Physics

In this work, chiral fibrils are shown to manifest in P(NDI2OD-T2) polymers through the addition of chiral solvents and an off-center spin coating method. The aligned polymeric chains form without a residual chiral solvent in the films, and circular dichroism spectroscopy reveals successful chiral imprinting. Spectroscopic measurements point to rotation of the conjugated polymer backbone, along with modified lamellar stacking, which promotes enhanced crystallinity along the backbone in a chiral fashion. Magneto field-effect transistors (mFETs), composed of chiral conjugated polymers, showed a strong dependence on the orientation of the externally applied magnetic field, leading to a robust asymmetric response in spin polarization current and charge carrier mobility that was sensitive to the handedness of the polymer. These findings are rationalized within the context of the chiral-induced spin-selectivity (CISS) effect. Collectively, this study establishes design strategies for organizing achiral conjugated polymers into chiral assemblies and provides a pathway for their implementation in spintronic device applications.

Abstract Robophysics investigates the physical principles that govern living-like robots operating in complex, real-world environments. Despite remarkable technological advances, robots continue to face fundamental efficiency limitations. At the level of individual units, locomotion
remains a challenge, while at the collective level, robot swarms struggle to achieve shared purpose, coordination, communication, and cost efficiency. This perspective article examines the key challenges faced by bio-inspired robotic collectives and highlights recent research efforts that incorporate principles from active-matter physics and biology into the modeling and design of robot swarms.

Abstract In this article, we analyze the quantum and topological properties of graphene-based plasmonic systems. We consider the following plasmonic materials: single-layer graphene, twisted bilayer graphene, and other graphene stackings, as well as the following architectures: graphenebased gratings, grids, chains of graphene disks, and the kagomé lattice.

Lithium-rich oxide (LRO) cathodes are considered promising candidates for next-generation lithium-ion batteries due to their low cost and high capacity but face challenges of cyclic decay caused by irreversible oxygen loss and structural degradation. Herein, a spinel/disorder heterostructure attached to the LRO surface is demonstrated by quenching high-temperature LROs in a MgCl₂ solution, based on the quenching regulation mechanism discovered from a thermodynamic perspective. High-temperature calcination promotes lattice expansion, weakens metal-oxygen bonds, and generates significant lattice distortion and defects. These metastable structures are effectively preserved by rapid cooling and further optimized by the MgCl₂ solution, ultimately forming a spinel/disorder heterostructure enriched with abundant defects and Mg doping on the LRO surface. This multifunctional interface enhances structural stability and improves the reversibility of oxygen-anion redox reactions, effectively suppressing irreversible oxygen release and interface side reactions. Moreover, the increased d-layer spacing-coupled spinel phase promotes Li⁺ transport, and the quenching-induced Mg doping and Li/O vacancies synergistically stabilize the bulk with an optimized electronic structure. Therefore, the modified LRO has a significantly improved cycling and rate performance as well as suppressed self-discharge. These findings deepen the understanding of quenching engineering of nanomaterials and demonstrate the feasibility of optimizing Li-rich cathodes through a spinel/disorder heterostructure for sustainable energy storage.

Metasurface-based on-chip optical manipulation has attracted increasing attention recently, owing to its potential applications in single-cell analysis, atom cooling, and biosensing. So far, three-dimensional (3D) manipulation platforms based on metasurfaces remain unexplored, limiting the achievable degrees of freedom that are critical for practical applications. Here, we present an on-chip 3D manipulation platform with a multifunctional metasurface by leveraging the photonic spin Hall effect. The metasurface is designed via the combined use of geometric and propagation phases, with spatial multiplexing enabling independent control of different spatial degrees of freedom at distinct wavelengths. By varying the incident polarization or wavelength, the system can switch among four focal positions within a 3D volume, thereby enabling dynamic particle manipulation. Experimental results demonstrate stable and tunable 3D particle control, with lateral and longitudinal displacements of 24.2 and 90 μm, respectively. These results provide a platform for miniaturized 3D optical manipulation and highlight the potential of metasurface-based platforms for efficient on-chip manipulation.

