High-quality chabazite (CHA-type) zeolites are highly desirable for their excellent catalytic performance without significant cost. However, their optimal synthesis remains challenging due to the difficulty in simultaneously controlling crystallinity and hierarchical porosity, as well as the persistent issue of polymorph competition. To overcome these hurdles, we present a one-step approach for synthesizing high-quality hierarchical CHA zeolites through controlled etching-assisted crystallization. Moving beyond conventional ammonium fluoride (NH4F) and phenol, we systematically investigated a series of para-substituted phenols and structurally diverse ammonium salts as a single additive to manipulate CHA crystallization. Our research reveals that the etching capacity of the additives dictates the properties of the resulting zeolites. By balancing dissolution and growth kinetics, we achieve high crystallinity and tailored porosity while circumventing polymorphism and amorphization. Strikingly, the judicious selection of etchant acid strength and amount consistently yields optimized mesoporous CHA zeolites with similar structural features and catalytic performance in selective catalytic reduction with ammonia (NH3-SCR). We identify an inverse correlation between the optimal in situ nucleophile amount (defined as the etchant quantity multiplied by its number of dissociable protons) and its acid dissociation constant (Ka) for modulating zeolite synthesis, which closely aligns with the ex situ dissolution rate, underscoring the importance of employing mild etchants. This correlation unifies the mechanism of etching-assisted zeolite crystallization. The demonstrated wide applicability of mild in situ etchants encompassing organic or inorganic compounds for crystallization control offers a versatile approach for the rational design of targeted zeolites with tailored functional properties.

Drug-resistant bacterial infections are a growing crisis that severely threatens global public health, creating an urgent need for novel antibacterial strategies beyond traditional antibiotics. Two-dimensional (2D) metal-organic frameworks (MOFs) have emerged as a promising class of nanomaterials for antibacterial applications due to their high specific surface area, tunable porosity, structural diversity, atomically thin morphology, and exceptional structural tunability. However, the antibacterial activity of pristine 2D MOFs is often limited, making structural engineering essential for optimizing their performance. This review systematically summarizes recent advances in the structural engineering of 2D MOF-based nanomaterials for enhanced antibacterial therapy. Five primary engineering strategies are elaborated: dimension and morphology control, heterojunction construction, functional modification, element ratio regulation, and defect engineering. These approaches enable precise modulation of physicochemical properties, leading to significantly improved reactive oxygen species generation, charge separation, catalytic activity, and bacterial targeting. Subsequently, the diverse antibacterial mechanisms enabled by these engineered 2D MOFs are discussed, including photoresponsive therapy (photodynamic and photothermal), nanozyme-catalyzed therapy, controlled ion release, ultrasound-activated therapy, physical membrane disruption, and synergistic multimodal strategies. Finally, current challenges in clinical translation are critically analyzed, including synthesis scalability, long-term biocompatibility, targeting specificity, and stability, and an outlook on future directions is provided. By incorporating the latest developments in synthesis, mechanisms, and applications, this review seeks to provide guidance on the rational design of advanced 2D MOF-derived antibacterial agents and to inspire innovative approaches for combating drug-resistant bacterial infections.

Metal ion migration under operational gradients triggers irreversible decomposition and performance collapse in thermoelectric (TE) materials. β-Zn 4 Sb 3 has high TE performance but suffers from severe zinc (Zn) ion migration under an external field. This work uses powder atomic layer deposition (pALD) to engineer atomic-scale zinc oxide (ZnO) interfaces that simultaneously suppress Zn ion migration and enhance phonon scattering. Through precise ZnO coatings (50 to 200 cycles), we create continuous barriers that immobilize interstitial Zn ions, eliminating Zn motion and inhibiting phase decomposition. Optimized 100 ALD cycle coatings reduce lattice thermal conductivity by >20% through intensified boundary-phonon scattering, yielding a stabilized, nondegrading figure of merit compared to uncoated performance. Crucially, the thermal stability of 100-ALD-cycle-coated sample persists through 39,260 thermal cycles under gradients of 220 kelvin, and Seebeck coefficient mapping exhibits a uniform distribution along temperature difference. Our approach establishes pALD as a promising atomic-level interface design in migration-prone TE materials, bridging high performance with long-term operational reliability.

