CrO42- can originate from the oxidation of chromium present in electrode materials (e.g., stainless steel or Cr-containing alloys) during anodic polarization in alkaline media. They have long been regarded as an inert species in electrocatalysis, which simply dissolves away in the electrolyte. In this work, based on the studies of model catalysts and surface treated stainless steel, we find that CrO42- dynamically adsorbs onto the readily formed NiFeOOH during the surface reconstruction which strongly coordinate with the oxyhydroxide surface, forming both monodentate mononuclear and bidentate binuclear structures. This elevates the Ni oxidation state and promotes a partial shift of the reaction pathway from the adsorbate evolution mechanism toward the lattice oxygen mechanism in both the oxygen evolution reaction (OER) and the ethylene glycol oxidation reaction. Importantly, the chromate-containing electrode enables high ethylene glycol conversion (>95%) while maintaining a high Faradaic efficiency (>90%) toward formate by effectively suppressing competing side reactions such as the OER and substrate overoxidation. This work reveals the unique role of interfacial chromate ions on the lattice‑oxygen reactivity, structural stability and catalytic selectivity of NiFeOOH, offering a promising strategy for designing high‑performance anodes for both water splitting and electrosynthesis of value‑added chemicals.

Gel polymer electrolytes (GPEs) paired with abundant sodium (Na) and high-voltage polyanionic cathode, offer improved energy density and superior safety, positioning them as scalable alternatives for resource-limited lithium batteries. However, such technologies are plagued by critical interfacial engineering challenges: existing GPEs fail to sustain (electro)-chemical stability and mechanical close contact at high-loading cathodes and highly reactive anodes. Here, we report a rationally engineered GPE featuring biphasic polymer, creating step channels and polymer-solvent dipole adsorption to address the key issues. It enables volume-constrained bidirectional transport of infilling linear ether and cyclic carbonate solvents and endows the polymer with differential mechanical viscoelasticity for high-loading cathodes and ductile Na anodes. Therefore, a high-energy-density full cell of Na||Na3V2(PO4)3 (34.1 mg cmcathode -2, 194.4 Wh kg-1, based on total cell mass) and a stable pouch cell of 4.5 V-class Na||Na2.466Fe1.724Mg0.043(SO4)3 (18.7 mg cmcathode -2, ∼100% after 100 cycles) were demonstrated, with safety validation included. The design principles were established for this new chemical engineering pathway towards practical solid-state batteries.

Solid electrolytes (SEs) are central to next-generation metal batteries, yet their discovery remains constrained by fragmented data, limited transferability of simulations, and slow experimental iteration. Unlike catalysis, where surface reactivity dominates, SEs require simultaneous optimization of bulk ion transport, defect chemistry, mechanical integrity, and interfacial stability. Here, we outline a framework for autonomous SE discovery enabled by large artificial intelligence (AI) models, including machine learning interatomic potentials (MLIPs) and large language models (LLMs). We discuss the evolution from static materials databases to dynamic, self-updating knowledge systems, the role of MLIPs in bridging density functional theory (DFT) and long-timescale ion migration, and the emergence of LLMs as engines for literature mining, hypothesis generation, and scientific reasoning. We further describe a closed-loop architecture integrating AI-driven candidate design, multiscale simulation, uncertainty-aware selection, and experimental validation. Such systems shift SE research from intuition-guided exploration to data-informed, self-improving cycles. We conclude by highlighting challenges in data standardization, interfacial complexity, and reproducibility, and we propose design principles for building autonomous laboratories for solid-state battery materials.

