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In this study, we prepared Pt/29.3 wt % LaFeO 3 on a commercial carrier of γ-Al 2 O 3 by inserting a CaO interlayer between LaFeO 3 and γ-Al 2 O 3 (i.e., Pt/LaFeO 3 /CaO/γ-Al 2 O 3 ) via atomic layer deposition. With the interaction between CaO and LaFeO 3 , the Pt supported on LaFeO 3 /CaO/γ-Al 2 O 3 demonstrated diverse dispersion characteristics, with regions showing well-dispersed Pt particles of approximately 2 nm, while others displayed some larger Pt nanoparticles. Interestingly, after redox treatments, the CO adsorption over Pt/LaFeO 3 /CaO/γ-Al 2 O 3 was significantly attenuated, and high-resolution transmission electron microscope analysis on the Pt surface revealed the presence of FeO x layers covering the Pt. Postoxidation, a thick FeO x layer was generated on Pt, leading to the inertness of the catalyst toward CO oxidation. However, after reduction, a thinner FeO x layer (approximately two atomic layers) developed on Pt, which facilitated the oxidation of CO through the Pt-FeO x interface.

Noncanonical amino acids (ncAAs) are synthetic building blocks that, when incorporated into proteins, confer novel functions and enable precise control over biological processes. These small yet powerful tools offer unprecedented opportunities to investigate and manipulate various complex life forms. In particular, ncAA incorporation technology has garnered significant attention in the study of animals and their constituent cells, which serve as invaluable model organisms for gaining insights into human physiology, genetics, and diseases. This review will provide a comprehensive discussion on the applications of ncAA incorporation technology in animals and animal cells, covering past achievements, current developments, and future perspectives.

Type I interferons (IFNs) are essential for activating dendritic cells (DCs) and presenting tumor-associated antigens to T cells. IFNs are primarily produced from DCs among immune cells. A combination of chemotherapy and metalloimmunotherapy induces IFN production by activating the cyclic GMP-AMP synthase-stimulator of interferon genes (cGAS-STING) pathway. However, chemotherapeutic agents deplete DC populations, suppressing immunostimulatory activities, despite their potent anticancer activities. Furthermore, an optimal ratio between chemotherapeutic agents and metal for activating DCs at the highest level has not been reported, and evidence for ensuring DC survival is lacking. In this study, we hypothesized that there is an optimal ratio to yield the highest DC maturation and anticancer activity with minimal DC depletion. To demonstrate it, we have designed a pH and redox dual-responsive nanoparticle, MnO 2 @BSA@DOX (MD), to prevent DCs from depleting and activate the cGAS-STING pathway both in cancer cells and DCs, inducing considerable levels of IFNs and maturation. MD consists of a core-layer structure, a manganese dioxide (MnO 2 ) core, and a cross-linked layer with bovine serum albumin (BSA) and doxorubicin (DOX), with a specific ratio of DOX to manganese. MD exhibits structure-based selectivity between cancer cells and DCs by targeting the extracellular pH of the tumor microenvironment and intracellular redox reactions in cancer cells. Among various formulations, the 1:1 ratio shows the highest maturation with no significant depletion. Moreover, it induces distinct cytotoxicity in cancer cells through apoptosis and cGAS-STING activation, leading to increased calreticulin expression and enhanced DC phagocytosis. Consequently, it results in superior tumor suppression and prolonged survival with the high accumulation of MD in the tumor and no observed systemic toxicities, highlighting its potential as a therapeutic agent in cancer treatments.

Transition metal carbenes have emerged as versatile intermediates for various types of alkylations. While reactions of metal carbene species with alkenes have been extensively studied, most examples focus on cyclopropanation and allylic C-H insertion. Herein, we present the first example of a catalytic strategy for the carbene-involved regioselective remote C-H alkylation of internal olefins by synergistically combining two iridium-mediated reactivities of olefin chain walking and carbenoid migratory insertion. The present method, utilizing sulfoxonium ylides as a bench-stable robust carbene precursor, was found to be effective for a series of olefins tethered with alkyl chains, heteroatom substituents, and complex biorelevant moieties. Combined experimental and computational studies revealed that reversible iridium hydride-mediated olefin chain walking proceeds to lead to a terminal alkyl-Ir intermediate, which then forms a carbenoid species for the final migratory insertion, resulting in regioselective terminal-alkylated products.

Fiber-based organic light-emitting diodes (OLEDs) are gaining attention as promising candidates to achieve truly wearable textile displays because of their favorable electrical and mechanical characteristics. However, although fiber OLEDs have been developed into passive-matrix displays, it has not been possible to achieve active OLED operation because of the difficulty of realizing fiber-based thin film transistors (TFTs) with the proper electrical and mechanical performance at the same time. Here, 1D cylindrical fiber-based IGZO TFTs, which simultaneously exhibit a high electrical performance and flexibility, are reported. To address this trade-off relationship, four key stages of a novel fabrication process and unique device structures that suitable for the thermal properties and cylindrical structure of the fiber were applied: (I) prethermal treatment, (II) partially patterned layers, (III) coplanar structure, and (IV) continuous postannealing (CPA) process. As a result, the fabricated fiber-based IGZO TFTs showed high mobility (8.6 cm 2 /(V s)) and low off-current (∼10 -12 A), comparable to that glass-based TFTs, as well as flexibility. Furthermore, based on these valid performances, it was demonstrated that fiber phOLEDs could be driven by fiber-based IGZO TFTs using a wiring connection with Cu wire and Ag paste. The results suggest that this may allow the potential fabrication of fully textile AMOLED displays, integrated with TFTs.

Two-dimensional conductive metal-organic frameworks (2D cMOFs) stand at the forefront of chemiresistive sensing innovations due to their high surface areas, distinctive morphologies, and substantial electronic conductivity. Particularly, 2D cMOFs crafted using 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) and 2,3,6,7,10,11-hexaiminotriphenylene (HITP) organic ligands have garnered a large amount of attention due to their designable active sites and proper conductive characteristics. Nevertheless, a deeper exploration into their sensing mechanisms is imperative for a comprehensive understanding of the intrinsic chemistry, which is crucial for the intricate design of specialized 2D cMOF chemiresistive sensors. In this study, we fabricate six M-HXTP (M = Co, Ni, and Cu; X = H and I) chemiresistive sensors, focusing on the application of hydrogen sulfide (H 2 S) detection. Among these, the 2D cMOFs incorporating Cu metal manifested a remarkably enhanced response to H 2 S. A combination of experimental and computational studies unveils the mechanisms of sulfur oxidation and Cu reduction, wherein distortion of the reduced MX 4 cluster markedly amplifies the sensing response. Lastly, a real-time and portable wireless H 2 S sensing module has been demonstrated by using the Cu-HHTP composite material, highlighting the substantial practical significance and potential applicability.

