Physics

ABSTRACT Sensory‐neuromorphic computing endows wearable devices with capabilities of environmental perception and active service, acting as a pivotal driver for the revolution in human–computer interaction. However, its implementation in textile electronics is hampered by incompatibility between conventional electronic device structures and the fabric‐woven manufacturing methodology. Here, we demonstrate a tactile‐neuromorphic interface integrating a textile‐type resistive random‐access memory (RRAM) array for constructing human–machine sensing‐computing interactive systems. The 3D stacked TiO 2 /Ti 3 C 2 T x textile RRAM exhibits an order‐of‐magnitude reduction in switching voltage (85 mV) compared to prevailing counterparts, ultra‐stable resistive switching over 10 3 operation cycles with ultralow 1.15% LRS coefficient of variation, ideal for actualizing weavable neuromorphic computing. An all‐textile integrated near‐sensor computing system, featuring monolithically co‐integrated pressure sensor and RRAM arrays, demonstrates quasi‐linear conductance modulation under pressure stimuli, allowing for the embedded computation‐memory nodes knitted into garment textiles to achieve in situ tactile processing for contactless vehicular maneuvering. This work demonstrates the potential to integrate an embedded sensing‐logic‐memory electronic device into smart textiles, propelling a transformative paradigm shift in human–machine interaction.

ABSTRACT Constructing robust nanofibrillar networks in layer‐by‐layer (LbL) organic solar cells (OSCs) is challenging since small‐molecule acceptors lack polymer‐like interlocking capabilities. Herein, we propose a topology‐driven strategy using bulky siloxane‐terminated side chains to induce fibrillation. We synthesized asymmetric acceptors BTP‐2Ph and BTP‐3Ph by substituting one alkyl chain of L8‐BO with diphenylmethylsilyl and triphenylsilyl groups, respectively. We reveal a size‐dependent competition between steric hindrance and intermolecular interlocking. The bulkier triphenylsilyl group in BTP‐3Ph provides strong interlocking that overrides steric‐induced crystallinity loss, driving the formation of an interconnected acceptor nanofibrillar network. This creates an ideal dual‐fiber morphology with the D18 donor. Consequently, the D18/BTP‐3Ph device achieves an impressive 20.31% efficiency, significantly outperforming L8‐BO (19.28%). Crucially, this physically interlocked framework kinetically freezes the optimal phase separation, enabling excellent operational stability with 85% initial efficiency retention after 650 h of continuous one‐sun illumination.

ABSTRACT The practical implementation of two‐dimensional (2D) transistors is fundamentally limited by the lack of gate dielectrics that can simultaneously deliver a high dielectric constant, a wide bandgap, strong breakdown strength, and long‐term environmental stability‐an often‐overlooked yet critical requirement for reliable device integration. Here, we report 2D single‐crystalline TbOCl nanosheets as gate dielectrics that uniquely reconcile these competing demands. TbOCl exhibits a high dielectric constant (12.5), an ultrawide bandgap (∼6.6 eV), and a high breakdown field (11.9 MV cm −1 ). MoS 2 field‐effect transistors (FETs) gated by TbOCl exhibit excellent electrostatic control, yielding a near‐ideal subthreshold swing of 72 mV dec −1 , a small hysteresis of only 8 mV, and an ultra‐low gate leakage current of ∼10 −13 A. Notably, TbOCl‐based devices maintain ultrastable electrical performance after more than 9 months of ambient storage with negligible performance degradation. The superior stability originates from an intrinsic dual‐antioxidation mechanism that effectively suppresses oxidative degradation of the dielectric. Furthermore, logic inverters fabricated with TbOCl gate dielectrics exhibit fast switching behavior, with rise and fall times of 80 and 16 µs, respectively. Together, these results establish TbOCl as a stable, high‐performance 2D dielectric platform, offering a viable pathway toward reliable 2D electronic devices.

ABSTRACT Two‐dimensional (2D) indium selenide (InSe) has attracted considerable interest due to its superior ballistic transport properties, superplasticity, and thermoelectric properties. Ferroelectricity and a variety of other intriguing physical characteristics. These arise from its van der Waals (vdW) layered structure, interlayer coupling, and intralayer interactions. The vibrational modes of 2D InSe are highly sensitive to thickness. The phase transitions in 2D materials, which are critical to their properties and applications, are closely related to interlayer and intralayer vibrations. However, the effect of the thickness on these vibrational behaviors during phase transitions remains insufficiently understood. In this study, we investigate the Raman spectra of β ‐InSe with layer numbers (LN) ranging from 4 to 33 under high pressure and construct a pressure LN phase diagram. Unexpectedly, due to the quantum confinement and defect effects, InSe flakes with fewer layers require more energy to undergo phase transitions which is confirmed by PL experiments and DFT calculations, irrespective of whether pressure is being increased or decreased. This research establishes a solid foundation for exploring and characterizing interlayer and intralayer lattice dynamics through pressure engineering in vdW materials.

