Nature Energy
intl_tech
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Anion-reduction catalytic centres regulate interfacial solvation structures for fast-charging Si anodes
发布:2026-05-27
· 事件:2026-05-27
Download PDF Subjects Batteries Abstract Anion-rich interfacial solvation structures (ISS) are critical for stable fast charging of anodes. Here we propose interfacial anion-reduction catalysis as a n...
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Subjects
Batteries
Abstract
Anion-rich interfacial solvation structures (ISS) are critical for stable fast charging of anodes. Here we propose interfacial anion-reduction catalysis as a new paradigm, in which catalytic centres regulate the ISS to direct solid electrolyte interphase formation. Using S vacancies as prototypical catalytic sites, we demonstrate that electrostatic potential wells induced by these centres attract bis(fluorosulfonyl)imide (FSI
−
) to the interface and form contact ion pairs during charging, creating FSI
−
-rich ISS in commercial electrolytes. This catalytically regulated ISS promotes preferential FSI
−
reduction and ultrafine LiF grain formation, generating a compact LiF-rich solid electrolyte interphase with rapid Li
+
transport pathways. Si-based anode with catalytic interface demonstrates stable cycling with an average coulombic efficiency of ~99.94%. Pouch cells achieve ~91.4% and ~85.3% charge in 10 min and 6 min, respectively, while providing ~240.4 Wh kg
−1
under 6 min charging. This work establishes catalytic regulation of ISS as a promising strategy for fast battery charging.
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Main
Lithium-ion batteries (LIBs) combining high energy density and fast charging capability are essential for accelerating the adoption of electric vehicles
1
,
2
,
3
,
4
. High-capacity anodes, such as Si and metallic Li, enable batteries with high energy densities
5
,
6
. However, their large volume changes during cycling repeatedly fracture and reform the solid electrolyte interphase (SEI), leading to continuous consumption of active lithium and rapid capacity fade
7
,
8
,
9
,
10
. In addition, the instability of conventional SEI results in its uncontrolled growth, which increases interfacial resistance under fast-charging conditions, impedes Li
+
transport and facilitates lithium plating at elevated overpotentials
11
. This polarization-induced overpotential enhances heat generation during fast charging, which accelerates electrolyte decomposition and interfacial side reactions, thereby exacerbating battery degradation and safety risks. To address these fast-charging limitations, strategies have included materials-level interface engineering targeting interfacial physicochemical processes and system-level thermal management
4
,
12
,
13
. For the former, electrolyte engineering has focused on tailoring solvation environments to promote the formation of a robust SEI with high Li
+
conductivity
14
,
15
,
16
. Yet because the SEI forms at the electrode/electrolyte interface, its properties are determined by the interfacial solvation structure (ISS) rather than the bulk solvation structure
17
. Unlike the thermodynamically stable bulk solvation, ISS is dynamically reconfigured in interfacial fields with surface interactions
18
. In conventional electrolytes (~1 M), strong interfacial electric fields exclude anions from the inner Helmholtz plane (IHP), leading to solvent-dominated ISS that yields unstable organic-rich SEI
19
,
20
. However, the evolution and regulation of ISS in practical electrolytes remain poorly understood.
Anion-rich ISS that enable preferential reduction of anions (for example, PF
6
−
and FSI
−
) promote the formation of inorganic-rich SEI containing species such as LiF, which is particularly valued for its mechanical robustness, stability and ability to enhance Li
+
transport
21
,
22
. Electrolyte strategies, including concentrated or weakly solvating electrolytes, have been used to achieve anion-rich ISS, by promoting the formation of Li
+
-anion contact ion pairs (CIPs) and aggregates that co-migrate with Li
+
towards the interface under electric fields
23
,
24
,
25
,
26
,
27
,
28
. Yet such electrolytes suffer from trade-offs: high viscosity or low conductivity that limit fast charging. Until now, achieving more than 90% charge within 10 min without sacrificing energy density (for example, >250 Wh kg
−1
) and cycle life remains a formidable challenge.
Achieving an anion-rich ISS while maintaining solvent-dominated bulk solvation for high conductivity is essential for fast charging. This raises a fundamental question of whether anion-rich ISS can be realized in conventional electrolytes without compromising bulk ionic transport. Indeed, the ISS is shaped not only by electrolyte composition but also critically by the physicochemical nature of the electrode surface
29
,
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. Such interfacial regulation is well established in electrocatalysis
31
, where catalytic sites can regulate local potential landscapes, influence the adsorption of reactive species and determine reaction selectivity. Inspired by this concept, we propose interf