Fine inhalable particulate matter (PM 2.5 ) is a harmful airborne pollutant, with serious repercussions to public health worldwide. To prevent the influx of PM 2.5 into the indoor living and working space, we conceived the design of a "filtration window" that exhibits efficient PM 2.5 filtration capabilities while having sufficient transparency and physical durability. In this work, we demonstrate the successful fabrication of a transparent (∼80%) PM 2.5 filter based on nanofibrous poly(vinylidenefluoride- co -trifluoroethylene) (PVDF-TrFE), which captures PM 2.5 by electrostatic mechanisms originating from the ferroelectric property of the copolymer. The embedded PVDF-TrFE-based nanofibrous filter exhibits a notable PM 2.5 removal efficiency of 93%, which is on par with those of medical-grade face masks. Simultaneously, owing to its dense packing, the PVDF-TrFE nanofibrous filter is highly durable, allowing it to be cleaned with water for reuse, and withstands its structural integrity even under a wind flow of 15 m/s, altogether making it practically viable as a functional window unit.

Enabling reversible control over the topological invariants, transitioning them from nontrivial to trivial states, has fundamental implications for quantum information processing and spintronics. It offers a promising avenue for establishing an efficient on/off switch mechanism for robust and dissipationless spin-currents. While mechanical strain has traditionally been advantageous for such manipulation of topological invariants, it often comes with the drawback of in-plane fractures, rendering it unsuitable for high-speed, time-dependent operations. This study employs ultrafast optical and THz spectroscopy to explore topological phase transitions induced by light-driven strain in Bi 2 Se 3 . Bi 2 Se 3 requires substantial strain for Z 2 switching. Our observations provide experimental evidence of ultrafast switching behavior, demonstrating a transition from a topological insulator with spin-momentum-locked surfaces to hybridized states and normal insulating phases under ambient conditions. Notably, applying light-induced strong out-of-plane strain effectively suppresses surface-bulk coupling, facilitating the differentiation of surface and bulk conductance even at room temperature─significantly surpassing the Debye temperature. We expect various time-dependent sequences of transient hybridization and manipulation of topological invariant through photoexcitation intensity adjustments. The sudden surface and bulk transport alterations near the transition point enable coherent conductance modulation at hypersound frequencies. Our findings on the potential of light-triggered ultrafast switching of topological invariants hold promise for high-speed topological switching and its related applications.

Tumor-infiltrating lymphocyte (TIL) therapy has shown promising responses in clinical trials for highly aggressive cancers such as advanced melanoma and metastatic colorectal cancer. However, TIL therapy is still limited in clinical practice due to the complex ex vivo cell preparation process. Here, we report an " in situ TIL therapy" for the treatment of solid tumors. We utilized lipid nanoparticles for the delivery of an mRNA encoding membrane-anchored anti-CD3 single-chain variable fragment (scFv) (MA-aCD3), efficiently engineering both tumor-associated macrophages (TAMs) and tumor cells following intratumoral delivery. Expression of MA-aCD3 resulted in enhanced TIL activation, proliferation, and tumor cell engagement directly within the tumor microenvironment. In B16F10 and MC38 tumor models, concurrent expression of MA-aCD3 on TAMs and tumor cells mediated by mRNA delivery resulted in significant antitumor effects via in situ polyclonal CD8 + TIL expansion and directed cytotoxic effector functions. In addition, combinatorial treatment of MA-aCD3-encoding mRNA and antiprogrammed cell death 1 (anti-PD-1) antibodies exhibited synergistic antitumor effects on anti-PD-1 refractory B16F10 tumors. Together, our findings suggest that in situ TIL therapy is a practical and effective mRNA-based therapeutic modality for the treatment of solid tumors.

Derivatives of polythiophene (PT) have garnered considerable attention in organic solar cells (OSCs) because of their relatively uncomplicated molecular structures and cost-effective synthesis. Herein, we have developed two regioisomeric fluorinated PT donors, PEI3T-FITVT and PEI3T-FOTVT, to realize efficient OSCs. PEI3T-FITVT and PEI3T-FOTVT are strategically designed with different fluorine atom arrangements on thiophene-vinyl-thiophene (TVT) units. Notably, PEI3T-FOTVT possesses enhanced backbone planarity induced by F···S noncovalent interactions between two constituent building blocks. Consequently, PEI3T-FOTVT with the higher aggregation and crystalline properties leads to a 2.5-fold increase in hole mobility over PEI3T-FITVT (from 1.4 × 10 -4 to 3.6 × 10 -4 cm 2 V -1 s -1 ). Furthermore, PEI3T-FOTVT exhibits higher domain purity than PEI3T-FITVT, leading to faster charge transport and reduced charge recombination in OSC devices. These characteristics lead to a higher power conversion efficiency of 14.4% for PEI3T-FOTVT-based OSCs, compared to 12.9% for PEI3T-FITVT-based OSCs.

Owing to the growing interest in wearable ionotronics, the demand for ionogels with outstanding mechanical and electrochemical characteristics has increased dramatically. Nevertheless, it remains challenging to simultaneously enhance the mechanical robustness and conductivity of ionogels because of their trade-off relationship. In this work, we propose physically/chemically dual-cross-linked ionogels designed to improve the mechanical strength without reducing ionic conductivity by introducing metal-ligand complexation only within the physically cross-linked domains. In particular, the impact of metal-ligand complexation, a crucial parameter in this strategy, on ionogel performance is systematically examined using various metal ions. The mechanical resilience and thermal stability of ionogels are effectively enhanced with Co 3+ having the highest coordination number, which can be explained by the highest metal-ligand complexation (i.e., chemical cross-linking) density. Additionally, there is no degradation in ionic conductivity when compared to the pristine ionogel because these complexations occur within physically cross-linking domains that are irrelevant to the ion conductive channels. The dual-cross-linked ionogels are successfully applied to alternating-current electroluminescent displays (ACEDs). Moreover, a versatile mixed-emitter strategy is suggested to improve practicality, enabling the realization of frequency-controlled multicolor ACEDs.

Perovskite oxides are promising candidates for chemiresistive-type gas sensors owing to their exceptional thermal and chemical stability during solid-gas reactions. However, perovskites suffer from critical issues such as low surface area and poor surface activity, which negatively influence the sensing characteristics. While metal nanoparticles can be incorporated in perovskites to improve their reactivity, the fundamental incompatibility between catalytic metals and perovskite oxides often leads to substantial structural degradation as well as phase instability. Herein, we overcome this challenge through the introduction of an intermediary phase that forms coherent interfaces with both the perovskite phase and catalyst metals. Specifically, we present the case study of p-type La 0.8 Ca 0.2 Fe 0.98 Pt 0.02 O 3 perovskite, whose hole accumulation layer was modulated by the incorporation of metal-organic framework (MOF)-derived n-type α-Fe 2 O 3 nanoparticles decorated with highly dispersed Pt catalysts. The resulting composite exhibited significantly improved surface activity over the nonmodified La 0.8 Ca 0.2 FeO 3 perovskite, leading to exceptional chemiresistive sensing performance toward acetone gas ( R g = 39.8 toward 10 ppm of acetone at 250 °C) with high cross-sensitivity against interfering gases. Importantly, our findings reaffirm the critical influence of interfacial engineering in facilitating surface chemical reactions on perovskite oxides and, by doing so, effectively provide a general synthetic guideline to the design of perovskite-based chemiresistors.R a = 39.8 toward 10 ppm of acetone at 250 °C) with high cross-sensitivity against interfering gases. Importantly, our findings reaffirm the critical influence of interfacial engineering in facilitating surface chemical reactions on perovskite oxides and, by doing so, effectively provide a general synthetic guideline to the design of perovskite-based chemiresistors.

