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Abstract Direct implementation of metal-organic frameworks as the catalyst for CO 2 electroreduction has been challenging due to issues such as poor conductivity, stability, and limited > 2e − products. In this study, Au nanoneedles are impregnated into a cupric porphyrin-based metal-organic framework by exploiting ligand carboxylates as the Au 3+ -reducing agent, simultaneously cleaving the ligand-node linkage. Surprisingly, despite the lack of a coherent structure, the Au-inserted framework affords a superb ethylene selectivity up to 52.5% in Faradaic efficiency, ranking among the best for metal-organic frameworks reported in the literature. Through operando X-ray, infrared spectroscopies and density functional theory calculations, the enhanced ethylene selectivity is attributed to Au-activated nitrogen motifs in coordination with the Cu centers for C-C coupling at the metalloporphyrin sites. Furthermore, the Au-inserted catalyst demonstrates both improved structural and catalytic stability, ascribed to the altered charge conduction path that bypasses the incoherent framework. This study underlines the modulation of reticular metalloporphyrin structure by metal impregnation for steering the CO 2 reduction reaction pathway.more » « less
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Highly active and selective oxygen reduction to H2O2 on boron-doped carbon for high production ratesnull (Ed.)Abstract Oxygen reduction reaction towards hydrogen peroxide (H 2 O 2 ) provides a green alternative route for H 2 O 2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. Here we report a boron-doped carbon (B-C) catalyst which can overcome this activity-selectivity dilemma. Compared to the state-of-the-art oxidized carbon catalyst, B-C catalyst presents enhanced activity (saving more than 210 mV overpotential) under industrial-relevant currents (up to 300 mA cm −2 ) while maintaining high H 2 O 2 selectivity (85–90%). Density-functional theory calculations reveal that the boron dopant site is responsible for high H 2 O 2 activity and selectivity due to low thermodynamic and kinetic barriers. Employed in our porous solid electrolyte reactor, the B-C catalyst demonstrates a direct and continuous generation of pure H 2 O 2 solutions with high selectivity (up to 95%) and high H 2 O 2 partial currents (up to ~400 mA cm −2 ), illustrating the catalyst’s great potential for practical applications in the future.more » « less
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Abstract Nanomaterial‐based stretchable electronics composed of conductive nanomaterials in elastomer can seamlessly integrate with human skin to imperceptibly capture electrophysiological signals. Despite the use of transfer printing to form embedded structures, it remains challenging to facilely and stably integrate conductive nanomaterials with thin, low‐modulus, adhesive elastomers. Here, a facile‐yet‐simple laser‐induced graphene (LIG)‐assisted patterning and transfer method is demonstrated to integrate patterned silver nanowires onto an ultra‐low modulus silicone adhesive as ultra‐conformal epidermal electrodes. The resulting thin epidermal electrodes of ≈50 µm exhibit a low sheet resistance (0.781 Ω sq−1), tissue‐like Young's modulus (0.53 MPa), strong self‐adhesion, and excellent breathability. The breathable electrodes dynamically conformed to the skin with low contact impedance allow for long‐term, high‐fidelity monitoring of electrophysiological signals in complex environments (even during exercise and heavy sweating). Moreover, the LIG‐assisted transfer can provide a robust interface to establish a stable connection between the soft electrodes and rigid hardware. The large‐scale fabrication further provides an eight‐channel electromyography system combined with a deep learning algorithm for gesture classification and recognition with remarkable accuracy (95.4%). The results from this study also provide design guidelines and fabrication methods of the next‐generation epidermal electronics for long‐term dynamic health monitoring, prosthetic control, and human‐robot collaborations.more » « less
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