Environmentally adaptive hydrogels undergo reconfiguration under external stimuli, suitable for intelligent sensing, bioinspired actuation, and soft robotics. However, achieving programmable three-dimensional (3D) morphing in homogeneous hydrogels under constant stimuli remains quite challenging despite the tremendous research efforts. Herein, inspired by the directional ion-transport actuation of starfish, supramolecular poly(amic acid) salt (PAAS) hydrogels with predictable 3D structure formation were developed through directional metal ion transport imparted by seawater. These hydrogels were prepared through aqueous polymerization of 3,3',4,4'-biphenyltetracarboxylic dianhydride (s-BPDA) and <i>p</i>-phenylenediamine (PDA) in the presence of organic bases with imidazole moieties (1,2-dimethylimidazole (DMZ), imidazole (IM), and 1-(2-hydroxyethyl)imidazole (HIM)), followed by thermal treatment at 50 °C. The resultant hydrogels, featuring high-density carboxylates, enable programmable 3D shape-morphing under seawater stimulation through spatially asymmetric (Ca²⁺/Mg²⁺)-carboxylate cross-linking and swelling/contraction. The dynamic supramolecular networks provide remarkable reconfigurability, with repeated reconstruction of complex 3D architectures. Specifically, the hydrogels show exceptional stability with low equilibrium swelling ratios (<50%), increased tensile strength (up to 2.1 MPa), and all 180° deformations completed within 70 s. Overall, programming 3D morphologies of homogeneous hydrogels using a single stimulus has potential for advancing shape-morphing engineering.

Radiation therapy induces DNA damage primarily through reactive oxygen species, leading to cancer cell apoptosis. However, intratumoral heterogeneity and spatial dose variations often result in the survival of polyploid giant cancer cells (PGCCs), a therapy-resistant subpopulation characterized by multinucleation, genetic instability, and stem-like features. Particularly in malignant breast cancer, PGCCs contribute to recurrence by adopting a dormant yet invasive phenotype. Despite their clinical relevance, reliable tools to identify or characterize these cells remain lacking. Here, we present a nanomechanical single-cell profiling platform that enables high-resolution mechanomics of radiation-induced PGCCs. Through integrated cytoskeletal imaging and nanoscale stiffness mapping, we identify a distinct mechanical dormancy state, marked by cortical actin remodeling, nuclear enlargement, and biomechanical stiffening. This dormant mechanotype is coupled with suppressed proliferation yet sustained expression of invasion-associated markers, representing a latent therapeutic threat. Our findings position mechanical dormancy as a mechanobiological hallmark of radiation resistance and propose a predictive framework for optimizing radiotherapy thresholds. This platform enables mechanotype-guided stratification and precision-targeted intervention in radiation-refractory cancer.

Origami-inspired materials enable sophisticated three-dimensional (3D) structural designs, yet conventional materials face an intrinsic conflict between strength and flexibility. Herein, foldable bamboo (FB) is fabricated by mimicking the rove beetle wing's microstructure and bidirectional folding mechanism, coupled with a microwrinkling engineering and waterborne polyurethane (WPU) loading strategy to decouple mechanical trade-offs. Selective lignin removal and cellulose framework softening induce rearrangement of the hydrogen bond network, driving microfibril aggregation and formation of surface microwrinkles. These features enhance interfacial friction and mechanical interlocking. Reinforced by WPU penetration and film formation, this multiscale structure (from molecular to macro levels) endows FB with exceptional folding endurance (24,793 cycles, >24× higher than bamboo veneer, BV). Simultaneously, FB achieves a 59.18% increase in transverse tensile strength, 16.06% higher elongation at break, and 54.48% improved bursting strength. These properties, especially folding endurance, not only surpass most biobased materials but also compete favorably with many polymers and metals. Notably, FB further demonstrates enhanced hydrophobicity, tunable light transmittance, inkjet compatibility, and unlimited splicing capability, enabling robust performance under tension, compression, and folding. These advantages underpin FB's large-scale applications in sustainable, sophisticated 3D structural designs, such as packaging, decoration, and outdoor engineering.

Observation of superconductivity, magnetism, and correlated insulating phases driven by the moiré potential in twisted graphene bilayer has opened the exciting new field of "twistronics". Even richer physics is expected if moiré superlattice could be generated on topological insulators; however, until now, experimental studies have been scarce. Here, we demonstrate topological moirés generated by adsorbing a monolayer of noble gas on a topological insulator. By angle-resolved photoemission spectroscopy, we show that the moiré potential replicates the topological surface state and affects it in a way fundamentally different from the trivial states. Replicated Dirac cones generally avoid crossings, except at the time-reversal invariant momenta that remain gapless. This creates van Hove singularities at the moiré Brillouin zone corners, providing the mechanism of enhancing correlations. Indeed, we observe a strong enhancement of the electron-phonon coupling strength that, if properly tuned, might lead to topological superconductivity and Majorana Fermions.