The physicochemical characterization of trivalent ions is limited due to a lack of accurate force fields. By leveraging the latest machine learning force field to model aqueous AlCl 3 , we discover that upon dissolution of Al 3+ , water molecules beyond the second hydration shell are involved in the hydration process. A combination of scissoring of coordinating water is followed by synchronized secondary motion of water in the second solvation shell due to hydrogen bonding. Consequently, the water beyond the second solvation penetrates through the second solvation shell and coordinates to the Al 3+ . Our study reveals a novel microscopic understanding of solvation dynamics for the trivalent ion.

Plasmon resonance using metal nanostructures enables the realization of high-performance optoelectronic devices via field enhancements in the vicinity of the metal nanostructure. This study proposes an ultrabroadband MoS 2 photodetector based on the gap-mode plasmon of gold nanorods. The use of MoS 2 as a gap spacer for the gap-mode plasmon effect and as a channel material for the photodetector is demonstrated. The proposed photodetector demonstrates superior performance, a high photoresponsivity of 2.8 A/W at a near-infrared wavelength of 1100 nm, and a fast response time of 17 μs. In addition to the gap-mode plasmon effect of the gold nanorod enhancing the photoresponsivity from 1.13 to 8.7 A/W, the lateral surface plasmon resonance of the gold nanorods enhances the absorption of the longitudinal mode of the gold nanorods (near-infrared to infrared range). Further, the gap-mode plasmon effect of the gold nanorods enhances the absorption of the transverse mode of the gold nanorods (visible range), thus realizing ultrabroadband photodetection. Therefore, the proposed device design strategy contributes significantly to overcoming the trade-off between photoresponsivity and response time.

Rashba states have been actively revisited as a platform for advanced applications such as spintronics and topological quantum computation. Yet, access to the Rashba state is restricted to the specific material sets, and the methodology to control the Rashba state is not established. Here, we report the Rashba states on the (001) surface of KZnBi, a 3D Dirac semimetal. Using angle-resolved photoemission spectroscopy and first-principles calculations, we investigated the evolution of Rashba states under different surface conditions controlled by alkali metal deposition. We observed that restoring surface ordering enables a Rashba state, which is absent in freshly cleaved surfaces. Interestingly, we were able to modify the dispersion of the Rashba state from an ordinary parabolic dispersion to a linearly dispersing Dirac-like state by additional alkali-metal deposition. Our findings provide a methodology for engineering the properties of Rashba states for advanced applications and redefine topological systems as generic hosts of Rashba states.

MXenes possess a wide range of materials properties owing to their compositional and stoichiometric diversities, facilitating their utilization in various technological applications such as electrodes, catalysts, and supercapacitors. To explore their applicability, identification of thermodynamically stable and synthesizable MXenes should precede. The energy above the convex hull ( E ) calculated using the density functional theory (DFT) is a powerful scale to probe the thermodynamic stability. However, the high calculation cost of DFT limits the search space of unknown chemistry. To address this challenge, this study proposes an active learning (AL) framework consisting of a surrogate model and utility function for expeditious identification of thermodynamically stable MXenes in the extensive chemical space of 23,857 MXenes with compositional and stoichiometric diversity. Exploiting the fast inference speed and the capability of the AL framework to accurately identify stable MXenes, only 480 DFT calculations were required to identify 126 thermodynamically stable MXenes; among these, the stabilities of 89 MXenes have not been previously reported. In contrast, only two stable MXenes were identified among randomly selected 1693 MXenes, demonstrating the inefficiency of using only DFT calculations in exploring a large chemical space. The AL framework successfully minimized the number of DFT calculations while maximizing that of thermodynamically stable MXenes identified and can contribute to future studies in finding stable MXenes expeditiously.hull ) calculated using the density functional theory (DFT) is a powerful scale to probe the thermodynamic stability. However, the high calculation cost of DFT limits the search space of unknown chemistry. To address this challenge, this study proposes an active learning (AL) framework consisting of a surrogate model and utility function for expeditious identification of thermodynamically stable MXenes in the extensive chemical space of 23,857 MXenes with compositional and stoichiometric diversity. Exploiting the fast inference speed and the capability of the AL framework to accurately identify stable MXenes, only 480 DFT calculations were required to identify 126 thermodynamically stable MXenes; among these, the stabilities of 89 MXenes have not been previously reported. In contrast, only two stable MXenes were identified among randomly selected 1693 MXenes, demonstrating the inefficiency of using only DFT calculations in exploring a large chemical space. The AL framework successfully minimized the number of DFT calculations while maximizing that of thermodynamically stable MXenes identified and can contribute to future studies in finding stable MXenes expeditiously.

The performance of mid-infrared (MIR) on-chip gas sensors, operating via laser absorption spectroscopy, hinges critically on light-matter interaction dynamics, significantly influenced by external confinement and the effective light path length. Conventional on-chip sensors, however, face challenges in achieving the required limit of detection for highly sensitive applications, primarily due to their intrinsically short effective light path. Furthermore, these sensors are limited in their spectral range coverage within the MIR spectrum by the constraints of standard silicon-based platforms. To overcome these limitations, our research presents a novel approach to fabricate a freestanding germanium (Ge) photonic crystal waveguide (PCW) on a germanium-on-insulator (Ge-OI) platform, utilizing yttrium oxide (Y 2 O 3 ) as the buried oxide layer. This device leverages the broad transparent windows of Ge and Y 2 O 3 , broadening the spectral coverage across the MIR range. The introduction of the PCW and its slow light effect significantly elevate external confinement and light-matter interactions, enabling a notable reduction in waveguide length, which traditionally limits on-chip configurations. The freestanding structure not only expands the sensing region and enhances external confinement but also prevents the emergence of leaky modes within the PCW. As a result, our compact sensor achieves an exceptionally low LoD of 7.56 ppm for carbon dioxide (CO 2 ) sensing at the operational wavelength of 4.23 μm, with a compact waveguide length of only 800 μm.

