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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Directing electrochemical reaction mechanism via interfacial control for better sulfur cathode

Lei Hu,Haifeng Xue,Lingli Liu,Sheng Liang,Tao Ding,Ningning Zhou,Lili Wang,Chonghai Deng,Yongsheng Han

The “shuttle effect” in ether electrolyte or nucleophilic reaction in carbonate electrolyte are major obstacles to developing of lithium-sulfur (Li–S) batteries. Superficial sulfur on the outside of microporous carbon host can occur“shuttle effect” in ether electrolyte or nucleophilic reaction in carbonate electrolyte, which may affect the electrochemical reaction mechanism for lithium-sulfur batteries and need to be further clarified. Herein, we rationally designed microporous carbon and non-microporous carbon as the sulfur hosts, and manipulated the distribution of sulfur via interfacial control in cathode material, exhibiting diverse electrochemical behavior in carbonate electrolyte and ether electrolyte. The surface composition of the electrode was confirmed by ex-situ XPS and verified by in-situ XRD, which contributes to demonstrating the definite reaction mechanisms of lithium-sulfur batteries in the different electrolytes. The results show only the sulfur confined in microporous structure is active via “solid–solid” pathway, and the presence of sulfur on the outer surface of the cathode electrode has the negative effect on electrochemical performance in both electrolytes, which should be avoided in the fabrication of carbon/sulfur composites. Based on microporous carbon/sulfur composites, the lithiated Ge-S full cell was proposed and exhibited superior cycling performance and high Coulombic Efficiency.

CAS / MDL: 7704-34-9
研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Multichalcogen-Integrated Cathodes for Novel Lithium-Chalcogenide Batteries in Ether and Ester Electrolytes

Zewen Yang,Dandan Jia,Qing Zhao,Depeng Song,Yuan Zhang,Jing Gao,Xiaolin Sun,Takeo Ohsaka,Futoshi Matsumoto,Qiang Shen,Jianfei Wu

Lithium–sulfur (Li–S) batteries and lithium–selenium (Li–Se) batteries that contain only one single active element have unique advantages and disadvantages. Inspired by ternary lithium batteries, multielement chalcogenide compounds with integrated advantages may improve upon the performance of lithium-chalcogenide batteries at the source. In this work, activated carbon (AC) with an Al2O3@SiO2 heterojunction is used as the carrier, and the performances and mechanisms of elemental substances (X/AC, X = S, Se, and Te) are studied in ether and ester electrolytes as the basis for preparing multielement chalcogenide composites (SST/AC, SST: S–Se–Te compound). In the ester electrolyte system, SST811/AC (where S/Se/Te = 8:1:1, molar ratio) exhibited the best cycling performance, and the capacity remained at 1024.9 mA h g–1 after 300 cycles. The characterization results revealed the mechanisms and sequences of the gradual liquid-phase reactions of SST/AC in ether electrolytes and the direct solid-phase reactions in ester electrolytes. The active elements in SST/AC fully demonstrated their own functions, enabling the effective construction of new lithium-chalcogenide battery systems. This work provides inspiration for the subsequent research of multielement lithium-chalcogenide batteries and paves the way for their application.

CAS / MDL: 7782-49-2 13494-80-9
研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

Multi-layered MXene V4C3Tx as new low-voltage insertion anode for Na-ion battery applications

Krishnan Subramanyan,Sanming Chen,Na Li,Tingting Ma,Yongping Liu,Sundaram Chandrasekaran,Vanchiappan Aravindan