ABSTRACT Near‐infrared (NIR) mechanoluminescence (ML) materials that directly convert mechanical stimuli into optical signals are highly desirable for mechanically adaptive optoelectronics. To date, however, this field has been overwhelmingly dominated by Cr 3+ ‐based phosphors, whose emission relies on piezoelectric‐field‐driven excitation. While effective in rigid inorganic hosts, such systems suffer from pronounced performance degradation when transferred into flexible matrices, resulting in poor repeatability, limited cyclic stability, and restricted applicability. Here, we move beyond the Cr 3+ paradigm by introducing Bi 2+ as an alternative and fundamentally distinct activator for flexible NIR ML. By incorporating a newly developed Sr 3 (BO 3 ) 2 :Bi 2+ phosphor into a polydimethylsiloxane (PDMS) matrix, a chromium‐free NIR ML elastomer is developed, leveraging a triboelectrification‐induced interfacial charge transfer mechanism to achieve robust broadband emission peaking at 815 nm under diverse mechanical excitations. The composite demonstrates highly repeatable and cyclically stable NIR ML over 10,000 continuous stretching cycles, with an impressive initial power density (29.0 mW·m −2 ) and self‐recovery behavior (24.1%@1 min and 91.5%@24 h). Notably, its initial ML intensity exceeds that of state‐of‐the‐art Cr 3+ ‐based counterparts (e.g., Ga 2 O 3 :Cr 3+ /PDMS) by more than 2.2‐fold, while simultaneously exhibiting markedly enhanced cyclic stability. This work presents a chromium‐free, self‐powered, and self‐recoverable NIR ML system, paving the way for mechanically adaptive optoelectronic devices.

Silicon nitride (SiNx), an effective barrier layer in advanced electronic devices thanks to its exceptional resistance to both chemical and environmental degradation, is typically deposited via plasma-enhanced atomic layer deposition (PE-ALD). Among various plasma configurations, very high-frequency (VHF) plasma sources have attracted significant interest for the deposition of SiNx because of their potential to enhance film density and conformality, as well as to minimize substrate damage. Additionally, since the precursor properties play an important role in determining the growth behavior and quality of thin films, exploring various precursors is essential for optimizing SiNx deposition. Therefore, in this study, we introduce [SiHN(CH3)2CH3]2NH (bis(dimethylaminomethylsilyl)amine; NSi-01) as a dual-Si atomic precursor for VHF PE-ALD and compare it with two conventional counterparts─[(CH3)3CNH]2SiH2 (bis(tert-butylamino)silane; BTBAS) and SiH2[N(CH2CH3)2]2 (bis(diethylamino)silane; BDEAS). A comprehensive analysis of the dual-Si atomic structure and adsorption mechanism of NSi-01 reveals that only one methyl ligand actively participates in surface reactions. This distinctive adsorption behavior yields SiNx with a lower dielectric constant and better electrical characteristics compared to those obtained from BTBAS and BDEAS. These results provide a key understanding of the precursor selection that influences the properties and quality of thin films deposited via VHF PE-ALD.

Lithium nitrate (LiNO3) can be preferentially reduced on Li metal to induce an inorganic-rich solid–electrolyte interphase (SEI) (e.g., Li2O/Li3N), making it an effective handle to regulate Li-metal interfacial chemistry. However, the extremely low solubility of LiNO3 in conventional low-donor-number carbonate electrolytes prevents LiNO3 from evolving beyond an additive, whereas high-donor-number solvents that dissolve LiNO3 typically suffer from insufficient oxidative stability at high voltages, limiting their compatibility with Ni-rich cathodes (e.g., NCM811). Herein, we developed a LiNO3-based electrolyte that simultaneously delivers high-voltage stability and high LiNO3 solubility via synergistic anion-coordination regulation using an oxazolidinone solvation platform, a tunable cosolvent, and a fluorinated dilution. Specifically, the introduction of TTE (1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether) increases the fraction of anion-paired species and strengthens NO3– coordination in the solvation sheath. This solvation reconstruction promotes the transition from monodentate to bidentate NO3– coordination, thereby favoring nitrate-derived interfacial reduction. The optimized electrolyte enables >3000 h stability in Li||Li symmetric cells, 97.64% average Coulombic efficiency (CE) in Li||Cu cells, and 83.44% capacity retention after 500 cycles at 4.3 V (1C) in Li||NCM811 cells, offering a practical design paradigm for LiNO3 electrolytes that combine high solubility with high-voltage stability.

