Balanced d-Band Model: A Framework for Balancing Redox Reactions in Lithium–Sulfur Batteries DOI
Wei Xiao, Kisoo Yoo, Jong‐Hoon Kim

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(47), P. 32732 - 32745

Published: Nov. 11, 2024

Managing the redox reactions of polysulfides is crucial for improving performance lithium-sulfur batteries (LSBs). Herein, we introduce a progressive theoretical framework: balanced d-band model, which based on classical center theory. Specifically, by optimizing position in middle between highest occupied molecular orbital (HOMO) and lowest unoccupied (LUMO) each sulfur species, fast oxidation reduction species can be achieved simultaneously. To validate this theory, synthesized catalyst featuring an situ phosphorized heterostructure (NOP) nickel oxide (NiO), effectively optimizes at HOMO LUMO species. Aided kinetics NOP-based cell high reversible capacity, superior cycling stability, prolonged cycle life. This study extends conventional theory introduces innovative model to expand our understanding internal reaction mechanisms LSBs.

Language: Английский

Rechargeable Metal-Sulfur Batteries: Key Materials to Mechanisms DOI
Weiqi Yao, K. T. Liao, Tianxing Lai

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(8), P. 4935 - 5118

Published: April 10, 2024

Rechargeable metal-sulfur batteries are considered promising candidates for energy storage due to their high density along with natural abundance and low cost of raw materials. However, they could not yet be practically implemented several key challenges: (i) poor conductivity sulfur the discharge product metal sulfide, causing sluggish redox kinetics, (ii) polysulfide shuttling, (iii) parasitic side reactions between electrolyte anode. To overcome these obstacles, numerous strategies have been explored, including modifications cathode, anode, electrolyte, binder. In this review, fundamental principles challenges first discussed. Second, latest research on is presented discussed, covering material design, synthesis methods, electrochemical performances. Third, emerging advanced characterization techniques that reveal working mechanisms highlighted. Finally, possible future directions practical applications This comprehensive review aims provide experimental theoretical guidance designing understanding intricacies batteries; thus, it can illuminate pathways progressing high-energy-density battery systems.

Language: Английский

Citations

70

Accelerated Li+ Desolvation for Diffusion Booster Enabling Low‐Temperature Sulfur Redox Kinetics via Electrocatalytic Carbon‐Grazfted‐CoP Porous Nanosheets DOI Creative Commons
Xin Zhang, Xiangyang Li, Yongzheng Zhang

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(36)

Published: May 19, 2023

Abstract Lithium–sulfur (Li–S) batteries are famous for their high energy density and low cost, but prevented by sluggish redox kinetics of sulfur species due to depressive Li ion diffusion kinetics, especially under low‐temperature environment. Herein, a combined strategy electrocatalysis pore sieving effect is put forward dissociate the + solvation structure stimulate free diffusion, further improving reaction kinetics. As protocol, an electrocatalytic porous diffusion‐boosted nitrogen‐doped carbon‐grafted‐CoP nanosheet designed via forming NCoP active release more react with species, as fully investigated electrochemical tests, theoretical simulations in situ/ex situ characterizations. result, cells booster achieve desirable lifespan 800 cycles at 2 C excellent rate capability (775 mAh g −1 3 C). Impressively, condition mass loading or environment, cell 5.7 mg cm −2 stabilizes areal capacity 3.2 charming 647 obtained 0 °C after 80 cycles, demonstrating promising route providing ions toward practical high‐energy Li–S batteries.

Language: Английский

Citations

57

Unveiling the Pivotal Parameters for Advancing High Energy Density in Lithium‐Sulfur Batteries: A Comprehensive Review DOI Creative Commons
Yue Fei, Ge Li

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(21)

Published: Jan. 29, 2024

Abstract The lithium‐sulfur (Li‐S) battery stands as a strong contender for the next‐generation energy storage system, characterized by abundant sulfur resources, environmental sustainability, and high specific capacity. However, its density remains constrained factors such low loading fraction in cathode, excessive electrolyte, an excess of anode. These mild conditions significantly limit Li‐S batteries, making them less competitive. To achieve higher density, harsh operation are necessary, but these remain challenging to implement, even lab‐scale production. In this comprehensive review, emphasis will be on recent advancements specifically realm designing loading, fraction, lean limited negative electrode batteries. A visualizable model that illustrates relationship between cell various parameters, underscoring importance exploring batteries under extreme operating further development is provided. Furthermore, it discussed possibilities achieving challenges need addressed make practical real‐world applications.