We report an MXene V 4 C 3 T x new low-voltage insertion anode and a comparison of the electrochemical performance with ester and ether-based electrolytes in half– and full–cell configuration with Na 3 V 2 (PO 4 ) 3 @C (NVPC). Though MXene has been explored for Na-ion batteries (SIB), M n +1 X n T x with n  = 3 has been hardly explored. Moreover, the ether-based electrolyte has not been used with any MXenes for electrochemical energy storage , especially in the SIB perspective. The initial irreversibility in the carbonate-based half–cell (V 4 C 3 T x –C) is 128 mAh g −1 more than the tetraglyme–based half–cell (V 4 C 3 T x –T). After 100 cycles, V 4 C 3 T x –T maintains 84 mAh g −1 , while V 4 C 3 T x –C shows only 60 mAh g −1 , which shows the better retention ability in the ether-based system. As for the rate performance, though V 4 C 3 T x –T has a higher capacity in low currents, at higher currents, V 4 C 3 T x –C shows higher values. This showed that the carbonate-based system has diffusion and capacitive-based Na–ion storage, which enabled it to have a high–rate performance. An extensive in–situ impedance study revealed significant formation of the passivation layer in V 4 C 3 T x –C by irreversibly consuming Na–ions, which causes an increased initial Coulombic inefficiency, whereas no such significant SEI layer formation is evident for V 4 C 3 T x –T. Full–cells were assembled with NVPC cathode in tetraglyme and carbonate-based electrolytes. The full–cell with ether electrolyte exhibited enhanced capacity, capacity retention, and rate performance compared to ester-based electrolytes. The full-cell displayed an energy density of ∼66 and ∼74 Wh kg −1 for tetraglyme and ester-based electrolytes, respectively.

研究领域: 材料科学 · 电化学 · 储能技术
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Joule · 2022 · IF 46.048

A high-voltage and stable zinc-air battery enabled by dual-hydrophobic-induced proton shuttle shielding

Yang-feng Cui,Yun-hai Zhu,Jia-yi Du,Yong-lai Zhang,Kai Li,Wan-qiang Liu,Gang Huang,Xin-bo Zhang

Rechargeable zinc-air batteries (ZABs) stand out among next-generation battery technologies due to their high energy density and high safety but suffer from electrochemical irreversibility. Herein, we report a hybrid ZAB with a long lifespan and high working voltage; it uses a neutral anolyte, an acidic catholyte, and a proton-shuttle-shielding dual-hydrophobic membrane to isolate the two electrolytes. The hybrid ZAB operates through the stable electrochemical plating and stripping of zinc (Zn) in a neutral anolyte and a high-voltage O 2 redox reaction in acidic catholyte. The designed proton-shuttle-shielding dual-hydrophobic membrane selectively transports hydrophobic bis(trifluoromethylsulfonyl)imide anions (TFSI − ) and effectively avoids the crossover of protons. As a result, the hybrid ZAB exhibits a high working voltage (1.50 V) and stable operation (up to 2,000.0 h) in ambient air. This strategy not only overcomes the severe irreversibility of conventional ZABs but also promotes development of electrolyte-decoupled systems.

研究领域: 材料科学 · 电化学
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Journal of Energy Chemistry · 2023 · IF 13.1

Regulating solid electrolyte interphases on phosphorus/carbon anodes via localized high-concentration electrolytes for potassium-ion batteries

Wei Xiao,Peiyi Shi,Zhengkui Li,Chong Xie,Jian Qin,Huijuan Yang,Jingjing Wang,Wenbin Li,Jiujun Zhang,Xifei Li