Navigating the multifaceted compositional landscape of quinary thermoelectric (TE) materials via classical trial-and-error is impractical due to high labor and material costs. To address this, we present an AI-guided methodology to accelerate the discovery of high-performance Zintl phases in the Ca9–xEuxZn4.5–yCuySb9 system, leveraging a synergistic Eu–Cu cosubstitution strategy. Three machine learning (ML) models were developed to predict electrical conductivity, Seebeck coefficient, and thermal conductivity, enabling systematic screening for a high figure-of-merit, ZT value. Experimental validation confirmed the orthorhombic Ca9Mn4Bi9-type crystal structure for the title compounds, with Eu showing a strong site preference for the interlayer A4 site. This substitution, combined with charge compensation of Cu+ for Zn2+, increased interstitial site occupancy, enhancing anionic framework connectivity and charge transport. Density functional theory and crystal orbital Hamilton population analyses also indicated that cosubstitution optimized interatomic interactions, yielding simultaneous enhancements in σ and S via boosted carrier mobility. A maximum ZT of 0.60 at 810 K was achieved for Ca8.5Eu0.5Zn4.4Cu0.1Sb9, a substantial improvement over the ternary parent Ca9Zn4.5Sb9, that aligned with ML predictions within a 7.7% margin. This work demonstrated that an integrated AI-experimental workflow effectively bridged the gap between ML prediction and the realization of high-performance TE materials.

For centuries, scientists have been captivated by the way molecules arrange themselves in the rigid beauty of crystals. Polymorphism, the ability of a compound to crystallize in more than one distinct lattice, is a central property of crystals as structure controls every material property relevant to their manufacture, durability, and performance. In the special case of active pharmaceutical ingredients, polymorph selection determines essential behaviors that range from solubility and hygroscopicity to tableting and long-term stability. Recent advances in molecular thermodynamics and analytics have radically expanded our understanding of polymorphic free energy landscapes. This review provides a comprehensive synthesis of up-to-date theoretical foundations of the relative stability of different polymorphs of a compound. Drawing on real-world case studies, we discuss challenges related to evaluation of crystal form stabilities. We conclude by highlighting necessary prospective developments in the fundamental understanding of polymorphism that focus on the roles of solvents, conformational variability, and entropy, and in the experimental approaches such as automation and the use of artificial intelligence.

Ribociclib (RBC), an antitumor drug, is categorized as a BCS Class IV drug with low solubility and permeability. Despite achieving clinically relevant bioavailability in its marketed malate salt form, the limited aqueous solubility of RBC still poses significant challenges for formulation development. In this work, three novel RBC salts with nonsteroidal anti-inflammatory drugs (diclofenac, DIC; ibuprofen, IBU; loxoprofen, LOX) were successfully synthesized and comprehensively characterized. Among them, compared with pure RBC, the multicomponent RBC-LOX salt showed 2.97-fold higher solubility and 1.90-fold faster dissolution rate in pH 7.4 buffer, and 1.73-fold stronger in vitro cytotoxicity against MDA-MB-231 breast cancer cells. Moreover, in vivo pharmacokinetic evaluations revealed that the RBC-LOX salt significantly improved the oral bioavailability of RBC (1.49-fold), demonstrating enhanced bioavailability. Overall, these findings highlight the potential of RBC-NSAID salts as a strategy to enhance the solubility, anticancer activity, and bioavailability of ribociclib, offering a promising approach for optimizing its therapeutic efficacy.

