http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

A molybdenum aluminum boride-guided charge-buffered sulfidation strategy is proposed to stabilize anionic boron (Bδ−) dopants in metallic phase molybdenum disulfide. The Bδ− substitution not only generates a high-energy-state of empty pz orbital to unlock the rapid H2O dissociation, but also facilitates the H adsorption through modulating the electronic environment of adjacent sulfur, hence improving alkaline HER performance.

The sp3 hybridization of surface sulfur in metallic phase molybdenum disulfide (1T MoS2) is identified as the intrinsic bottleneck for alkaline hydrogen production (HER), where their electron-saturated nature elevates the kinetic barrier for water dissociation. To overcome this limitation, a charge-buffered sulfidation strategy is reported to stabilize anionic boron (Bδ−) within 1T MoS2. By employing molybdenum aluminum boride as the precursor, the Bδ− dopants can be efficiently preserved via the topological confinement imposed by Mo─B─Mo network. This approach also maintains the 1T phase integrity through Al-mediated electron compensation. Theoretical and experimental analyses reveal that Bδ− substitution generates vertically oriented empty pz orbitals through sp2 hybridization, which elevates orbital energy to align with molecular orbitals of water, significantly reducing the O─H cleavage barrier by over 80% compared to 1T MoS2. Concurrently, the B─Mo─S networks upshift adjacent sulfur 3p band centers to optimize the hydrogen adsorption path. These dual functionalities endow the pz-functionalized 1T MoS2 with a low overpotential of −30 mV at 10 mA cm−2, and high-current operation of 1 A cm−2 at 1.779 V in an anion-exchange membrane electrolytic cell. This work not only establishes orbital alignment as a transformative design principle for advanced electrocatalysts, but also paves a novel synthetic pathway for 1T transition metal disulfides.

A natural moisturizing material, hyaluronic acid, is developed to enhance electrolyte adsorption and polysulfide capture via intramolecular hydrogen bonds, eliminate polysulfides by its superior radical-scavenging capability, and expedite electron/Li+ transport by spiral acceleration effect, thus boosting sulfur redox reaction kinetics and achieving outstanding electrochemical performance of lean-electrolyte Li–S batteries.

Catalyzing sulfur conversion is an efficient solution to overcome poor ion transfer, severe shuttle effect, and unfavored electrode passivation in lean-electrolyte lithium–sulfur batteries. Herein, a natural moisturizing material, hyaluronic acid (HA), is experimentally and theoretically demonstrated to promote the adsorptions of electrolyte and polysulfides via intramolecular hydrogen bonds, providing sufficient electrolyte contacts for subsequent catalytic reactions. Rely on its radical-scavenging capability, HA facilitates the conversion of polysulfide radicals at N sites, suppressing shuttle effect. Due to the spiral acceleration effect of double helix structure, HA accelerates Li+ migration, enhancing the lithiation kinetics of system. Consequently, under sulfur loading of 8 mg cm−2 and lean electrolyte of 3 µL mg−1 conditions, the HA-modified cells deliver a high areal capacity of 11.76 mAh cm−2 and a gravimetric energy density of 409 Wh kg−1. This work provides a fresh insight into developing natural moisturizing materials as electrocatalysts toward practical Li–S batteries.

In p-i-n structure perovskite solar cells, conventional self-assembled monolayers (SAMs) such as [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) exhibit limited buried interfacial adhesion, compromising device stability. A donor-acceptor SAM, 4-(7-(4-(bis(4-methoxyphenyl)amino-2,5-difluorophenyl)benzo[c][1,2,5]thiadiazol-4-yl)benzoic acid (PAFTB), featuring an enhanced dipole moment and tailored functional groups, improves adhesion by 2.8 times, thereby enhancing both stability and efficiency of the devices.