Tunneling nanotubes (TNTs) mediate intercellular exchange of organelles, yet the mechanical basis of cargo transport in these confined structures remains unclear. Here, we combine optical trapping with confocal imaging to quantify lipid droplet (LD) transport in TNTs. Bidirectional LD movement relies on MTs and is driven by kinesin and dynein. Both transport directions exhibit multimotor cooperation, characterized by trimodal anterograde stall forces (∼2.1, 4.2, 6.3 pN; 1-3 kinesins) and bimodal retrograde forces (∼1.5, 2.9 pN; 1-2 dynins), with conserved ∼8 nm step size. Dynein inhibition eliminated higher-order kinesin force peaks and narrowed step distributions, revealing dynamic force coupling between bidirectional motors. Although the highly viscoelastic microenvironment of TNTs reduces the transport speed of LDs, multimotor engagement sustained long-range transport. These findings define a quantitative description of force-dependent motor coordination in TNTs and clarify how confined intercellular structures regulate organelle transport.

Idiopathic Pulmonary Fibrosis (IPF) is a severely irreversible chronic disease affecting approximately 3 million individuals worldwide, with its pathogenic mechanisms remaining incompletely elucidated. Currently, treatment options of IPF are very limited, with only two FDA-approved drugs. The development of innovative therapeutics and advanced delivery technologies represents a pivotal step to overcoming the current clinical challenges of IPF. CO-based gas therapy is recognized as a potential IPF therapeutic strategy. However, a safe and efficient delivery of CO to pulmonary fibrosis tissue remains a challenge, constraining advancements in this field. To address the above issues, a lung-targeted carrier of CO (LTCoCO) was developed in this study by directly encapsulating CO within phospholipid microspheres, leveraging size-dependent pulmonary retention and selective organ targeting (SORT) principles. By regulating the TGF-β1/Smad signaling pathway and exerting anti-inflammatory, antioxidant, and antifibrotic activities, LTCoCOs have demonstrated in vivo inhibition of IPF, resulting in significant recovery from bleomycin-induced pulmonary fibrosis. Mechanistic in vitro studies identified LTCoCOs as potent inhibitors of epithelial-mesenchymal transition (EMT), endothelial-to-mesenchymal transition (E(nd)MT), and fibroblast activation (FA), acting through both canonical and noncanonical TGF-β1 pathways to achieve robust antifibrotic effects. In summary, an LTCoCO-based strategy for IPF inhibition has been established. These findings expand treatment options and provide a theoretical framework for the IPF clinical application of gas therapy.

Type I photosensitizers (PSs), which generate Type I reactive oxygen species (ROS) through the electron transfer pathway and remain effective under hypoxic conditions, provide a promising solution to overcome the oxygen dependence of the currently dominant Type II PSs in photodynamic therapy (PDT). Yet, the lack of a mechanistic framework for designing Type I PSs has made their discovery largely empirical. Here, we present an excited-state-guided molecular design system that treats key excited-state properties, low first triplet-state (T₁) energy, and a small singlet-triplet (Δ<i>E</i>_ST) energy gap as joint optimization objectives to suggest candidates with Type I characteristics. Starting from 147 molecular fragments, the system generates 713 candidate molecules designed for Type I behavior. Two representative molecules (NIDPP and NAAID) are further synthesized and experimentally validated, both exhibiting robust superoxide anion (O₂^•-) radical production, thereby confirming Type I behavior. This study demonstrates that the excited-state-guided molecular design strategy is effective toward the discovery of next-generation PSs for hypoxia-resilient PDT.

The integration of two-dimensional materials into van der Waals heterostructures provides a powerful strategy for developing advanced optoelectronic devices. Nevertheless, efficient photodetection remains challenging, as it demands precise management of carrier dynamics in terms of effective dissociation of excitons and rapid transport of charges across the heterointerfaces. Herein, we demonstrate a sandwich-type InSe/graphene/MoTe₂ heterostructure by employing a band structure engineering strategy. The graphene interlayer establishes a step-like band alignment, thus promoting efficient separation and transport of photogenerated carriers at the interfaces. Consequently, alongside a prominent improvement in carrier mobility, the InSe/graphene/MoTe₂ photodetector exhibits a fast photoresponse with a rise/fall time of 2.87/3.68 μs, 2 orders of magnitude faster than its bilayer InSe/MoTe₂ counterpart. Furthermore, the InSe/graphene/MoTe₂ photodetector is employed in imaging and optical signal encoding/decoding, demonstrating its potential for low-error-rate data transmission in the near-infrared region. This study opens new avenues for developing high-performance optoelectronic devices through interlayer band alignment engineering.

