Surface vacancy engineering is crucial for enhancing charge separation in catalytic reactions. Traditional approaches have largely focused on single-type vacancies that trap either electrons or holes, limiting the effectiveness of overall redox reactions. Constructing dual-type metal-oxygen vacancies (VM-VO) facilitates trapping electrons and holes simultaneously and selectively. However, it poses significant challenges under equilibrium conditions due to the incompatible vacancy-formed conditions. Here, we utilize the non-equilibrium effect of the femtosecond-laser-processing technique to construct surface VM-VO. Taking TiO2 as a model, we confirm the surface engineering of dual-type titanium and oxygen vacancies (VTi-VO), synergistically boosting charge lifetime from 281.4 ps to 1507.6 ps, by 5.4 times. Remarkably, a dramatic enhancement of the apparent quantum efficiency in photocatalytic hydrogen evolution from 12.4% to 80.7% under 365 nm illumination is achieved. This work demonstrates a non-equilibrium femtosecond laser processing strategy for accurately carving VM-VO on metal oxides and highlights the significantly enhanced photocatalysis empowered by VM-VO-induced charge separation.

This study employed cross-linking units with star-like topology of varying sizes ethoxylated trimethylolpropane triacrylate(ETPTA), polyhedral oligomeric silsesquioxanes(POSS) and nano-zirconia) as cross-linking cores to chemically cross-link with poly(ethylene glycol) diacrylate(PEGDA), constructing three polymer networks(EP, PP and ZP) for application in quasi-solid-state dye-sensitized solar cells(DSSCs). The results demonstrate that the strategy of increasing the size of the cross-linking core effectively enlarges the free volume of the polymer, reduces its glass transition temperature, and consequently enhances its low-temperature electrochemical performance. At a low temperature of -40 degrees C, the power conversion efficiency(PCE) of the ZP-based device shows a significant increase of 37.4% compared to the EP-based device. This research provides a novel and effective strategy for developing quasi-solid-state electrochemical devices suitable for high altitude environment.

Abstract Solar-powered electrochromic devices (SP-ECDs) are promising for zero-energy smart optical systems, holding potential applications in energy-saving windows, augmented reality displays, and adaptive camouflage. State-of-the-art SP-ECDs typically rely on the physical stacking of solar cells and electrochromic components. This approach inevitably introduces multiple heterogeneous interfaces, which severely limit the switching speed, operational stability, and color diversity of integrated devices. Herein, we introduce an all-in-one photoelectrochromic device that molecularly integrates dye-sensitized photoanodes and viologen electrochromic molecules within a single redox electrolyte. This innovative device achieves a record switching time of ∼7 s under optical, electrical, or hybrid stimuli, enabling real-time light adaptation to various dynamic illumination situations. The device presents high operational stability, enduring over 103 cycles under continuous AM 1.5G illumination. Furthermore, it offers a wide range of designable color palette (red, green, blue, purple, and cyan) with uniform, full-frame coloring appearance, facilitating further aesthetic and functional designs. Our strategy establishes a monolithic architecture that overcomes the integration complexity in conventional SP-ECDs, inspiring the creation of customized material platforms and the advancement of self-adaptive optoelectronics.

While gel polymer electrolytes (GPEs) are safer and more flexible than liquid electrolytes, their inherently disordered polymer networks drastically hinder ion transport and reduce ionic conductivity by two or three orders of magnitude. Thus, achieving liquid-level conductivity in GPEs continues to be a challenge in advancing ionic and energy devices. This study successfully constructs a high conductivity GPE of a liquid-comparable level by ordered network design with selective, efficient photoinitiated thiol–ene click chemistry. The ordered polymer networks suppress crystallization and topological defects, thereby enabling the rapid gelation (< 10 s) at ultra-low content (5 wt%), and they minimize diffusion resistance by reducing ion transport activation energy (5.8 kJ/mol) to the liquid level (6.7 kJ/mol). The optimized GPEs deliver high conductivity across nine widely used electrolytes, achieving a record-high 11.3% efficiency in quasi-solid-state dye-sensitized solar cells utilizing bulky copper complexes, and enabling ultrafast-charging lithium-metal batteries with 83% capacity retention after 1,000 cycles at 5C. This click-enabled GPE design overcomes the long-term conductivity gap between liquid and solid electrolytes, and unlocks the monomer engineering potential for scalable, multifunctional development of electrochemical energy devices.

