The Origin of Strain Effects on Sulfur Redox Electrocatalyst for Lithium Sulfur Batteries

Advanced Energy Materials, Год журнала: 2023, Номер 14(5)

Опубликована: Дек. 8, 2023

Abstract Introducing strain is considered an effective strategy to enhance the catalytic activity of host material in lithium‐sulfur batteries (LSB). However, introduction through chemical methods often inevitably leads changes composition and phase structure, making it difficult truly reveal essence root cause enhancement. In this paper, into MoS 2 introduced a simple heat treatment quenching. Experimental research theoretical analysis show that raises parts antibonding orbitals Mo─S bonds above Fermi level weakens Li─S S─S bonds, resulting tight anchoring accelerating conversion for lithium polysulfides (LiPSs). The cells based on with high delivers initial discharge specific capacity as 1265 mAh g −1 under 0.2 C low average fading 0.041% per cycle during 1500 cycles 1 C. This work deeply reveals origin effects reaction process LSB, providing important design principles references rational high‐performance materials future.

Язык: Английский

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Chlorine bridge bond-enabled binuclear copper complex for electrocatalyzing lithium–sulfur reactions

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Апрель 15, 2024

Abstract Engineering atom-scale sites are crucial to the mitigation of polysulfide shuttle, promotion sulfur redox, and regulation lithium deposition in lithium–sulfur batteries. Herein, a homonuclear copper dual-atom catalyst with proximal distance 3.5 Å is developed for batteries, wherein two adjacent atoms linked by pair symmetrical chlorine bridge bonds. Benefiting from their unique coordination, increased active interface concentration synchronously guide evolutions species. Such delicate design breaks through activity limitation mononuclear metal center represents concept battery realm. Therefore, remarkable areal capacity 7.8 mA h cm −2 achieved under scenario content 60 wt. %, mass loading 7.7 mg electrolyte dosage 4.8 μL −1 .

Язык: Английский

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Ni Single Atoms on Hollow Nanosheet Assembled Carbon Flowers Optimizing Polysulfides Conversion for Li−S Batteries

Advanced Functional Materials, Год журнала: 2023, Номер 33(44)

Опубликована: Авг. 30, 2023

Abstract The sluggish conversion kinetics and shuttling behavior of lithium polysulfides (LiPSs) seriously deteriorate the practical application lithium–sulfur (Li–S) batteries. Herein, Ni single atoms on hollow carbon nanosheet‐assembled flowers (Ni‐NC) are synthesized via a facile pyrolysis‐adsorption process to address these challenges. as‐designed Ni‐NC with enhanced mesoporosity accessible surface area can expose more catalytic sites facilitate electron/ion transfer. These advantages enable Ni‐NC‐modified separator exhibit both confinement‐catalysis ability suppressed LiPSs. Consequently, Li−S battery shows an initial capacity 1167 mAh g −1 low decay ratio (0.033% per cycle) over 700 cycles at 1 C. Even sulfur loading 6.17 mg cm −2 , high areal 5.17 is realized 0.1 C, together superior cycling stability 300 cycles. This work provides catalyst design strategy for development high‐performance

Язык: Английский

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A Review on Engineering Transition Metal Compound Catalysts to Accelerate the Redox Kinetics of Sulfur Cathodes for Lithium–Sulfur Batteries

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Янв. 29, 2024

Abstract Engineering transition metal compounds (TMCs) catalysts with excellent adsorption-catalytic ability has been one of the most effective strategies to accelerate redox kinetics sulfur cathodes. Herein, this review focuses on engineering TMCs by cation doping/anion doping/dual doping, bimetallic/bi-anionic TMCs, and TMCs-based heterostructure composites. It is obvious that introducing cations/anions or constructing can boost capacity regulating electronic structure including energy band, d / p -band center, electron filling, valence state. Moreover, doped/dual-ionic are adjusted inducing ions different electronegativity, ion radius, resulting in redistribution, bonds reconstruction, induced vacancies due interaction changed crystal such as lattice spacing distortion. Different from aforementioned two strategies, heterostructures constructed types Fermi levels, which causes built-in electric field electrons transfer through interface, induces redistribution arranged local atoms regulate structure. Additionally, lacking studies three comprehensively for improving catalytic performance pointed out. believed guide design advanced boosting lithium batteries.

Язык: Английский

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An Electrolyte Engineered Homonuclear Copper Complex as Homogeneous Catalyst for Lithium–Sulfur Batteries

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Июль 17, 2024

Abstract Lithium–sulfur (Li–S) batteries suffer from severe polysulfide shuttle, retarded sulfur conversion kinetics and notorious lithium dendrites, which has curtailed the discharge capacity, cycling lifespan safety. Engineered catalysts act as a feasible strategy to synchronously manipulate evolution behaviors of species. Herein, chlorine bridge‐enabled binuclear copper complex (Cu‐2‐T) is in situ synthesized electrolyte homogeneous catalyst for rationalizing Li–S redox reactions. The well‐designed Cu‐2‐T provides completely active sites sufficient contact homogeneously guiding Li 2 S nucleation/decomposition reactions, stabilizing working interface according synchrotron radiation X‐ray 3D nano‐computed tomography, small angle neutron scattering COMSOL results. Moreover, with content 0.25 wt% approaching saturated concentration further boosts optimization function really operated batteries. Accordingly, capacity retention battery elevated 51.4% 86.3% at 0.2 C, reaches 77.0% 1.0 C over 400 cycles. Furthermore, cathode assistance realizes stable under practical scenarios soft‐packaged pouch cell high loading (6.5 mg cm −2 usage 4.5 µL −1 ).