Lithium-oxygen (Li-O2) batteries overcome the ion-intercalation chemistry in lithium-ion batteries by employing oxygen conversion reactions beyond the solid cathode framework. However, sluggish kinetic limit practical discharge voltages below 2.85 V, establishing a "high capacity, low power output" dilemma that severely compromises achievable energy and power densities. Herein, a CO2-mediated Li-O2 battery (CLOB) is constructed to redefine the oxygen redox chemistry by strategically optimizing gas composition and catalytic architecture, successfully elevating the discharge voltage to 3.30 V comparable to the LiFePO4-based lithium-ion batteries. O2 and CO2 are gradually reduced to form the intermediates of Li2CO4 and Li2C2O6, and finally Li2CO3 as the discharge product. It leads to an equilibrium voltage of 3.30 V in a two-electrode electrochemical cell. Furthermore, iron phthalocyanine (FePc) is introduced as a soluble molecular carrier to mitigate the kinetic constraint. The demonstrated FePc-based CLOB delivers an exceptional discharge voltage of 3.30 V and the assembled pouch cell exhibits a 1.38 Ah capacity with an ultrahigh energy density of 870.1 Wh kg-1. This voltage enhancement substantially improves energy output and offers a new paradigm for the commercialization of metal-gas batteries.

The mounting mining royalties, particularly on cobalt ore, within the Democratic Republic of the Congo have introduced a sustained tension within the battery industry. This challenge is notably significant given cobalt’s critical role in the battery industry. The predicament surrounding cobalt has been further exacerbated by the rapid expansion of battery production and the burgeoning electrical vehicle (EV) market, leading to a notable upswing in wholesale cobalt prices and a decelerated pace in the advancement of transportation electrification. In response, the battery scientific community is actively engaged in developing new electrode materials to alleviate reliance on cobalt. However, achieving complete liberation from cobalt appears to be currently impractical, primarily due to the irreplaceable role of cobalt in battery chemistry and the limited feasibility of proposed non-cobalt alternatives. This necessitates a nuanced approach to finding a balance between reducing dependence on cobalt and maintaining the performance and stability required in advanced battery technologies. In this perspective, our emphasis is directed towards cultivating a fundamental understanding of the pivotal role that cobalt plays in the layered structure. This strategic focus aims to pave the way for exploring the feasibility of advanced cobalt-free cathode materials.

ABSTRACT The development of high‐energy low‐cost lithium‐ion batteries has sparked interest in ultrahigh‐Ni Co‐free layered cathodes that offer high capacity, low cost, and environmental friendliness. Yet, their widespread deployment is impeded by the challenges posed by the large magnetic moments of Ni and Mn, as well as the aggregation of the highly spin‐unstable high‐spin state of Ni 3+ at the interface. Herein, an efficient three‐in‐one strategy of internal Al and external Zr is proposed to achieve an ultrastable single‐crystal ultrahigh‐Ni Co‐free cathode, Li(Ni 0.90 Mn 0.08 Al 0.02 ) 0.98 Zr 0.02 O 2 (NMAZ). The strong AlO 6 ligands prevent the formation of high‐spin Ni 3+ . Surface‐enriched Zr restricts the diffusion of Ni within the NiO 6 octahedron. The single‐crystal structure reduces unwanted reactions with the electrolyte. Consequently, NMAZ achieves a favorable unity of material cost and electrochemical performance by reducing the resource expense by >7.5% than conventional Co‐containing single‐crystal LiNi 0.88 Mn 0.08 Co 0.04 O 2 (NMC) and demonstrating excellent calendar lifespan performance. Moreover, it shows better phase stability under high dissociation conditions, alleviates the harmful H2‐H3 phase transformation, and avoids the release of lattice oxygen due to the overlap of Co 3+/4+ 3d and O 2− 2p orbitals upon deep delithiation.

Microbial fuel cells (MFCs) represent a green and promising technology for interconverting electrical and chemical energy. However, the efficiency of microbial catalysts is often fundamentally limited by inherent catalytic constrains of natural enzymes and insulating barrier of the cell membrane. In this study, we heterologously expressed leghemoglobin 4 (LB4) in Escherichia coli (E. coli) and displayed it on the cell surface using an ice nucleation protein (INP). LB4 serves as an efficient electrocatalyst for the oxygen reduction reactions (ORR), exhibiting high intrinsic activity. The surface-display strategy not only increased the protein level of active LB4 but also effectively circumvented the insulating cell membrane barrier. As a result, the engineered strain INP-Soya achieved an ORR current density of 3.46 mA cm-2 (vs. RHE) and an onset potential of 0.78 V. The MFC constructed with INP-Soya generated a maximum power density of 300 μW cm-2. This work demonstrates that the surface display of catalytically active proteins provides a viable strategy for achieving efficient bioelectrocatalysis.

