lycerol, a low-cost and abundant byproduct of biodiesel production, has attracted attention as a feedstock for conversion into value-added chemicals. To maximize the economic value of products, maintaining three carbons (C3) as the dominant product is important yet difficult to achieve at high potentials due to the favorable C–C bond scission. We demonstrate that an atomically dispersed Pt catalyst anchored on defect-rich ceria-carbon selectively controls the glycerol electrooxidation reaction (GEOR), favoring C3 products. The isolated Pt sites favored single-carbon adsorption, preventing multi-carbon binding and subsequent cleavage up until high potential of 1.2 VRHE. The catalyst maintained nearly 70% of C3 selectivity across various potentials with high glycerate productivity and selectivity. In contrast, catalysts with Pt nanoparticles rapidly shifted towards C2 and C1 products, especially glycolate and formate as potential increases. Moreover, Pt single atoms on the catalyst maintained high glycerate productivity without much Pt agglomeration under 48 h operation. Beyond batch operation, the Pt single atom catalyst was validated in a continuous flow-cell reactor. Glycerate remained as the major product, reaching a selectivity of 51.6% as potential increases and exhibited a productivity of 37.0 mmol L−1 mgPt−1 h−1 at 1.2 VRHE. This work highlights atomic dispersion on defect-engineered supports as a powerful strategy to control electrocatalytic pathways in the GEOR via suppressing C–C cleavage.

Supramolecular assembly of biological materials into fibrous structures often provides exceptional functionalities. In the case of synthetic polymers, however, it is challenging to construct fibrous structures in the condensed matrix, primarily due to limited ordering and chain mobility for supramolecular assembly. We present a design strategy of using hydrogen bonding units to facilitate supramolecular assembly in self-healing PDMS-based polymer films, exploring how subtle changes in alkyl spacers affect dynamic mechanical responses. We observed that increasing structural flexibility in hydrogen bonding units enables long-range supramolecular assemblies, leading to the formation of fibrous structures. These structures endow the material with improved mechanical stability under tensile, compressive, and frictional stresses. Notably, the supramolecular assembly responds to molecular-level changes, allowing selective self-healing between corresponding polymers. This molecular-level recognition gave self-alignment in multilayer laminates, enabling autonomous healing and alignment of damaged and misaligned layers. Our findings provide new insights for designing mechanically robust, self-healable, and multi-functional polymers.

The electrocatalytic nitrate reduction reaction (NO3RR) provides a sustainable pathway to convert excess nitrate into ammonia, yet realizing high selectivity requires a fundamental understanding of dynamic structural changes occuring at active sites during reactions. Here, we investigate how in situ Cu clustering dynamically activates dual catalytic sites in Fe–Cu bimetallic single-atom catalysts (FeCu–N–C) during NO3RR, through combined density functional theory calculations and operando spectroscopy. Under reductive potentials, atomically dispersed Cu spontaneously aggregates into nanoclusters that efficiently activate NO3–. Concurrently, Cu clustering induces pronounced structural strain and electronic distortion in adjacent Fe–Nx moieties, triggering a spin-state transition in the Fe active site from low-spin to high-spin configuration. This spin modulation dramatically enhances the activity for subsequent NO2– conversion to NH3. The synergistic coupling between Cu clusters and spin-modulated Fe establishes a highly effective tandem pathway, yielding superior NO3RR activity and NH3 selectivity, compared to Cu–N–C and Fe–N–C counterparts. These findings provide new insights into the rational design of advanced multicomponent electrocatalysts with dynamically tunable active site properties.

