiF and Sn–Li alloy stabilizes the electrochemical interface, enhances Li+ diffusion kinetics, and reduces charge transfer resistance. As expected, the SnF2–SiO delivers a remarkable ICE (99.7%) and cycling stability (1126.0 mAh g–1 after 200 cycles), together with superior overall performance for lithium-ion full batteries (SnF2–SiO//LiFePO4). This work confirms the significance of chemical prelithiation and regulation of the hybrid SEI layer for advancing silicon-based anodes in high-performance lithium batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Guocui Cai,Helong Jiang,Fangyi Chu,Xiangcun Li,Xiaobin Jiang,Xiao Wu,Gaohong He,Yan Dai
Here, the conventionally disordered Co(OH)F filaments are rearranged to form highly-ordered flower-like Co(OH)F architectures in a conductive membrane substrate. The important findings contribute to designing delicate nanostructures and improving the catalytic activity of advanced materials for energy applications. The hierarchically porous CNT@NC membrane with CNT as the core and N -doped carbon as the crosslinking shell is scalably designed firstly for strengthening the transport of Li + and electrons in the electrode, providing an ultrahigh porosity for growing flower-like Co(OH)F on both surfaces and interior of the membrane, as well as offering electrons for the redox reactions through the roots of the Co(OH)F flowers. Furthermore, the ordered Co(OH)F bundles with divergent and open-ended structures provide the catalyst with the broad reaction interface and active sites for polysulfides (LiPSs) anchoring and catalytic conversion at a low energy barrier, significantly facilitating the diffusion of ions and electrolyte in the catalyst, and thus effectively alleviating the shuttle effect. Owing to the synergistic effect between the conductive membrane substrate and the grown Co(OH)F catalyst, the Co(OH)F-CNT@NC cathode generates a high reversible capacity and excellent long-term cycling performance (622 mAh·g −1 at 1C after 600 cycles). Conclusively, the proposed facile strategy provides insights regarding the design of novel cathode materials for high-areal-capacity Li–S batteries.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Liyuan Li,Tao Li,Yifan Sha,Chi Zhang,Baozeng Ren,Lan Zhang,Suojiang Zhang
Silicon-based anode materials attract ever-increasing attention owing to their high theoretical capacity. However, their practical application is significantly hindered by the dramatic volume change during the charge/discharge process, during which not only the solid electrolyte interface (SEI) but also the electrode might be ruined. Here, we propose a H-bond network-regulated binder by introducing low-molecular-weight cross-linkers, lithium oxalate and α-cyclodextrin (α-CD), into alginate (Alg). The balance between the binding strength and Li ion diffusion is realized through the control of the ratio between them. Lithium oxalate and α-CD can effectively regulate the H-bond network of the binder by forming intermolecular dynamic H bonds with Alg and reducing the intramolecular ones. Although the hybrid binder shows lower adhesion force than Alg, better electrode integrity is obtained during the charge/discharge process. Meanwhile, Li+ transportation is facilitated due to extra Li+ supplied by lithium oxalate, thereby achieving better rate capability.
研究领域:
材料科学
·
电化学
·
能源存储
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高影响因子
Nano Energy
·
2020
·
IF 16.602
Huajin He,Fucheng Ren,Jianping Zhu,Yuxuan Xiang,Bizhu Zheng,Sheng Li,Shijian Chen,Yixiao Li,Qi-Hui Wu,Yong Yang
Li-SF 6 battery has been proposed as a novel energy conversion device for both reducing greenhouse-effect SF 6 and potentially providing large specific energy . However, the real discharge process of SF 6 remains ambiguous with fast cathode passivation and large polarization. Here we report that the Li-SF 6 chemistry is able to deliver an unprecedented capacity of >20,000 mA h g c −1 with reduced polarization and excellent rate capability by using a low-cost, high-surface-area porous carbon as cathode host. More importantly, by adjusting the SF 6 atmosphere, an approximately eight-electron transfer process with predominant products of LiF and Li 2 S is realized via two voltage steps, whereas previously only a little Li 2 S could be found with one plateau appearing. The eight-electron process leads to a high energy density about 2,300 W h kg −1 based on the mass of carbon and discharge products, which sheds light on SF 6 as a promising high-energy-density cathode.
研究领域:
能量转换
·
电化学
·
材料科学
·
环境科学
·
电源技术
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