Inverted p-i-n structure perovskite solar cells (PSCs) have outperformed traditional n-i-p PSCs in recent years. A key advancement is the use of self-assembled monolayers (SAMs) as hole transport layers. One class of widely used SAMs is carbazole-based phosphonic acids. However, it is found that these SAMs lack strong binding with transparent conducting oxides (TCO) and perovskite. The weak binding strength results in suboptimal interfacial adhesion of the buried interface, which limits the device's stability. Here, interfacial binding is enhanced by increasing the dipole moment that creates a strong interfacial electric field that enhances electrostatic interactions at the TCO/perovskite interface, while incorporating tailored functional groups in SAMs to improve chemical anchoring to TCO and binding to perovskite. Specifically, the donor-acceptor SAM molecule 4-(7-(4-(bis(4-methoxyphenyl)amino)-2,5-difluorophenyl)benzo[c][1,2,5]thiadiazol-4-yl)benzoic acid (PAFTB) is employed, which features an enhanced dipole moment along with electron-donating and electron-withdrawing functional groups to optimize interfacial interactions. Compared to extensively used [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz), PAFTB enhances total interfacial adhesion by 2.8 times, thereby improving the thermal stability of the layer. Using this approach, PSCs are demonstrated with a certified quasi-steady-state power conversion efficiency of 24.9% and maintain 80% of the initial efficiency after 900 h of maximum power point tracking at 85 °C.

A plasmonic MoO3− x /Ag photocatalyst is designed for efficient N2 photofixation. It exhibits superior light absorption, a Schottky-barrier-free feature, and plasmonic photothermal conversion. A diphase reaction platform is designed by loading the photocatalyst in a polymer film to suppress the light absorption of water and accelerate the mass transfer kinetics, giving a high photocatalytic efficiency of >0.28% from air.

Storing solar energy in chemical bonds through photocatalysis under ambient conditions is of great importance for sustainable development and carbon neutrality. In addition to the design of new photocatalysts with high activities, efficient solar energy delivery and the acceleration of reactant mass transfer kinetics are also crucial for efficient energy conversion. Herein, a new type of plasmonic Schottky-barrier-free MoO3− x /Ag photocatalyst is designed for efficient NH3 production. The photocatalyst exhibits strong light absorption and utilization under sunlight illumination. The construction of a bilayer system reduces the light attenuation by water in the near-infrared region and accelerates the N2 mass transfer kinetics. As a result, the photocatalytic activity is largely boosted. A high solar-to-chemical energy conversion efficiency of over 0.28% (±0.01%) is reached with air directly used as the feeding gas. The study offers a promising pathway for the rational design of photocatalysts and photocatalytic platforms, enabling greatly enhanced solar-to-chemical energy conversion.

Large-format fiber lithium-ion batteries (L-FLIBs) beyond 2 m in length are developed by homogenizing the electric field along fiber axis. The as-assembled L-FLIBs can deliver a 0.4 W high power output, corresponding to a 40% power increment. Furthermore, an unprecedented single-cell capacity of >1 Ah is achieved.

Large-format fiber-shaped lithium-ion batteries (L-FLIBs) hold great promise for next-generation flexible and wearable electronics but suffer significant cell polarization and insufficient active material utilization after scaling up. The heterogeneous spatial electric field distribution fundamentally affects the electrochemical behavior and jeopardizes the performance of L-FLIBs, yet its influence on 1D fiber structures remains unexplored. Here, the electron transport mechanisms are systematically investigated and develop an optimized dual-terminal cell configuration for field homogenizing. Through equivalent circuit modeling and experimental validation, it is revealed that strategic electron collection terminal design establishes symmetric electric fields along the fiber length, effectively addressing the fundamental challenge of electrochemical heterogeneity and enhancing the redox kinetics for L-FLIBs. Thereby, a 60% internal resistance reduction is achieved and successfully fabricated a 10-m-long L-FLIBs with an unprecedented 1 Ah high capacity for a single fiber cell. The practical capability of this design is demonstrated by integrating large-format batteries into a fabric power bank for portable electronics.

This work presents a strategic molecular design utilizing fused B/N and C ═ O/N units within the MR-TADF framework to enhance molecular rigidity and accelerate RISC, resulting in efficient sky-blue OLEDs. BNTO-based hyper-fluorescence OLEDs achieved a moderate EQE of 19.4% and a LT70 of 500 h at 1000 cd m−2, emphasizing the importance of structural rigidification and excited-state engineering for color purity and stability.

