Machine-learning-assisted design of a binary descriptor to decipher electronic and structural effects on sulfur reduction kinetics

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(11), P. 1073 - 1086

Published: Oct. 19, 2023

Language: Английский

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Fundamental, application and opportunities of single atom catalysts for Li-S batteries

Energy storage materials, Journal Year: 2022, Volume and Issue: 55, P. 322 - 355

Published: Dec. 5, 2022

Language: Английский

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Dilute Alloying to Implant Activation Centers in Nitride Electrocatalysts for Lithium–Sulfur Batteries

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(7)

Published: Nov. 23, 2022

Dilute alloying is an effective strategy to tune properties of solid catalysts but rarely leveraged in complex reactions beyond small molecule conversion. In this work, dilute dopants are demonstrated serve as activating centers construct multiatom catalytic domains metal nitride electrocatalysts for lithium-sulfur (Li-S) batteries, which the sulfur cathode suffers from sluggish and conversion reactions. With titanium (TiN) a model system, cobalt shown greatly improve reaction kinetics while inducing negligible catalyst reconstruction. Compared pristine TiN, alloy enables onefold increase high rate (2.0 C) capacities Li-S well impressively low cyclic decay 0.17% at loading 4.0 mgS cm-2 . This work opens up new opportunities toward rational design by also enlightens understandings domain-catalyzed energy applications.

Language: Английский

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Transition Metal Compounds Family for Li–S Batteries: The DFT‐Guide for Suppressing Polysulfides Shuttle

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(32)

Published: April 29, 2023

Abstract Lithium–sulfur batteries (LSBs) are considered as one of the best candidates for next generation high‐energy‐density storage devices owing to their superior theoretical energy density, high specific capacity, and sufficient sulfur reservoirs. However, shuttle effect soluble polysulfides sluggish LiPSs redox kinetics restrict further application LSBs. The can be efficiently alleviated conversion accelerated by designing optimal transition metal compounds (TMCs) multifunctional catalyst materials. Herein, recent advances about TMCs in LSBs systematically summarized analyzed. First all, intrinsic structural characteristics relevant on works adsorption energies studies described detail. Second, bonding manners properties analyzed density functional theory (DFT)‐guided calculations, focusing diffusion behavior between LiPSs. Furthermore, mechanism reaction is studied from aspects, thus developing continuous dynamic analysis “adsorption–diffusion–conversion” toward Eventually, this study particularly highlights importance modification engineering provides a forward‐looking overview its prospects introduction previous advanced

Language: Английский

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Nanoreactors Encapsulating Built‐in Electric Field as a “Bridge” for Li–S Batteries: Directional Migration and Rapid Conversion of Polysulfides

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(9)

Published: Dec. 27, 2023

Abstract Lithium–sulfur batteries (Li–S) are recognized as the next generation of secondary due to their satisfactory theoretical specific capacity and energy density. However, a series problems such disordered migration behavior, sluggish redox kinetics, serious shuttle effect lithium polysulfides (LiPSs) greatly limit commercial application. Herein, nanoreactors encapsulate heterostructure guarantee sulfur conversion in hosts where consists FeP with moderate adsorption ability, excellent catalytic active low work function, Fe 3 O 4 strong ability high function. This rational configuration controls direction interface built‐in electric field (BIEF) between catalyst adsorbent, realizing successive “trapping‐directional migration‐conversion” reaction mechanism species. Thanks BIEF bridge connect trapping site site, /FeP@C─S cathode delivers an ultrahigh initial 1402 mAh g −1 at 0.1 C remains more than 450 5 after 350 cycles. Even loading 5.20 mg cm −2 , it displayed 970 . provided effective strategy design high‐performance electrocatalysts for Li–S batteries.

