Small
·
2023
·Vol. 19
·期 46
·2305326
·
IF 13.3
Shida Xue,Shiming Chen,Yanda Fu,Hengyao Zhu,Yuchen Ji,Yongli Song,Feng Pan,Luyi Yang
Composite solid electrolytes (CSEs) consisting of polyethylene oxide (PEO) matrix and active inorganic fillers have shown great potential for practical applications. However, mechanisms of how different active fillers enhance ion transport in CSEs still remain inconclusive. In this work, the component dependencies of ionic conductivity of PEO-based CSEs are investigated by comparing two widely investigated active fillers: NASICON-type (LATP) and garnet-type (LLZTO). In terms of ionic conductivity, the optimum ratios are strikingly different for LLZTO (10 wt%) and LATP (50 wt%). Through experimental and computational studies, it is demonstrated that the high affinity between LATP and PEO facilitates unhindered interfacial Li + transfer so that LATP functions as a bulk-active filler to provide additional inorganic ion pathways. By contrast, Li + transfer between LLZTO and PEO is found to be sluggish. Instead, LLZTO mainly improves ionic conductivity by dissociating lithium salt, making it a surface-active filler. Through categorizing active fillers based on their Li + conductive mechanisms, this work provides new understanding and guidelines for componential design and optimization of solid composite electrolytes.
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高影响因子
Inorganics
·
2023
·Vol. 11
·期 6
·257
·
IF 2.9
Rui Yan,Fangchao Liu,Zhengwen Fu
Li-SeS2batteries balance the opposing and complimentary qualities of Li-S and Li-Se batteries by having a high specific capacity and high electrical conductivity. However, there is still a lack of knowledge regarding the electrochemical characteristics of Li-SeS2all-solid-state batteries (ASSB). Herein, transmission electron microscopy (TEM) is used to reveal the electrochemistry of a Li-SeS2battery. It is discovered that, without the Polyethylene glycol (PEG), amorphous SeS2in Li-SeS2ASSB change into crystalline selenium and a small amount of sulfur. The continuous loss of sulfur from the active material may be related to the failure of the cell at 15 cycles and the severe instability of the Coulombic efficiency. It was found that the PEG coating selenium disulfide graphene composite (PEG@rGO-SeS2) cathode maintained a specific capacity of 258 mAh g−1and a stable Coulombic efficiency of about 97% after 50 cycles. TEM analysis shows that the charging product remains as a granular amorphous selenium disulfide with a constant Se/S ratio during cycling. The PEG-protected selenium disulfide can effectively limit the loss of elemental sulfur and regulate the reaction mechanism of the Li-SeS2batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yiding Li,Qiang Zhang,Simin Shen,Siqi Wang,Liangliang Shi,Dequan Liu,Yujun Fu,Deyan He
Effectively limiting the shuttle effect is the key to improving the electrochemical performance of Li-S batteries. Here, the synthesis of WO 3 -WS 2 heterostructures is reported by electrospinning and in situ sulfurization strategies, combining the initial WO 3 nanoparticles with the sulfurization product WS 2 . It was found that the obtained bifunctional heterostructures enhance the electrolyte wettability, optimize intermediate regulation performance, accelerate Li + /e − diffusion, and thus exhibit excellent electrochemical characteristics in Li-S batteries. Through experiments and density functional theory (DFT) calculations, the WO 3 -WS 2 heterostructures were considered as a coupled creative solution with multiple advantages. Different from the batteries using single-component or single-configuration catalyst, the prepared Li-S batteries with the WO 3 -WS 2 heterostructures exhibited synergistic enhanced electrochemical performance and high-temperature crushing resistance. Even under severe conditions, including high sulfur loading (10.3 mg cm −2 ), lean electrolyte (5.8 μL mg −1 ), high current density (7.0 A g −1 ), extended cycling (1600 cycles), and high temperature (90 °C), the representative battery exhibited stable cycling performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xinjian Li,Yanhui Su,Yong Ma,Le Wei,Ying He,Yuting Gu,Shiwei Mei,Qiaoqiao Mu,ChengYuan Peng,Yang Peng,Zhao Deng
Photo-assisted charge/discharge has witnessed marked success in Li-O 2 batteries (LOBs) to overcome the sluggish kinetics of triphasic reactions at the cathode, but challenges remain to develop high-efficiency but low-cost photocathode catalysts. Herein, a photoactive electron mediator is applied, for the first time, as bifunctional photocathode catalyst in solar-assisted LOBs. The facilely synthesized tris(2,2-bipyridine) cobalt(II) complex (Co-bpy) manifests good electrocatalytic activity in dark and high photoactivity under illumination, concertedly affording an superior charge/discharge voltage gap of 0.12 V and round-trip efficiency of 97%. Moreover, a significantly enhanced charge/discharge reversibility was attained under illumination and attributed to the light-induced amorphization of Li 2 O 2 that further extends the cycle life. A two-circuit model is proposed to rationalize the better reduction of charge/discharge polarization at lower operating current density. This work not only extends the family of photocathode catalysts to small-molecule complexes, but also offers new insights into the mechanism of photoenergy storage in LOBs.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Shan Yin,Xin He,Xiande Zhang,Yan Hao,Kaipeng Wu,Yun Zhang