Blue-emitting multiple-resonance thermally activated delayed fluorescence (MR-TADF) emitters with high photoluminescence quantum yield (PLQY), high robustness with short-lived emission lifetime is particularly desired for the development of organic light-emitting diodes (OLEDs). In this study, a series of MR-TADF molecules featuring fused boron/nitrogen (B/N) and C ═ O/N frameworks is reported. These emitters namely BNO, BNDO, and BNTO are systematically designed and synthesized to investigate the impact of molecular rigidity or planarity toward their excited-state dynamics through stepwise intramolecular electrophilic acylation reactions. Computational studies and single-crystal X-ray diffraction data revealed the enhanced planarity of BNDO and BNTO. Upon photoexcitation, these compounds exhibited blue emission with PLQYs of approaching unity and short-lived delayed lifetimes (<2 µs). BNTO-based OLEDs achieved sky-blue emission peaking at 489 nm, a moderate device operational lifetime of over 500 h at 70% of the initial brightness (LT70) at 1000 cd m−2, which shows longer device stability when compared with BNO and greener emission when compared to BNDO. This study highlights that manipulation of the rigidity of compounds and emissive states of MR-TADF compounds is essential in achieving blue emission and improving OLED operational stability.

This study reports two compounds crystallizing in achiral point groups (2/m and 1¯$\bar{1}$) that exhibit circularly polarized room-temperature phosphorescence. Mechanistic investigations reveal that the synergistic effect of intermolecular π–π stacking and C─H···N hydrogen bonding during crystallization induces symmetry breaking, facilitating directed helical assembly. The photoluminescence dissymmetry factors (g lum) reach 5.5 × 10−2 (543 nm) and 4.3 × 10−2 (550 nm), respectively.

Very recently, considerable attention has been given to pure organic circularly polarized room-temperature phosphorescent (CP-RTP) materials due to their unique photophysical properties. However, the directed construction of optically active phosphorescent signals within achiral systems remains a formidable challenge. In this study, two achiral crystals, 2CN4S and 2F4S, belonging to the achiral point groups 2/m and 1¯$\bar{1}$, exhibit strong CP-RTP emission with high photoluminescence dissymmetry factors (g lum) up to 5.5 × 10−2 (543 nm) and 4.3 × 10−2 (550 nm), respectively. This phenomenon is attributed to the intrinsic mirror-antiparallel molecular conformations induced by the targeted substitution of cyano/fluoro groups, which spontaneously assemble into symmetry-breaking helical superstructures through synergistic C─H···N hydrogen bonding and π–π interactions. This work not only establishes a novel approach for CP-RTP material design but also overcomes structural constraints in optically active materials within achiral point group systems.

A stretchable, adhesive, anti-freezing hydrogel electrolyte with dual-functional water regulation is constructed via a one-pot strategy, integrating acetate anions and the hydrophilic amide groups on polyacrylamide chains. This design disrupts the intrinsic water hydrogen-bond network and suppresses interfacial side reactions, enabling aqueous zinc-ion batteries to operate over a broad temperature range spanning from −20 to 100 °C.

Aqueous zinc-ion batteries (AZIBs) are promising candidates for next-generation energy storage due to their intrinsic safety and environmental compatibility. However, parasitic reactions induced by active water molecules in conventional aqueous electrolytes severely degrade electrochemical performance and cycling stability. Herein, a stretchable, adhesive, anti-freezing hydrogel electrolyte with dual-functional water regulation is synthesized via a one-pot radical polymerization strategy, where acetate (Ac−) anions and hydrophilic amide (─CONH2) groups on polyacrylamide (PAM) chains synergistically regulate water activity. This design disrupts water's intrinsic hydrogen bond network and suppresses interfacial side reactions, enabling stable AZIBs operation across a wide temperature range (−20 to 100 °C). Consequently, Zn||Cu cells employing PAM-Zn(Ac)2-4KAc (denoted PAM-ZnK4Ac) hydrogel electrolyte achieve an average Coulombic efficiency of 99.7% over 500 cycles, demonstrating outstanding reversibility. Meanwhile, Zn||polyaniline (PANI) cells retain 81.4% capacity after 1100 cycles at −20 °C and operate effectively up to 100 °C. This work establishes a facile yet effective strategy for preparing hydrogel electrolytes, advancing all-climate AZIBs toward extreme-environment energy storage and flexible electronics.

This Perspective comprehensively reviews the research progress of high-entropy oxides as electromagnetic wave absorbing materials from four aspects: high-entropy characteristics, crystal structure, synthesis methods, and elemental composition. The key scientific issues that urgently need attention at present and the development are proposed, aiming to provide insights for high-entropy oxides to become the next generation of promising electromagnetic wave absorbing materials.