Language: Английский

Citations

47

Accelerated Sulfur Redox Kinetics on Transition Metal Sulfide Electrocatalysts by Modulating Electronic‐State of Active Sites DOI
Xiaoting Wang, Siyu Liu, Juan Yang

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(25)

Published: April 5, 2024

Abstract Lithium‐sulfur (Li‐S) batteries are considered a competitive next‐generation electrochemical energy storage device, while the shuttle effect of soluble lithium polysulfides (LiPSs) resulting from sluggish redox kinetics severely impedes their practical applications. Herein, novel cation doping strategy is demonstrated for substantially accelerating sulfur on transition metal sulfide (TMS) electrocatalysts by partially substituting cobalt atoms with in situ dissolved Ni dopants (Ni x Co 3‐x S 4 , 0<x≤1). Theoretical calculations revealed that spinel 3 phase enables electronic‐state modulation active sites realizing upshift d‐orbital center, thus leading to good chemical adsorption intermediates and low conversion barriers between LiPSs solid Li 2 products. This confirmed in‐depth dynamics Raman characterizations, which obtained 0.5 2.5 hierarchical nanosheet structure delivers stronger affinity 6 higher precipitation/dissociation capacity comparison monometallic sulfides. Benefiting these outstanding attributes, assembled Li‐S incorporating into S@carbon nanotube cathode (S@Ni /CNT) exhibit high specific 1189 mAh g −1 excellent rate performance 596 at 5 C long‐term cycling over 600 cycles decay 0.06% per cycle 1 C. More importantly, an ultrahigh reversible areal 6.6 cm −2 can be achieved S@Ni /CNT even loading 6.1 mg . work demonstrates new insight designing TMS toward rapid batteries.

Language: Английский

Citations

26

Rare Earth Single‐Atom Catalysis for High‐Performance Li−S Full Battery with Ultrahigh Capacity DOI
Rong Zhou,

Yongqiang Ren,

Weixin Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(31)

Published: May 18, 2024

Lithium-sulfur (Li-S) batteries have many advantages but still face problems such as retarded polysulfides redox kinetics and Li dendrite growth. Most reported single atom catalysts (SACs) for Li-S are based on d-band transition metals whose d orbital constitutes active valence band, which is inclined to occur catalyst passivation. SACs 4f inner of rare earth challenging their great difficulty be activated. In this work, we design synthesize the first metal Sm has electron-rich promote catalytic conversion uniform deposition Li. enhance catalysis by activated through an f-d-p hybridization. Using Sm-N

Language: Английский

Citations

19

Advanced preparation and application of bimetallic materials in lithium-sulfur batteries: A review DOI

Yongbing Jin,

Nanping Deng, Yanan Li

et al.

Journal of Energy Chemistry, Journal Year: 2023, Volume and Issue: 88, P. 469 - 512

Published: Oct. 5, 2023

Language: Английский

Citations

36

Binary Transition-Metal Sulfides/MXene Synergistically Promote Polysulfide Adsorption and Conversion in Lithium–Sulfur Batteries DOI
Yuchen Cui, Xiaoya Zhou, Xin Huang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(42), P. 49223 - 49232