Solvated electrons are strong homogeneous reducing agents, and their generation with visible light can unlock new redox chemistry. Water imposes a high photoemission energy barrier for gold, restricting the accessible spectral window for plasmon-mediated solvated electron generation to the near-ultraviolet region. Here, we first demonstrate that by using hexamethylphosphoramide, an organic solvent that supports large applied cathodic potentials without decomposition, the photoemission threshold is lowered to provide access to the entire visible spectrum. Next, we achieve solvated electron yields up to 150-fold higher with coupled plasmon modes from clustered gold nanoparticles, as compared to a smooth gold electrode. The observed quantum yield correlates with the local electric field enhancement by gap plasmon modes for these nanostructured electrodes as identified by varying the particle density. Overall, this study offers mechanistic insights into how coupled plasmon modes and threshold optimization can be used to enhance solvated electron generation with visible light.

Owing to well-defined topologies and structural orderings, metal-organic frameworks (MOFs) can serve as a prototype platform for designing new energy materials with predesigned structures for efficient energy and electron transfer. This study explores the photoinduced electron transfer dynamics of monoanionic radicals within two different UiO-type MOFs, distinguished by their degree of interpenetration. In 0-MOF, which has relatively large pores (18.6 Å), electron transfer is primarily facilitated by solvent-assisted electron hopping, with dimethylformamide (DMF) molecules serving as bridges between naphthalenediimide (NDI)-based ligands. In contrast, the smaller pores (12.1 Å) of 100-MOF admit only one or two DMFs, favoring direct through-space electron transfer between neighboring NDI units. This comparative study highlights the role of pore size and intermolecular interactions in governing the electron transfer mechanisms within MOFs. These findings contribute to a better understanding of the photophysical properties of MOFs and open new avenues for their potential use in future energy applications.

Li metal is a promising anode for high-energy-density batteries, suffering from rapid capacity fading and uncontrolled volume expansion. Herein, an innovative method is employed to fabricate a 3D current collector. Laser processing is used to form through-holes on ultrathin Cu foil, which is integrated with Cu foam by one-step stacking. A hybrid copper composite (HCC) current collector is constructed efficiently. Through-holes serve as guided channels, promoting inward deposition to the bottom Cu foam. Owing to the high surface area and interconnected porous network, Cu foam offers ample space and reaction interfaces. A synergistic effect enables precise regulation of deposition behavior, effectively suppressing uncontrolled dendrite growth and volume expansion. The HCC half cell enables stable Li plating/stripping for 580 cycles with CE exceeding 98.2% at 0.5 mA cm^-2. For a full cell assembled with a commercial LiFePO₄ cathode, it maintains an 82% capacity retention rate after 280 cycles at 2 C, providing a promising pathway toward practical applications.

The syntheses of solid-solution alloys consisting of elements with large redox-potential differences remain significant challenges. In this work, by a slow synthesis method, we precisely controlled the reduction, nucleation, and growth processes of Au and Os and successfully synthesized homogeneous Au_<i>x</i>Os_1-<i>x</i> solid-solution NPs for the first time, which cannot mix with each other over most composition ranges up to 3000 °C. The reaction-area confinement effect in the spray method was proved to be favorable for preventing Au phase segregation. In NO_<i>x</i> reduction tests, Au_0.1Os_0.9 NPs showed much higher activity with a temperature at 50% conversion (<i>T</i>₅₀) of 239 °C than the state-of-the-art monometallic Rh catalysts (<i>T</i>₅₀ of 267 °C). Based on <i>in situ</i> Fourier transform infrared measurements and density functional theory calculations, the modifications of Os electronic states via Au alloying significantly enhanced CO and NO activation at Os sites, leading to the excellent NO_<i>x</i> reduction catalytic activities for Au_<i>x</i>Os_1-<i>x</i> solid-solution NPs.