In recent decades, data-driven methodologies have emerged as irreplaceable tools in materials science, particularly for elucidating structure-property relationships and facilitating the discovery of novel materials. However, despite the rapid development witnessed in other domains, amorphous materials have received relatively less attention in this context. The disordered atomic structure of amorphous materials resulting from irreversible reactions between building blocks has posed a difficulty in structural modeling, leading to a lack of databases that accurately reflect the amorphous nature of these materials. In this work, a database composed of 10,237 porous polymer networks (PPNs) was constructed from self-assembly simulations, resulting in the largest database of PPNs considering their amorphous characteristics. Through the distinct differences observed in comparison with existing databases, we emphasize that carefully considering the structural disorder of PPNs is essential for accurately characterizing their chemical behaviors. Machine learning models trained on the constructed database have confirmed that the macroscopic properties of amorphous PPNs can be predicted solely from the atomic structures of their monomers, implying that the characteristics of previously unseen PPNs can be assessed without the need for additional self-assembly simulations.

The precise characterization and control of single-electron wave functions emitted from a single-electron source are essential for advancing electron quantum optics. Here, we introduce a method for tailoring a single-electron emission distribution using energy filtering, enabling selective control of the distribution under various energy barrier conditions of the filter. The tailored electron is studied by reconstructing its Wigner distribution in the time-energy phase space using the continuous-variable tomography method. Our results reveal that the filtering cuts the portion of the distribution below the energy-barrier height of the filter in the time-energy space. While the filtering is demonstrated in a classical regime of the emitted electrons, we expect that this study significantly contributes to the design and implementation of advanced experiments toward quantum information processing based on single electrons.

The pursuit of harnessing superior mechanical properties achieved through the size effect on a macroscopic scale has been a prominent focus in engineering, as size-induced strengthening is enabled only in the nanoscale regime. This study presents a metal/ceramic/metal (MCM) nanocomposite reinforced by ceramic nanoarchitectures. Through proximity-field nanopatterning, the inch-scale production of nanoarchitecture films is enabled in a single fabrication step. The developed three-dimensional (3D) Ni/Al 2 O 3 /Ni nanocomposite film exhibits significantly high compressive strength, corresponding to an increase of approximately 30% compared with that calculated using the upper limits of the conventional rule of mixtures. The exceptional strength of the 3D MCM nanocomposite can be attributed to the extrinsic size effect of the ceramic nanoarchitectures. By combining size-induced strengthening of ceramics with the strengthening law for composites, a new type of strengthening model is derived and experimentally validated using the 3D MCM nanocomposite.

Reconstructing the surface nature of metal-organic frameworks (MOFs) as precatalytic structures is a promising methodology for improving electrocatalytic performance. However, regulating the structural evolution of MOFs during electrolysis remains highly uncontrollable and lacks an in-depth understanding of the role of in situ -derived active sites. Here, we suggest a simple approach to fine-tune the symmetry of Co-MOFs with an oxo-coordinated asymmetric coordination that acts as a prototypical structure motif for the oxygen evolution reaction (OER). Through a facile thermal treatment, the Co-N4 configuration of Co-MOFs transforms to the distorted Co-N3-oxo configuration of defective Co-ligand nanoclusters. By operando spectroscopic characterization, the reconstructed Co-N3-oxo structure enables a rapid structural transition toward homogeneous oxyhydroxides. Moreover, the defective nature of the precatalytic structure regulates the surface Co-O bonding environment with abundant μ 2 -O-Co 3+ sites, thereby exhibiting highly enhanced OER activity with an overpotential of 256 mV at 10 mA cm -2 and excellent durability for 100 h, compared with the pristine Co-MOFs. Atomistic simulations reveal that the effect of OER intermediates on the oxyhydroxides gets distributed among neighboring Co ions, promoting balanced binding of the intermediates. This work highlights an effective strategy to design the MOF-based structure for optimizing the surface nature, thus enhancing the electrocatalytic activity.

Modern graphics processing units (GPUs) provide an unprecedented level of computing power. In this study, we present a high-performance, multi-GPU implementation of the analytical nuclear gradient for Kohn-Sham time-dependent density functional theory (TDDFT), employing the Tamm-Dancoff approximation (TDA) and Gaussian-type atomic orbitals as basis functions. We discuss GPU-efficient algorithms for the derivatives of electron repulsion integrals and exchange-correlation functionals within the range-separated scheme. As an illustrative example, we calculate the TDA-TDDFT gradient of the S 1 state of a full-scale green fluorescent protein with explicit water solvent molecules, totaling 4353 atoms, at the ωB97X/def2-SVP level of theory. Our algorithm demonstrates favorable parallel efficiencies on a high-speed distributed system equipped with 256 Nvidia A100 GPUs, achieving >70% with up to 64 GPUs and 31% with 256 GPUs, effectively leveraging the capabilities of modern high-performance computing systems.

Single-crystal hexagonal boron nitride (hBN) is used extensively in many two-dimensional electronic and quantum devices, where defects significantly impact performance. Therefore, characterizing and engineering hBN defects are crucial for advancing these technologies. Here, we examine the capture and emission dynamics of defects in hBN by utilizing low-frequency noise (LFN) spectroscopy in hBN-encapsulated and graphene-contacted MoS 2 field-effect transistors (FETs). The low disorder of this heterostructure allows the detection of random telegraph signals (RTS) in large device dimensions of 100 μm 2 at cryogenic temperatures. Analysis of gate bias- and temperature-dependent LFN data indicates that RTS originates from a single trap species within hBN. By performing multispace density functional theory (MS-DFT) calculations on a gated defective hBN/MoS 2 heterostructure model, we assign substitutional carbon atoms in boron sites as the atomistic origin of RTS. This study demonstrates the utility of LFN spectroscopy combined with MS-DFT analysis on a low-disorder all-vdW FET as a powerful means for characterizing the atomistic defects in single-crystal hBN.

Europium halide perovskites are promising candidates for environmentally benign blue-light emitters with their narrow emission line width. However, the development of high-photoluminescence quantum yield (PLQY) colloidal europium halide perovskite nanocrystals (PNCs) is hindered by limited synthetic methods and elusive reaction mechanisms. Here, we provide an effective synthetic route for achieving high-PLQY deep-blue-emitting colloidal CsEuBr 3 PNCs. Using two Br-organic ligand precursors, oleylammonium bromide (OLAMHBr) and trioctylphosphine dibromide (TOPBr 2 ), we identified distinct phase evolution routes involving Eu 2+ :CsBr, Cs 4 EuBr 6 , and CsEuBr 3 . The OLAMHBr precursor initially promotes the formation of the Eu 2+ :CsBr phase, which reorganizes into the CsEuBr 3 perovskite phase via proton transfer. In contrast, the TOPBr 2 precursor induces the formation of core/shell Cs 4 EuBr 6 /CsBr PNCs, which subsequently transform into CsEuBr 3 through nucleophilic addition. The TOPBr 2 route exhibited enhanced CsEuBr 3 phase homogeneity, resulting in a significantly higher PLQY (40.5%; full width at half-maximum (fwhm) = 24 at 430 nm), compared to the OLAMHBr route (16.5% at 418 nm). Notably, the phase-pure CsEuBr 3 PNCs demonstrated a world-record PLQY among the reported blue-emitting lead-free PNCs that exhibit a narrow emission line width (fwhm <25 nm). This work highlights the significant role of organic ligands in the colloidal synthesis of CsEuBr 3 PNCs and their potential as nontoxic, solution-processable blue-light emitters.