ABSTRACT PbS quantum dots (QDs) are highly promising visible–near‐infrared materials for low‐noise broadband photodetectors, particularly in a state‐of‐the‐art homojunction device made solely from p‐ and n‐doped QDs. However, the performance of these QD photodetectors is frequently bottlenecked by the inferior quality of p‐doped PbS QDs. This limitation originates from the poor ligand control of p‐doped QDs during the constrained and incomplete solid‐phase synthesis, resulting in significant energy‐level disorder and aggravated carrier recombination in the device. Here, we propose an ethylenediamine (EDA) post‐treatment strategy to refine the ligand environment of p‐doped PbS QDs after synthesis. This EDA treatment efficiently removes the residual insulating oleate ligands by 91.4%, while promoting further bonding of the target thiol ligands. The mild chemical nature of EDA ensures that pre‐deposited functional layers remain entirely unaffected. Photodetectors incorporating EDA‐treated p‐doping QDs exhibit significantly suppressed noise (3.07 × 10 −14 A Hz −1/2 ) and achieve an ultrawide bandwidth of 205 kHz for high‐speed operation. These high‐performance detectors enable rapid and clear broadband single‐pixel imaging through various opaque media, demonstrating their considerable potential for machine vision, autonomous sensing, and imaging under challenging environments.

The energy-inefficient and environmentally unsustainable nature of conventional ammonia synthesis necessitates alternative nitrogen fixation pathways powered by renewable electricity. Herein, we develop a coupled in-water plasma-electrochemical strategy for sustainable ammonia production, in which dinitrogen is first activated by in-water plasma to generate a dilute NOx- solution, followed by electrochemical reduction to ammonia. Enabled by a nano-Cu4O3 electrocatalyst, ammonia is produced from low-concentration NOx- at a rate of 5.58 mg mgcat-1 h-1 at -0.47 V vs. RHE. Mechanistic investigations attribute the superior activity to in situ formed Cu-Cu4O3 interfacial sites, which markedly reduce the energy barriers for proton-coupled electron transfer. As a result of the plasma-electrochemical synergy, the system achieves an electrical-to-chemical energy conversion efficiency of 14.8%. And the energy consumption of this system attains 4.63 MJ mol-1 with air as the nitrogen source. These performance metrics position this work among the state-of-the-art electrically powered nitrogen-to-ammonia technologies, offering a carbon-neutral and energy-sustainable paradigm for ammonia synthesis.

Photo-plasma catalysis, combining the controllability of photocatalysis with the high reactivity of plasma, presents a promising platform for reactive oxygen species (ROSs) generation. However, efficient coupling of photocatalysis and plasma requires interfaces that integrate multiple catalytic functions to reconcile differences between the two processes. Herein, we report the tuning of the TiO2/Co3O4 nano-interface for efficient photo-plasma catalytic ROS generation by loading a Co3O4 nanozyme onto a surface-disordered TiO2 photocatalyst. For bisphenol A (BPA) removal, the composite catalyst achieves a degradation rate that is 17.3-fold and 12.6-fold higher than those of plasma and photocatalysis alone, respectively. Combined ROS scavenging and probe analyses reveal that the enhanced bisphenol A removal is directly related to the efficient singlet oxygen (1O2). Further mechanistic analyses suggest that the yield of 1O2 is linked to the conversion of superoxide radicals (•O2-). The heterogeneous nano-interface serves as the key reaction center. Specifically, surface disorder and heterojunction-driven electron accumulation promote •O2- generation via photocatalytic O2 reduction on TiO2, while holes in Co3O4 oxidize plasma-generated H2O2 to •O2- through a sustained Co3+/Co2+ redox cycle. Compared with TiO2/Fe2O3 and TiO2/CuO, TiO2/Co3O4 exhibits superior photo-plasma catalytic performance due to the more efficient conversion between H2O2 and •O2- enabled by the stable Co3+/Co2+ redox cycle. This work provides a general paradigm for developing interfacial reaction centers in catalysts to improve coupled catalytic ROS generation.