Manganese dioxide (MnO2) is a promising cathode material for aqueous zinc ion batteries (AZIBs) due to its high theoretical capacity and natural abundance. However, its practical application is hindered by severe structural degradation caused by Jahn-Teller distortion and dissolution in aqueous environments. Herein, we report high-crystallinity layered MnO2 synthesized via high-temperature calcination at 800 °C, in contrast to conventional low-temperature hydrothermal methods. The calcinated MnO2 (MnO2-cal) exhibits ordered lamellar morphologies with robust crystallinity and enhanced structural integrity, enabling a superior cycling stability even without Mn2+ electrolyte additives. Electrochemical tests reveal a reversible capacity of ∼135 mAh g-1 with negligible capacity fading. Detailed ex situ XRD and XAS characterizations confirm the highly reversible structural evolution and stable Mn-O coordination during electrochemical operations. This work sheds light on the structural design and synthesis routes of manganese oxides, offering a novel viewpoint on developing long-life AZIB cathodes beyond traditional hydrothermal synthesis.

We develop a Ni-Cu dual single-atom catalyst (DSAC) as a model catalyst to investigate the neighboring synergy in dual single-atom sites for promoting the electrocatalytic carbon dioxide reduction reaction (ECO2RR) kinetics. Through detailed electrochemical tests, in situ spectroscopic observations and theoretical calculations, we found that during ECO2RR, the neighboring Ni-Cu dual single-atom sites synergistically weaken the rigidity of the hydrogen-bond networks of interfacial water and optimize the spatial configuration of water molecules surrounding the Ni-Cu dual single-atom sites, which increases the proportion of easily dissociated water species in the interfacial water, thus accelerating the CO2 protonation kinetics during the conversion of CO2 to CO. As a result, Ni-Cu DSAC exhibits a 1.5-fold increase and a 15-fold increase in ECO2RR activity compared to Ni SAC and Cu SAC, respectively. In flow cell electrolyzer, Ni-Cu DSAC achieves almost 100% Faradaic efficiency for CO production (FECO) from applied current density of 50 to 400 mA cm−2, with the optimal full-cell energy efficiency of 61.1% for CO production, reflecting the excellent catalytic performance of neighboring Ni-Cu dual single-atom sites for selective conversion of CO2 to CO. Benefiting from the efficient suppression of carbonates formation in acidic media, Ni-Cu DSAC achieves an outstanding single-pass carbon efficiency of 67.3% for CO2-to-CO conversion at 200 mA cm−2. Additionally, Ni-Cu DSAC also exhibits excellent long-term stability, with less than 10% decay of FECO throughout a 170-h continuous electrolysis in strong acid (pH = 1, j = 200 mA cm−2).

The pursuit of high-energy-density lithium-ion batteries demands high-silicon silicon-graphite composite negative electrodes, yet their commercialization remains hindered by interfacial incompatibility and mechanical instability. While an ideal binder must simultaneously achieve robust adhesion to both silicon and graphite, accommodate substantial silicon volume changes, and maintain high binder bulk stability, existing systems fail to harmonize these requirements. Here, we present a molecularly engineered binder that resolves this trilemma through interfacial-mechanical synergy. By integrating a hydrophobic-soft copolymer and hydrophilic-hard copolymer, our design enables amphiphilic interfacial adhesion and provides mechanical properties specifically tailored to accommodate silicon volume changes. A supramolecular crosslinker further reinforces interchain cohesion, ensuring binder bulk stability during long cycling life. This design enables a 2 Ah-level pouch cell to sustain 500 cycles at 0.3 C with 99.83% average Coulombic efficiency. At a commercial binder loading of 5 wt%, 1 Ah cells deliver over 2000 cycles at 1 C with an average Coulombic efficiency of 99.93%. Our work has the potential to not only resolve the long-standing trade-off between interfacial and mechanical stability in silicon-based negative electrodes but also provide a practical framework for designing next-generation binders targeting energy-dense, durable batteries.

