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ACS Sustainable Chemistry & Engineering · 2017 · IF 5.951

Highly Active IrOx Nanoparticles/Black Si Electrode for Efficient Water Splitting with Conformal TiO2 Interface Engineering

Miao Kan,Xufang Qian,Taiyang Zhang,Dongting Yue,Yixin Zhao

Here we report a highly active electrochemical water splitting electrode fabricated from colloidal IrOx nanoparticles and nanoporous Si stabilized by conformal TiO2. The colloidal amorphous IrOx nanoparticles are highly active for oxygen evolution reaction. However, their application for water splitting has a dilemma that the traditional annealing process could lead to low activities but the nanoparticles based electrode without annealing usually exhibited low stability. This nanostructured water splitting electrode exhibited both the high activities as the colloidal IrOx nanoparticles and comparable stability as a traditional thermal annealing fabricated electrode. The impedance study revealed that conformal TiO2 significantly inhibits the interface oxidation and maintains the high activity of colloidal IrOx nanoparticles catalysts. The conformal TiO2 interface engineering combined with nanocatalysts would be a promising strategy to achieve balanced activities and stability for water splitting.

CAS / MDL: 16920-56-2
研究领域: 材料科学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Lithium Carbide Prelithiation Agent-Coated Separator Facilitates Compact Expansion of Silicon Electrode

Liewu Li,Xiaoyu Gong,Chufang Chen,Zhencheng Huang,Weibin Chen,Qianqian Jiang,Jing Chen,Jionghui Wang,Liqing He,Tengfei Cheng,Hongbin Wang,Shenghua Ye,Xuming Yang,Xiangzhong Ren,Xiaoping Ouyang,Jianhong Liu,Qianling Zhang,Jiangtao Hu

The high specific capacity and safety nature of silicon (Si) anode has garnered significant attention and investment for its application in high-energy-density lithium-ion batteries (LIBs). However, the Si anode exhibits low initial Coulombic Efficiency (CE) and compromised cycle stability due to interfacial side reactions and the volume expansion of Si particles. Here, a straightforward strategy is proposed to prelithiate Si anodes and enhance the cycle stability by utilizing a lithium carbide (LiC 6 ) coated separator. By incorporating a LiC 6 prelithiation agent-coated PP/PE separator (PP/PE@LiC 6 ), a robust interaction between PP/PE@LiC 6 and Si anode forms during cycling, which significantly reduces subsequent contact between the electrolyte and Si particles, thereby minimizing excessive electrolyte decomposition during cycling, and facilitates the compact expansion of the Si electrode. In Si|PP/PE@LiC 6 |Li cell, the initial CE reaches 108.51%, showcasing enhanced electrochemical stability (77.93% after 100 cycles). Moreover, the Si|PP/PE@LiC 6 |LiFePO 4 cell also exhibits exceptional initial CE of ≈93.02% and improved electrochemical stability (100.94% after 100 cycles at 0.33C). This study introduces a secure and readily attainable prelithiation method for industrial applications of high-energy density Si-based batteries.

CAS / MDL: 9005-38-3
研究领域: 材料科学 · 能源技术
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Energy & Environmental Science · 2011 ·Vol. 4 ·期 3 ·1037-1042 · IF 9.488

Facile fabrication of a nanoporous silicon electrode with superior stability for lithium ion batteries

Chunyu Du,Cuihua Gao,Geping Yin,Meng Chen,Long Wang

In this paper, we demonstrate that a novel silicon electrode with a large amount of nanopores can be fabricated by an in-situ thermal generating approach using triethanolamine as a sacrificing template. The fabrication process is simple, green, low cost, and easy to be scaled up. This electrode achieves high reversible capacities (2500 mAh g−1) with excellent cycling stability (∼90% capacity retention after 100 charge–discharge cycles), showing great potential as a high-performance anode for lithium-ion batteries. It is revealed that the high void volume with pore size of <200 nm can both enlarge the interface between active silicon particles and the electrolyte, and accommodate the severe volume change of silicon, thus leading to remarkably improved reversible capacity and cycling stability. The design concept and the fabrication approach used in the nanoporous silicon electrode may also be extended to other electrodes for electrochemical applications.

