Jian-Jun Wang

Aluminum‐ion batteries are a promising energy storage technology for high resource abundance, safety, and cost‐effectiveness advantages, but practical implementation is hindered by two degradation mechanisms in Al metal anode: electrically isolated metallic aluminum (iAl ⁰ ) and electrochemical side‐reaction products (iSEI Al ³⁺ ). Precise quantification of these inactive species and relationships with cycling reversibility have rarely been established, limiting rational anode design. Here, we develop a basic titration gas chromatography technology to accurately quantify iAl ⁰ and iSEI Al ³⁺ , revealing a current density‐dependent Al loss mechanism: iSEI Al ³⁺ loss dominates at low current, while metallic iAl ⁰ loss prevails at high current. We discover that an inorganic‐dominated interphase favors significant suppression of inactive Al formation. Applying an optimal stack pressure strategy (780 kPa) constructs tip‐localized stack pressure/electric field, effectively reducing inactive Al loss by 81.99% and prolonging battery cycling life by ≥500%. These advancements offer fundamental theory and techniques for Al anode reaction mechanism research and provide design principles for high‐performance aluminum‐ion battery.

Aluminum‐ion batteries (AIBs) are promising for large‐scale energy storage owing to their elemental abundance, low cost, safety, and high anode capacity. However, their development is hindered by the limited reversibility of Al plating/stripping on Al metal anodes and cathode structural degradation under high‐voltage operation, resulting in short cycle life and limited energy density. These challenges originate from an incomplete understanding of how interphase components and properties regulate electrode reactions. Here, we systematically investigate the interphase properties in AIBs and reveal that AlF ₃ exhibits the highest interfacial energy, mechanical strength against dendrite growth, and electrochemical stability with electron‐blocking capability against parasitic reactions, making it an ideal artificial interphase component. Based on these findings, AlF ₃ ‐enriched artificial interphases are constructed in Al||graphene batteries, enabling 99.9% Al plating/stripping Coulombic efficiency with uniform deposition morphology. The Al||graphene full cell delivers a high specific capacity of 122.6 mAh g ⁻¹ , ultrahigh‐rate capability (817 C, charged in 2.936 s), and long‐term cyclability exceeding 100 000 cycles. This AlF ₃ ‐enriched interphase strategy establishes fundamental principles for designing high‐performance AIBs.

This work proposes a water regulation strategy. 3-Hydroxypropionitrile (HPN) modulates bulk solvation and interfacial environment, endowing cells with 8000 h cycling stability and wide-temperature adaptability from −40 to 50 °C.

Nonoxide electrocatalysts hold great promise for high-efficiency seawater oxidation, yet their practical application is hindered by the inevitable surface reconstruction and pronounced corrosion under high anodic potentials. Herein, we solve this longstanding challenge by developing a rational anionic ligand passivation strategy that stabilizes phosphide lattices against oxidative degradation while preserving inherent electrocatalytic activity. Leveraging Lewis acid–base interactions, we grow an ultrathin, undercoordinated TiOx overlayer on a FeNiP (FNP) support. This overlayer withdraws electrons from lattice phosphorus, downshifts the P p-band center, and thermodynamically stabilizes the entire anionic sublattice against oxidative leaching. The oxidation-resistant scaffold further enables the anchoring of atomically ordered Ir arrays with a well-defined interatomic spacing of ∼2.8 Å, promoting direct O–O radical coupling via the oxide pathway mechanism and effectively circumventing the corrosive lattice oxygen route. Operando spectroscopy and 18O isotope tracing confirm fully reconstruction-free OER behavior with negligible lattice oxygen participation. The as-developed TiIr@FNP catalyst achieves ultralow overpotentials (only 310 mV at 1 A cm–2), operates stably for over 1200 h in alkaline seawater, and maintains near-unity Faradaic efficiency. The work demonstrates a generalizable strategy for designing durable, high-performance nonoxide anodic electrocatalysts under industrially relevant conditions.