In this Perspective, we present the recent advancement and the prospects of atomic-scale friction and adhesion measurements across the pressure gap between ultrahigh vacuum and ambient pressure environments using variable-pressure atomic force microscopy (VP-AFM). We introduce the VP-AFM that enables nanotribological studies under various gas conditions with partial pressure ranging from UHV (1.0 × 10 -10 mbar) to 1 bar. We highlight the frictional behaviors of ultrananocrystalline diamond surface in oxygen and water gas environments, as well as the chemical states probed with near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS). The atomic scale degradation processes of MA(CH 3 NH 3 )PbBr 3 , which is an organic-inorganic hybrid perovskite (OHP) investigated with VP-AFM are introduced. Finally, we discuss the potential works on catalytic model systems including bimetallic Pt 3 Ni(111) and TiO 2 (110) and the future perspective of nanotribology under ambient conditions.

Achieving structural and stereogenic diversity from the same starting materials remains a fundamental challenge in organic synthesis, requiring precise control over the selectivity. Here, we report divergent catalytic methods that selectively yield either cycloaddition or addition/elimination products from bicyclo[1.1.0]butanes and α,β-unsaturated ketones. By employing chiral Lewis acid or Brønsted acid catalysts, we achieved excellent regio-, diastereo-, and enantioselectivity across all three distinct transformations, affording a diverse array of synthetically valuable chiral bicyclo[2.1.1]hexanes and cyclobutenes. The divergent outcomes are controlled by the differential activation of the substrates by the specific chiral catalyst with the reaction conditions dictating the pathway selectivity. This strategy demonstrates the power of divergent catalysis in creating molecular complexity and diversity, offering a valuable tool for the synthesis of enantioenriched chiral building blocks.

Rh(III)-catalyzed B(4)-azo coupling reactions of o -carborane acids with aryl diazonium tetrafluoroborates have been developed, leading to the regioselective formation of B(4)-azo-coupled o -carboranes. Moreover, B(4)-azo-coupled o -carboranes can be further functionalized by introducing a second azo group, producing B(4)-C(1)-di(arylazo) o -carborane. The B(4)-azo group as an efficient directing group enables catalytic C-H amidation reactions, providing a new synthetic route for complex o -carborane derivatives.

Assessing the mechanical robustness of metal-organic frameworks (MOFs) is crucial to enhance their applicability in various fields. Although considerable research has been conducted on the relationship between the mechanical properties of MOFs and their structural features (such as pore size, surface area, and topology), the insufficient exploration of metal elements has prevented researchers from fully understanding their mechanical behavior. To plug this knowledge gap, we constructed a database of mechanical properties for 20,342 MOFs included in the QMOF database using molecular simulations to investigate the impact of metal elements on mechanical stability. Through Shapley additive explanations (SHAP) analysis, we found that Co and Ln could enhance the structural stability of MOFs. We validated these findings using newly generated hypothetical MOFs. Notably, we adopted an interpretable machine learning technique to analyze the contribution of remarkably diverse metal elements in the 20,342 MOFs to the mechanical properties of each MOF. We anticipate that this research will serve as a valuable tool for future studies on identifying mechanically robust MOFs suitable for various industrial applications.

There is a growing need to develop artificial intelligence technologies capable of accurately predicting the properties of materials. This necessitates the expansion of material databases beyond the scope of density functional theory, and also the development of deep learning (DL) models that can be effectively trained with a limited amount of high-fidelity data. We developed a DL model utilizing a crystal structure representation based on the orbital field matrix (OFM), which was modified to incorporate information on elemental properties and valence electron configurations. This model, effectively capturing the interrelation between the elemental properties in the crystal, was coined the PRoperty-networking Orbital Field maTrix-convolutional neural Network (PROFiT-Net). Remarkably, PROFiT-Net demonstrated high accuracy in predicting the dielectric constant, experimental band gaps, and formation enthalpies compared with other leading DL models. Moreover, our model accurately identifies physical patterns, such as avoiding the prediction of unphysical negative band gaps and exhibiting a Penn-model-like trend while maintaining the scalability. We envision that PROFiT-Net will accelerate the development of functional materials.

Industrial implementation of highly thermally conductive polymeric composites has been hindered by several hurdles, such as the low intrinsic thermal conductivity (TC) of polymers, the use of expensive thermally conductive fillers, and difficulty in processing composites with high filler loading. In this study, we introduce a straightforward fabrication method for a high TC polymeric composite with a programmed internal structure of a highly interconnected thermal conduction highway (HITCH) by the simple addition of partially cured resin fragments into the conventional filler/resin combination. Critical variables, such as the concentration of the added resin fragments and the local concentration of hexagonal boron nitride (hBN) in the HITCH, as well as the packing density of the fragments, were systematically tuned to maximize the TC with the use of the least amount of the filler. Careful choice of the compositions enabled a significant TC enhancement of the composite by 2.6 times (6.5 W/mK) compared to the value of the conventional composite at the same overall concentration of hBN (∼2.5 W/mK). Finally, a composite with high TC (∼12 W/mK) and strong tensile strength (∼22.6 MPa), which is good enough for most practical thermal management applications, could be successfully fabricated with the use of the least amount of the filler (∼34 wt %). The comprehensive study of the HITCH composite here can be easily extended to other combinations with various fillers and matrices and may provide a library to researchers looking for advanced materials for future thermal management systems.

Herein, we report halide nanocomposite solid electrolytes (HNSEs) that integrate diverse oxides with alterations that allow tuning of their ionic conductivity, (electro)chemical stability, and specific density. A two-step mechanochemical process enabled the synthesis of multimetal (or nonmetal) HNSEs, MO 2 -2Li 2 ZrCl 6 , as verified by pair distribution function and X-ray diffraction analyses. The multimetal (or nonmetal) HNSE strategy increases the ionic conductivity of Li 2 ZrCl 6 from 0.40 to 0.82 mS cm -1 . Additionally, cyclic voltammetry test findings corroborated the enhanced passivating properties of the HNSEs. Notably, incorporating SiO 2 into HNSEs leads to a substantial reduction in the specific density of HNSEs, demonstrating their strong potential for achieving a high energy density and lowering costs. Fluorinated SiO 2 -2Li 2 ZrCl 5 F HNSEs exhibited enhanced interfacial compatibility with Li 6 PS 5 Cl and LiCoO 2 electrodes. Cells employing SiO 2 -2Li 2 ZrCl 5 F with LiCoO 2 exhibit superior electrochemical performance delivering the initial discharge capacity of 162 mA h g -1 with 93.7% capacity retention at the 100th cycle at 60 °C.