Language: Английский

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Unraveling Polysulfide's Adsorption and Electrocatalytic Conversion on Metal Oxides for Li‐S Batteries

Advanced Science, Journal Year: 2022, Volume and Issue: 10(5)

Published: Dec. 11, 2022

Abstract Lithium sulfur (LiS) batteries possess high theoretical capacity and energy density, holding great promise for next generation electronics electrical vehicles. However, the LiS development is hindered by shuttle effect sluggish conversion kinetics of lithium polysulfides (LiPSs). Designing highly polar materials such as metal oxides (MOs) with moderate adsorption effective catalytic activity essential to overcome above issues. To design efficient MOs catalysts, it critical necessary understand mechanism associated processes LiPSs. most reviews still lack a comprehensive investigation basic always ignore their in‐depth relationship. In this review, systematic analysis toward understanding underlying in chemistry well discussion typical works concerning electrocatalysts are provided. Moreover, improve “adsorption‐diffusion‐conversion” process caused low conductive nature MOs, oxygen vacancies heterostructure engineering elucidated two strategies. The challenges prospects also provided last section. authors hope review will provide instructive guidance catalyst explore practical possibilities commercialization batteries.

Language: Английский

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Regulating the Spin State Configuration in Bimetallic Phosphorus Trisulfides for Promoting Sulfur Redox Kinetics

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(41), P. 22516 - 22526

Published: Oct. 3, 2023

Lithium-sulfur (Li-S) batteries suffer from sluggish kinetics due to the poor conductivity of sulfur cathodes and polysulfide shutting. Current studies on redox catalysis mainly focus adsorption catalytic conversion lithium polysulfides but ignore modulation electronic structure catalysts which involves spin-related charge transfer orbital interactions. In this work, bimetallic phosphorus trisulfides embedded in Prussian blue analogue-derived nitrogen-doped hollow carbon nanocubes (FeCoPS3/NCs) were elaborately synthesized as a host reveal relationship between activity spin state configuration for Li-S batteries. Orbital splitting FeCoPS3 drives transition low-spin high-spin states, generating more unpaired electrons 3d orbit. Specifically, nondegenerate orbitals involved result upshift energy levels, active states. Such tailored increases transfer, influences d-band center, further modifies with potential reaction pathways. Consequently, cell FeCoPS3/NC exhibits an ultralow capacity decay 0.037% per cycle over 1000 cycles. This study proposed general strategy sculpting geometric configurations enable topology regulation battery catalysts.

Language: Английский

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Synergizing Spatial Confinement and Dual‐Metal Catalysis to Boost Sulfur Kinetics in Lithium–Sulfur Batteries

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(44)

Published: July 19, 2023

Sluggish kinetics and parasitic shuttling reactions severely impede lithium-sulfur (Li-S) battery operation; resolving these issues can enhance the capacity retention cyclability of Li-S cells. Therefore, an effective strategy featuring core-shell-structured Co/Ni bimetal-doped metal-organic framework (MOF)/sulfur nanoparticles is reported herein for addressing problems; this approach offers unprecedented spatial confinement abundant catalytic sites by encapsulating sulfur within ordered architecture. The protective shells exhibit long-term stability, ion screening, high lithium-polysulfide adsorption capability, decent multistep conversion. Additionally, delocalized electrons MOF endow cathodes with superior electron/lithium-ion transfer ability. Via multiple physicochemical theoretical analysis, resulting synergistic interactions are proved to significantly promote interfacial charge-transfer kinetics, facilitate conversion dynamics, inhibit shuttling. assembled batteries deliver a stable, highly reversible marginal decay (0.075% per cycle) 400 cycles at 0.2 C, pouch-cell areal 3.8 mAh cm-2 200 under loading, as well remarkably improved performance.

Language: Английский

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Controllable catalysis behavior for high performance lithium sulfur batteries: From kinetics to strategies

EnergyChem, Journal Year: 2022, Volume and Issue: 5(1), P. 100096 - 100096

Published: Nov. 18, 2022

Language: Английский

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Interfacial engineering of transition metal dichalcogenide/carbon heterostructures for electrochemical energy applications

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(22), P. 7802 - 7847

Published: Jan. 1, 2023

This review provides a fundamental understanding of three types interfacial engineering in TMDC/C heterostructures and guidance for designing electrochemical energy applications.

Language: Английский

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