The escalating impact of electromagnetic radiation on human health and electronic device stability has driven intensive research into advanced electromagnetic wave absorption (EMA) materials in recent decades. Among them, high-entropy oxides (HEOs) have evolved into increasingly popular research in the material field since they were first reported in 2015. They are particularly promising for EMA applications due to their remarkable tunability and almost infinite compositional flexibility. The advantages of HEOs as EMA material from four key aspects are systematically clarified: the intrinsic properties of the high-entropy system, crystal structure, compositional design, and synthesis strategies. A forward-looking view on the future development of HEOs in EMA is highlighted, demonstrating six crucial points: dielectric genes, high-throughput computational methods, material integration strategies, microstructural modulation, the high-entropy concept expansion, and functional expansion. This perspective offers theoretical insights and technological references to advance high-performance HEO research by systematically connecting the HEO family and EMA functionality.

A synthetic high-density lipoprotein (sHDL) nanodisc, referred as sHDL@Pt, is engineered to load a Pt(IV) prodrug (C2-Pt(IV)-C12), activating the innate immune system through the cGAS-STING pathway. Using near-infrared II fluorescence imaging and single photon emission computed tomography imaging technology, it is found that sHDL@Pt can be effectively accumulated in tumor sites.

Cisplatin is a first-line, broad-spectrum anti-tumor drug used to treat various types of cancer. However, immune-suppressive tumor microenvironments (TME) are often induced by cisplatin. Here, a first synthetic high-density lipoprotein (sHDL) nanodisc, referred as sHDL@Pt, is engineered to load a Pt(IV) prodrug (C2-Pt(IV)-C12), inducing a 2.2-fold increase in dsDNA release compared to cisplatin. This further activates the innate immune system through the cGAS-STING pathway. Using near-infrared II fluorescence imaging and single photon emission computed tomography imaging technology, it is found that sHDL@Pt can be effectively accumulated in tumor sites. The sHDL@Pt can induce severe DNA damage, which subsequently results in a more pronounced activation of the cGAS-STING pathway, further promoting dendritic cell maturation and T cell proliferation, triggering strong cytotoxic T lymphocyte responses, and inhibiting tumor growth. This work introduces a novel approach for delivering Pt(IV) prodrug that effectively initiates and activates innate immunity through the activation of the cGAS-STING pathway.

This work presents a molecularly engineered conjugated polycarbazole framework that enables efficient, stable, and bias-free photoelectrochemical synthesis of H2O2. Scaled to a 1 m2 panel reactor operating under natural sunlight, the system achieves a solar-to-chemical conversion efficiency of 1.10%, setting a new benchmark as the largest and most efficient solar-driven PEC system for H2O2 production demonstrated to date.

Solar-driven photoelectrochemical (PEC) synthesis emerges as a promising pathway to produce hydrogen peroxide (H2O2), reimagining the energy-intensive anthraquinone method. However, scaling PEC systems from laboratory-scale prototypes to practical large-area installations remains a significant scientific and engineering challenge, primarily due to limited catalytic selectivity at photoelectrode surfaces and rapid performance degradation during upscaling. This study presents a modular, bias-free PEC system designed for scalable solar-driven H2O2 production. Conjugated polycarbazole frameworks (CPFs) containing rationally designed diacetylene and anthraquinone moieties functions as molecularly precise catalytic layers, enabling concurrent two-electron pathways at both the photoanode and photocathode. The resulting photoanode and photocathode deliver faradaic efficiencies of 94.08% and 95.50%, respectively, for H2O2 production. Integrating these photoelectrodes into a 1 cm2 unbiased tandem PEC device achieves a solar-to-chemical conversion (SCC) efficiency of 2.11%. More importantly, scaling these devices to a 1 m2 membrane-free PEC panel reactor via a modular assembly strategy yields an average SCC efficiency of 1.10% under natural sunlight, representing the largest reported solar-driven PEC system for H2O2 production to date. This study bridges the gap between laboratory-scale experimentation and real-world applications, providing a scalable framework for decentralized, solar-driven H2O2 production.