All-perovskite tandem solar cells are promising for achieving both high efficiency and thermal stability. Taking Cs(Sn, Pb)I3 as a representative example, this issue severely limits the open-circuit voltage and operational stability of the corresponding devices. Here, we reveal that lattice distortion in Cs(Sn, Pb)I3 fundamentally drives Sn2+ oxidation and phase separation, generating defects such as edge-sharing octahedral domains and anti-phase boundaries. Using ultralow-dose scanning transmission electron microscopy, we visualize these defects and correlate them with enhanced oxidation pathways. Incorporating dimethylammonium cations stabilizes the tetragonal perovskite phase, reducing perovskite structural distortion and suppressing Sn2+ oxidation. This structural engineering yields a narrow-band-gap (NBG) subcell with champion power conversion efficiency (PCE). Integrated with a 1.92 eV CsPbI2Br top cell, the resulting two-terminal tandem solar cells achieve a PCE of 19.3% (steady-state efficiency). These findings uncover the structural origin of Sn2+ instability, guiding the design of highly durable all-perovskite tandems.

Direct seawater electrolysis is severely constrained by the activity-durability trade-off and chloride-induced corrosion. Herein, we design corrosion-resistant, highly selective layered double hydroxide (LDH) catalysts by transitioning interlayer bonding from weak electrostatic attraction to strong coordination. Amphiphilic dodecylbenzenesulfonate (SDBS) coordinates with Fe active centers, forming robust Fe─O─S bonds that establish a securely locked microenvironment. Density functional theory reveals this coordination upshifts the Fe d-band center and enhances Fe─O covalency, lowering the thermodynamic oxygen evolution barrier. Simultaneously, molecular dynamics simulations show that hydrophobic alkyl tails reorganize the interfacial hydrogen-bond network. This creates a kinetic barrier against chloride, enabling high hydroxide-to-chloride diffusion selectivity (DOH -/DCl - ≈ 1.94). Consequently, the NiFe-SDBS electrode decouples stability from activity, delivering an ultralow overpotential of 239 mV at 10 mA cm-2 and sustaining 1000 mA cm-2 for >1000 h with negligible degradation. In a zero-gap anion exchange membrane (AEM) electrolyzer, it achieves 1000 mA cm-2 at ∼4.64 kWh Nm-3 and maintains robust stability (>600 h at 500 mA cm-2) with an ultra-low degradation rate of 0.18 mV h-1. This work establishes coordination-driven microenvironment engineering as a generalizable paradigm for durable electrocatalyst design.

Photoelectrochemical (PEC) water splitting offers low-cost, sustainable hydrogen fuel production, but the insufficient photoanode performance limits overall water splitting efficiency. Herein, PFeMo polyoxometalate nanoparticles embedded into a BiVO4 (bismuth vanadate [BVO]) photoanode boost the photon utilization efficiency by employing a novel strategy of enhancing the interfacial electric field and broadening light absorption pathways. Additionally, it can accelerate hole extraction by facilitating the dissociation of self-trapped excitons and reducing transmission voltage loss to achieve efficient charge separation. As a result, the BVO/PFeMo/NiFeOx photoanode demonstrates light absorption exceeding 90% in the 300-450 nm wavelength range, with charge separation efficiency approaching 100% at 1.23 VRHE. Furthermore, a perovskite solar cell with photoanodes in tandem delivers a remarkable solar-to-hydrogen efficiency of 7.23%. Overall, this work proposes a new light absorption strategy on the basis of increasing BVO charge carrier separation, providing a new perspective for further improving the performance of photoanodes.

Fe-based oxygen evolution reaction (OER) catalysts are thwarted by intrinsic charge transport bottleneck and active sites dissolution. Herein, we report a NiCo@FePOx catalyst assembled from core-shell building blocks, wherein the core comprised nano-twinned NiCo alloys with amorphous FePOx as shell wrapped around. The NiCo@FePOx catalyst achieved low overpotential (η10 = 228 mV) and Tafel slope (29.8 mV dec−1), and the resulting anion-exchange membrane (AEM) water electrolyzer demonstrated durability for 800 h at 1 A cm−2 with negligible voltage increase. Experimental analysis showed the nano-twinned NiCo core provided conductive pathways and robust scaffolds, while the amorphous FePOx shell hosted coordinatively unsaturated Fe active sites. Density functional theory (DFT) calculations revealed FePOx as the catalytic entity, where coordinatively unsaturated Fe sites served as the adsorption center and POx reduced the overpotential by stabilizing OOH* intermediate through hydrogen bonds. This work provides valuable insights for constructing the crystalline-amorphous interphase frameworks to develop efficient and durable electrocatalysts.