Lithium-rich oxide cathodes present high specific capacities (> 250 mAh g−1) and wide operating voltage windows (2.0–4.8 V), making them promising candidates for next-generation high-energy batteries. Their practical deployment, however, is limited by sluggish ion transport kinetics that arise from inherent structural constraints, including confined two-dimensional diffusion channels, transition metal migration, and local lattice distortions. These structural perturbations narrow Li+ pathways, intensify cation mixing, and generate localized strain fields, collectively increasing the Li+ migration energy barrier. To facilitate the rational design of fast-kinetic lithium-rich oxides through intrinsic structural optimization, a comprehensive elucidation of the structure–diffusion interplay is presented, with emphasis on the roles of lattice distortion and oxygen redox chemistry in modulating Li+ pathways and associated energy barriers. Structural design strategies that aim to improve ionic diffusivity are systematically evaluated, including interface engineering, morphology-directed design, and the modulation of redox chemistry. Advanced operando characterization techniques that capture dynamic structural and chemical evolution are also described as essential tools for guiding precise structure–performance analysis. The mechanistic insights and integrated analytical approaches summarized in this review establish a robust conceptual foundation for engineering lithium-rich oxides with enhanced ion transport kinetics, thereby supporting the advancement of next-generation high-power battery technologies.

The development of high-energy low-cost lithium-ion batteries has sparked interest in ultrahigh-Ni Co-free layered cathodes that offer high capacity, low cost, and environmental friendliness. Yet, their widespread deployment is impeded by the challenges posed by the large magnetic moments of Ni and Mn, as well as the aggregation of the highly spin-unstable high-spin state of Ni3+ at the interface. Herein, an efficient three-in-one strategy of internal Al and external Zr is proposed to achieve an ultrastable single-crystal ultrahigh-Ni Co-free cathode, Li(Ni0.90Mn0.08Al0.02)0.98Zr0.02O2 (NMAZ). The strong AlO6 ligands prevent the formation of high-spin Ni3+. Surface-enriched Zr restricts the diffusion of Ni within the NiO6 octahedron. The single-crystal structure reduces unwanted reactions with the electrolyte. Consequently, NMAZ achieves a favorable unity of material cost and electrochemical performance by reducing the resource expense by >7.5% than conventional Co-containing single-crystal LiNi0.88Mn0.08Co0.04O2 (NMC) and demonstrating excellent calendar lifespan performance. Moreover, it shows better phase stability under high dissociation conditions, alleviates the harmful H2-H3 phase transformation, and avoids the release of lattice oxygen due to the overlap of Co3+/4+ 3d and O2- 2p orbitals upon deep delithiation.

Manganese dioxide (MnO2), known for its low-cost, high-theoretical capacity, and environmental friendliness, has garnered great attention in developing mild aqueous Zn-MnO2 batteries (AZMBs). However, Mn2+ dissolution severely compromises cycling stability and practical viability; moreover, the ambiguity of charge storage mechanisms (e.g., Zn2+ vs. H+) makes the direction of strategic engineering uncertain. Herein, via advanced electron microscopy, we show that the charge storage in MnO2 is dominated by H+ intercalation rather than Zn2+ insertion. Inspired by this finding and by referring to the recipe of proton exchange membrane, we uniformly coat individual MnO2 particles with a proton-selective surface, that is, Nafion, which successfully suppresses Mn2+ dissolution as an "ion filter" and simultaneously facilitates reversible H+ insertion/extraction as a "proton channel". Therefore, the MnO2@Nafion cathode exhibits an outstanding specific capacity (277 mAh g-1 after 100 cycles at 0.2 A g-1) and remarkable cycling stability, retaining 91.7% of its capacity after 3000 cycles at 2 A g-1. These results outperform previously reported manganese-based cathodes, demonstrating the potential of MnO2@Nafion as a high-performance and durable cathode material for AZMBs. This work rationalizes the rising endeavors in the mechanism understanding of MnO2-based aqueous battery systems and provides new insights for developing more sustainable aqueous battery materials.