Short-chain molecular ligands (SMLs) are favored for producing colloidal quantum dot (CQD) inks for solution-processed optoelectronics, since they enable more efficient charge transport than conventional long-chain ligands. However, their weak steric or electrostatic stabilization makes CQD inks vulnerable to aggregation or coalescence. To overcome this challenge, here we report a hydrogen-bond-mediated strategy for preparing SML-capped CQD inks with excellent colloidal stability and solution processibility. Through theoretical and experimental evaluation of hydrogen-bond strengths across polar organic solvents and small thiol molecules, we identify 1-thioglycerol (TG) in dimethylsulfoxide (DMSO) as an optimal pair. This combination enables one-step synthesis of CQDs of binary, ternary, and quaternary metal sulfide under ambient conditions, while strong ligand-solvent hydrogen bonding ensures robust colloidal stability. Optoelectronic devices fabricated by stacking these p-type PbS CQDs on n-type PbS CQDs achieve a record power conversion efficiency of 12.2% solar cells in all-ink-processed devices and an enhanced detectivity of 9.4 × 1011 Jones in near-infrared photodetectors. This hydrogen-bond-mediated approach demonstrates a straightforward and cost-effective route to produce p-type PbS CQD conductive inks, holding great promise for advancing all-ink scalable-manufacturing optoelectronic devices.

Clean synthesis of key oxidants is central to decentralized and sustainable chemical manufacturing. Herein, we report an electricity-powered solution plasma method coupled with phenyl porphyrin catalysts for production of hydrogen peroxide (H2O2). The catalytic efficiency of H2O2 synthesis is significantly influenced by the substituents on the porphyrin ring. In particular, meso-tetra(4-carboxyphenyl)porphyrin (TCPP) exhibited the highest catalytic performance, achieving a H2O2 production rate of 5.7 mmol L-1 h-1. To enhance catalyst dispersion and interfacial accessibility under discharge, the TCPP structure was dispersed via self-assembly (SA-TCPP) and ultrasonication (US-TCPP). Under identical solution plasma conditions, the H2O2 concentrations in the SA-TCPP and US-TCPP systems reached 6.58 mmol L-1 h-1 and 7.0 mmol L-1 h-1, respectively, representing 46% and 55% improvements compared to that of the pure water control group. It is found that singlet oxygen (1O2) acts as a decisive reactive oxygen species (ROS) in promoting H2O2 formation. Under plasma excitation, O2 is converted into 1O2via energy transfer, while the H2O and H2 in the solution are ionized to produce a large number of H+ ions. Subsequently, 1O2 directly reacts with H+ to form H2O2. This research confirms the high efficiency of porphyrin-based catalysts in solution plasma-driven H2O2 synthesis and provides a new perspective for the green production of H2O2.

Porphyrin supramolecules catalysts with CO convert O 2 to 1 O 2 via energy transfer in plasma; 1 O 2 + 2H + + 2e − → H 2 O 2 . Dispersion engineering boosts US‑TCPP to 7.0 mmol L −1 h −1 .