Iron oxide/graphene hybrids are outstanding electrodes with high specific capacity for secondary batteries. However, in practice there still remains challenges in alleviating the poor electrical conductivity and significant volume changes of FeO x during the lithiation/delithiation process. Herein, we describe the discovery of fabricating graphene-wrapped Fe 3 O 4 (3D-rGO/Fe 3 O 4 ) via a solution-based self-assembly process. During which, GO/Fe 3 O 4 /Na 2 SO 4 precursor was first formed by the corrosion reaction of metallic Fe in GO aqueous solution and antisolvent self-assembly, which was then quenched into water to dissolve the Na 2 SO 4 template and meanwhile enable the GO to shrink and encapsulate the Fe 3 O 4 nanoparticles spontaneously, followed by a final thermal reduction. Fe 3 O 4 nanoparticles, with a diameter of tens of nanometers, are homogeneously enwrapped into rGO framework, guaranteeing the “plane-to-plane” interconnection. The obtained 3D-rGO/Fe 3 O 4 demonstrates unprecedented Li-storage behaviors when utilized as Li-ion battery anode. Furthermore, quantitative kinetic analysis revealed that both capacitance and diffusion mechanisms account for Li-storage behavior. This contribution not only presents a ultrahigh-performance Li-storage electrode but also shows a novel methodology to design and construct other graghene-based metallic compounds for various applications.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Junqin Xie,Kangning Liu,Sha Fu,Xian-Xiang Zeng,Congshan Zhou,Tong-Tong Zuo,Xiongwei Wu
Among all energy storage systems, lithium metal batteries (LMBs) show great advantages in terms of energy density. Nevertheless, the challenges of lithium metal anodes, namely, dendrite formation and low Coulombic efficiency, hinder the practical application of LMBs. In this work, we used the ZnO/carbon shell/carbon cloth as a host for the lithium metal anode. The introduction of ZnO sites reduces the nucleation barrier of lithium deposition, and the existence of a 3D current collector alleviates the volume change during lithium plating/stripping. In addition, the combination of ZnO/C and 3D carbon cloth decreases the local current density and contributes to uniform lithium plating/stripping. The half cells assembled with modified carbon cloth electrodes cycle for more than 125 cycles with a high Coulombic efficiency of 99.34%, even under a high areal capacity of 6 mA h cm–2. By and large, our work provides a simple and effective strategy to modify the current collector for high Li-content anodes.
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Shuai Wang,Liuyuan Zhu,Rujie Yang,Minliang Li,Fangfang Dai,Shiqi Sheng,Liang Chen,Shanshan Liang
Lithium extraction from brine or seawater using membrane technology has attracted extensive attention in recent years. Graphene oxide (GO), as one of the two-dimensional materials, has been proven as a competitive candidate for membranes. However, the GO membranes still suffer challenges for ion sieving due to the swelling in the aqueous solution. In this work, a GO–PEI membrane with positively charged channels was constructed by polyelectrolyte polyethyleneimine (PEI) molecular chain-grafted GO nanosheets. The GO–PEI membrane showed a high selectivity of 22.2 for Li+/Mg2+, together with a competitive Li+ permeation rate of 0.09 mol m–2 h–1 in a binary permeation test. In addition, the membrane showed excellent stability during the separation process. The enhanced Li+/Mg2+ separation performance of the GO–PEI membrane could be mainly attributed to the synergistic effect of size sieving and electrostatic repulsion. We further systematically studied the influence of various variables, such as PEI molecular weight, PEI content, membrane thickness, and ion concentration, on separation performance. This work deepens the understanding of membrane ion selectivity from multiple perspectives and puts forward a strategy to design a two-dimensional membrane structure from microscopic materials.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Hengyu Li,Yunhao Li,Meng Li,Yan Jin,Guodong Kang,Yiming Cao
Extraction of lithium from salt lakes is an important route for lithium sources. Due to the unique structure and separation mechanism, i.e., size exclusion and Donnan effect, nanofiltration (NF) is considered as a promising way to separate magnesium (Mg 2+ ) and lithium (Li + ) ions. However, the Mg 2+ /Li + separation factor of NF membrane fabricated by traditional interfacial polymerization (IP) is usually dissatisfactory. Here, a swelling-embedding-shrinking strategy was proposed to modify polyethyleneimine (PEI)/trimesoyl chloride (TMC) NF membranes using diethylenetriamine (DETA) to improve the performance in Mg 2+ /Li + separation. The pristine PEI/TMC NF membrane was swollen with methanol to increase the polyamide chain spacing followed by embedding electropositive DETA as a modifier. The charge properties and pore structure of the active layer could be regulated by optimizing the modification conditions. Within comparison to the pristine membrane (TFC-0), the pure water flux of modified NF membrane (TFC-3) increased by 63.6% because of the rougher surface and the larger pore size. Meanwhile, the embedding of electropositive DETA reduced the electronegative property of membrane surface. In consequence, TFC-3 membrane exhibited higher rejection of MgCl 2 (93.9% against 88.4%) and lower rejection of LiCl (31.0% against 32.1%), thus showing a twofold improvement in Mg 2+ /Li + separation factor ( S Li, Mg = 11.38 against 5.87). The swelling-embedding-shrinking strategy in this article provided a good reference for the modification of NF membranes in the separation of multivalent and monovalent ions.