The fundamental question regarding the fractionation phenomenon is whether diffusion alone is responsible for it or whether an additional advection dynamic is involved. We studied the fractionation by diffusion of particles in spatially heterogeneous environments. By experimentally observing the time-sequential fractionation patterns of dye particles diffusing across a solid-solid interface of varying polyacrylamide gel densities, we found that the two-component diffusion model accurately captures the observed fractionation dynamics. In contrast, single-component diffusion models by Fick, Wereide, and Chapman do not. Our results indicate that diffusion alone can explain the fractionation phenomenon and that additional advection dynamics are not involved. The underlying physics in the fractionation phenomenon is discussed by using a two-component random walk model.

Ice, one of the most enigmatic materials on Earth, exhibits diverse polymorphism, with research mainly focusing on the most commonly observed phases: hexagonal ice (I h ), cubic ice (I c ), and stacking-disordered ice (I sd ). While their formation or structural changes are crucial for advancements in cloud science, climate modeling, and cryogenic technology, the molecular mechanisms driving these phenomena remain unexplored. Herein, utilizing cryogenic transmission electron microscopy, we investigate the formation of ice at two different temperatures, demonstrating a size-dependent phase shift from I c to I sd . Furthermore, a relatively metastable cubic phase in I sd transitions to a hexagonal phase under electron beam radiation. This transition, facilitated by crystal defects, contrasts with perfect crystalline I c , which maintains its original phase, emphasizing the importance of defects in polymorphic phase transitions. Our findings provide novel insights on phase control during the ice growth processes and polymorphic phase transitions from the cubic-to-hexagonal phases.

Nanofiltration (NF) technology is pivotal for ensuring a sustainable and reliable supply of clean water. To address the critical need for advanced thin-film composite (TFC) polyamide (PA) membranes with exceptional permselectivity and fouling resistance for emerging contaminant purification, we introduce a novel high-performance NF membrane. This membrane features a selective polypiperazine (PIP) layer functionalized with amino-containing quaternary ammonium compounds (QACs) through an in situ interfacial polycondensation reaction. Our investigation demonstrated that precise QAC functionalization enabled the construction of the selective PA layer with increased surface area, enhanced microporosity, stronger electronegativity, and reduced thickness compared to the control PIP membrane. As a result, the QAC NF membrane exhibited an approximately 51% increase in water permeance compared to the control PIP membrane, while achieving superior retention capabilities for divalent salts (>99%) and emerging organic contaminants (>90%). Furthermore, the incorporation of QACs into the PIP selective layer was proved to be effective in mitigating mineral scaling by allowing selective passage of scale-forming cations, while simultaneously exhibiting strong antimicrobial properties to combat biofouling. The in situ QAC incorporation strategy presented in this study provides valuable guidelines for the fit-for-purpose design of the selective PA layer, which is crucial for the development of high-performance NF membranes for efficient water purification.

The chemical conversion of CO 2 into value-added products is the key technology to realize a carbon-neutral society. One representative example of such conversion is the reverse water-gas shift reaction, which produces CO from CO 2 . However, the activity is insufficient at ambient pressure and lower temperatures (<600 °C), making it a highly energy-intensive and impractical process. Herein, we report indium oxide nanofibers modified with palladium catalysts that exhibit significantly potent redox activities toward the reduction of CO 2 splitting via chemical looping. In particular, we uncover that the doped palladium cations are selectively reduced and precipitated onto the host oxide surface as metallic nanoparticles. These catalytic gems formed operando make In 2 O 3 lattice oxygen more redox-active in H 2 and CO 2 environments. As a result, the composite nanofiber catalysts demonstrate the reverse water-gas shift reaction via chemical looping at record-low temperatures (≤350 °C), while also imparting high activities (CO 2 conversion: 45%). Altogether, our findings expand the viability of CO 2 splitting at lower temperatures and provide design principles for indium oxide-based catalysts for CO 2 conversion.

This study aims to develop a method for the chiral analysis of organoboron compounds using nuclear magnetic resonance (NMR) spectroscopy. It addresses the longstanding challenge associated with these chiral organoboron compounds, which often require derivatization and pretreatment prior to chromatographic analysis. Our method utilizes tridentate ligands to facilitate effective ligand exchange and incorporates fluorine labels, allowing for the precise discrimination of 19 F NMR signals. This is achieved in conjunction with a chiral cationic cobalt complex, serving as the chiral solvating agent. This approach provides reliable and rapid determination of enantiomeric excess in a wide range of organoboron compounds, featuring various functional groups, and establishes a universal tool for assessing the optical purity of these substances., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Nanoparticle monolayers (NPMLs) exhibit unique collective properties that are highly desirable for applications in sensors, catalysts, and optics. However, their practical use is often hindered by structural instability, especially when they are exposed to solvents. In this study, we developed a method for the spontaneous deposition of gold nanoparticle monolayers (AuNPMLs) on silicon substrates via covalent bonding interactions that provides excellent structural stability in solvents with varying polarities. The esterification reaction between carboxyl-functionalized gold nanoparticles and alkyl-chloride-functionalized silicon substrates spontaneously forms AuNPMLs on the substrate in which single-crystalline domains are interconnected, forming a percolation network morphology. The ex situ scanning electron microscopy measurements show that the surface coverage of AuNPMLs rapidly increases up to ca. 60% during the initial 10 min, followed by gradual growth and saturation at ca. 70% at 360 min of deposition time. On the other hand, the single-crystalline domain size reaches its maximum at 45 min and then gradually decreases, which may be attributed to the desorption of AuNPs by the hydrolysis of ester bonds. The reflectance spectra of AuNPMLs showed the red shift as the deposition time increases up to 45 min with a subsequent blue shift thereafter, which is consistent with the change of the single-crystalline domain size with the deposition time. The covalent bonding interaction-mediated nanoparticle deposition method can be used to form stable AuNPMLs with controlled surface coverage and domain size, allowing for fine control of the optical properties and possibly other properties. The excellent structural stability of AuNPMLs and their controlled properties may provide new opportunities for practical applications of NPMLs.