ABSTRACT Hydrogel–based evaporators have long been regarded as star materials in the field of photothermal interfacial evaporation owing to their remarkable performance. However, achieving the synergistic optimization of water–state regulation and structural stability remains a highly appealing yet challenging goal. In this work, a multifunctional photothermal evaporator was designed by incorporating MXene nanosheets and magnesium ions (Mg 2+ ) into a poly(vinyl alcohol) (PVA) hydrogel matrix, which was subsequently anchored onto a nonwoven fabric substrate. Density functional theory (DFT) calculations reveal that Mg 2+ forms stable hydrated coordination structures on MXene surfaces, achieving a favorable balance between water–binding strength and electronic coupling, thereby enabling effective water–state regulation and energy transfer. Finite element simulations further demonstrate that a 10° inclination of the evaporator relative to the water surface markedly enhances light harvesting and vapor diffusion. As a result, the as–prepared PFMs evaporator achieves an evaporation rate of 3.88 kg·m −2 ·h −1 under 1 sun, ranking among the high–performing hydrogel–based evaporators reported to date while exhibiting excellent long–term stability. Large–scale tests using a 100 cm device verify its good scalability. This work provides a feasible strategy for developing efficient, durable, and scalable solar evaporators.

ABSTRACT Lightweight, high strength and toughness, outstanding thermal conductivity, and superior shielding effectiveness (SE) are critical yet challenging to achieve simultaneously in advanced electromagnetic interference (EMI) shielding materials. Herein, by integrating aramid nanofibers (ANFs) and silver nanowires (Ag NWs) into a highly dense, well‐aligned bilayer‐packed cross‐layer structure featuring an Ag NW top layer, simultaneously improved tensile strength (366 MPa), toughness (78 MJ m −3 ), electrical conductivity (11,363 S cm −1 ), in‐plane thermal conductivity (10.4 W m −1 K −1 ), and EMI SE (71 dB) are achieved. Notably, the EMI SE per unit thickness reaches 59,167 dB cm −1 . Additionally, the densified bilayer structure of the Ag NW‐ANF film endows it with remarkable resistance to bending fatigue, ensuring operational reliability in practical applications. The comprehensive performance of this nanocomposite film is superior to that of pure ANF, single‐layer Ag NW‐ANF, bilayer Ag NW‐ANF, and previously reported EMI‐shielding nanocomposites. Thus, the outstanding multifunctional performance of this nanocomposite film makes it a competitive candidate for EMI‐shielding materials in advanced electronic devices.

ABSTRACT Flexible magnetoelectronics face a major challenge in maintaining functionality under mechanical strain. This research investigates how biaxial multicracking affects the magnetic properties of nanometric thin films, specifically by separating magnetoelastic from magnetostatic effects. Using a unique experimental platform, we show that in magnetostrictive Co films, the magnetic behavior is dominated by stress‐induced magnetoelastic effects. In contrast, in non‐magnetostrictive films, the magnetic changes only appear once multicracking begins, allowing us to demonstrate the magnetostatic contributions from fragmentation. Our findings reveal that the variation in the saturation field correlates directly with fragment shape. This work demonstrates that fragmentation is not just a failure mechanism but a controllable process whose magnetic effects can be understood and leveraged for designing next‐generation flexible devices.

ABSTRACT Self‐assembled monolayers (SAMs) are widely used in inverted perovskite solar cells (PSCs) due to their high hole mobility, excellent interfacial modification capability, and low‐cost fabrication processes. However, conventional SAMs suffer from molecular aggregation during film formation, leading to non‐uniform and low coverage issues, which ultimately hinder the enhancement of PSCs performance. Herein, this work presents a strategy to tackle this challenge through the modification of [4‐(3,6‐dimethyl‐9H‐carbazol‐9‐yl)butyl]phosphonic acid (Me‐4PACz) with O‐Phospho‐L‐tyrosine (OPLt) molecules. The aggregation of Me‐4PACz molecules is suppressed through disrupting Me‐4PACz dimers and reducing the intermolecular π‐π stacking, while the anchoring sites for the SAM layer on the NiO x substrate are optimized, facilitating enhanced interfacial contact and consequent perovskite crystallization. Eventually, PSCs based on the Co‐SAM show a performance improvement, with a power conversion efficiency (PCE) of 26.03%. Meanwhile, the device stability has been effectively enhanced, with the efficiency retaining 81.90% of its initial value after 1200 h of continuous one‐sun illumination. This work focused on the coverage and film quality of hole transport layers and demonstrated a molecule‐assisted dispersion strategy toward high‐efficiency and stable PSCs.