The resourceful and inexpensive red phosphorus has emerged as a promising anode material of potassium-ion batteries (PIBs) for its large theoretical capacities and low redox potentials in the multi-electron alloying/dealloying reactions, yet chronically suffering from the huge volume expansion/shrinkage with a sluggish reaction kinetics and an unsatisfactory interfacial stability against volatile electrolytes. Herein, we systematically developed a series of localized high-concentration electrolytes (LHCE) through diluting high-concentration ether electrolytes with a non-solvating fluorinated ether to regulate the formation/evolution of solid electrolyte interphases (SEI) on phosphorus/carbon (P/C) anodes for PIBs. Benefitting from the improved mechanical strength and structural stability of a robust/uniform SEI thin layer derived from a composition-optimized LHCE featured with a unique solvation structure and a superior K + migration capability, the P/C anode with noticeable pseudocapacitive behaviors could achieve a large reversible capacity of 760 mA h g −1 at 100 mA g −1 , a remarkable capacity retention rate of 92.6% over 200 cycles at 800 mA g −1 , and an exceptional rate capability of 334 mA h g −1 at 8000 mA g −1 . Critically, a suppressed reduction of ether solvents with a preferential decomposition of potassium salts in anion-derived interfacial reactions on P/C anode for LHCE could enable a rational construction of an outer organic-rich and inner inorganic-dominant SEI thin film with remarkable mechanical strength/flexibility to buffer huge volume variations and abundant K + diffusion channels to accelerate reaction kinetics. Additionally, the highly reversible/durable full PIBs coupling P/C anodes with annealed organic cathodes further verified an excellent practical applicability of LHCE. This encouraging work on electrolytes regulating SEI formation/evolution would advance the development of P/C anodes for high-performance PIBs.

研究领域: 电化学 · 材料科学 · 储能技术
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Nanomaterials · 2018 ·Vol. 8 ·期 5 ·335 · IF 3.504

High Performance of Supercapacitor from PEDOT:PSS Electrode and Redox Iodide Ion Electrolyte

Xing Gao,Lei Zu,Xiaomin Cai,Ce Li,Huiqin Lian,Yang Liu,Xiaodong Wang,Xiuguo Cui

Insufficient energy density and poor cyclic stability is still challenge for conductive polymer-based supercapacitor. Herein, high performance electrochemical system has been assembled by combining poly (3,4-ethylenedioxythiophene) (PEDOT):poly (styrene sulfonate) (PSS) redox electrode and potassium iodide redox electrolyte, which provide the maximum specific capacity of 51.3 mAh/g and the retention of specific capacity of 87.6% after 3000 cycles due to the synergic effect through a simultaneous redox reaction both in electrode and electrolyte, as well as the catalytic activity for reduction of triiodide of the PEDOT:PSS.Keywords:PEDOT:PSS;catalysis;redox electrolyte;stability

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 电化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2021 · IF 4.464

The investigation for electrodeposition behavior of lithium metal in a crown ether/propylene carbonate electrolyte

Xianli Huang,Dongmei Zhuang,Zhihui Chen,Hao Gong,Tao Wang,Jianping He,Xiaogang Zhang

It is so far an efficient way for depressing dendrite growth to adjust the electrolyte composition . Therefore, we study the electrochemical behavior of lithium metal electrodeposited in a LiPF 6 -propylene carbonate (PC) electrolyte by adding two kinds of crown ether . The effect of crown ether concentration on the Coulombic efficiency of lithium electrodes has be evaluated, and the electrodeposition behavior of lithium metal on negative electrode has be analyzed by cyclic voltammetric curve, electrodeposition curve and lithium metal deposition morphology. The results show that a certain amount of crown ether (15-crown-5 and 12-crown-4) can preferentially coordinate with lithium ion in the electrolyte and form complex compounds, which reduce the lithium ions concentration in the “hot spot” and level the lithium electrode greatly by inhibiting the preferential growth of lithium dendrite . A uniform and dense nano-columnar lithium layer could be obtained at the current density of 2.0 mA cm −2 when the deposition amount is 1.0 mAh cm −2 , and the concentration of 15-crown-5 and 12-crown-4 ether are 0.3 M and 0.2 M, respectively. Gaussian calculation results show that the lithium-crown complex has a relatively lower lowest unoccupied molecular orbit (LUMO), where electrons could be injected during the charging process, leading to decreased Coulumbic efficiency.