Thermoelectric (TE) materials with high efficiency near room temperature are crucial for low‐temperature waste‐heat recovery and solid‐state cooling applications. Among them, Mg3(Sb, Bi)2‐based Zintl compounds have emerged as leading n‐type materials due to their intrinsically low lattice thermal conductivity and favorable electronic structure. However, their performance is still constrained by the relatively low carrier mobility in the low‐temperature regime because of the dominated grain‐boundary charge scattering, which limits the achievable power factor and thus the overall figure of merit (zT). Hereby, we proposed an interface modification strategy based on powder atomic layer deposition (pALD) of metallic Cu to enhance the carrier mobility of n‐type Mg3(Sb, Bi)2. The ALD‐Cu addition is found to be beneficial for improving carrier mobility by promoting grain growth, compensating Mg deficiencies at some of the grain boundaries (particle boundaries), and thereby mitigating the interfacial transport barriers. Metallic Cu was precisely deposited on TE powders without introducing oxygen‐ or water‐based precursors, thereby avoiding surface oxidation and degradation of the powders. Simultaneously, despite the more than twofold increase in grain size, the formation of Cu‐rich domains near particle boundaries acts as effective phonon‐scattering centers, leading to a lower lattice thermal conductivity. Benefiting from this synergistic modification of electrical and thermal transport, both peak and average zT over 303–573 K were enhanced by 14% and 13.3%, respectively. This work demonstrates a feasible metallic pALD approach for interface modification and establishes a new strategy to decouple transport parameters in n‐type Mg3(Sb, Bi)2‐based alloys for near room temperature applications.

The photocatalytic conversion of CO2 into high-value C2 products presents a promising green route toward renewable energy storage, fine chemical production and carbon neutrality. However, this process is limited so far by the high energy barrier for C & horbar;C coupling and the low efficiency of intermediate protonation. In this study, we constructed a 3hCuO/(Cu0.7Co0.3)Co2O4 heterojunction photocatalyst and identified the formation of elongated interfacial Cu & horbar;O & horbar;Co bridging bonds. This catalyst delivers a record-high C2H4 production rate of 211.5 & micro;mol g-1 h-1 in a CO2/water vapor system under 300 W Xenon lamp illumination, a 7.8-fold improvement over the control sample. Mechanistic studies indicate that the elongated Cu & horbar;O & horbar;Co bridges strengthen the synergy between the Cu and Co dual-metal sites: not only can this structural feature leave room for *CO migration, which facilitates proton transfer to Cu sites and accelerates the rate-determining step (*CO -> *COH), it also mitigates steric hindrance caused by the accumulation of reaction intermediates, thus promoting asymmetric *COH-CO coupling. Consequently, both the yield and selectivity of C2H4 are significantly enhanced. By offering atomic-level insights into the bimetallic cooperative catalysis, this work paves the way for the rational design of heterojunction bridging structures to efficiently steer CO2 reduction pathways toward C2 and beyond.

All-inorganic perovskite solar cells (PSCs) have emerged as a prominent research focus because the high thermal/photo stability they can offer is critical to commercialization of the burgeoning photovoltaic (PV) technology. However, there remain issues pertaining to the susceptibility of the all-inorganic perovskites to surface degradation from moisture ingress under ambient conditions and the suboptimal PV efficiency that still lags substantially behind that of their organic-inorganic hybrid counterparts. To address these challenges, this work employs an in situ self-assembly strategy to construct a 1D/3D perovskite heterojunction on top of the all-inorganic perovskite using tetrabutylammonium trifluoromethanesulfonate (TTFS). While typical ammonium salts only provide a cationic barrier or weak passivation, the TTFS-based design uniquely synergizes a hydrophobic cationic barrier with strong anionic passivation, and concurrently creates fast electron extraction channels through a nanostructured interface. This approach overcomes the conventional trade-off between stability and efficiency. By exploiting it to optimize a semi-transparent wide-band PSC for 4-terminal (4-T) tandem devices, a certified power conversion efficiency (PCE) of 17.10% was achieved together with exceptional operational stability under maximum power point (MPP) tracking-maintaining 80% of the initial PCE (T80) after operating for 1210 hours at 65 °C and 650 hours at 85 °C (ISOS-L-2). When it is combined with a narrow-band all-inorganic PSC in the 4-T tandem configuration, a certified efficiency of 21.54% was obtained, which is the highest reported for this type of tandem cells. Through synergistic optimization of interface stabilization and tandem optoelectronic management, this work provides valuable insights for developing efficient and stable all-inorganic perovskite tandem solar cells.