Renowned for their high porosity and structural diversity, metal-organic frameworks (MOFs) are a promising class of materials for a wide range of applications. In recent decades, with the development of large-scale databases, the MOF community has witnessed innovations brought by data-driven machine learning methods, which have enabled a deeper understanding of the chemical nature of MOFs and led to the development of novel structures. Notably, machine learning is continuously and rapidly advancing as new methodologies, architectures, and data representations are actively being investigated, and their implementation in materials discovery is vigorously pursued. Under these circumstances, it is important to closely monitor recent research trends and identify the technologies that are being introduced. In this Perspective, we focus on emerging trends of machine learning within the field of MOFs, the challenges they face, and the future directions of their development., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Specific targeting of tumor cells is a key to achieving high therapeutic efficacy while minimizing off-target side effects. As a general approach to targeting diverse tumor cells, considerable attention has been paid to the tumor microenvironment, particularly its slightly acidic pH (6.5-6.8). However, existing pH-sensitive nanomaterials, based on organic polymers and proteins, often lack sufficient pH sensitivity and specificity. Here, we demonstrate a strategy to construct a pH-responsive protein assembly through clustering of a single amino acid repeat as a charge-tunable moiety. As a proof of concept, a histidine peptide with varying lengths was displayed on the surface of a ferritin assembly composed of 24 subunits by genetic fusion to a subunit. The resulting self-assembled ferritin particles, termed "pHerricle (pH-responsive ferritin particle)", were shown to exhibit a specific binding to tumor cells in response to pH changes through cooperative effects of histidine peptides. Increasing the histidine peptide length from 0 to 12 residues increased the pHerricle's cell-binding capacity by 21-fold and allowed modulation of the targetable pH range. General applicability as a tumor cell-targeting platform was shown by specific delivery of a cytotoxic cargo by the pHerricle into tumor cells of various origins in a pH-dependent manner.

Stacking semiconductor chips allows for increased packing density within a given footprint and efficient communication between different functional layers of the chip, leading to higher performance, improved speed, and reduced power consumption. In such vertical stacking, achieving homogeneous electrical and mechanical bonding between heterogeneous chips is crucial, which is termed Cu to Cu direct bonding (CCDB) technology. However, conventional CCDB required a high temperature of over 250 °C to allow Cu diffusion and a vacuum condition for inhibiting Cu oxidation, limiting its practical utilization. Here, we propose that the covering of the Ru layer enables a reliable CCDB as low as 200 °C without concerns regarding oxidation. The bonding strength was as high as 2.24 MPa, and it was endurable at the -45 and 125 °C temperature cycle test for 500 cycles. Through microscopic analysis, we have identified that Cu diffuses through the intercluster boundaries of the Ru layer and moves to the surface, and these atomic Cu ions are recrystallized at the bonding interface, enabling stable bonding at lower temperatures. Specifically, we observed a trade-off between Cu diffusion distance and oxidation inhibition capability depending on the thickness of Ru and found that a 6 nm-thick Ru is optimal, balancing these factors.

Multiple emulsions are used as templates for producing functional microcapsules due to their unique core-shell geometry. Employing glass capillary devices with coaxial channels has proven effective in creating uniform multiple-emulsion droplets. However, the use of partially miscible fluids, crucial for microcapsule production, often results in clogging and disrupts the stability of these devices. Here, we introduce innovative capillary microfluidic devices with concentric capillary channels, specifically designed to optimize the production of multiple-emulsion droplets while mitigating issues of precipitation and clogging. The key aspect of these devices is their configuration of two or three concentrically aligned capillaries, which form separate, coaxial microchannels for fluid injection. This unique alignment, achieved through rotational adjustments that leverage the natural off-center positioning of tapered capillaries, facilitates the simultaneous coaxial injection of various fluids into a droplet-forming junction, significantly reducing fluid contact before emulsification. The devices, featuring double and triple concentric capillary channels, consistently produce highly uniform double-, triple-, and quadruple-emulsion droplets with precisely controlled diameters and layer thicknesses. The minimal contact between fluids prior to emulsification in these devices broadens the usable range of fluid combinations, heralding new possibilities in microcapsule development for pharmaceutical and cosmetic applications.

Interfacial interactions between polymers and fillers play a crucial role in determining the performance of composite materials. In this study, mechano-responsive spiropyran (SP) beads, which exhibit fluorescence changes under stress, serve as force probes to evaluate force transfer efficiency across two types of interfaces: noncovalent and covalent. These interfaces are engineered by respectively employing physical blending and grafting polymerization to integrate hydroxyl SP beads with a polyurethane (PU) matrix. A custom-built in situ opto-mechanical setup quantitatively assesses force transfer by monitoring changes in fluorescence intensity and peak wavelength during specimen stretching. The analysis reveals that the covalent interface significantly outperforms the noncovalent interface, demonstrating a 100% improvement in force magnitude and transfer rate from the PU matrix to the SP beads. Direct observation of SP beads within the PU matrix during tension unveils that enhanced force transfer efficiency is closely linked to changes in the SP beads' aspect ratio. Fluorescence changes in SP beads are solely a function of aspect ratio, making them effective independent force probes.

Proton exchange membrane fuel cells (PEMFCs) for automotive applications are required to achieve mechanical reliability at various temperatures ranging from subfreezing to 80 °C. The thermal behavior of the electrode should be considered at the initial design stage to design a robust automotive fuel cell electrode. Recently, a behavior different from that of the bulk state has been reported for ionomers with a few nanometers of thickness. Therefore, the intrinsic thermal behavior of ionomer films with thicknesses from micrometers to nanometers is quantitatively investigated in this study. By introducing the fabrication of a pseudo-freestanding Nafion thin film and in-plane thermal strain measurement method on the water surface, the thermal expansion of the freestanding Nafion thin film was successfully measured with minimizing substrate constraints. Thermal strain measurement and X-ray scattering studies revealed that the weakening of intermolecular interaction within the hydrophobic and hydrophilic domains in the Nafion thin film caused thermal expansion, and well-structured hydrophobic domains could suppress thermal expansion. The thermal expansion behavior with different heat treatments provides evidence of the thin-film-to-bulk transition of the fully hydrated Nafion film. Intrinsic thermal behavior without substrate interactions can facilitate an understanding of the thermal behavior of electrodes and provide insight into designing a robust PEMFC in temperature-varying environments.

The delivery of mRNA into the lungs is the key to solving infectious and intractable diseases that frequently occur in the lungs. Since inhalation using a nebulizer is the most promising method for mRNA delivery into the lungs, there have been many attempts toward adapting lipid nanoparticles for mRNA inhalation. However, conventional lipid nanoparticles, which have shown great effectiveness for systemic delivery of mRNA and intramuscular vaccination, are not effective for pulmonary delivery due to their structural instability during nebulization and their inability to adapt to the pulmonary microenvironment. To address these issues, we developed an ionizable liposome-mRNA lipocomplex (iLPX). iLPX has a highly ordered lipid bilayer structure, which increases stability during nebulization, and its poly(ethylene glycol)-free composition allows it to infiltrate the low serum environment and the pulmonary surfactant layer in the lungs. We selected an inhalation-optimized iLPX (IH-iLPX) using a multistep screening procedure that mimics the pulmonary delivery process of inhaled nanoparticles. The IH-iLPX showed a higher transfection efficiency in the lungs compared to conventional lipid nanoparticles after inhalation with no observed toxicity in vivo . Furthermore, analysis of lung distribution revealed even protein expression in the deep lungs, with effective delivery to epithelial cells. This study provides insights into the challenges and solutions related to the development of inhaled mRNA pulmonary therapeutics.