CAS / MDL: 102-71-6
研究领域: 材料科学 · 能源存储
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Biomimetics-Inspired Architecture Enables the Strength–Toughness of Ultrahigh-Loading Silicon Electrode

Baoyu Sun,Shuai Wang,Shijie Zhou,Jiangning Liu,Caiwang Mao,Kefang Liu,Hao Fan,Jingying Xie,Jiangxuan Song

Silicon (Si), as one of the most promising anode candidates, is expected to improve the energy density of Li−ion batteries due to its high specific capacity (≈4200 mAh g −1 ). However, the cyclic performance of Si anode is unsatisfactory for practical usage due to its inadequate toughness when exceeding the mass loading beyond 2 mg cm −2 , which triggers unceasing electrode breakage. Here, a biomimetic Si electrode is created by interconnecting vertically aligned graphene oxide sheets with conductive carbon nanotubes (AGO−Si/C). Unlike reported structures, the AGO−Si/C electrode exhibits superior interlaminar toughness owing to its unique crumpling architecture of reversible interlayer slipping. The elastic structure releases the accumulative lithiation stress of Si nanoparticles to address the degraded inactivation. Thus, the AGO−Si/C electrode shows long−lived cycles by toughening the structure, allowing the fabrication of very thick loading (4.1 mg cm −2 ) with an impressive areal capacity of 10.0 mAh cm −2 . This discovery offers an easily scalable method for graphite/Si anode with high areal capacity that exceeds the commercial−level of 5 mAh cm −2 .

CAS / MDL: 9004-32-4 308068-56-6
研究领域: 材料科学 · 能源存储 · 纳米技术
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Suppression of hydrogen evolution reaction in CO2 reduction by functionalizing Ag-decorated Si electrode with phthalocyanine

Weiting Yu,Zhe Yang,Rendan Zhu,Mengzhi Lu,Tingjiang Lu,Yan Yu,Shuang Song

The photo-assisted electrochemical CO 2 reduction reaction (CO 2 RR) toward CO stands as a highly promising pathway for addressing environmental challenges and produces valuable chemicals. In this study, a novel pl-Si/Ag/Pc electrode was developed with the surface enveloped by an amorphous phthalocyanine overlayer. The pl-Si/Ag/Pc electrode has gained recognition as a catalyst of exceptional quality, displaying superior activity, selectivity toward CO, and stability. A synergistic mechanism has been revealed from experimental results that Ag served as active centers for CO 2 RR, Pc facilitated CO 2 adsorption and suppressed the competing HER reaction. Functionalizing the surface of electrode with Pc enhanced the CO selectivity (FE CO at 90.8 % under −1.5 V vs RHE) during the CO 2 RR process and reduced the cost in following product separation procedures. This study presents an uncomplicated yet effective approach for formulating durable and discerning electrocatalysts dedicated to the utilization of CO 2 .

CAS / MDL: 7664-39-3 574-93-6
研究领域: 材料科学 · 环境科学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

In situ preparation of an advanced binder with a triple-crosslinking network for high-performance silicon anodes

Yu Qin,Haowen Jiang,Kanghui Cai,Zhenzhen Liu,Jing Su,Xiaoyan Lv,Yanxuan Wen

Silicon serves as a promising anode material for lithium-ion batteries. However, silicon suffers from low initial coulombic efficiency (ICE) and poor cycling performance due to large volume change, lithium consumption, the formation of a solid-electrolyte interphase (SEI), and low conductivity. To improve the performance of silicon anodes, this work proposed a new strategy for the design of silicon electrode binders based on β -cyclodextrin, citric acid, and sodium alginate, where a binder with a chemical/ionic/hydrogen-bonded triple-crosslinked network was constructed in situ during electrode preparation. The binder with a triple-crosslinked network provided the silicon electrode with a high binding strength, excellent ion/electron permeation network, and robust interfacial protective layer, providing better tolerate volume changes, and inhibiting the interfacial side reactions and the formation of solid-electrolyte interphase, as well as accelerating Li + diffusion during the charge/discharge processes. The prepared silicon electrodes had a higher ICE (92.8%), better cycling stability (1429 mAh/g after 400 cycles at 0.5 C), and superior rate performance (1274 mAh/g at 4 C). This work may guide the design of high-performance binders for silicon electrodes.