Nonmetallic polymers are promising materials for the production of H2O2 by O2 reduction reactions in water, since they activate oxygen to reactive oxygen species under photo/electrical excitation. However, the slow kinetics of water activation restricts the rate of H2O2 production. Solution plasma technology has emerged as a promising strategy, as it effectively activates water molecules, thereby facilitating the water oxidation process while simultaneously introducing an oxygen reduction pathway that consumes H+ ions for efficient H2O2 production. Here, we loaded meso-tetra(4-carboxyphenyl) porphyrin (TCPP) with photosensitizing properties onto cyano-modified carbon nitride (CCN) to form pi-pi-stacked solution plasma catalysts that exhibited excellent H2O2 activity. The H+ concentration in the CCN/TCPP polymer solution decreased by a factor of 104 after 1 h of discharge compared to the noncatalyst system, indicating that the catalyst promoted the O2 reduction reaction. The CCN/TCPP accumulated 32 mM H2O2 with an energy conversion efficiency of 0.91%. The lower intersystem crossing (ISC) energy barrier of CCN/TCPP allows CCN/TCPP and O2 to produce 1O2 at a faster energy transfer rate to consume H+ from the discharge and produce H2O2. This study widens the design of solution plasma catalysts for the production of H2O2 and provides an effective strategy for the sustainable development of solution plasma catalytic technology.

Holographic steganography is considered a highly secure information transmission method that relies on active optical media to achieve multifunctionality. Transition metal oxides undergo reversible color changes during photoelectrically driven cation migration, providing a platform for tunable holography. However, single-ion migration systems suffer from rapid attenuation of holographic fringe contrast under repeated electrical switching, leading to the loss of diffraction efficiency and hindering reliable information readout. In this Letter, we develop a WO x /electrolyte/TiO 2 optoelectronic memory based on Li + -Ag + dual-cation synergistic regulation. The excitation of near-ultraviolet coherent light not only constructs an initial hologram in the WO x layer but also generates latent nucleation sites for Ag particles on the TiO 2 surface. During subsequent electrical switching, the dual-cation device can either hide holograms by modulating the Li + ions distribution or reproduce signals by selectively depositing Ag particles on the pre-defined latent sites. The device integrates the color-changing pathway of WO x /Li + with the silver electrodeposition of TiO 2 /Ag + , improving the diffraction efficiency and cycling durability. By programming specific voltage sequences, the holographic steganography based on spatiotemporal multiplexing is achieved. This work paves a bright path for high-density information security storage.

SnO2 is considered an ideal electron transport layer (ETL) material for solar cells due to its excellent stability, high transparency, and high electron mobility, however, its performance in near-infrared quantum dots photovoltaics has remained unsatisfactory. This underperformance is mainly linked to generally-used chemical bath deposition (CBD) method of SnO2 ETLs which is prone to incomplete oxidation of Sn2+ precursor. The resulting Sn2+ residues and oxygen vacancy (Ov) induce severe interfacial traps limiting further efficiency gains. In this study, we utilized dielectric barrier discharge technology to generate high-activity oxygen plasma for gas-phase post-treating the CBD-SnO2 surface. This oxygen plasma reduced the amount of Sn2+ and Ov by similar to 20%, which suppressed trap-assisted recombination and collectively reduced interfacial energy band alignment offset. Compared with untreated devices (efficiency: 11.32%), PbS QDSCs with optimized SnO2 ETL increased carrier lifetime by nearly twofold and enhanced interfacial carrier collection efficiency by 10.7%, significantly raising efficiency to 13.28%. This distinctive gas-phase post-treatment method, which introduces no additional chemicals and leaves no residues, offers a new technical avenue for developing high-performance ETL.