The energy conversion efficiency of a single-junction photovoltaic device is mainly constrained by its bandgap setting a theoretical upper bound known as Shockley-Queisser (S-Q) limit. In this work, carbon-based perovskite solar cells (C-PSCs) are harnessed to transcend the S-Q limit through a synergistic integration of photovoltaic and photothermal conversion for water splitting: the above-bandgap photons are converted into electrical energy, while the below-bandgap photons are all transformed into thermal energy through the carbon composite electrode. Correlative investigations into photovoltaic performance under varying solar driven heat-accumulation conditions, irradiance spectra, and incident light intensity reveal that C-PSCs exhibit lower temperature coefficients and higher full-spectrum solar energy utilization than conventional silicon cells. Furthermore, we calculated the S-Q efficiency limits under varying temperatures, irradiation spectra, and bandgap configurations, thereby offering critical insights for optimizing graded utilization of full solar spectrum. By integrating C-PSCs with water-splitting electrolytic cells, a graded utilization of full solar spectrum through both photovoltaic and photothermal conversion within the single-junction device is achieved. This integration elevates the solar-to-hydrogen (STH) efficiency from 11.30% to 12.98%, representing an enhancement of 14.86%, and achieves a remarkable STH-to-power conversion efficiency (PCE) ratio of up to 71.0%, highlighting its profound transformative potential.

Spray coating has emerged as a transformative technique for fabricating high-quality perovskite thick films, which are essential for advanced photodetectors such as X-ray and narrowband sensors. This review surveys and systematically elucidates the physicochemical mechanisms underlying the aerosol-liquid-solid (ALS) transformation during spray deposition, focusing on three core stages: aerosol generation (via pneumatic, electrospray, or ultrasonic methods), droplet deposition and wetting dynamics, and liquid-to-solid crystallization. The interplay among precursor properties, spray parameters, and substrate characteristics dictates film morphology, crystallinity, and defect density. We highlight optimization strategies, including solvent engineering, additive incorporation, and process control, that enable the growth of dense, vertically aligned, and large-grained perovskite films with thicknesses up to hundreds of micrometers. Furthermore, the integration of dimensional engineering and heterojunction design through sequential spray deposition enhances charge transport, suppresses ion migration, and improves detection performance. Applications of these films are demonstrated in direct X-ray detectors and filter-free narrowband photodetectors with high sensitivity, low detection limits, and excellent spatial resolution. Remaining challenges are also discussed in understanding dynamic phase transitions and ensuring large-area uniformity of the spray-deposited films. Advancing in situ characterization and intelligent process control will accelerate the transition of spray coating from a laboratory technique to a scalable precision-manufacturing platform for next-generation perovskite optoelectronics.

ABSTRACT Stability at industrially relevant current densities remains a central challenge for transition‐metal phosphide based hydrogen evolution electrocatalysts operating in alkaline condition. To combat catalyst degradation, here the interfacial hydroxyl chemistry is regulated by robustly constructing an amorphous CoP/CeO 2− x heterostructure through a facile two‐step electrodeposition strategy. Operando Raman spectroscopy combined with density functional theory calculations reveals that oxygen‐vacancy‐rich CeO 2− x selectively captures *OH intermediates generated on Co sites, enabling efficient hydroxyl spillover away from CoP and thereby suppressing P oxidation and dissolution. The amorphous CoP framework further facilitates interfacial coupling and hydroxyl migration by providing abundant unsaturated coordination sites and dense Co/Ce interfacial contact. Benefiting from this synergistic effect, CoP/CeO 2− x delivers enhanced activity together with remarkable durability, sustaining 1 A cm −2 for over 320 h in alkaline electrolyte. When implemented as the cathode in an anion exchange membrane water electrolyzer, the catalyst operates stably for 750 h at 1 A cm −2 and 60°C with a low degradation rate of ≈52 µV h −1 . This work demonstrates the effectiveness of interfacial hydroxyl‐spillover engineering for stabilizing CoP‐based electrocatalysts under practical operating conditions.

