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

Advanced Materials, Год журнала: 2023, Номер 35(44)

Опубликована: Июль 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.

Язык: Английский

---

Rechargeable Metal-Sulfur Batteries: Key Materials to Mechanisms

Chemical Reviews, Год журнала: 2024, Номер 124(8), С. 4935 - 5118

Опубликована: Апрель 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.

Язык: Английский

---

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

---

Co/Mon Invigorated Bilateral Kinetics Modulation for Advanced Lithium–Sulfur Batteries

Advanced Materials, Год журнала: 2023, Номер 36(13)

Опубликована: Дек. 22, 2023

Abstract Sluggish sulfur redox kinetics and Li‐dendrite growth are the main bottlenecks for lithium–sulfur (Li–S) batteries. Separator modification serves as a dual‐purpose approach to address both of these challenges. In this study, Co/MoN composite is rationally designed applied modifier modulate electrochemical on sides cathode lithium anode. Benefiting from its adsorption‐catalysis function, decorated separators (Co/MoN@PP) not only effectively inhibit polysulfides (LiPSs) shuttle accelerate their conversion but also boost Li + flux, realizing uniform plating/stripping. The accelerated LiPSs excellent reversibility triggered by modified evidenced performance, in‐situ Raman detection theoretical calculations. batteries with Co/MoN@PP achieve high initial discharge capacity 1570 mAh g −1 at 0.2 C low decay rate 0.39%, transportation 1 mA cm −2 over 800 h. Moreover, areal 4.62 achieved under mass loadings 4.92 mg . This study provides feasible strategy rational utilization synergistic effect multifunctional microdomains solve problems anode S toward long‐cycling Li–S

Язык: Английский

---

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

---

Recent advances and strategies of metal phosphides for accelerating polysulfide redox and regulating Li plating

Coordination Chemistry Reviews, Год журнала: 2024, Номер 510, С. 215836 - 215836

Опубликована: Апрель 12, 2024

Язык: Английский

---

Green synthesis and applications of MXene for lithium–sulfur batteries

Energy storage materials, Год журнала: 2024, Номер 67, С. 103257 - 103257

Опубликована: Фев. 11, 2024

Язык: Английский

---

Regulate transportation of ions and polysulfides in all–solid-state Li-S batteries using ordered-MOF composite solid electrolyte

Science Advances, Год журнала: 2024, Номер 10(11)

Опубликована: Март 13, 2024

A dilemma arises when striving to balance the maximum desired ion conductivity and minimize undesired lithium polysulfide shuttling effect for all-solid-state lithium-sulfur batteries (ASSLSBs). Here, we introduce a strategy of using ordered MIL-125-NH

Язык: Английский

---

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

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(31)

Опубликована: Май 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

Язык: Английский

---

Breaking the Passivation Effect for MnO₂ Catalysts in Li−S Batteries by Anion‐Cation Doping

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(46)

Опубликована: Июль 22, 2024

Transition metal oxides (TMOs) are recognized as high-efficiency electrocatalyst systems for restraining the shuttle effect in lithium-sulfur (Li-S) batteries, owing to their robust adsorption capabilities polysulfides. However, sluggish catalytic conversion of Li

Язык: Английский

---