Lithium‐ion batteries (LIBs) suffer rapid capacity fade at low temperatures. Weakly coordinating electrolytes via adding low‐polarity or non‐coordinating co‐solvents (such as fluorinated ethers) have shown promise in rapid desolvation, yet these electrolytes often exhibit low ionic conductivity at low temperature, limiting the application of high‐energy density LIBs. Here, we design a weakly coordinating electrolyte by incorporating the non‐coordinating co‐solvent (pentafluoroethyl)trimethylsilane (PFTMS) into the coordinating solvent diethyl carbonate (DEC) via orbital‐overlap‐enhanced dipole–dipole interactions. The slight Si─O orbital overlap drives strong dipole–dipole interactions between PFTMS and DEC. This interaction lowers the negative electrostatic potential at the carbonyl oxygen of DEC, thereby weakening Li ⁺ ‐DEC coordination. Thus, by leveraging enhanced dipole–dipole interactions, this strategy realizes a weak Li ⁺ ‐solvent coordination through a lower content of PFTMS (10 vol%) compared to traditional fluorinated solvents. Besides, the designed electrolyte delivers sufficient ionic conductivity of 1.56 mS cm ⁻¹ at −40°C. Accordingly, the graphite || LiNi _0.8 Co _0.1 Mn _0.1 O ₂ (NCM811) coin cell shows reversible capacity of 156.5mAh g ⁻¹ at −40°C. Notably, 4.7 Ah graphite || NCM811 pouch cell also demonstrates 219.8 Wh kg ⁻¹ at −20°C. This work advances the design of traditional weakly coordinating electrolytes via an orbital overlap strategy, which paves the way for application in extreme environments.

ConspectusAqueous zinc-ion batteries (ZIBs) are increasingly recognized as leading candidates for grid-scale energy storage owing to their intrinsic safety, material abundance, and low cost. However, their practical deployment is fundamentally constrained by a self-amplifying failure cycle at the zinc anode, wherein inhomogeneous Zn²⁺ flux induces dendritic growth, which exacerbates the hydrogen evolution reaction (HER) and promotes the formation of insulating passivation layers (e.g., Zn₄SO₄(OH)₆·xH₂O). Conventional mitigation strategies, such as structural engineering of the anode, surface coatings, or electrolyte optimization, are largely static and lack the dynamic adaptability required to stabilize the evolving electrode-electrolyte interface over extended cycling. In this context, supramolecular chemistry, governed by reversible noncovalent interactions, molecular recognition, and self-assembly, offers a transformative and dynamic platform to address the root causes of ZIB instability. This Account systematically elucidates the core mechanisms by which supramolecular systems operate: (1) host-guest recognition, wherein macrocyclic hosts (e.g., cyclodextrins, cucurbiturils, crown ethers) selectively bind Zn²⁺ or anions to reconfigure solvation structures and direct uniform ion transport; (2) interface stabilization via self-assembled supramolecular layers that create water-deficient, flexible artificial SEI layers to suppress parasitic reactions; and (3) dynamic hydrogen-bond networks that enable real-time adaptation, self-repair, and mechanical buffering against volume fluctuations. We highlight key contributions from our group and others across diverse application domains, including host-guest electrolyte additives, supramolecular gel electrolytes, and interfacial engineering, demonstrating precise control over Zn²⁺ deposition behavior (e.g., epitaxial (002) growth), effective HER suppression, and enhanced performance under extreme conditions such as low temperature. Through integration of advanced in situ characterization and multiscale simulations, we establish structure-property relationships that inform the rational design of next-generation supramolecular systems. Finally, we outline critical challenges and future directions, including elucidation of noncovalent interaction dynamics under operando conditions, development of multifunctional hosts with tailored selectivity, scalable and sustainable synthesis, and full-cell validation (e.g., suppression of cathode dissolution). This Account underscores that supramolecular chemistry, through its dynamic and adaptive nature, overcomes the inherent limitations of conventional static approaches and paves the way toward durable, high-performance ZIBs for sustainable energy storage.