Published: Oct. 15, 2023

Currently, severe shuttle effects and sluggish conversion kinetics are the main obstacles to advancement of lithium-sulfur (Li-S) batteries. Modification battery separator by a catalyst is promising approach tackle these problems, but simultaneously obtaining rich catalytic active sites, high conductivity, remarkable stability remains great challenge. Herein, flower-like MXene/MoS2/SnS@C heterostructure as functional intercalation Li-S batteries was prepared for accelerating synergistic adsorption-electrocatalysis sulfur conversion. The MXene skeleton constructs three-dimensional conductive network that anchors polysulfides enhances charge transfer. Meanwhile, MoS2/SnS has sites polysulfide conversion, leading excellent electrochemical performances. A with displays an extraordinary capacity 836.1 mAh g-1 over 200 cycles at 0.5C demonstrates cycling attenuation approximately 0.051% per cycle during 1000 2C. When loading reaches 5.1 mg cm-2, still maintains 722.4 50 cycles. This research proposes novel strategy design stable catalysts extended lifespan.

Language: Английский

Citations

31

RuOx Quantum Dots Loaded on Graphdiyne for High‐Performance Lithium–Sulfur Batteries DOI
Zhongqiang Wang,

Congying Song,

Han Shen

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(9)

Published: Nov. 4, 2023

Abstract Here, a strategy to strengthen d–p orbital hybridization by fabricating π backbonding in the catalyst for efficient lithium polysulfides (LiPSs) conversion is reported. A special interface structure of RuO x quantum dots (QDs) anchored on graphdiyne (GDY) nanoboxes (RuO QDs/GDY) prepared enable strong Ru‐to‐alkyne backdonation, which effectively regulates d‐electron structures Ru centers promote between and LiPSs significantly boosts catalytic performance QDs/GDY. The affinity with Li ions fast Li‐ion diffusion QDs/GDY also ultrastable metal anodes. Thus, S@RuO cathodes exhibit excellent cycling under harsh conditions, Li@RuO anodes show an ultralong life over 8800 h without dendrite growth. Lithium‐sulfur (Li–S) full cells can deliver impressive areal capacity 17.8 mA cm −2 good stability practical conditions low negative‐to‐positive electrode (N/P) ratio (N/P = 1.4), lean electrolyte (E/S 3 µL mg −1 ), high S mass loading (15.4 ).

Language: Английский

Citations

31

Electron delocalization-enhanced sulfur reduction kinetics on an MXene-derived heterostructured electrocatalyst DOI
Yunmeng Li, Yinze Zuo,

Xiang Li

et al.

Nano Research, Journal Year: 2024, Volume and Issue: 17(8), P. 7153 - 7162

Published: May 15, 2024

Language: Английский

Citations

15

Electronic State‐Modulated Ni4N/Zn3N2 Heterogeneous Nanosheet Arrays Toward Dendrite‐Free and Kinetic‐Enhanced Li‐S Full Batteries DOI Creative Commons
Qiwen Ran, Jintao Liu, Lei Li

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(38)

Published: April 26, 2024

Abstract The applications of lithium (Li)–sulfur (S) batteries are simultaneously hampered by the unlimited dendritic Li growth and sluggish redox kinetics polysulfides (LiPSs). In this work, an electronic state‐modulated Ni 4 N/Zn 3 N 2 heterogeneous nanosheet arrays is painstakingly fabricated on surface carbon cloth (CC@Ni ) as efficient bi‐service host to promote uniform deposition boost LiPSs catalysis. It found that structure heterostructure modulated realize a rational transition metal d‐band center, its built‐in electric field (BIEF) within heterointerfaces facilitates interfacial charge transfer, resulting in low deposition/migration energy barrier adsorption/catalytic conversion kinetics. As result, as‐prepared CC@Ni ‐Li anode can enable Li||Li symmetrical cells possess long‐term lifespan over 500 h even at 10 mA cm −2 /20 mAh , as‐assembled LiNi 0.8 Co 0.1 Mn O ||CC@Ni full cell also shows excellent cycling performance (95.8% capacity retention after 100 cycles). When used for both S loading, ‐S||CC@Ni exhibits outstanding stability (744 g −1 1000 cycles 2C). This work highlights great potential heterostructures fabricating ideal bi‐serve hosts electrodes.

Language: Английский

Citations

13