CAS / MDL: 7440-70-2
研究领域: 材料科学 · 能源存储
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IONICS · 2023 ·Vol. 29 ·期 6 ·2241-2248 · IF 2.8

Dual function high efficiency silicon electrode prelithiation strategy

Deng Rongfeng,Wang Zhilong,Chen Kanghua

The Si anode holds the most potential among anode materials, however, its low initial coulombic efficiency has been a serious impediment to commercial progress. In this study, we immersed Si electrode in the prelithiation reagent of lithium-biphenyl(Li-Bp)/2-methyltetrahydrofuran(2-Me-THF) for 5 min, resulting in an initial coulomb efficiency was increased to 135%. The full cell assembled with LiFePO 4 has a coulomb efficiency of 89.1% for the first turn and the capacity retention rate of 87.2% after 100 cycles. Prelithiation reagent after drying can form a protective layer on the surface of the Si electrode, and the prelithiated Si electrode can stably exist for more than 9 h at the dew point (DP) of -25 ℃, which provides a strategy for industrial production.

研究领域: 材料科学 · 电化学 · 能源技术
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Constructing a Stable Integrated Silicon Electrode with Efficient Lithium Storage Performance through Multidimensional Structural Design

Fenghui Li,Hao Wu,Hong Wen,Chen Wang,Chaoqi Shen,Liwei Su,Sheng Liu,Yifan Chen,Lianbang Wang

Silicon (Si) stands out as a highly promising anode material for next-generation lithium-ion batteries. However, its low intrinsic conductivity and the severe volume changes during the lithiation/delithiation process adversely affect cycling stability and hinder commercial viability. Rational design of electrode architecture to enhance charge transfer and optimize stress distribution of Si is a transformative way to enhance cycling stability, which still remains a great challenge. In this work, we fabricated a stable integrated Si electrode by combining two-dimensional graphene sheets (G), one-dimensional Si nanowires (SiNW), and carbon nanotubes (CNT) through the cyclization process of polyacrylonitrile (PAN). The integrated electrode features a G/SiNW framework enveloped by a conformal coating consisting of cyclized PAN (cPAN) and CNT. This configuration establishes interconnected electron and lithium-ion transport channels, coupled with a rigid-flexible encapsulated coating, ensuring both high conductivity and resistance against the substantial volume changes in the electrode. The unique multidimensional structural design enhances the rate performance, cyclability, and structural stability of the integrated electrode, yielding a gravimetric capacity (based on the total mass of the electrode) of 650 mAh g–1 after 1000 cycles at 3.0 A g–1. When paired with a commercial LiNi0.5Co0.2Mn0.3O2 cathode, the resulting full cell retains 84.8% of its capacity after 160 cycles at 2.0 C and achieves an impressive energy density of 435 Wh kg–1 at 0.5 C, indicating significant potential for practical applications. This study offers valuable insights into comprehensive electrode structure design at the electrode level for Si-based materials.

研究领域: 材料科学 · 能源技术
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ACS Applied Energy Materials · 2022 · IF 6.959

Self-Healing Silicon Anode via the Addition of GaInSn-Encapsulated Microcapsules

Jian Yang,Junfeng Li,Ziyu Yang,Jiarun Liu,Yong Xiang,Fang Wu

Silicon materials as promising anodes for lithium-ion batteries own a high specific capacity and a low discharge potential, while their application is restricted by their huge volumetric expansion and poor conductivity. In this study, a self-healing GaInSn–MS/Si hybrid electrode using an additive of microencapsulated gallium- liquid metal (GaInSn) with high electrical conductivity and mobility (LM microcapsule) was fabricated via an aqueous casting process. With the added LM microcapsule in the GaInSn–MS/Si hybrid electrode, the dispersed GaInSn could not only avoid its oxidation into a solid-state gallium oxide with decreased conductivity but also make it easy for uniform dispersion and quick fluidity. Consequently, the constructed self-healing GaInSn–MS/Si anode does not require manual splicing when the anode forms cracks, realizing a spontaneous self-healing performance, and the GaInSn–MS/Si hybrid electrode displays superior cycle stability and structural integrity, which retains a capacity of 806.7 mAh g–1 after 100 cycles at 2.1 A g–1. The constructed self-healing Si electrode structure design via LM microcapsule additives would provide a simple synthesis strategy for manufacturing advanced Si electrodes.

