Modulation of Solvation Structure and Electrode Work Function by an Ultrathin Layer of Polymer of Intrinsic Microporosity in Zinc Ion Batteries

Heo, Jiyun; Hwang, Young‐Eun; Doo, Gisu; Jung, Jae Hee; Shin, Kyung‐Jae; Koh, Dong‐Yeun; Kim, Hee‐Tak

doi:10.1002/smll.202201163

Cited by 14 publications

(9 citation statements)

References 53 publications

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“…The lower value of the work function for SiO x /Fe–N–C was beneficial for promoting its electron transfer and catalyze the electrochemical reactions such as the dissociation/formation of amorphous Li x Si. [ 58 , 59 ] Moreover, the electron‐density isosurface of SiO x /Fe–N–C also verified higher ability to transfer electrons compared with SiO x /N–C (Figure 6g,h ). [ 60 , 61 ]…”

Section: Resultsmentioning

confidence: 91%

Embedding Atomically Dispersed Iron Sites in Nitrogen‐Doped Carbon Frameworks‐Wrapped Silicon Suboxide for Superior Lithium Storage

Guo

et al. 2022

Advanced Science

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Silicon suboxide (SiO x ) has attracted widespread interest as Li-ion battery (LIB) anodes. However, its undesirable electronic conductivity and apparent volume effect during cycling impede its practical applications. Herein, sustainable rice husks (RHs)-derived SiO 2 are chosen as a feedstock to design SiO x /iron-nitrogen co-doped carbon (Fe-N-C) materials. Using a facile electrospray-carbonization strategy, SiO x nanoparticles (NPs) are encapsulated in the nitrogen-doped carbon (N-C) frameworks decorating atomically dispersed iron sites. Systematic characterizations including high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) verify the existence of Fe single atoms and typical coordination environment. Benefiting from its structural and compositional merits, the SiO x /Fe-N-C anode delivers significantly improved discharge capacity of 799.1 mAh g −1 , rate capability, and exceptional durability, compared with pure SiO 2 and SiO x /N-C, which has been revealed by the density functional theory (DFT) calculations. Additionally, the electrochemical tests and in situ X-ray diffraction (XRD) analysis reveal the oxidation of Li x Si phase and the storage mechanism. The synthetic strategy is universal for the design and synthesis of metal single atoms/clusters dispersed N-C frameworks encapsulated SiO x NPs. Meanwhile, this work provides impressive insights into developing various LIB anode materials suffering from inferior conductivity and huge volume fluctuations.

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Section: Resultsmentioning

confidence: 91%

Embedding Atomically Dispersed Iron Sites in Nitrogen‐Doped Carbon Frameworks‐Wrapped Silicon Suboxide for Superior Lithium Storage

Guo

et al. 2022

Advanced Science

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“…According to the Gaussian function, there were three states of H 2 O based on wide O–H stretching: (1) a long-range network formed by strong hydrogen bonding coordination [network water (NW), ∼3205 cm –1 ]; (2) distorted hydrogen bonds formed short-range networks with other H 2 O molecules [intermediate water (IW) ∼3410 cm –1 ]; and (3) free H 2 O or poorly connected to their environment [multimer water (MW), ∼3560 cm –1 )]. As shown in Figure e, in Zn(OTF) 2 + 1.14 m HMPA electrolyte, the O–H stretching band was shifted to a high wavenumber, indicating more free H 2 O and weaker coordination of H 2 O with Zn 2+ , which could be attributed to the fact that HMPA can disrupt the connection between H 2 O molecules or with Zn 2+ . , In other words, the introduction of HMPA may replace H 2 O in the solvation sheath of Zn 2+ , which leads to more electron shielding around the Zn atom as well as weakens the hydrogen bond of H 2 O.…”

Section: Resultsmentioning

confidence: 96%

Simultaneously Regulating Solvation Structure and Interphase by Strong Donor Cosolvent for Stable Zn-Metal Batteries

Yang

et al. 2023

J. Phys. Chem. C

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Aqueous Zn-metal battery has been regarded as the most scalable system for grid-scale energy storage, yet challenges arise from arbitrary dendrite growth and Zn anode corrosion, thus restricting its practical application. Herein, a strong donor cosolvent (hexamethylphosphoramide, HMPA) is introduced to enable highly reversible Zn anode. It is demonstrated that the HMPA can preferentially adsorb on the surface of Zn as well as regulate the solvation structure of Zn 2+ by excluding H 2 O from the solvation sheath and thus weakens the activity of H 2 O, which contributes to a dense and uniform SEI layer that enables the homogeneous Zn electrodeposition. Owing to the above advantages, the resultant HMPA-containing electrolyte enables highly reversible Zn plating/stripping for thousands of cycles in Zn||Ti and Zn||Zn cells. Consequently, the cycling stability of Zn|| V 2 O 5 full cells is also significantly improved with a high capacity of 155 mAh g −1 maintained after 1500 cycles.

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“…3c). 6,11,15,[21][22][23][24][25][26]31,41,49,51,[53][54][55][56][57][58][59][60][61][62][63][64][65][66] Note that the SnO 2 /Zn symmetric cell can still maintain a stable long-term life of over 1200 h at 1 mA cm −2 aer cycling at varied current densities (Fig. 3b), which suggests the excellent cycling stability of SnO 2 /Zn anodes.…”

Section: Resultsmentioning

confidence: 99%

Highly reversible, dendrite-free and low-polarization Zn metal anodes enabled by a thin SnO₂layer for aqueous Zn-ion batteries

et al. 2023

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Modulation of Solvation Structure and Electrode Work Function by an Ultrathin Layer of Polymer of Intrinsic Microporosity in Zinc Ion Batteries

Abstract: The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202201163.

Cited by 14 publications

References 53 publications

Embedding Atomically Dispersed Iron Sites in Nitrogen‐Doped Carbon Frameworks‐Wrapped Silicon Suboxide for Superior Lithium Storage

Embedding Atomically Dispersed Iron Sites in Nitrogen‐Doped Carbon Frameworks‐Wrapped Silicon Suboxide for Superior Lithium Storage

Simultaneously Regulating Solvation Structure and Interphase by Strong Donor Cosolvent for Stable Zn-Metal Batteries

Highly reversible, dendrite-free and low-polarization Zn metal anodes enabled by a thin SnO₂layer for aqueous Zn-ion batteries

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Modulation of Solvation Structure and Electrode Work Function by an Ultrathin Layer of Polymer of Intrinsic Microporosity in Zinc Ion Batteries

Abstract: The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202201163.

Cited by 14 publications

References 53 publications

Embedding Atomically Dispersed Iron Sites in Nitrogen‐Doped Carbon Frameworks‐Wrapped Silicon Suboxide for Superior Lithium Storage

Embedding Atomically Dispersed Iron Sites in Nitrogen‐Doped Carbon Frameworks‐Wrapped Silicon Suboxide for Superior Lithium Storage

Simultaneously Regulating Solvation Structure and Interphase by Strong Donor Cosolvent for Stable Zn-Metal Batteries

Highly reversible, dendrite-free and low-polarization Zn metal anodes enabled by a thin SnO2layer for aqueous Zn-ion batteries

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Highly reversible, dendrite-free and low-polarization Zn metal anodes enabled by a thin SnO₂layer for aqueous Zn-ion batteries