The development of high-performance, stable quantum dot (QD) inks is critical yet challenging for advancing the efficiency and scalability of next-generation solution-processed optoelectronic devices. Inorganic lead iodide ligands passivated lead sulfide QDs (PbS-PbI2) have been attractive for their superior surface passivation and strong inter-dot coupling. However, the state-of-the-art inks typically require strongly coordinating alkylamine solvents to dissociate and solvate the PbI2 ligand, yet these solvents can continuously etch the QDs, leading to rapid ink degradation within a few hours. Herein, an amine-vapor pre-solvation strategy is proposed using a facile butylamine (BA) vapor (u0026lt; 10 min) pretreatment of QDs, enabling stable dispersion of QDs in BA-free solvents (e.g., N-methyl-2-pyrrolidone (NMP) and propylene carbonate). The resulting QD inks remain stable for u0026gt; 60 days with no variation in QD size, while QD films exhibit reduced trap-related losses. Solar cells processed from 60-day-aged NMP inks retain 90% of their initial power conversion efficiency (12.1%), whereas BA-based inks degrade within hours, reducing their device efficiency from 11% to 0.3% after only 4 h of aging. The shelf-stable NMP ink further enables large-area blade-coating of uniform PbS-PbI2 films, manifesting the potential in scalable manufacturing of high-performance QD optoelectronic devices.

The optical encryption strategy based on the combination of fluorescence and polarization holography has significant advantages in multi-dimensional coding and visual security, and plays a crucial role in information protection. However, building a robust dual-functional platform with full-color fluorescence tunability and large storage capacity still remains a big challenge. Herein, fluorescent carbon dots (CDs) are assembled into gridded titania (TiO2) scaffolds for ultra-high-level holographic encryption. The construction of the fluorescence-holography encryption layer utilizes both the polarized spectral hole-burning of CDs/TiO2 based on directional interface charge transfer and the fluorescence emission characteristics of CDs monomers. Chromaticity information is assigned to Quick Response (QR) code patterns under UV excitation. Then, micrometric computer-generated holograms (CGHs) are written into the CDs/TiO2 region, which exhibits significant polarization dependence. The decryption of true information requires the super verification with color, coordinate, polarization, wavelength, and logical judgment. The platform demonstrates excellent optical and thermal stability, maintaining over 97% fluorescence intensity under prolonged UV irradiation, and persistent holographic reconstruction efficiency at 433 K for at least 30 h. This work integrates color display, fluorescence switch, and polarization holography, providing a promising path for high-security optical anti-counterfeiting and information encryption.

A universal molecular linker strategy enables the formation of high-quality CZTSSe/CdS heterojunctions by simultaneously controlling CdS nucleation and passivating CZTSSe surface defects, thereby enhancing photovoltaic efficiency.

The water-gas shift (WGS) reaction is pivotal for H2 production and purification, yet conventional processes rely on coupled middle and high temperature stages (180-300 °C). Development of wide-temperature-window catalysts could avoid temperature switching and reduce the energy demand. However, room-temperature WGS is particularly limited by sluggish water splitting. Here, we report a continuous-flow solution plasma (CSP) strategy to construct an oxygen vacancy-rich Au1/CeO2-Fe single-atom catalyst (SAC). Fe is uniformly doped into the CeO2 lattice to increase the density of oxygen vacancies and Au is stabilized as isolated atomic sites on the CeO2 surface. By photothermal excitation, the catalyst delivers high WGS activity across 25-300 °C. Notably, at 25 °C, the CO conversion rises from near-zero for conventional catalysts to 35%, overcoming the kinetic barrier of room-temperature WGS for a low CO conversion rate. Mechanistic studies reveal that Fe doping selectively promotes H2O dissociation, and Au SACs enhance CO adsorption and oxidation. Meanwhile, light activates CeO2 lattice oxygen and engages a Mars-van Krevelen cycle. The as-developed catalyst maintains significant activity from ambient temperature to 300 °C without temperature switching, providing a process toward energy-efficient H2 production and purification.