Nitrogen-doped carbon catalysts are promising metal-free candidates for the oxygen reduction reaction (ORR). However, the identification of genuine active species remains challenging due to the complexity of local N environments, where the role of lactam has long been overlooked. Herein, N-doped nanodiamond (NND) and carbon nanotubes (NCNT) as metal-free model catalysts are fabricated for ORR. Spectroscopic analyses and temperature-programmed desorption (TPD) measurements reveal the dominance of lactam in an sp3-hybridized carbon framework of NND, whereas NCNT is mainly composed of pyridinic and graphitic N, providing clear chemical tools for active site investigation. Through electrochemical Coulombic screening experiments, it was demonstrated that ORR on NND mainly proceeds via lactam-derived cationic N intermediates, while NCNT could expedite the reaction through anionic intermediates associated with pyridinic N. Further postreaction characterizations evidence the formation of cationic N+ in NND, which interacts strongly with neighboring carbon atoms (e.g., C–O−) to participate in ORR actively. Taken together, this work not only highlights the pivotal role of cationic lactam N toward ORR but also gives insights into the future design of metal-free carbon catalysts via fine N engineering.

Two-dimensional transition metal chalcogenides have attracted significant interest for advanced functional materials due to their tunable electronic structures and polymorphic phase transitions. However, achieving dynamically switchable room-temperature ferroelectricity remains a significant challenge. Here, we demonstrate that Ar+ ion beam irradiation induces controlled Te vacancies in monolayer 2H-MoTe2, triggering robust out-of-plane ferroelectric polarization at 300 K. Through polarization-resolved second-harmonic generation (SHG) microscopy and low-temperature spectroscopic characterization, we verify the ion-beam-induced symmetry breaking and the formation of nonuniform ferroelectric domains with switchable polarization states. Comprehensive switching spectroscopy piezoresponse force microscopy (SS-PFM) with rigorous artifact mitigation reveals reversible 180° polarization switching, confirmed by characteristic phase hysteresis and symmetric amplitude butterfly loops. Crucially, polarity-dependent linear sweep voltammetry (LSV) demonstrates that hydrogen evolution reaction (HER) activity can be reversibly modulated by polarization switching: positive poling reduces the overpotential, while negative poling degrades it, establishing a direct causal link between ferroelectric state and catalytic performance. Remarkably, this defect-engineered ferroelectric polarization modifies the interfacial charge distribution, optimizing the hydrogen adsorption free energy (ΔGH*) from 1.86 eV (pristine) to −0.27 eV (irradiated), thereby significantly enhancing the hydrogen evolution reaction (HER) activity. This work establishes ferroelectric polarization as a primary descriptor for electrocatalytic enhancement and provides a defect-engineering strategy for designing adaptive nanocatalysts.

The shuttling effect of lithium polysulfides (LiPSs) and sluggish redox kinetics are the primary obstacles hindering the commercial application of lithium–sulfur (Li–S) batteries. Most existing studies on two-dimensional-layered material-based sulfur hosts mainly focus on bulk electronic modulation, ignoring the impact of crystal growth geometry on the electrochemical performance. Herein, we designed carbon-cloth-supported, vertically oriented bismuth selenide with preferentially exposed (006) crystal planes (denoted as v-Bi2Se3@CC) as the sulfur host for Li–S batteries. Benefiting from the vertical structure, abundant active sites are exposed and a three-dimensional network is constructed to facilitate efficient mass transport, while the exposed Se active sites on the (006) planes reduce the reaction energy barrier of LiPSs conversion. Consequently, the Li–S batteries assembled with v-Bi2Se3@CC deliver a high specific capacity of 1396 mAh g–1 at 0.2 C, excellent cycling stability with a capacity fading rate of 0.058% per cycle over 500 cycles at 2 C, and a favorable performance even under a high sulfur loading of 11.3 mg cm–2. This work demonstrates that crystal orientation engineering is an effective strategy to optimize sulfur hosts, providing insights for the development of high-performance Li–S batteries.