Layered transition metal oxide cathodes (NaxTMO2) demonstrate a classic type of cathode for Sodium-ion batteries (SIBs), however their practical application faces a long-standing challenge of irreversible phase transitions at high voltages, which causes unsatisfied specific energy and cycling stability, particularly for P-type (Na+ located at prismatic sites) cathodes. This phenomenon is conventionally ascribed to the Na+ re-coordination from prismatic to octahedral (O-type) configuration upon Na+ extraction, whereby the TMO2 slab gliding and abrupt c-lattice change are always coupled, and a straightforward solution to this situation remains elusive. Here, we reveal that, the TMO2 slab gliding and the lattice contraction can be decoupled, and the rapid lattice contraction under high state-of-charge underlies the fundamental origin for the irreversible phase transitions. By pre-engineering 15.8

Microbial catalysts offer compelling advantages for oxygen reduction reaction (ORR) in microbial fuel cell (MFC) cathodes, including reduced costs and extended operational lifespans. However, their practical application remains limited by insufficient intrinsic activity at catalytic protein sites and restricted charge accessibility, both of which constrain ORR kinetics. Here, we report the development of an efficient trifunctional bioendogenous system based on menaquinone-7 (MK-7), enriched from Bacillus subtilis natto (natto digester strain (ND)) through a straightforward fermentation strategy. The engineered MK-7 simultaneously performs three critical functions: (i) facilitating mediated electron transfer between bacteria and electrodes, (ii) regulating the in-situ formation of size-controlled conductive polydopamine nanostructures that enhance direct electron transfer pathways, and (iii) modulating the electronic structure of cytochrome c (Cyt c) to activate its catalytic center and optimize O2 adsorption capacity. Through these synergistic effects, our engineered nano-hybrid ND-FM@sPDA (FM is fermentation and sPDA is size-controlled conductive polydopamine) achieves an oxygen reduction current density of 3.83 mAcm-2, representing a 1.54-fold enhancement over pristine ND (2.48 mAcm-2). MFCs constructed with the ND-FM@sPDA biocathode deliver a peak power density of 412 mu Wcm-2, surpassing previously reported microbial catalysts for similar applications. This work elucidates novel regulatory mechanisms for optimizing biocatalysts at the molecular level and provides critical insights for advancing sustainable bioelectrocatalytic technologies with enhanced performance.

Conventional transfer methods for wafer-scale graphene rely on sacrificial polymer supports and multi-step handling, making them incompatible with thin polymer substrates. Here, we report a one-step thermal pressing approach for graphene transfer, in which spin-coated polyimide serves simultaneously as the transfer medium and the flexible substrate, eliminating the need for sacrificial polymer layers and intermediate handling steps. Under experimentally optimized conditions, the semi-cured PI conformally contacts the graphene and establishes sufficient interfacial adhesion to enable delamination from the copper growth substrate during wet etching. Following transfer, the PI can be mechanically peeled from the rigid carrier to release freestanding flexible devices. This process is compatible with conventional photolithography, as demonstrated by the fabrication of flexible Hall sensors on 3 × 3 cm2 transferred graphene. The resulting devices exhibit an average current-normalized sensitivity of 130 ± 33 V A-1 T-1 and a carrier mobility up to 3640 cm2 V-1 s-1, comparable to devices produced via conventional multi-step wet transfer using graphene from the same batch. This work establishes a scalable route for wafer-scale graphene transfer onto ultrathin flexible substrates without the complexity of sacrificial polymer processing.

