Yao Dai

Soft bioelectronics require conductive hydrogels with balanced mechanical–electrical performance for high‐fidelity electrophysiological recording, yet conventional ones lack a balance between stretchability and electrochemical stability due to poor interfacial charge transfer. We present a molecularly engineered polyoxometalate‐functionalized mesoporous metal–organic framework (meso‐MOF@POM) nanoarchitecture that simultaneously reinforces the hydrogel network and enhances interfacial charge kinetics. The meso‐MOF serves as a hierarchical scaffold with multiscale channels for polymer anchoring, while the sub‐nanometer Keggin‐type POM layer creates abundant redox‐mediated electron transfer pathways. Upon integration of meso‐MOF@POM into a dual‐network poly(acrylic acid)/polyacrylamide hydrogel, the composite hydrogel enables high stretchability (>1000% strain), minimal electrical creep (3000 cycles). Crucially, the engineered organic–inorganic interface endows the hydrogel with excellent pseudocapacitive charge‐transfer kinetics, which achieves low skin–electrode impedance (64 kΩ at 1 Hz vs. 287 kΩ at 1 Hz for Ag/AgCl gel). As a result, the skin‐interfacing electrode enables high‐fidelity recording of on‐skin electrophysiological signals, including electrocardiogram, electromyogram, and electrooculogram, with an enhanced signal‐to‐noise ratio (e.g., 23.8 dB for ECG vs. 21.3 dB for Ag/AgCl gel). This work provides a novel fabrication strategy for highly conductive interfaces, enabling long‐term applications in wearable health monitors and human–machine interfaces.

Activation and cleavage of the inert O═O bond represent a central challenge in energy electrochemistry. Here, the Cu dual‐atom catalyst (Cu‐DAC) is constructed via bottom‐up pre‐coordination assembly and post‐encapsulation pyrolysis. The resulting Cu‐DAC features a well‐defined Cu–Cu distance (∼3.31 Å) with switchable Cu ¹⁺ /Cu ²⁺ states, enabling dynamic dual‐site coordination with O ₂ . Cu‐DAC achieves 0.87 V _RHE half‐wave potential for oxygen reduction reaction (ORR), a near‐unity 4e ⁻ selectivity, and outstanding stability. Multiple operando spectroscopic characterizations and ab initio dynamic simulations (AIMD) reveal that the dynamic heterovalent [Cu ^1+─ O─O ^{· −} ─Cu ²⁺ ] unit elongates the O–O bond and promotes its cleavage via dual‐site confinement and electron donation. By specifically elucidating how these dual‐atom sites dynamically evolve to facilitate O─O bond cleavage, we provide vital atomic‐level principles for the rational design of dynamically active catalysts.

Activation and cleavage of the inert O═O bond represent a central challenge in energy electrochemistry. Here, the Cu dual‐atom catalyst (Cu‐DAC) is constructed via bottom‐up pre‐coordination assembly and post‐encapsulation pyrolysis. The resulting Cu‐DAC features a well‐defined Cu–Cu distance (∼3.31 Å) with switchable Cu ¹⁺ /Cu ²⁺ states, enabling dynamic dual‐site coordination with O ₂ . Cu‐DAC achieves 0.87 V _RHE half‐wave potential for oxygen reduction reaction (ORR), a near‐unity 4e ⁻ selectivity, and outstanding stability. Multiple operando spectroscopic characterizations and ab initio dynamic simulations (AIMD) reveal that the dynamic heterovalent [Cu ^1+─ O─O ^{· −} ─Cu ²⁺ ] unit elongates the O–O bond and promotes its cleavage via dual‐site confinement and electron donation. By specifically elucidating how these dual‐atom sites dynamically evolve to facilitate O─O bond cleavage, we provide vital atomic‐level principles for the rational design of dynamically active catalysts.