ABSTRACT The pursuit of energy‐dense lithium metal batteries (LMBs) is often compromised by the catastrophic safety risks of flammable polymer electrolytes. Herein, we propose a hierarchical design paradigm for a 20‐µm‐thick composite solid electrolytes (CSE) that orchestrates high ionic influx and intrinsic safety management. This architecture integrates a thermally‐triggered molecular “firewall” composed of trimethyl phosphate (TMP) confined within HKUST‐1 metal‐organic frameworks (HKUST@TMP) and a rigid polyethylene terephthalate mechanical scaffold within the thin‐layer poly(ethylene oxide) (PEO) membrane formation. Notably, the HKUST‐1 framework effectively isolates chemically active TMP from the lithium anode under operating conditions to preserve interfacial integrity on the Li anode, while precisely releasing TMP to scavenge reactive radicals upon thermal abuse (&gt;120°C). Consequently, the as‐formed 20 µm CSE achieves the balanced mechanical strength (25.54 MPa), high ionic conductance (234 mS at 30°C), enhanced Li + transference number of 0.71 as well as the superior flame retardancy with a limiting oxygen index of 24.3%. This controlled‐release strategy enables the LiNi 0.8 Mn 0.1 Co 0.1 O 2 |Li pouch cell to deliver a competitive gravimetric/volumetric energy density of 368.2 Wh kg −1 /693.9 Wh L −1 , together with verified thermal abuse tolerance under the GB/T 31485–2015 protocol, providing a new roadmap for the next generation of safe, high‐energy‐density energy storage.

ABSTRACT Sodium‐ion batteries (SIBs) are gaining limelight for research owing to their large‐scale, all‐climate energy storage, yet their practical application remains plagued by unreliable performance at low temperatures. A key reason is the lack of cathode materials that can preserve both structural stability and ion‐transport kinetics under deep subzero conditions. Here, we report a hydrogen‐bonded organic framework (HOF) cathode for SIBs, HOF‐PZQ, with a rigid π‐conjugated backbone reinforced by an extensive network of directional O─H···O hydrogen bonds. HOF‐PZQ combines framework‐level structural coherence with adaptive supramolecular response, enabling stable Na + storage under deep subzero conditions where conventional organic cathodes often suffer from kinetic degradation and structural instability. As a result, HOF‐PZQ delivers stable cycling for 5000 cycles at 1 A g −1 at room temperature. Even at −40°C, it achieves a reversible capacity of 105 mAh g −1 , with 98% capacity retention after 1000 cycles at 100 mA g −1 . We demonstrate that Na + insertion and extraction occur at the C═N redox sites and are accompanied by reversible reorganization of the hydrogen‐bond network, which accommodates local electrostatic stress without loss of long‐range crystallinity. This work highlights HOFs as promising cathodes for reliable sodium‐ion storage in harsh cold environments.

ABSTRACT Coupling the oxidation of 5‐hydroxymethylfurfural (HMF) with the hydrogen evolution reaction can simultaneously reduce the energy barrier of HMF oxidation reaction and yield value‐added products. Nickel‐based catalysts demonstrate outstanding activity toward C─H bond activation, which is typically the rate‐determining step in the HMF oxidation reaction. However, their catalytic performance is often constrained by the sluggish formation of active sites and weak adsorption of organic reactants. In this study, we synthesized the Sr 0.1 Ni 0.9 (OH) 2 catalyst and investigated how carbonate ions in electrolytes promote the electrooxidation of HMF via proton‐coupled electron transfer (PCET). The comprehensive characterizations and density functional theory calculations collectively demonstrate that Sr incorporation effectively modulates the interfacial electronic structure and enhances carbonate adsorption, thereby facilitating PCET through a restructured interfacial hydrogen‐bond network that enhances proton relay efficiency. The Sr 0.1 Ni 0.9 (OH) 2 catalyst exhibits enhanced catalytic activity, delivering a Tafel slope of 29 mV dec −1 and a Faradaic efficiency of ∼90% for the production of 2,5‐furandicarboxylic acid. This work presents a cooperative catalyst–electrolyte strategy to modulate interfacial interactions, offering new avenues for ion‐regulated electrocatalysis in sustainable energy conversion applications.