Conductive metal-organic frameworks (cMOFs) offer high porosity and electrical conductivity simultaneously, making them ideal for application in chemiresistive sensors. Recently, incorporating foreign elements such as catalytic nanoparticles into cMOFs has become a typical strategy to enhance their sensing properties. However, this approach has led to critical challenges, such as pore blockage that impedes gas diffusion, as well as limited improvement in reversibility. Herein, single-atom catalyst (SAC)-functionalized cMOF is presented as a robust solution to the current limitations. Facile functionalization of SACs in a cMOF can be achieved through electrochemical deposition of metal precursors. As a proof of concept, a Pd SAC-functionalized cMOF is synthesized. The Pd SACs are stabilized at the interplanar sites of cMOF with Pd-N 4 coordination while preserving the porosity of the MOF matrix. Notably, the microenvironment created by Pd SACs prevents irreversible structural distortion of cMOFs and facilitates a reversible charge transfer with NO 2 . Consequently, the cMOF exhibits a fully recoverable NO 2 response, which was not previously attainable with the nanoparticle functionalization. Additionally, with the combination of preserved porosity for gas diffusion, it demonstrates the fastest level of response and recovery speed compared to other 2D-cMOFs of this class.

An enantioselective Cu(I)-catalyzed coupling of N-carboxyindoles with various 2-naphthols and phenols for the synthesis of axially chiral arylindoles has been developed. Our mechanistic studies, bolstered by experimental evidence and DFT calculations, reveal a novel closed-shell mechanism involving outer-sphere attack of N-carboxyindoles on the Cu-bound naphthols. This mechanism allows for unprecedented diversity of 2-naphthols and phenols in C-H arylation. Enantiocontrol is achieved through center-to-axis chirality transfer via a key dearomatized naphthol intermediate, which prevents undesired epimerization of the C-C axis.

Pyrolysis-based plastic chemical recycling has gained significant industrial attention due to its advantage of eliminating complex plastic sorting processes. However, plastic pyrolysis oil contains various components that require stringent removal before subsequent processes. In particular, Cl compounds originating from the decomposition of poly(vinyl chloride) can cause serious corrosion of reactors and catalyst deactivation in downstream processes. While extensive research has been conducted on the removal of other heteroatoms (S, N, and O) from organic compounds via hydrotreating, studies on the removal of Cl have been scarce. In this study, hydrodechlorination over Pt catalysts on various supports is comprehensively investigated using 1,2-dichloroethane as a model reactant. Our results demonstrate that Pt on γ-Al 2 O 3 can exhibit exceptionally high catalytic activity compared to those on other supports due to a distinct bifunctional mechanism. Rigorous studies reveal that the Lewis acidic pentacoordinated Al sites of γ-Al 2 O 3 activate C-Cl bonds, whereas Pt activates H 2 and provides spillover H to remove Cl as HCl. The bifunctional mechanism enables the minimized use of precious Pt (<0.1 wt %) to achieve high activity. Pt/γ-Al 2 O 3 also allows for efficient Cl removal (96.8%) with high stability in treating waste plastic pyrolysis oil containing 7500 ppm of Cl.

As global freshwater shortages worsen, solar steam generation (SSG) emerges as a promising, eco-friendly, and cost-effective solution for water purification. However, widespread SSG implementation requires efficient photothermal materials and solar evaporators that integrate enhanced light-to-heat conversion, rapid water transportation, and optimal thermal management. This study investigates using nonoxidized graphene flakes (NOGF) with negligible defects as photothermal materials capable of absorbing over 98% of sunlight. By combining NOGF with cellulose nanofibers (CNF) through bidirectional freeze casting, we created a vertically and radially aligned solar evaporator. The hybrid aerogel exhibited exceptional solar absorption, efficient solar-to-thermal conversion, and improved surface wettability. Inspired by tree structures, our design ensures rapid water supply while minimizing heat loss. With low NOGF content (∼10.0%), the NOGF/CNF aerogel achieves a solar steam generation rate of 2.39 kg m -2 h -1 with an energy conversion efficiency of 93.7% under 1-sun illumination, promising applications in seawater desalination and wastewater purification.

Iridium, the most widely used anode catalyst in proton exchange membrane water electrolysis (PEMWE), must be used minimally due to its high price and limited supply. However, reducing iridium loading poses challenges due to abnormally large anode polarization. Herein, we present an anode catalyst layer (CL) based on a one-dimensional iridium nanofiber that enables a high current density operation of 3 A cm -2 at 1.86 V, even at an ultralow loading (0.07 mg Ir cm -2 ). The performance is maintained even with a Pt coating-free porous transport layer (PTL) because our nanofiber CL circumvents the interfacial electron transport problem caused by the native oxide on the Ti PTL. We attribute this to the low work function and the low-ionomer-exposed surface of the nanofiber CL, which prevent the formation of Schottky contact at the native oxide interface. These results highlight the significance of optimizing the electronic properties of the CL/PTL interface for low-iridium-loading PEMWE.

As the potential adverse health and environmental effects of nanoscale pollutants have garnered significant attention, the demand for monitoring and capturing ultrafine particulate matter has been growing. With the rise in ultrafine dust emissions, this issue has become increasingly important. However, submicron particles require advanced strategies to be captured because of their limited inertial effect. For example, electrostatic air filters have been investigated for their improved performance in the fine particle regime. On the other hand, Raman spectroscopy was proposed as a promising analytical strategy for aerosol particles because it can be used to conveniently detect analytes in a label-free manner. Thus, the synergistic integration of these strategies can open new applications for addressing environment-related challenges. This study presents a multifunctional approach for achieving both air filtration and surface-enhanced Raman scattering (SERS) for analyte identification. We propose a nanoporous membrane composed of a thin gold layer, copper, and copper oxide to provide the desired functions. The structures are produced by performing scalable electrodeposition and subsequent electron-beam evaporation, attaining an excellent filtration efficiency of 95.9% with an applied voltage of 5 kV for 300 nm KCl particles and a pressure drop of 121 Pa. Raman intensity measurements confirm that the nanodendritic surface of the membrane intensifies the Raman signals and allows for the detection of 10 μL of nanoplastic particle dispersion with a concentration of 50 μg/mL. Rhodamine 6G aerosol stream with an approximate particle deposition rate of 0.040 × 10 6 mm -2 ·min -1 is also identified in a minimum detectable time of 50 s. The membrane is shown to be recyclable owing to its structural robustness in organic solvents. In addition, the fatigue resistance of the structure is evaluated through 22,000 iterative loading cycles at a pressure of 177 kPa. No performance degradation is observed after the fatigue loading.