Low-Cost, Facile, and Scalable Manufacturing of Single-Molecule-Integrated Catalytic Electrodes

To surmount the shortcomings of powder-based catalysts and small electrode sizes, the development of meter-scale integrated electrode materials is essential for practical electrocatalytic applications, which requires fine control over the effective surface grafting of catalytic active sites on large-size electrodes as well as addressing the challenge of balancing cost-effective and large-scale manufacturing with highly active and stable operation. Herein, we report a low-cost, facile, and scalable method for directly constructing meter-scale single-molecule-integrated catalytic electrodes using commercially available, flexible, and size-tailored conductive carbon textiles (e.g., graphite felt) and well-defined planar conjugated molecules (e.g., metallophthalocyanines) via heterostacking steered cross-scale heterointerfacial assembly. This universal method unlocks the limitations of traditional approaches that involve integrating powder-based catalysts, conductive carbon particles, binders (e.g., Nafion), and supported electrodes (e.g., carbon paper) through multiple processing steps and typically result in centimeter-level electrodes. Meaningfully, our method enables precise control over the size, composition, microenvironment, and structure of the single-molecule-integrated catalytic electrodes to match various electrocatalytic environments. As a proof of concept, an electrode integrated with thiophene-gilded cobalt phthalocyanine demonstrates outstanding catalytic activity and stability for CO2 electroconversion in alkaline, neutral, and acidic media under industrially relevant current densities, and even in flowing paired-electrolysis system. This study provides comprehensive scientific data and engineering guidance for the systematic design of scalable, binder-free catalytic electrodes, thereby promising to drive sustainable energy-efficient electrolysis on an industrial scene.