A narrow bandgap acceptor, BTA-4F, featuring a 2-methyl-2H-benzotriazole central core, is fabricated to construct the rear sub-cell of tandem organic solar cells (OSCs). By fine-tuning the optical field distribution in the BAT-4F-based tandem OSC, a power conversion efficiency of 21.5% is achieved (certified as 21.2%), respectively, which marks the arrival of 21% era in the field of OSCs.2

Tandem organic solar cells (OSCs) offer a promising strategy for enhancing light utilization and reducing energy loss, presenting significant potential in achieving high power conversion efficiency (PCE). Herein, a narrow bandgap acceptor, BTA-4F, featuring a 2-methyl-2H-benzotriazole (BTA) central core, is fabricated, which is designed for the rear sub-cell of tandem OSCs. Systematic characterizations demonstrate that incorporating strong electron donating groups BTA into central core unit can narrow the bandgap and enhance the electroluminescence external quantum efficiency. These improvements lead to increased current density and reduced voltage loss of single junction OSCs under AM 1.5G illumination and real incident light of the rear sub-cell. Inspiringly, BTA-4F-based single-junction and tandem OSCs achieve outstanding PCEs of 19.5% and 21.5% (Certified as 21.2%), respectively, which represents the milestone of 21% PCE in the field of OSCs. This study highlights the synergistic benefits of molecular design and implementation of tandem architecture as an effective strategy for enhancing photovoltaic performance of OSCs.

This systematic study of magnetic topological matter under hydrostatic pressure reveals strong material response to pressure, demonstrating a shrinking topological gap and enhanced magnetic order under compression. These findings establish strain engineering as an effective tuning parameter for manipulating and potentially enhancing the quantum anomalous Hall effect.

To date, the most widely-studied quantum anomalous Hall insulator (QAHI) platform is achieved by dilute doping of magnetic ions into thin films of the alloyed tetradymite topological insulator (TI) (Bi1 − x Sb x )2Te3 (BST). In these films, long-range magnetic ordering of the transition metal substituants opens an exchange gap Δ in the topological surface states, stabilizing spin-polarized, dissipationless edge channels with a nonzero Chern number C$\mathcal {C}$. The long-range ordering of the spatially separated magnetic ions is itself mediated by electronic states in the host TI, leading to a sophisticated feedback between magnetic and electronic properties. Here, a study is presented on the electronic and magnetic response of a BST-based QAHI system to structural tuning via hydrostatic pressure. A systematic closure of the topological gap under compressive strain is identified accompanied by a simultaneous enhancement in the magnetic ordering strength. Combining these experimental results with first-principle calculations, structural deformation is identified as a strong tuning parameter to traverse a rich topological phase space and modify magnetism in the magnetically doped BST system.

Fungal infections are worsened by biofilms and inflammation, reducing antifungal efficacy. Lipidic prodrug co-crystals (LPCCs) are developed that co-deliver antifungal and anti-inflammatory drugs. LPCCs self-assemble, load drugs efficiently, and respond to biofilm environments. They inhibit biofilms and inflammation, modulate immunity, and restore tissue health in mice, offering a promising antifungal treatment strategy.

Fungal infections are often complicated by biofilm formation and concurrent inflammation, limiting the efficacy of conventional antifungal therapies. To address these challenges, we developed a novel hybrid drug delivery platform—lipidic prodrug co-crystals (LPCCs)—that combines the benefits of lipidic self-assembly and pharmaceutical co-crystallization. In this study, a lipidic prodrug is synthesized by linking catechol-containing α-aminophosphonate with phenylboronic acid-modified bifonazole (Bfz), an antifungal agent, via boronate bonding. The resulting self-assembled structures exhibit high drug-loading capacity (up to 85%) and are capable of co-crystallizing with anti-inflammatory agents such as nonsteroidal antiinflammatory drugs (NSAIDs) through strong aromatic and ionic interactions. This dual-delivery system enables the controlled, site-specific release of both antifungal and anti-inflammatory agents in response to the acidic and oxidative microenvironment of fungal biofilms. LPCCs effectively prevent biofilm formation, eradicate mature biofilms, and enhance ROS-scavenging capacity. Mechanistically, LPCCs inhibit the NF-κB/COX-2 pathway, reduce pro-inflammatory cytokines, and promote an anti-inflammatory M2 macrophage phenotype. In a murine rectal candidiasis model, LPCCs significantly reduced fungal load, restored tissue integrity, and normalized immune and microbial environments. Our findings highlight LPCCs as a promising strategy for enhancing treatment efficacy, improving patient compliance, and overcoming the limitations of current antifungal therapies.

A Zn2+-conductive solid polymer electrolyte (SPE) is fabricated by in situ polymerization of 2-ethyl-2-oxazoline (EtOx) within sulfonated porous aromatic frameworks (SPAF). The solvation effect of PEtOx and the anchoring effect of SPAF synergistically promote the transport of Zn2+ ions, reduce the migration energy barrier, and improve the performance of the battery at cryogenic temperatures.