研究领域: 材料科学 · 电化学
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Materials Research Express · 2020 ·Vol. 7 ·期 1 ·016438 · IF 1.929

Characterization of micro-arc oxidation coatings on Ti6Al4V with addition of SiC particle

Yong Lian,Xianyi Dai,Jin Zhang

In the present work, particles of SiC were applied to the micro-arc oxidation (MAO) treatment of Ti6Al4V, characterization of MAO coatings with different SiC particle concentration were evaluated. X-Ray Diffraction (XRD) and Scanning Electron Microscope (SEM) results show that the structure and morphology of MAO ceramic coatings could change with different amounts of SiC in the electrolyte. Both of the number and size of the pores on the ceramic coating surface were decreased, while the layer thickness increased with the increase in SiC particles in the electrolyte. A dense double-layer structure coating composed of a Ti-based layer and a SiC-based layer with a thickness of about 40 μm was prepared. It was shown that the addition of SiC particles participated in the process of micro-arc oxidation and changed the microstructure of MAO coating.

CAS / MDL: 409-21-2
研究领域: 材料科学 · 表面工程
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Hollow nanosphere Fe-Cu-Co trimetallic selenides with high catalytic performances for hydrogen evolution reaction in both acidic and alkaline electrolytes

Yu Ma,Haitao Zhang,Haizhou Zhang,Xinyuan Ren,Xiaochun Ma,Xiaoming Zhou,Yanlu Mu,Jiemei Yu,Taizhong Huang

Developing non-precious metal based catalysts is one of the most feasible ways to accelerate the application of hydrogen production technology by full water electrolysis with low-cost and high efficiency. In this work, hollow nanosphere structured Fe–Cu–Co trimetallic selenide based catalysts were successfully prepared by one-step hydrothermal method. The hollow nano-spherical shell structure was examined by using XRD, Raman, BET, SEM, TEM, XPS, etc. technologies. The catalytic performance for hydrogen evolution reaction (HER) of the catalysts was tested by LSV, Tafel, CV, EIS, i-t , etc . methods. The overpotential of FeCo 0.1 Cu 0.9 Se 2 catalyzed HER was only 191 (alkaline) and 112 mV (acidic) at 10 mA/cm 2 . The corresponding Tafel slope for HER is 180 mV/dec (alkaline) and 110 mV/dec (acidic), respectively. In addition, the FeCo 0.1 Cu 0.9 Se 2 also showed excellent long-time running stability. The current decay after continuous running 12 h in 0.5 M H 2 SO 4 and 0.1 M KOH electrolytes are 0.07 % and 0.271 %, respectively. FeCo 0.1 Cu 0.9 Se 2 catalyst with the hollow nanospherical structure exhibited excellent catalytic activity for HER. Density functional theory calculations show that the introduction of Co and Cu adjusted the electronic structure of FeCo 0.1 Cu 0.9 Se 2 and the special hollow nano-spherical structure provides enough active catalytic sites for HER. The nano-spherical structured multi-metal selenides show great potential to be high performance catalysts for HER in both alkaline and acidic electrolytes.

研究领域: 材料科学 · 电化学 · 纳米催化 · 能源材料 · 物理化学
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Science Bulletin · 2025 · IF 21.1

Anion-mediated electrolyte engineering unlocks high-energy-density and long-cycling sulfur-based batteries at ultra-low N/P ratio

Huangwei Zhang,Yuluo Chen,Xiaoyu Ge,Kai Huang,Jiulin Wang,Jia-Qi Huang,Zhen Li,Yunhui Huang

High energy density and long cycle life are considered to be incompatible in battery design. Lithium metal batteries often have high energy density but poor cycle stability, while graphite (Gr)-based batteries usually have long cycle life but are limited in energy density. Therefore, mixing lithium with Gr as the anode is expected to balance high energy density and long cycle life. Reducing the negative/positive areal capacity (N/P) ratio to less than 1 is the simplest means to achieve a hybrid anode. The battery with sulfurized poly(acrylonitrile) (SPAN) as the cathode and an ultra-low N/P ratio (N/P=0.6) is expected to leverage the significant advantage of its cathode’s energy density far exceeding that of traditional cathodes, while maintaining stable cycling performance. This makes it a highly promising battery system. Through the design of anion-mediated electrolyte engineering, the capacity retention rate of the SPAN||Gr pouch cell at N/P=0.6 after 300 cycles was 92%, and its energy density was increased by 24% compared with that at N/P=1.1, achieving a balance between energy density and cycling stability. This strategy establishes N/P engineering coupled with electrolyte design as a scalable paradigm for next-generation energy-dense batteries.