Lithium extraction is of paramount importance for the emerging batteries. For salt lakes or recyclable lithium-containing materials, various metal ions are unavoidable, including Na+, K+, Ca2+ and Mg2+. Lithium aluminum layered double hydroxides (LiAl-LDHs), as the most mature adsorbent, have been intensively studied on adsorption capacity and stability, but the cation adsorption selectivity is confusing and sometimes contradictory. To decipher the intrinsic cation selectivity of this nanosheets adsorbent, we track the mass fluctuation using operando quartz crystal microbalance with dissipation (QCM-D) method. First, we establish this effective monitoring strategy through accurately discriminating the adsorption-desorption behavior of interference-free LiAl-LDH/LiAlFe-LDH nanosheets. Then, by combining adsorption process of metal ions and density functional theory (DFT) calculations, we determine the intrinsic ion-selectivity sequence of Li+ > Mg2+ >> Na+ approximate to K+ approximate to Ca2+. For ions larger than Li+ (0.76 & Aring;), a well-crystallized structure hardly adsorbs Na+ (1.02 & Aring;), K+ (1.38 & Aring;), and Ca2+ (1.00 & Aring;) limited by the steric hinderance. Meantime, the dehydration energy consumption of hydrated ions determines the trend of Li+ > Mg2+. Following, the SA-LiAl-LDH (composite binder-LDH adsorbent) directly corroborates that the misleading interfacial process result from sodium alginate binder adsorption. The work ends the confusion on the intrinsic properties of LiAl-LDHs and provides a clear insight for deciphering the myriad of ion adsorption selectivity.

Oxygen vacancy-rich bismuth vanadate (BiVO4- x) photoanodes usually exhibit excellent bulk charge separation efficiency and relatively low onset potential, but the Fermi-level pinning effect leads to a relatively low photovoltage (V ph). Herein, we propose a synergistic strategy of F element doping and in situ deposition of the NiCoBi co-catalyst to amplify the V ph of BiVO4- x. Systematic investigations demonstrate that F doping modifies the electronic structure of BiVO4- x, increases the electron work function, and synergizes with the NiCoBi co-catalyst to repair surface defect states, thereby enhancing the V ph of the F-BiVO4- x/NiCoBi photoanode by 37.78% compared to its unmodified BiVO4- x counterpart. Consequently, both organic oxidation reactions and water oxidation reactions are significantly activated. More importantly, the enhanced V p h can also improve the long-term operational stability of the photoanode. Such improvements in multiple performance metrics can provide a universal strategy for the design of next-generation photoelectrode materials.

Replacing the oxygen evolution reaction with the thermodynamically more favorable urea oxidation reaction (UOR) enables energy-efficient H2 production in seawater electrolysis. However, conventional UOR is plagued by sluggish kinetics and only generates low-value products. Herein, we report a NiCo2Se4 catalyst modified with vanadium-oxide layers containing oxygen vacancies (NiCo2Se4@VO), which via a new lattice oxygen mechanism (LOM) enables efficient NO2- electrosynthesis and enhanced H2 production from seawater electrolysis. In alkaline seawater containing 0.5 M urea, NiCo2Se4@VO required only 1.40 V vs. RHE to deliver 1 A cm-2 and maintained this performance for over 1200 h with an energy consumption of 3.72 kWh/m3H2. Additionally, at 1.35 V vs. RHE, the catalyst delivered a record-breaking NO2- Faradaic efficiency of 92.77% and a yield of 178.17 mg h-1 cm-2, setting a new benchmark for UOR catalysis. Mechanistic studies revealed that the Lewis-acidic layer captures active OH-, directing UOR toward NO2- instead of N2; meanwhile, UOR kinetics is accelerated by oxygen vacancies via LOM. More importantly, this study reveals for the first time that LOM is the governing pathway (> 60% contribution) for UOR and analogous small molecule electrooxidation reactions involving O-X bond coupling, establishing a new foundation for efficient sustainable energy conversion systems.