研究领域: 材料科学 · 能源存储
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Small · 2023 · IF 13.3

In Situ Constructing of Rigid-Soft Coupling Solid–Electrolyte Interphase on Silicon Electrode toward High-Performance Lithium Ion Batteries

Zhenxiao Li,Tingjie Hu,Juan Yang,Xia Yu,Fanyun Su,Qixian Bai,Yayun Ma,Yanchun Song,Ming Jia,Xiangyang Zhou,Jingjing Tang

The application of Si anodes is hindered by some critical issues such as large volume changes of bare Si and fragile solid–electrolyte interface (SEI), resulting in low coulombic efficiency and rapid capacity decay. Herein, a multifunctional SEI film with high content of LiF is in situ constructed via the surface grafting of carbon–fluorine functionalized groups on silicon nanoparticles (SiNPs) during cycling. Mechanical study demonstrates that the incorporation of LiF with high modulus and unbroken carbon–fluorine groups with highly elastic guarantee the rigid-soft coupling SEI film on Si electrode. Furthermore, it is demonstrated that the rigid-soft coupling SEI film can effectively accommodate the volume expansion of Si nanoparticles during lithiation process, with the electrode expanding rate of only 114.16% after 100 cycles (263.87% for bare Si without surface modification). Afterward, with the aid of well-designed rigid-soft coupling SEI, the initial Coulomb efficiency of 89.8% is achieved, showing a reversible capacity of 1477 mAh g −1 after 200 cycles at 1.2 A g −1 . This work provides a simple and efficient solution that can potentially facilitate the practical application of Si anodes.

研究领域: 材料科学 · 能源存储
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Materials Today Chemistry · 2025 · IF 6.7

A polymeric three-dimensional adhesive network for a high initial Coulombic efficiency silicon anode

Siying Li,Zhengwei Wan,Zhuoying Wu,Dan Qian,Kun Wang,Xingyu Sun,Chuhan Zhou,Min Ling,Chengdu Liang

The inevitable side reactions during the cycling of silicon electrodes lead to the low initial Coulombic efficiencies. Binders play a vital role as a crucial component of electrodes in enhancing the initial Coulombic efficiencies in the cycling process. The water-soluble grafted CMC/PAA binder can form a three-dimensional adhesion network to cover Si particles. A large proportion of hydroxyl and carboxyl groups in the binder can generate a strong interaction with Si–OH bond to attach to the surface of Si particles. The dynamic cross-linked network helps to maintain the structural integrity of the electrodes while simultaneously enhancing the kinetics of lithium ion transportation. The Si@CMC/PAA electrode achieves a high initial Coulombic efficiency of 90.61 %, stable cycling performance and high rate capacity of 880 mAh·g −1 at 2 C.

研究领域: 材料科学 · 能源存储
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ChemElectroChem · 2020 ·Vol. 7 ·期 17 ·3623-3631 · IF 4.154

Effects of Non-Ionic Surfactants on the Rheological, Electrical and Electrochemical Properties of Highly Loaded Silicon Suspension Electrodes for Semi-Solid Flow Batteries

Yuanyuan Wu,Defu Cao,Xiaojie Bai,Hao Liu,Huiying Hao,Jie Xing,Jingjing Dong,Libing Liao

Graphical Beyond the sticking point : The microstructure of the electrode paste is regulated. The conductivity and viscosity of the semi-solid lithium-ion liquid flow battery electrode paste are restricted by adding non-ionic surfactant. Low viscosity and good electrochemical cycling stability are obtained by adding a certain amount of nonionic surfactant. Silicon-based suspension electrodes represent one of the most promising candidates as negolyte to replace lithium metal for high energy density semi-solid flow batteries (SSFBs). Nevertheless, it remains a critical challenge to obtain Si-based negolyte with highly loaded active material and low viscosity, which are essential for its practical application. Here, the effects of two common non-ionic surfactants – polyvinylpyrrolidone (PVP) and Triton X-100 (TX-100) – on rheological, electrical and electrochemical properties of highly loaded Si (30 vol % Si) negolyte were systemically studied. It was found that the viscosity is effectively decreased by introducing steric and/or depletion interactions when adding a certain amount of non-ionic surfactant polyvinylpyrrolidone (PVP), while good electrochemical performance of the Si negolyte was maintained. An optimal Si negolyte (adding 0.4 wt % PVP) with a low viscosity of 240 mPa s at a shear rate of 40 s −1 (i. e. about five times lower than the PVP-free suspension) exhibits a high reversible capacity (ca. 1300 mAh/g) and stable cycling performance (>100 cycles) with a high coulombic efficiency (>98 %). In contrast, TX-100 can react with lithium salt in the electrolyte and is not suitable to decrease the viscosity of Si negolyte. The highly loaded Si negolyte with low viscosity reported in the present work is promising for practical high energy density lithium-free SSFBs.

研究领域: 材料科学 · 电化学
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