CAS / MDL: 7704-34-9
研究领域: 储能 · 电化学 · 电池技术 · 材料科学 · 化学工程
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Energy Storage Materials · 2024 · IF 18.9

A high-voltage and low-solvating electrolyte towards promising micro-Si/Ni-rich NMC full cells

Yiye Guo,Mouren Miao,Yun-Xiao Wang,Chunxing Yan,Jin Liu,Yuliang Cao,Hanxi Yang,Xinping Ai,Fu-Sheng Ke

A full cell via pairing high-capacity silicon anode with high-voltage NMC cathode (Li(Ni 0.83 Co 0.12 Mn 0.05 )O 2 ) holds great promise as a high-energy battery system for practical applications. Nevertheless, this potential has been hindered by challenges in terms of the pulverization of Si particles, unstable electrode/electrolyte interface, and severe dissolution of transition metals at high voltage. Herein, we present a novel high-voltage and weakly solvating electrolyte, consisted of lithium bis(fluorosulfonyl)imide in mixed solvent of diethyl carbonate and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether, which effectively enables the remarkable cycling stability of both micron silicon anode (a high reversible capacity of 1667 mAh g −1 after 200 cycles) and Ni-rich cathode (a notable capacity retention of 83% after 140 cycles at an ultrahigh cut-off voltage of 4.9 V). It is revealed that the tailored electrolyte leads to the formation of a robust and reinforced concrete-like solid electrolyte interphase, characterized by a distinctive vertical side-by-side columnar structure comprised of LiF and sulfide on the micro-silicon anode. Meanwhile, a uniform and thin cathode-electrolyte interphase is observed on the surface of NMC particles when cycled in the designed electrolyte. Furthermore, coupled with high-capacity micro-Si and high-voltage NMC, this designed electrolyte endows a remarkable full-cell with high energy density (475 Wh kg −1 ), excellent rate capability, and high-voltage cycling stability. This research contributes a pioneering approach to enabling the utilization of micron-sized silicon anodes and Ni-rich cathodes for next-generation high-energy lithium-ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Materials Chemistry A · 2017 ·Vol. 5 ·期 19 ·9350-9357 · IF 8.867

A high performance lithium–selenium battery using a microporous carbon confined selenium cathode and a compatible electrolyte

Jingjing Zhou,Jun Yang,Zhixin Xu,Tao Zhang,Zhenying Chen,Jiulin Wang

Rechargeable lithium–selenium (Li–Se) batteries are promising electrochemical systems with higher energy density than traditional Li ion batteries. Nevertheless, the dissolution of high-order lithium selenides and the shuttle effect in electrolytes lead to low Se utilization, inferior capacity and poor cycling performance. This study proposes a combination of nanostructured Se cathode materials and compatible carbonate electrolytes for promoting the performance of Li–Se batteries. Se/MC composite nanoparticles (∼35 nm) with a moderate Se content (≈51.4 wt%) were prepared by embedding Se into a metal–organic framework derived microporous carbon. The resulting Se/MC cathode exhibits significantly high rate capability and cycling stability in LiDFOB/EC-DMC-FEC electrolyte. It delivers a capacity of 511 mA h gSe−1 after 1000 cycles at 5C, with an inappreciable capacity decay of 0.012% per cycle. Even at a very high rate of 20C, a large capacity of 569 mA h gSe−1 can be obtained, corresponding to a decrease of only 5.6% compared to that at 0.5C. The impressive high rate performance is attributed to the co-effect of selenium confined in ultra-small microporous carbon particles and excellent compatibility of the electrolyte with both the Li anode and selenium composite cathode.

研究领域: 材料科学 · 电化学
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