Simultaneously achieving uniform zinc deposition and stable interfaces remains a critical challenge for aqueous zinc metal batteries. Herein, we present a synergistic electrolyte design integrating β‐cyclodextrin (β‐CD) as a supramolecular regulator with trimethyl phosphate (TMP) as a bulk cosolvent to enable multiscale regulation from the electrode interface to the electrolyte bulk. The β‐CD additive dynamically adsorbs on the Zn surface, guiding homogeneous Zn ²⁺ flux and fostering a robust solid electrolyte interphase. Concurrently, TMP reconstructs the primary solvation shell of Zn ²⁺ and disrupts the hydrogen‐bond network, effectively suppressing hydrogen evolution and corrosion. Spectroscopic and electrochemical analyses confirm that this cooperative mechanism optimizes both interfacial kinetics and bulk electrolyte stability. Consequently, Zn||Zn symmetric cells achieve outstanding cycling stability over 2000 h, and Zn||Cu asymmetric cells maintain a high Coulombic efficiency of 99.52% for over 1100 cycles. Full cells paired with NH ₄ V ₄ O ₁₀ cathodes further demonstrate superior capacity retention and reduced self‐discharge. This work provides a novel electrolyte design paradigm through molecular co‐regulation, offering a general strategy for stabilizing metal anodes in aqueous batteries.

Enhancing cycling reversibility in high-energy-density lithium metal batteries necessitates precise management of electrolyte-derived electrochemical reactions at electrodes and interphases, yet recently developed localized high-concentration electrolytes suffer from limited tunability of these reactions for the non-solvation-participating nature of oxygen-proximal fluorinated diluents. Here we address this issue by synthesizing an oxygen-distal fluorinated di-2,2,3,3-tetrafluoropropoxyethane diluent whose molecular skeleton is strategically edited to position fluorine atoms distal to oxygen centers that attenuate electron-withdrawing effects at Li⁺-coordination sites, enabling: enhanced diluent/anion participation and reduced volatile solvents in solvation shells; atypical H-F bonding between diluent and solvent toward enhanced oxidation resistance; and promotion of diluent and salt-derived highly stable inorganic-rich interphase formation. This electrolyte achieves 99.8% Li plating/stripping Coulombic efficiency, 450 stable cycles in 4.5 V high-voltage Li || LiNi_0.8Mn_0.1Co_0.1O₂ cells, and 5.9-Ah, 504.6 Wh kg^–1 (based on mass of all components including packaging) pouch cells that exhibits 0.053% per-cycle capacity decay. This work introduces oxygen-distal fluorination as a potential molecular skeleton editing strategy for stable energy-dense lithium metal batteries.

Electrocatalytic amine dehydrogenation to nitriles has emerged as a green and sustainable synthetic route, providing a promising alternative to traditional energy-intensive and polluting nitrile production processes. However, this field still faces significant challenges, such as limited catalytic activity and selectivity, insufficient mechanistic understanding, and a lack of systematic integration of catalyst and system design. To address these issues, this review comprehensively summarizes recent advances in electrocatalytic nitrile synthesis from amines. Beginning with the fundamental electrocatalytic mechanisms, we focus on rational design strategies for high-performance catalysts, highlighting how catalyst structures and electrolyte components regulate interfacial properties and reaction pathways. By integrating in situ characterization, theoretical calculations, and performance evaluation, we further identify key future research directions, including multi-scale optimization of catalytic systems, electrolyzer design, and techno-economic analysis. This review aims to offer theoretical insights and practical guidance for the development of efficient, stable, and scalable electrocatalytic systems for green nitrile synthesis.

Solid-state lithium metal batteries (SSLMBs), particularly in anode-less configurations, are severely hindered by catastrophic electrochemomechanical degradation at the Li anode–solid electrolyte interface caused by infinite anode volume fluctuations during Li plating/stripping reaction, posing significant challenges to its cycling reversibility. Here, we report a zero-volume-change cellular void-structured host that changes the solid-state Li metal anode reaction mechanism, from infinite volume-changing Li deposition/dissolution at the anode–solid electrolyte interface to Li deposition/dissolution inside the voids of the host with zero-volume-changing feature. Operando pressure/microscopy characterization verifies that the zero-volume-change cellular void host architecture terminates the critical Li anode volume-change-induced solid–solid interface delamination failure that has constrained SSLMB development for decades, thus achieving a record-breaking Coulombic efficiency (≥99.9%) that surpasses prior benchmarks by 1–3 orders of magnitude. Meanwhile, anode-less SSLMBs using the zero-volume-change host with a negative:positive capacity ratio of 0 can realize 95.5% capacity retention after 400 cycles at low stack pressure (440 kPa), representing one of the best SSLMB performances so far. By resolving the root cause of the Li anode volume-change-driven fluctuated interface contact failure mechanism in the SSLMB, this work provides an anode design strategy for cycling-stable solid-state lithium metal battery construction.