Solid polymer electrolytes (SPEs) are vital for zinc-ion solid-state batteries (ZSSBs) for dendrite suppression but face low-temperature hurdles from poor ionic conductivity and crystallization. Here, a supramolecularly engineered SPE is constructed by in situ polymerization of 2-ethyl-2-oxazoline (EtOx) within sulfonated porous aromatic frameworks (SPAFs), acting as macroinitiators and nanoconfined reactors. Resulting poly(2-ethyl-2-oxazoline) (PEtOx) chains assemble with the SPAF via strong non-covalent interactions, forming cohesive SPAF-PEtOx (SPP) with interconnected ion transport pathways. −SO3 − groups anchor Zn2+, while confined PEtOx chains modulate solvation dynamics, facilitating efficient Zn2+ migration. SPE based on SPP embedded in polyvinylidene fluoride (PVDF) matrices (SPP@PVDF) achieves high ionic conductivity (5.04 × 10−4 s cm−1) and a wide electrochemical window (2.74 V) at room temperature. A Zn || Zn symmetric battery exhibits stable plating/stripping over 3000 h, while a full Zn || V2O5 battery retains capacity over 1000 cycles at −40 °C with no decay. Notably, the ionic conductivity of SPP@PVDF at −40 °C is 8-fold higher than SPAF@PVDF, as PEtOx reduces Zn2+ migration barriers. This work offers a molecular-level strategy for designing cryogenically robust SPEs, advancing ZSSB technologies for extreme environments.

3D temperature sensing has recently advanced rapidly for comprehensive thermal characterization. In this review, representative research progress is summarized in systems with typical thermal sensing materials and their applications for 3D temperature sensing. The systems include optical-based and non-optical-based systems for surface and volumetric 3D temperature sensing. Challenges and future outlooks are also discussed in the end.

Temperature sensing has broad applications in everyday life and serves as a crucial tool for ensuring safety, efficiency, and sustainable development across various industries. Recently, 3D temperature sensing has become increasingly vital in modern society due to the boosted demand for comprehensive thermal information in various applications. This field has attracted global efforts in developing temperature-sensitive materials, spatial positioning technologies, and new mechanisms of heat transfer to improve temperature resolution and spatial resolution in various systems. This review summarizes representative research progress of thermal sensing materials and systems in 3D temperature sensing. The systems include optical-based systems (X-ray computed tomography, luminescence thermometry, optical tomography, Raman spectroscopy, infrared thermography, photoacoustic thermometry) and non-optical-based systems (thermocouple, scanning thermal microscopy, magnetic resonance imaging, magnetic particle imaging). Emphases are placed on introducing the thermal sensing materials, the mechanism of temperature sensing in 3D, and discussing the feasibility of different applications. Artificial intelligence-enhanced 3D temperature sensing is also summarized. Perspectives on current challenges and future research directions are discussed at the end. It is anticipated that this review will stimulate further in-depth research in materials and systems for 3D temperature sensing and help accelerate the growth of this emerging field.

This remarkable work combines supercritical CO2 chemical engineering, two-dimension plasmon photophysical science, and perovskite photovoltaic technology. It introduces novel concepts like broad - spectrum coupled photon absorption, the intermediate - localized - states model, and optoelectrical - bimodal - coupling engineering. It aims to combat optoelectronic dissipation and enhance energy harvesting via a heterodimensional van der Waals optically coupled system.

All-inorganic CsPbX3 (X = I, Br, Cl) perovskites emerged as a crucial material for addressing the stability bottleneck due to their exceptional resistance to both light-thermal stress. However, their performance is limited by adverse optoelectronic dissipation arising from inadequate photon conversion and chaotic carrier energetics. Herein, the mechanism of the unique nonlinear plasmonic effect in van der Waals 2D MoO3-x is elucidated, which is mediated by electronic intermediate states. It demonstrates that the 2D MoO3-x serves as a light-capture-antenna in heterodimensional CsPbX3-MoO3-x optically coupled system, contributing to the accumulation the optical field energy on the nanoscale and resulting in a remarkable 59% increase in photon convergence. Additionally, facet-oriented carrier channels can be established through heteroepitaxy along matched Mo-O octahedron. This optoelectrical-bimodal-coupling engineering combined with a bifacial light-harvesting configuration yields a bifacial equivalent efficiency of 27.33%, which stands as the supreme performance in all-inorganic perovskite photovoltaics.