Achieving high solar-to-hydrogen (STH) efficiency in photoelectrochemical (PEC) water splitting is fundamentally limited by the challenge of simultaneously optimizing light absorption and charge separation in photoanodes. Herein, we overcome this bottleneck by fabricating ~20 nm thick B:C3N5-x nanosheets featuring a macroscopic gradient of B dopants and N vacancies on Mo:BVO via a substrate-mediated stabilization strategy. This unique architecture not only broadens the visible-light absorption range of BiVO4 (BVO), but also establishes a robust macroscopic dipole field. Originating from the breaking of inversion symmetry and synergistically reinforced by localized interlayer B-N bonding, this dipole field provides a powerful internal driving force for ultrafast carrier separation. Consequently, achieving a record 2.89% ABPE, the Mo:BVO/B:C3N5-x/NiFeBi photoanode delivers an outstanding 8.52% STH efficiency in tandem with a perovskite solar cell. This work demonstrates that combining gradient engineering with interlayer coupling effectively reconciles the intrinsic trade-off between optical thickness and charge extraction. Furthermore, this strategy presents a versatile blueprint for rationally designing of complex 2D/3D heterostructures for next-generation solar energy conversion and related applications.

Inorganic CsPbI3 perovskite, known for its high chemical stability and near-ideal bandgap, offers a promising solution to the instability of organic-inorganic hybrid perovskites that limit perovskite solar cells (PSCs) longevity. However, the conventional intermediate phase (dimethylammonium lead iodide, DMAPbI3) templating method suffers from inefficient phase conversion, hindering high-performance PSC development. To overcome this limitation, we engineered the crystallographic orientation of DMAPbI3 to promote rapid volatilization of DMAI and accelerating the transformation. Through in situ anchoring of Pb2+-complexing groups (-F < -Cl < -SO4) on TiO2 substrates during chemical bath deposition, we direct the preferential in-plane growth of Pb-rich (100) planes of DMAPbI3, enhancing its [100] orientation. Crucially, stronger complexing groups yield higher orientation degrees, accelerating thermal conversion into highly oriented CsPbI3 perovskite with higher purity and better optoelectronic properties. This strategy enables carbon-based, hole-transport-layer-free CsPbI3 PSCs to achieve a record 20.72% efficiency (certified as 20.35%). Unencapsulated device retains > 85% of their initial efficiency after 1156 h of continuous maximum power point tracking under 1-sun illumination.

The escalating global energy demand has spurred the emergence of diverse solar-powered systems. As a typical example, photocathodic protection (PCP) is a promising technology to prevent metal corrosion via a “solar-electric-chemical” energy conversion process. However, the implementation of reported PCP systems has been greatly restricted by two key issues, that is, severe electron–hole recombination and sluggish surface water oxidation reaction. Herein, we report a high-performance bilayer PCP photoanode composed of single-domain ferroelectric PbTiO3 nanoplates at the bottom and NiCo-LDH nanosheets at the top. Controlled external poling aligns the depolarization fields of individual PbTiO3 nanoplates and adds up to a much enhanced “macroscopic electric field” through the entire photoanode, which is harnessed to steer the charge flow inside the PCP system. In addition, the integration of NiCo-LDH nanosheets on top of the PbTiO3 nanoplates not only introduces an electric field at the heterostructure interface to further promote the interfacial charge transfer, but more importantly, accelerates the oxygen evolution reaction (OER) kinetics and suppresses the electron–hole recombination. Such a rational design allows for the synergistic contribution of the ferroelectric polarization of PbTiO3 and the superior OER catalytic activities of 2D LDH to the overall energy conversion efficiency, leading to stable cathodic protection for 304 stainless steel. This work provides a feasible design strategy for efficient PCP systems through precise optimization of the core photoelectrochemical reaction steps. A “ferroelectric-catalytic” bilayer was tailored to harness synergistic contributions from the intrinsic spontaneous polarization of ferroelectrics and the superior water oxidation activity of catalysts to improve “solar-electric-chemical” energy conversion for efficient cathodic metal protection.