Plasmonic dimers are versatile platforms for manipulating light–matter interactions at the nanoscale, supporting hybridized modes such as capacitive plasmons (CPs) and charge transfer plasmons (CTPs), which are highly sensitive to the nature of the interparticle junction. However, these junctions have largely been restricted to noble metals, limiting fundamental understanding and design flexibility. Here, we report gold nanosphere dimers interconnected by a metal–semiconductor hybrid junction that enables selective regulation of plasmonic modes. Single-particle scattering measurements show that the hybrid junction, comprising metallic Ag pathways embedded within a high-permittivity AgI matrix, produces enhanced CPs and suppressed CTPs. Supported by electromagnetic simulations, we reveal that interfacial field localization driven by induced dipoles in AgI governs the mode selectivity by trapping oscillating surface plasmons and impeding long-range electronic conduction. This hybrid junction offers a tunable plasmonic platform, expanding opportunities in surface-enhanced Raman spectroscopy, optothermal therapeutics, nanophotonics, and optoelectronics that benefit from enhanced CP modes.

Zinc-halogen batteries (ZHBs) offer a safer, cost-effective alternative to lithium-ion batteries, leveraging abundant zinc resources and high energy density. Among ZHBs, dual-plating zinc bromine batteries (ZBBs) utilizing ionic liquid (IL)-forming bromine complexing agents (BCAs) exhibit enhanced performance by minimizing halogen crossover and enabling high conductivity via Grotthuss-type halide transport. In this study, the electrochemical impedance of the bromide redox reaction in the presence of 1-ethyl-1-methylpyrrolidinium bromide (MEPBr), an IL-forming BCA, was analyzed. Potentiodynamic operando impedance measurements revealed pronounced asymmetry in mass transport impedance between polybromide ionic liquid (PBIL) formation and dissolution. This asymmetry significantly influenced the potential and impedance trends during galvanostatic cycling of dual-plating ZBBs. During charging, facilitated Br− transport lowered the positive electrode impedance, resulting in minimal positive electrode overpotential even at high current densities. In contrast, during discharging, PBIL dissolution at the positive electrode exhibited large overpotential at high current densities due to the relatively sluggish internal mass transport of Br2n+1−. Furthermore, similar asymmetry was observed across various IL-forming BCAs, indicating that the mass transport disparity is an intrinsic property of PBIL rather than limited to MEPBr. These findings provide new insights into PBIL mass transport dynamics and their impact on high-current-density operation in dual-plating ZBBs.

DNA exhibits programmable self-assembly through complementary hydrogen bonding between nucleobases introduced to sugar-phosphate backbones in defined sequences, inspiring the development of synthetic analogs with nucleobases as recognition motifs. However, most nucleobase-containing polymers lack defined monomer sequences or molecular uniformity, limiting their biomimetic precision. In this work, we synthesized sequence-defined polymers bearing adenine and thymine units via a Passerini iterative exponential growth strategy. Butoxycarbonyl (Boc)-protected nucleobase-functionalized isocyanides were employed to construct poly(hydroxybutyrate) bearing butyl- and bp-thymine side chains and poly(hydroxybutyrate) with butyl- and bp-adenine side chains with uniform molecular weights. After Boc deprotection, NMR analyses revealed complementary adenine–thymine hydrogen bonding, showing characteristic downfield shifts in a 1:1 mixture, an association constant of 320 M–1 obtained by NMR titration, and thermoreversible behavior in variable-temperature NMR experiments. Furthermore, adenine and thymine were incorporated into a single polymer backbone, demonstrating the method’s ability to encode programmable hydrogen-bonding motifs into uniform synthetic macromolecules.

