Plasmonic photothermal polymerase chain reaction (PPT-PCR) is a nucleic acid amplification technique that utilizes the localized surface plasmon resonance effect of plasmonic nanomaterials under the irradiation of light with specific wavelengths to achieve rapid thermal cycling. PPT-PCR is considered as a next-generation PCR technique due to the potential to be applied to the development of point-of-care diagnostics and the fast, sensitive and accurate detection performance. In this study, we present PHANTOM, a proof-of-concept system that functionally integrates plasmonic photothermal PCR, magnetic nanoparticle removal, and swCNT-FET-based label-free electrical readout for rapid molecular diagnostics. The swCNT-FET sensor exhibits high sensitivity, capable of detecting low concentrations of target nucleic acids within minutes after PPT-PCR amplification. Besides, to improve the specificity of the assay, we introduce a hairpin structured primer to generate amplicons with an external single-strand tail that can hybridize with probes modified on the swCNT-FET sensor. With this design, an estimated limit of detection of 1.5 aM (experimentally validated down to 10 aM) was achieved within 20 min.

Practical applications of MXene-based hydrogels have been limited owing to their poor oxidation stability and mechanical performance. To overcome these issues, numerous efforts have been devoted to the surface modification of MXenes, but the optimal type of surface modifier has not been systematically explored. Herein, MXene is modified with diverse polymeric modifiers, including polyphenols (PPs) and linear synthetic polymers (LSPs), and the resulting properties are investigated in relation to their molecular structures. LSPs outperform PPs in improving oxidation resistance and mechanical performance of hydrogels, among which poly(acrylic acid) (PAA) provides the highest overall performance. Subsequently, the PAA-modified MXene hydrogel (PMH) is converted into organohydrogels (PMOH) to enhance mechanical performance and environmental durability. The PMOH exhibits substantially improved mechanical performance, including a tensile strain of 1487.5%, a tensile strength of 750 kPa, and a toughness of 5.27 MJ m(-3) with a tissue-like modulus of 71.9 kPa. The PMOH also shows enhanced conductivity compared with the bare organohydrogel (0.105 to 0.133 S m(-1)), robust adhesion to the skin (55.3 kPa), and outstanding resistance to freezing, dehydration, and oxidation. Owing to these properties, the PMOH is employed as a wearable strain and electrophysiological sensor. This study provides rational insights into the development of durable and high-performance MXene hydrogels for biomedical applications.

Lithium-oxygen batteries (LOBs) offer exceptionally high energy density but are limited by poor reversibility and large charging overpotentials owing to sluggish lithium oxide decomposition. We propose a rational Fe-4d dualatom catalyst (DAC) strategy to regulate oxygen evolution and stabilize NO2- redox mediation. Fe-Zr/Nb/Mo pairs are atomically dispersed onto defect-rich nitrogen-doped carbon nanotubes (NCNTs) and evaluated as oxygen-electrode catalysts. Among these, Nb-Fe-NCNT exhibits a superior performance, enabling excellent cycling for over 290 cycles with significantly reduced polarization. Electrochemical analysis reveals that Nb-Fe enhances charge-transfer kinetics and sustains low-voltage redox-mediated oxygen evolution while suppressing high-voltage direct Li2O2 oxidation. Ex situ characterization confirms highly reversible Li2O2 formation and decomposition. Density functional theory shows favorable reaction energetics and enhanced electron redistribution, which strengthens mediator interaction. These results demonstrate that metal-dependent electronic synergy in Fe-4d DACs governs oxygen-evolution pathways and provide practical design guidelines for durable, nonprecious catalysts for high-performance LOBs.

Bone morphogenetic protein-2 (BMP-2) is a potent osteoinductive factor for bone regeneration, but its rapid clearance and dose-dependent adverse effects limit its clinical use. This study developed calcium-binding poly(butyl methacrylate-co-methacryloyloxyethyl phosphate) (PBMP)-coated poly(lactide-co-glycolide) (PLGA) microparticles to enhance calcium-rich surface anchoring and enable sustained BMP-2 release. Microparticles were characterized for morphology, zeta potential, encapsulation efficiency, release kinetics, and hydroxyapatite (HA)-binding affinity, and were further evaluated for in vivo efficacy. PBMP coating markedly increased the HA-binding affinity of PLGA microparticles. Encapsulation efficiency was over 55%, and BMP-2 was released in a sustained manner over 30 days, with the cumulative release gradually approaching a plateau during the later incubation period. When applied to a rat calvarial defect model, the PBMP-coated microparticle (BMP-2-PLGA/PBMP) group showed the greatest bone volume fraction, bone surface area, and trabecular number, along with the lowest trabecular separation compared to the free BMP-2 and control groups. Histological analysis confirmed denser and more mature bone matrix formation in the BMP-2-PLGA/PBMP group. These findings demonstrate that PBMP-coated PLGA microparticles provide HA-targeted, sustained BMP-2 delivery, resulting in improved bone regeneration and microarchitecture. This delivery platform represents a promising strategy for more effective bone defect repair.