An important obstacle to long-term hydrogen sustainability is the lack of efficient and stable non-noble-metal catalysts for hydrogen generation through water electrolysis. Cobalt phosphides have emerged as earth-abundant catalysts for the hydrogen evolution reaction (HER), and its activity can be augmented by admixing synergistic elements to produce heteroatom-doped catalysts. Herein, we report an integrated computational and experimental study leading to the synthesis of Co1–xMnxP nanocrystals (NCs) displaying superior activity and stability for the alkaline HER compared to the benchmark Pt/C catalyst at higher current densities (j ≥ −35 mA/cm2). Density functional theory calculations predicted that Mn doping modulates the hydrogen adsorption energies (ΔGH) of orthorhombic CoP toward thermoneutral values. Accordingly, a series of Co1–xMnxP NCs (x = 0.038–0.169) with control over structure, morphology, and composition was produced via colloidal synthesis. Physical characterization of Co1–xMnxP NCs revealed an orthorhombic structure, pseudospherical morphology, and average diameters of ∼5.7–10.2 nm. The incorporation of Mn caused significant modulation of the electronic structure prompting a decrease in Co(2p) and P(2p) binding energies, suggesting an increase in electron density on both surface sites. Among NCs investigated, Co0.909Mn0.091P composition displayed the highest HER activity with an overpotential (η–10) of 136.29 mV at j = −10 mA/cm2, consistent with composition-dependent ΔGH studies. With a Tafel slope of 65.77 mV/dec, Co0.909Mn0.091P NCs showed similar kinetics to the Pt/C catalyst (62.31 mV/dec), indicating the Volmer-Heyrovsky HER mechanism. The highest-performing Co0.909Mn0.091P NCs showed a prominent increase in electrochemically active surface area and significantly lower charge transfer resistance compared to parent CoP NCs. The Co0.909Mn0.091P NCs showed exceptional stability in alkaline media compared to CoP NCs and commercial Pt/C catalysts. Co0.923Mn0.077P, Co0.909Mn0.091P, and Co0.831Mn0.169P compositions displayed superior HER activity and stability compared to monometallic CoP NCs suggesting that dopant-induced compositional and surface modification is an effective strategy for designing high-efficiency, durable nanostructures for numerous heterogeneous (electro)catalytic studies.

Nanothermites offer the dual advantages of high energy density and exceptional reactivity, making them highly promising for advanced energetic applications such as aerospace and microelectromechanical systems (MEMS). However, their mass transfer efficiency is hindered by nanoparticle agglomeration. Achieving structurally modified nanothermites with large, controllable interfacial contact without sacrificing energy release is challenging. To address this issue, we propose a strategy to mediate the heterogeneous growth of metal–organic frameworks (MOFs) on nanoaluminum (nano-Al) using layered double hydroxides (LDHs). The resulting Al@porous metal oxide (Al@pMO) from Al@MOF maximizes interfacial contact without introducing interlayers. The composition of Al@pCuO derived from Al@HKUST-1 is precisely adjusted by varying the feed rate of HKUST-1. Uniform growth of HKUST-1 thin films on nano-Al at high feed rates results in a sub-10 nm layer thickness in 10% Al@HKUST-1. Lower feed rates promote MOF growth to encapsulate nano-Al. Al@pCuO with 33 wt % CuO demonstrates a 3-fold enhancement in energy release in argon compared to Al/CuO mixtures, achieving 78% of the theoretical heat release. The growth mechanisms of LDH and MOF are further discussed. Notably, 10% Al@pCuO with an extreme equivalent ratio (Φ = 48.9) is successfully ignited, indicating more efficient mass transfer. The larger flame areas and higher dynamic pressures of Al@pCuO compared to Al/CuO mixtures highlight its enhanced energetic performance. This strategy provides a solution to the dilemma of interfacial contact and energy release. Al@pCuO with highly efficient energy release and precisely adjustable compositions shows excellent potential for MEMS and aerospace applications.

Interfacial bubbles in two-dimensional semiconductors can generate large, spatially varying strain fields for deterministic band-structure and exciton engineering. Here we develop reproducible bubble platforms in few-layer (1–3L) WS2 using controlled exfoliation onto Au films and artificial PDMS spherical caps. The resulting tensile strain induces strong, layer-dependent reconstruction of excitonic pathways. Monolayer WS2 exhibits up to ∼150 meV direct band gap tunability and enhanced trion emission via strain-gradient-driven carrier funneling. In bilayers, strain enhances and redshifts the indirect exciton emission by reordering valley-mediated recombination channels. In trilayers, strain activates momentum-forbidden or dark-exciton-related states and modifies competing indirect recombination pathways. These results establish bubble-induced strain as a programmable route to exciton control and band-structure engineering in two-dimensional semiconductors.