Electrochemical reactive carbon capture (eRCC) is a promising route for carbon utilization, but its performance is limited by fundamental constraints in conventional membrane electrode assembly (MEA) configurations. The key steps of eRCC, such as CO2 desorption, mass transport, and conversion, are detrimentally coupled at the zero-gap MEA interface. Here, we demonstrate that incorporating a dedicated stripping compartment enables the direct supply of CO2-laden solution to the membrane interface without electrode obstruction, and effectively decouples the mass transport of desorbed CO2 from its conversion in an interface-modulated three-compartment flow cell (3CFC), by modulating the pressure differential across compartments to drive directed CO2 transport. The in situ/operando Raman spectroscopy revealed its unique pH-buffering capability near the electrode, contributing to high C2+ selectivity and enhanced eRCC performance. This unique platform achieves remarkable stability and selectivity in the direct conversion of bicarbonate across diverse catalysts. At −200 mA/cm2, a Cu(OH)2-derived catalyst achieved an unprecedented C2+ selectivity of 52.0%, representing a 17-fold increase from 3.1% in the MEA cell. Moreover, Ag electrodes exhibit long-term stability for more than 155 h at −100 mA/cm2 from bicarbonate conversion, in contrast to the rapid increase in H2 observed in the MEA configuration. The CO selectivity of a Ni single-atom-catalyst from eRCC was dramatically enhanced to 96.7% utilizing 3CFC, compared to 38.0% in the MEA cell. This work presents a new principle for controlling the interfacial chemical environment in complex electrochemical systems.

The nervous system processes information by translating chemical signals into electrical and biochemical responses, ultimately driving biological adaptation and computation. Chemical synapses are the primary communication channels between neurons, operating with remarkable speed and precision to enable complex neural information processing. In this perspective, we focus on these native signaling principles and explore the potential of synaptic structures as neurointerface modules. Building on this view, we argue that electrodes can be engineered to function as complementary synaptic terminals, enabling neuron–device communication that directly leverages the chemical, electrical, and biological logic of neural systems. In particular, we discuss whether synaptic cell adhesion molecules can be harnessed as synaptogenic cues to redefine electrode surfaces as functional synaptic counterparts of neuronal terminals, and we examine the distinctive properties and emerging applications of such interfaces.

Light-programmable transistors are promising for next-generation electronics, but their reliance on high-energy UV light undermines stability and safety. Here, we demonstrate visible-light-only photoprogramming of organic field-effect transistors (OFETs) by integrating an all-organic triplet-sensitized diarylethene system into the channel layer. Rather than redesigning the photoswitch, this modular additive strategy renders a conventional UV-responsive diarylethene visible-addressable in solid-state transistors. A ternary blend of a polymer semiconductor (DPP-DTT), a diarylethene photoswitch (DAE-HP), and an organic triplet sensitizer (4CzIPN) enables fully reversible current modulation via photocyclization at 450 nm and photocycloreversion at 520 nm. The devices achieve a switching ratio up to 2.8 × 103 and remain stable over 100 cycles. Mechanistic studies show that DAE-HP and 4CzIPN co-localize within amorphous domains without perturbing polymer crystallinity, maintaining charge-transport continuity while ensuring the short-range proximity required for triplet exchange. Transient absorption spectroscopy supports efficient triplet–triplet energy transfer (TTET) from 4CzIPN to DAE-HP as the driver of visible-light photoswitching. These results identify nanoscale organization as the key lever for UV-free operation and provide a practical blueprint for safer, durable, and solution-processable light-programmable organic electronics.

Nickel has recently emerged as a promising catalytic center for single-atom catalysts, owing to its biological relevance, redox versatility, and favorable coordination chemistry. Herein, we report the synthesis of a multifunctional nanozyme (Ni/PEG-FA) comprising atomically dispersed nickel sites anchored on a nitrogen-doped carbon support. The nanozyme is functionalized with poly(ethylene glycol) to improve colloidal stability and biocompatibility, and further conjugated with folic acid to enable the selective targeting of cancer cells overexpressing folate receptors. Ni/PEG-FA exhibits dual enzyme-mimicking activity, catalyzing both peroxidase-like and superoxide dismutase-like reactions for efficient reactive oxygen species generation under physiological conditions. In addition, Ni/PEG-FA shows strong photothermal conversion upon near-infrared laser irradiation, enabling effective thermal ablation of tumor cells. In vitro and in vivo evaluations demonstrate that Ni/PEG-FA elicits synergistic antitumor effects by combining catalytic oxidative stress with photothermal therapy, with minimal systemic toxicity. These findings underscore the potential of Ni-based single-atom nanozymes as a safe and effective platform for reactive oxygen species–powered cancer therapy.