ABSTRACT Suppressing the formation of secondary phases during selenization has long been recognized as essential for achieving high‐efficiency Cu 2 ZnSn(S, Se) 4 (CZTSSe) photovoltaics. However, Se depletion arising from the kinetic imbalance between Se supply and consumption at the buried interface significantly increases the propensity of secondary phase formation. Here, we introduce a self‐sacrificing polymethyl methacrylate (PMMA) interlayer to mitigate Se depletion, thereby avoiding the formation of secondary phases and improving device performance. During selenization, the PMMA layer inhibits the competitive reaction of the Mo substrate for Se, alleviates local Se deficiency, and promotes a direct one‐step phase conversion into CZTSSe without generating secondary phases. As selenization proceeds, the PMMA layer gradually decomposes and disappears, leaving no additional barrier to carrier transport across the buried interface. We provide direct visualization of the composition and spatial distribution of secondary phases formed under Se‐depletion conditions at the buried interface, including ZnS, Zn x Sn 1‐x S, SnSe, and Cu 2 SnS(Se) x . Transient photocarrier dynamics analysis verifies enhanced carrier extraction at the buried interface upon introduction of the PMMA buried layer. Incorporating a PMMA buried layer enhances the device efficiency from 12.81% to 13.91%. This work provides new strategies for controllable phase transformation at buried interfaces in CZTSSe and related chalcogenide photovoltaic systems.

A high-quality CdS/Cu2ZnSn(S,Se)4 (CZTSSe) heterojunction interface is considered essential for obtaining efficient CZTSSe solar cells. However, the inherent surface defects of CZTSSe films, along with the non-uniform nucleation of CdS, pose non-negligible challenges to constructing a high-quality heterojunction. In this work, we proposed an innovative molecular linker strategy for dual-sided modulation of CdS/CZTSSe heterojunction, simultaneously passivating CZTSSe surface defects and regulating uniform CdS nucleation. We systematically screened 10 amino acid-based molecules and identified cysteine (Cys) as exhibiting outstanding bifunctional properties. The introduction of Cys improved device efficiency from 10.35% to 11.15% in the dimethylformamide (DMF) solution preparation system, and significantly enhanced efficiency from 11.22% to 12.79% in the 2-methoxyethanol (MOE) solution preparation system, demonstrating the broad applicability of this strategy. Experimental and theoretical analyses revealed that the passivation effect of Cys primarily originated from the effective interactions between its thiol (-SH) and amino (-NH2) groups and the intrinsic surface defects of CZTSSe, leading to stable defect passivation. Meanwhile, the outward-facing carboxyl (-COOH) group in Cys helped homogenize the nucleation sites on the CZTSSe surface, promoting the dense and uniform nucleation of CdS. This work established a scalable strategy for interfacial optimization, advancing the development of CZTSSe thin-film photovoltaic devices.

PbS quantum junction photodetectors (QJPDs), composed solely of sequentially stacked n- and p-doped quantum dot layers on a fluorine-doped tin oxide (FTO) electrode, are promising for high-speed photodetection. Their simplified architecture minimizes carrier transport distance, enabling rapid photoresponse and high-bandwidth signal processing. However, carrier concentration mismatch between the FTO electrode and the quantum dot layers induces interfacial charge accumulation and increases device capacitance, limiting the temporal response of device. Although inserting interfacial layers can mitigate this issue, it inevitably increases structural complexity. Here, we develop an oxygen plasma modification to remove fluorine-rich surface species of commercial FTO, reducing the surface fluorine concentration from 25% to 14%. This suppresses interfacial charge accumulation at the FTO/PbS interface, reducing the device capacitance by approximately 47% at 100 kHz. The optimized QJPD achieves a response time of 0.32 μs at 980 nm (theoretical bandwidth of 1.06 MHz) a 63% improvement over unmodified QJPDs. Our high-speed QJPD realized the indoor near-infrared optical communication with swift data transmission at 1.6 Mbps. This work reveals electrode-induced capacitance as a speed-limiting factor in QJPDs, and provides a simple, additional-layer-free route to mitigate interfacial capacitance, offering a pathway to high-speed near-infrared communication and imaging.