Achieving atomic-level insight into how dopants regulate the electrocatalytic CO2 reduction reaction (eCO2RR) of metal nanoparticles is challenging due to the lack of well-defined, compositionally tunable, and structurally identical model systems. Herein, we report two isostructural nanoclusters: [Au10Ag4(DPPP)5Cl4]2+ (Au10Ag4) and [Au9Ag2Cu3(DPPP)5Cl4]2+ (Au9Ag2Cu3), which differ only in metal composition (Au & horbar;Ag vs. Au & horbar;Ag & horbar;Cu). Together with the isostructural monometallic [Au14(DPPP)5Br4]2+ (Au14), they serve as ideal platforms to elucidate dopant effects on eCO2RR. Electrochemical studies reveal that Ag doping (Au10Ag4) suppresses both CO selectivity and activity of Au14, whereas further Cu incorporation (Au9Ag2Cu3) not only enhances these metrics relative to Au10Ag4 but also surpasses Au14. Specifically, Au9Ag2Cu3 exhibits an enhanced CO Faradaic efficiency (FECO, 73.7%-95.5%), exceeding that of Au14 (63.6%-95.0%) and Au10Ag4 (66.2%-79.5%), and its CO partial current densities were improved by 1.5- and 2.6-fold compared to those of Au14 and Au10Ag4, respectively. Theoretical calculations and in situ experiments reveal that Ag & horbar;Cu co-doping lowers the energy barrier for *COOH formation and weakens CO binding, promoting CO2-to-CO conversion. In contrast, Ag doping alone raises the energy barrier for *COOH formation and impedes CO desorption, diminishing catalytic activity. These findings provide atomistic insights into dopant-regulated eCO2RR and inspire the rational design of advanced alloy electrocatalysts.

Understanding how degradation reshapes lithium (de)insertion pathways in high-nickel cathodes is crucial for extending battery lifetime. Here, we integrate operando synchrotron X-ray diffraction (sXRD) with electrode-level transmission X-ray microscopy (TXM) to quantitatively resolve how degradation redistributes lithium accessibility in Ni-rich NCA cathodes. Using a 26-state deconvolution framework, we show that degraded electrodes exhibit nonmonotonic Li-content population evolution: delithiation kinetics are initially suppressed, transiently synchronized, and ultimately diverge, leaving similar to 7% discharge-like states and similar to 13% intermediate Li-content states at the end of charge. Spatially resolved TXM reveals that this divergence originates from size-dependent accessibility constraints-large particles develop persistent intra-particle state-of-charge gradients, while small particles exhibit pronounced inter-particle disparity. This work establishes a quantitative framework linking bulk Li-content population dynamics to particle-level degradation mechanisms in high-nickel cathodes.

The chemical space explored through synthesis is largely shaped by the availability of building blocks supplied by nature. Because biosynthesis follows defined metabolic logic, naturally occurring compounds are unevenly distributed across carbon count, creating intrinsic biases in synthetic accessibility. Consequently, molecules differing by only a single carbon atom can require markedly different synthetic effort. To overcome this longstanding challenge, we report a bidirectional coupling strategy that assembles alkenes and nucleophiles across an intervening methylene unit. In contrast to conventional alkene hydrofunctionalization, which joins these partners directly, this approach retains the modularity of the parent reaction while increasing product carbon count. We show that a designer methylene-bridged thianthrenium dication reagent exploits distinct redox properties and strain-release reactivity to differentiate two C-S bonds at a single carbon center. This design enables sequential alkene hydroalkylation and downstream nucleophile incorporation via substitution, cross-coupling or radical manifolds. This divergent reactivity accommodates diverse nucleophile classes (N, O, B, S, Se, C and halides), facilitates the hybridization of complex biorelevant fragments and expands retrosynthetic flexibility in the synthesis of marketed drugs. By rerouting two abundant substrate classes through a single-carbon linchpin, this platform opens one-carbon-shifted chemical space beyond the reach of conventional alkene hydrofunctionalization.