Multinary metal oxide photoelectrodes remain fundamentally limited by poor charge transport despite theoretical promise for solar fuel production. α-SnWO4 exemplifies this challenge: while density functional theory predicts highly anisotropic charge transport with orientation-dependent band-edge positions, synthetic barriers to achieving phase-pure films with controlled crystallographic orientation have prevented its exploitation. Here, we demonstrate that rapid thermal processing (RTP) of pulsed-laser-deposited films overcomes these synthetic limitations, creating percolation networks of co-oriented grains. Multiscale characterization reveals that aligned crystallographic orientations produce well-aligned band edges, lowering contact potential difference by 0.35 eV and enhancing the local conductivity by more than 2 orders of magnitude compared to furnace heating (FH). These results directly correlate enhanced transport properties with previously reported improved photoelectrochemical performance of the RTP-treated films compared to those treated by FH and suggest a microscopic mechanism for this improvement. Our findings establish that controlling grain orientation connectivity, not simply grain size, provides a scalable pathway for exploiting anisotropic transport in multinary metal oxide photoelectrodes, directly linking the microstructure to the enhanced charge transport required for practical solar fuel devices.

The emergence of convenient blading technology has enabled the development of large-area polymer solar cells (PSCs). However, the smart, efficient enhancement and transparency adaption of bladed PM6:Y6 solar cells requires demonstration of key performance indicators. Herein, we report the enhanced efficiency and adapted transparency of PSCs by binary lanthanide (Eu3+/Sm3+)-induced diblock polymer aggregates (EIPAs/SIPAs) with inclusion of ZnO (ZnO:EIPAs:SIPAs). First, the EIPA- and SIPA-cocapsulated ZnO nanoclusters (ESPAs-Z) were employed as the electron-transport layer (ETL). Owing to their distinct excitation and emission spectra, EIPAs and SIPAs can synergistically boost solar light harvesting and energy conversion. Thus, bladed devices using a PM6:Y6 active layer, with EIPAs and SIPAs in the ETL, have achieved an enhanced power conversion efficiency (PCE) of 13.47% that is notably enhanced by the ratio of 11.4% from 12.03% of the single ZnO ETL. Simultaneously, this ESPAs-Z-in-ETL improves the compatibility between ITO and the active layer and optimizes the energy-level alignment at the interface. In PM6:Y6-based semitransparent polymer solar cells (ST-PSCs), doping EIPAs and SIPAs yielded an optimal PCE of 6.09% while maintaining a high AVT of 39.32%. This work demonstrates that incorporating Eu3+/Sm3+ nanoaggregates into PSCs is a critical advance for the scalable fabrication of ST-PSCs.

Polyolefins such as polyethylene represent one of the most significant environmental hazards nowadays, and the high chemical inertness of polyolefin plastics makes their degradation or chemical recycling challenging. Herein, we demonstrate a chlorine-ion-enabled photocatalytic approach for converting low-density polyethylene (LDPE) under ambient conditions. With an oxygen vacancy-rich bismuth oxychloride (BiOCl-Ov) photocatalyst in a Cl– anion-containing aqueous solution, chlorine radicals (•Cl) are generated from the activation of interlayer lattice chloride (ClL–) via a hole-mediated process in BiOCl-Ov, enabling to break the C–H and C–C bonds of LDPE into different carbonic products. Meanwhile, the interlayer ClL– anions are replenished by Cl– in the electrolyte to maintain sufficient Cl– species in the catalyst. Under 1-sun illumination intensity and ambient conditions, the BiOCl-Ov photocatalyst exhibited one of the highest LDPE conversion performances without the addition of photosensitizers or sacrificial reagents, including 16.9% LDPE conversion rate and 365 μmol·gcat–1 liquid product formation rate, as well as efficient conversion capability for other plastics including polypropylene and polyvinyl chloride.

Manganese oxide cathodes are promising candidates for aqueous batteries owing to their high operating voltage and large capacity. However, they suffer from severe Mn3+ disproportionation and Mn2+ dissolution in acidic aqueous batteries, hindering their practical applications. Herein, we construct an in situ trifunctional (conductive, hydrophobic, self-adaptive) interphase using PDMS-DE@PANI (epoxypropoxypropyl-terminated polydimethylsiloxane@polyaniline) core–shell nanocapsules for encapsulating Mn2O3. The electrochemically driven release of the liquid PDMS-DE core, synergizing with the PANI shell, effectively suppresses Mn2+ dissolution while ensuring rapid electron/ion transfer. Consequently, the PD-Mn2O3 cathode delivers a record-high capacity of 340 mAh g–1 at 0.2 A g–1 and retains 201 mAh g–1 (92% capacity retention) after 800 cycles at 1 A g–1. Paired with a HATN anode, the full proton battery achieves an exceptional energy density of 140 Wh kg–1 with 80% capacity retention over 800 cycles. This dynamic interphase engineering provides a robust strategy for developing high-energy, ultrastable aqueous proton batteries.