Modulating e orbitals through ligand engineering to boost the electrocatalytic activity of NiSe for advanced lithium-sulfur batteries

Yan, Tianran; Feng, Jie; Zhang, Pan; Zhao, Gang; Wang, Lei; Cheng, Yuan; Cheng, Chen; Li, Youyong; Zhang, Liang

doi:10.1016/j.jechem.2022.07.025

Cited by 25 publications

(11 citation statements)

References 52 publications

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“…Notably, an inflection at the final stage around 1.8 V emerges, which may result from the inadequate infiltration of the cathode by electrolyte. 44 The battery with a D-MVO separator still maintains the conspicuous plateaus even at a high current rate of 4C with reduced overpotentials (Figure 4d), indicative of a kinetically favorable process regulated by D-MVO, as in sharp contrast to that of MVO and pristine separators (Figure S5). Long-term cycling performance was also evaluated at a current rate of 1C.…”

Section: ■ Results and Discussionmentioning

confidence: 97%

“…In Figure c, two discharge plateaus at about 2.3 and 2.1 V can be observed, which correspond to the two-step conversions of sulfur, respectively. Notably, an inflection at the final stage around 1.8 V emerges, which may result from the inadequate infiltration of the cathode by electrolyte . The battery with a D-MVO separator still maintains the conspicuous plateaus even at a high current rate of 4C with reduced overpotentials (Figure d), indicative of a kinetically favorable process regulated by D-MVO, as in sharp contrast to that of MVO and pristine separators (Figure S5).…”

Section: Results and Discussionmentioning

confidence: 97%

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Surface Defect Engineering of a Bimetallic Oxide Precatalyst Enables Kinetics-Enhanced Lithium–Sulfur Batteries

Zhao

Kao

et al. 2022

ACS Appl. Mater. Interfaces

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Developing efficient electrocatalysts to accelerate the sluggish conversion of lithium polysulfides (LiPSs) is of paramount importance for improving the performances of lithium–sulfur (Li–S) batteries. However, a consensus has not yet been reached on the in situ evolution of the electrocatalysts as well as the real catalytic active sites. Herein, defective MnV2O6 (D-MVO) is designed as a precatalyst toward LiPSs’ adsorption and conversion. We reveal that the introduction of surface V defects can effectively accelerate the in situ sulfurization of D-MVO during the electrochemical cycling process, which acts as the real electrocatalyst for LiPSs’ retention and catalysis. The in situ-sulfurized D-MVO demonstrates much higher electrocatalytic activity than the defect-free MVO toward LiPSs’ redox conversion. With these merits, the Li–S batteries with D-MVO separators achieve superior long-term cycling performance with a low decay rate of 0.056% per cycle after 1000 cycles at 1C. Even under an elevated sulfur loading of 5.5 mg cm–2, a high areal capacity of 4.21 mAh cm–2 is still retained after 50 cycles at 0.1C. This work deepens the cognition of the dynamic evolution of the electrocatalysts and provides a favorable strategy for designing efficient precatalysts for advanced Li–S batteries using defect engineering.

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Section: ■ Results and Discussionmentioning

confidence: 97%

Section: Results and Discussionmentioning

confidence: 97%

Surface Defect Engineering of a Bimetallic Oxide Precatalyst Enables Kinetics-Enhanced Lithium–Sulfur Batteries

Zhao

Kao

et al. 2022

ACS Appl. Mater. Interfaces

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“…Correspondingly, the anti‐bonding state occupation, orbital energy level, and orientation of the hybrid orbitals determine the strength of hybridization. [ 120,178,211–219 ]…”

Section: Discussionmentioning

confidence: 99%

“…Correspondingly, the antibonding state occupation, orbital energy level, and orientation of the hybrid orbitals determine the strength of hybridization. [120,178,[211][212][213][214][215][216][217][218][219] When we are constantly looking at a bright future with field-assisted electrocatalysts, we cannot help but worry about whether the field effects can be used as a commercial boosting method or only as a supplementary means to experimentally elucidate the mechanisms behind enhanced sulfur redox kinetics in the conceptual stage. Admittedly, a highly interdisciplinary field-assisted electrochemistry, referring to a considerable amount of uncertainty constrained by multi-interferences in physical parameter variability, weakens the universality and inevitability of the corresponding conclusion.…”

Section: Discussionmentioning

confidence: 99%

Field‐assisted electrocatalysts spark sulfur redox kinetics: From fundamentals to applications

Zhang

et al. 2023

Interdisciplinary Materials

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The chief culprit impeding the commercialization of lithium–sulfur (Li–S) batteries is the parasitic shuttle effect and restricted redox kinetics of lithium polysulfides (LiPSs). To circumvent these key stumbling blocks, incorporating electrocatalysts with rational electronic structure modulation into sulfur cathode plays a decisive role in vitalizing the higher electrocatalytic activity to promote sulfur utilization efficiency. Breaking the stereotype of contemporary electrocatalyst design kept on pretreatment, field‐assisted electrocatalysts offer strategic advantages in dynamically controllable electrochemical reactions that might be thorny to regulate in conventional electrochemical processes. However, the highly interdisciplinary field‐assisted electrochemistry puzzles researchers for a fundamental understanding of the ambiguous correlations among electronic structure, surface adsorption properties, and catalytic performance. In this review, the mechanisms, functionality explorations, and advantages of field‐assisted electrocatalysts including electric, magnetic, light, thermal, and strain fields in Li–S batteries have been summarized. By demonstrating pioneering work for customized geometric configuration, energy band engineering, and optimal microenvironment arrangement in response to decreased activation energy and enriched reactant concentration for accelerated sulfur redox kinetics, cutting‐edge insights into the holistic periscope of charge‐spin‐orbital‐lattice interplay between LiPSs and electrocatalysts are scrutinized, which aspires to advance the comprehensive understanding of the complex electrochemistry of Li–S batteries. Finally, future perspectives are provided to inspire innovations capable of defeating existing restrictions.

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“…The sulfur electrochemical reaction process demonstrates low electric and ionic conductivity, which would restrict the sulfur redox kinetics and reduce the corresponding conversion efficiency. 1,[86][87][88] Thus, incorporating electrocatalysts such as metals, 89,90 single-atom metals, [91][92][93] metal carbides, 62,94,95 metal sulfides 96 and composites [97][98][99] with high electric and ionic conductivity into sulfur cathodes promotes interfacial electron/ion transport to expedite the sulfur redox kinetics.…”

Section: Ion/electron Transport-induced Interactionmentioning

confidence: 99%

Dynamic evolution of electrocatalytic materials for Li–S batteries

Cheng

Liu

et al. 2023

Mater. Chem. Front.

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Modulating e orbitals through ligand engineering to boost the electrocatalytic activity of NiSe for advanced lithium-sulfur batteries

Cited by 25 publications

References 52 publications

Surface Defect Engineering of a Bimetallic Oxide Precatalyst Enables Kinetics-Enhanced Lithium–Sulfur Batteries

Surface Defect Engineering of a Bimetallic Oxide Precatalyst Enables Kinetics-Enhanced Lithium–Sulfur Batteries

Field‐assisted electrocatalysts spark sulfur redox kinetics: From fundamentals to applications

Dynamic evolution of electrocatalytic materials for Li–S batteries

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