Catalytic activity and electrical conductivity are critical to the performance of electrocatalysts and electrochemical devices, yet their combined assessment under operating conditions remains challenging. Here, we introduce operando Fourier-transform electrochemical source-drain impedance spectroscopy (FT-ESDIS), which simultaneously measures catalyst-film conductivity and charge-transfer resistance (R ct) with high temporal resolution at high current densities. During Fe incorporation into nickel (oxy)hydroxide (NiO x H y ), FT-ESDIS revealed that catalytic activation and charge transport properties evolve on distinct time scales, demonstrating that activity alone cannot capture catalyst-layer evolution during operation. At higher overpotentials, nickel-containing (oxy)hydroxides (Ni(Fe)O x H y ) showed an abrupt apparent conductivity increase upon oxidation, with conductivity remaining nearly unchanged thereafter, whereas iron (oxy)hydroxide (FeO x H y ) exhibited a gradual increase in apparent conductivity. Previous reports attributed this overpotential-dependent increase to the formation of high-valent Fe species. However, we show that the increase arises predominantly from an electrolyte-mediated current artifact, in which a potential perturbation at one electrode changes the local solution potential at the neighboring electrode surface and modulates its Faradaic current, producing an apparent conductivity response without direct through-film transport. We further establish a quantitative relationship between this artifact and R ct, enabling its estimation and subtraction from the apparent conductivity. The corrected FeO x H y conductivity exhibits substantially weaker potential dependence, suggesting that charge transport involving high-valent Fe species, if present, contributes much less than inferred from the uncorrected response. By resolving kinetic and transport properties under operating conditions, FT-ESDIS provides a more comprehensive basis for interpreting electrocatalyst behavior and establishes transport and reactivity as complementary descriptors for electrochemical energy-conversion systems.

Ni-based catalysts have been widely studied as promising alternatives to Pt group metal catalysts in anion exchange membrane water electrolysis. However, their insufficient durability at the membrane electrode assembly (MEA) poses a significant limitation. In this study, we evaluated the performance and durability of Ni₃Mo, PtNi/C, and Pt/C catalysts in MEAs under various intermittent protocols that mimic electricity production from renewable energy sources. In the intermittent protocols, sets of open circuit voltage (OCV) and constant current densities of 0.1 A cm−2 and/or 1 A cm−2 with different duration times were repeated for overall test time of 165 h. The Ni3Mo catalyst demonstrated severe degradation in cell performance for the long OCV duration of 1 h, while shorter exposure of 1 or 30 min presented little degradation, although the metal dissolution still occurred significantly. The cell degradation mainly resulted from phase transformation of the metallic Ni3Mo to Ni(OH)2. The Pt/C catalyst showed substantial degradation in the cell performance when the current density was frequently changed with short duration (1 min) at OCV, resulting from the Pt aggregation. The PtNi/C presented the most stable cell performance under various intermittent protocols, due to the formation of surface Ni hydroxide species that inhibit aggregation. The changes in the overpotentials at cathode, membrane, and anode were further investigated using 3-electrode MEA system. The PtNi/C catalysts were synthesized with various compositions of Pt:Ni ratios, and also the Pt1Ni1/C catalysts were synthesized with various sizes, but the effect of composition and sizes were insignificant for the cell performance.

Electrochemical synthesis offers a promising route toward renewable-energy-based chemical production and a sustainable carbon cycle. Maleic acid (MA) production from biomass-derived furfural (FF) via electrochemical oxidation (FFOR) represents a valuable model system for multi-step electro-organic oxidation reactions. However, oxygenation and dehydrogenation are conventionally treated as indistinguishable oxidation processes, obscuring key factors and the rational design of complex electro-organic reactions. Herein, we decouple oxygenation and dehydrogenation kinetics in FFOR, identify the key controlling factors for each step, and demonstrate that independent regulation enables high selectivity with 81.0% yield using a PbO x anode. Employing (bi)carbonate electrolytes moderates center dot OH-mediated oxygenation, improving carbon efficiency. 2,2,6,6-Tetramethylpiperidine 1-oxyl (TEMPO) mediator selectively accelerates dehydrogenation of the key intermediate (5-hydroxy-2(5H)-dihydrofuran-2-one, HFN, or cis-beta-formylacrylate, FAA-) to MA without perturbing FF-to-HFN/FAA- oxidation, shifting the rate-determining step. Mechanistic studies reveal that oxidation by TEMPO+ promotes oxoammonium-mediated proton transfer, driving the selective dehydrogenation toward MA. Systematic control of pH, cation/anion, and TEMPO concentration demonstrates that these factors strongly influence kinetics between center dot OH-mediated oxygenation and TEMPO-mediated dehydrogenation, with selective MA production achieved under their optimal balance. These mechanistic insights highlight strategies for the rational design of electro-organic synthesis by independently controlling oxygenation and dehydrogenation pathways under complex aqueous conditions.