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2018
·
IF 2.88
Yichen Jin,Tao Pang
Upconversion luminescence and optical temperature sensing properties of Yb 3+ /Er 3+ /Li + tri-doped ZnMoO 4 phosphors were investigated. It has been demonstrated that Li + doping affected not only the local symmetry of Yb 3+ and Er 3+ but also the distribution of them in the host lattice. As a result, the significantly improved green upconversion luminescence was obtained when excited at 980 nm. The pumping power dependent photo-thermal behavior was used to evaluate the reliability of upconversion temperature sensing. An accurate temperature scale was established by eliminating the impact of thermal effect, and the sensing ability was evaluated via a comparison with the results reported in literatures.
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Nanoscale Research Letters
·
2018
·Vol. 13
·期 1
·1-8
·
IF 3.125
Wang Zhifeng,Zhang Xiaomin,Zhao Yan,Li Meixian,Tan Taizhe,Tan Minghui,Zhao Zeren,Ke Chengzhi,Qin Chunling,Chen Zhihong,Wang Yichao
Due to the severe volume expansion and poor cycle stability, transition metal oxide anode is still not meeting the commercial utilization. We herein demonstrate the synthetic method of core-shell pomegranate-shaped Fe 2 O 3 /C nano-composite via one-step hydrothermal process for the first time. The electrochemical performances were measured as anode material for Li-ion batteries. It exhibits excellent cycling performance, which sustains 705 mAh g −1 reversible capacities after 100 cycles at 100 mA g −1 . The anodes also showed good rate stability with discharge capacities of 480 mAh g −1 when cycling at a rate of 2000 mA g −1 . The excellent Li storage properties can be attributed to the unique core-shell pomegranate structure, which can not only ensure good electrical conductivity for active Fe 2 O 3 , but also accommodate huge volume change during cycles as well as facilitate the fast diffusion of Li ion.
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Energy Storage Materials
·
2019
·
IF 0
Zhikang Liu,Jing Huang,Bin Liu,Dong Fang,Tao Wang,Quanling Yang,Lijie Dong,Guo-Hua Hu,Chuanxi Xiong
For lithium ion batteries , fast charging technology is one of the most important research topics in current society. Transition metal oxides show broad application prospects due to their obvious pseudocapacitive effect. We choose Fe 3 O 4 as the template to design the enhanced pseudocapacitance effect considering of its high theoretical specific capacity and superior structural adjustability . The nanohybrid materials with multiple ionically bonded interfaces accumulated the giant pseudocapacitive effect to obtain superior specific capacity. As a result, the nanohybrid shows a ranking specific capacity over 800 mAh g −1 at 1 A g −1 for 1000 cycles as well as excellent rate capabilities. The existence of interfacial pseudocapacitive effect was confirmed by the kinetic analysis calculating from CV curves. Furthermore, the computation simulation based on the density functional theory (DFT) highly corresponded with our viewpoint about interfacial lithium storage. Our findings pave a novel path for designing novel electrode materials and could further advance the development of lithium-ion batteries with long-term stability and superhigh capacity.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2018
·Vol. 165
·期 5
·A757
·
IF 3.662
Shijia Mu,Ding Zhu,Wei Liu,Shengrong Cai,Kaifang Zhang,Yungui Chen
Due to the sluggish oxygen reduction reaction (ORR) process of an O2 cathode, the power delivery of aprotic Li-O2 batteries (A-LOBs) is widely considered to be very poor. However, this work demonstrates the transient high-power output of A-LOBs based on the capacitive feature of the O2 cathode, including the intrinsic capacitance of cathode material and the ORR pseudocapacitance of the absorbed O2 on the cathode surface, by using graphene with high specific surface area. The O2 cathode delivers a high specific power of 12 026 W kggraphene−1 while also providing a large specific energy of 1216 Wh kggraphene−1. Pulse-discharge tests show that A-LOBs can achieve the transient high power output at high current via the "capacitor-type", while maintaining the high energy output at low current due to the "battery-type" (ORR). This work indicates that A-LOBs can deliver both high energy density and high transient power, which may be an appeal for the next-generation electric vehicles.
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