Язык: Английский

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Sulfur Vacancies and 1T Phase‐Rich MoS₂ Nanosheets as an Artificial Solid Electrolyte Interphase for 400 Wh kg⁻¹ Lithium Metal Batteries

Advanced Materials, Год журнала: 2024, Номер 36(21)

Опубликована: Фев. 13, 2024

Abstract Constructing large‐area artificial solid electrolyte interphase (SEI) to suppress Li dendrites growth and consumption is essential for high‐energy‐density metal batteries (LMBs). Herein, chemically exfoliated ultrathin MoS 2 nanosheets (EMoS ) as an SEI are scalable transfer‐printed on Li‐anode @Li). The EMoS with a large amount of sulfur vacancies 1T phase‐rich acts lithiophilic interfacial ion‐transport skin reduce the nucleation overpotential regulate + flux. With favorable Young's modulus homogeneous continuous layered structure, proposed @Li effectively suppresses repeat breaking/reforming SEI. As result, assembled @Li||LiFePO 4 @Li||LiNi 0.8 Co 0.1 Mn O demonstrate high‐capacity retention 93.5% 92% after 1000 cycles 300 cycles, respectively, at ultrahigh cathode loading 20 mg cm −2 . Ultrasonic transmission technology confirms admirable ability inhibit in practical pouch batteries. Remarkably, Ah‐class battery exhibits energy density 403 Wh kg −1 over 100 low negative/positive capacity ratio 1.8 electrolyte/capacity 2.1 g Ah strategy constructing by vacancies‐rich provides new guidance realize LMBs long cycling stability.

Язык: Английский

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Upcycling Spent Cathode Materials to Bifunctional Catalysts for High‐Stability Lithium–Sulfur Batteries

Advanced Functional Materials, Год журнала: 2024, Номер 34(29)

Опубликована: Апрель 13, 2024

Abstract In order to enhance the sluggish kinetics and suppress polysulfide shuttle effect in high‐loading lithium–sulfur (Li–S) batteries, it is crucial design synthesize catalysts exhibiting both high conversion rate strong anchoring toward species. Herein, based on theoretical predictions, spent cathode materials (LiCoO 2 LiMn O 4 ) from lithium‐ion batteries are converted into a bifunctional catalyst (Co─MnO) for Li–S through high‐temperature shock method. Owing synergistic catalytic of species exhibit by Co─MnO, superior electrochemical performance, including excellent performance (707 mAh g −1 at 4C) stability (capacity fading 0.058% per cycle over 400 cycles 1C) can be delivered under low areal loading (<0.5 wt%). This work not only offers new strategy catalysts, but also proposes promising approach transform LIBs highly efficient catalysts.

Язык: Английский

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Chemomechanics Engineering Promotes the Catalytic Activity of Spinel Oxides for Sulfur Redox Reaction

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Май 13, 2024

Abstract Cooperative catalysis is a promising approach to enhance the sluggish redox kinetics of lithium polysulfides (LiPSs) for practical lithium–sulfur (Li–S) batteries. However, elusory synergistic effect among multiple active sites makes it challenging accurately customize electronic structure catalysts. Herein, strategy precisely tailoring e g orbitals spinel oxides through chemomechanics engineering porposed regulate LiPSs retention and catalysis. By manipulating regulable cations in Mn x Co 3‐ O 4 , theoretically experimentally revealed that lattice strain induced by Jahn–Teller high‐spin 3+ at octahedral (Oh) can increase occupancy low‐spin Oh which effectively regulates chemical affinity toward establishes an unblocked channel intrinsic charge transfer. This leads volcano‐type correlation between sulfur activity. Benefitting from cooperative dual‐active sites, MnCo 2 with average 0.45 affords most appropriate adsorption strength rapid LiPSs, leading remarkable rate performance capacity assembled Li–S work demonstrates promise optimizing achieve efficient

Язык: Английский

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Redox mediators for high performance lithium-sulfur batteries: Progress and outlook

Chemical Engineering Journal, Год журнала: 2024, Номер 495, С. 153648 - 153648

Опубликована: Июль 1, 2024

Язык: Английский

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Entropy‐Driven Highly Chaotic MXene‐Based Heterostructures as an Efficient Sulfur Redox Electrocatalysts for Li‐S Battery

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Июнь 3, 2024

Abstract Both the sluggish sulfur redox reaction (SRR) kinetics and lithium polysulfides (LiPSs) shuttle effect limit practical application of Li‐S batteries. Designing heterostructure hosts has emerged as an effective way to address these two issues with one material. However, principles heterostructures reinforced batteries remain inadequately understood. Here, it is demonstrated for first time that increasing entropy can promote its SRR catalytic activity alleviate LiPSs shuttling. By a simple solution‐based strategy, highly chaotic MXene‐based (HCMH, TiS 2 /TiN/TiO /Ti 3 C T x ) fabricated. The smart integration “high entropy”, heterostructure, MXene endow HCMH catalyst significantly improved performance, by much smaller Tafel slope 62.9 mV dec −1 higher electron transfer number 7.10, compared moderately (MCMH, TiO /TiN/Ti MXene. DFT theoretical calculations reveal introducing new phases lowers Gibbs energy barriers both rate‐limiting Li S /Li reduction decomposition. Upon addition only 5 wt.% cathode, reversible capacity rate capability cells are greatly improved, which further highlights importance high “cocktail effect” in design electrocatalysts future.

Язык: Английский

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