Aqueous zinc-ion batteries (AZIBs) face persistent challenges in reversibility, Coulombic efficiency (CE), and long-term cycling stability, primarily due to uncontrolled dendrite growth, parasitic hydrogen evolution reaction (HER), and sluggish desolvation kinetics of hydrated Zn2 + ions. Here, we introduce a zincophobic-hydrophobic synergistic strategy by incorporating a trace amount of tiron (TR) into a 2 M Zn(OTf)2 electrolyte. Contrary to conventional belief that zincophobicity impedes Zn deposition, TR simultaneously addresses all major failure modes. It preferentially adsorbs onto Zn surfaces, effectively blocking low nucleation overpotential sites and thereby guiding Zn2+ to deposit as uniform, petal-like nanostructures rather than dendrites. Concurrently, TR disrupts micelle-like [Zn(H2O)n]2+ solvation clusters via competitive coordination, forming a more labile solvation shell that lowers desolvation barriers and accelerates Zn2+ transport. In addition, the hydrophobic TR layer repels interfacial water, suppressing HER effectively. As a result, Zn||Zn symmetric cells exhibit an ultra-long cycling life of 1520 h (vs. 96 h control), Zn||Cu half-cells achieve a high CE of 98.8 %, and Zn||AC hybrid capacitors retain 95.1 % capacity over 5000 cycles. This work pioneers a generalizable solvation-interface co-engineering strategy that redefines the role of zincophobicity and hydrophobicity in Zn electrochemistry-offering a robust pathway toward high-performance, long-life aqueous zinc-based energy storage systems.

ABSTRACT Aqueous Zn–I2 batteries (AZIBs) represent an efficient energy storage technology, with the emerging four‐electron redox mechanism further enhancing their application value. However, the advancement toward commercial implementation requires addressing key challenges inherent to the electrode–electrolyte interface. Apart from electrode optimization, electrolyte design is a pivotal strategy to tackle the interface issues and an inevitable road to realize the four‐electron redox reaction. In recent years, significant research efforts have been directed toward advancing AZIBs through electrolyte engineering. This review systematically summarizes recent progress in electrolyte‐regulated AZIBs. First, fundamental principles of AZIBs were presented, including their working mechanisms and inherent challenges related to both the zinc anode and iodine cathode. Furthermore, strategies based on functional additives, highly concentrated electrolytes, cosolvents, Zn salts, and hydrogel electrolytes are analyzed to evaluate their effectiveness in optimizing both traditional two‐electron and advanced four‐electron redox systems. After thoroughly discussing the zinc utilization and gas evolution of zinc anode, practical AZIBs configurations, that is, soft‐pack battery, flexible battery, and microbattery, are reviewed. Finally, prospective directions and development strategies are proposed to advance the practical implementation of AZIBs.

Lithium battery performance remains limited by sluggish kinetics, interfacial instability, and mass transport constraints. The application of magnetic fields as a non-invasive physical modulation tool offers a promising paradigm to fundamentally circumvent these pervasive bottlenecks. This review first outlines the fundamental physical principles of magnetic fields to establish the theoretical basis for their functionality in electrochemical systems. Building upon this foundation, we systematically elucidate the role of the magnetic field in addressing multiscale scientific challenges within lithium-based batteries, specifically regarding interfacial dynamics, bulk phase transport, and chemical reactions. Regarding the electrode/electrolyte interface, the magnetic field effectively inhibits lithium dendrite proliferation and stabilizes the solid electrolyte interphase through the homogenization of ionic flux. Within the bulk phase, macroscopic convection induced by the magnetohydrodynamic effect mitigates concentration polarization, while magnetic force facilitates the directional transport of paramagnetic molecules such as oxygen and the targeted capture of detrimental ions. At the reaction level, magnetic modulation inhibits cation mixing via spin-state regulation and accelerates sluggish multielectron reactions. The objective of this review is to clarify the transformative potential of magnetic fields as multiscale and multifunctional regulatory tool for advancing the development of next-generation lithium-based batteries, including lithium-sulfur, lithium-oxygen, and all-solid-state batteries.