Spatially and Dimensionally Programmed Amorphous Cu Electrocatalysts Using DNA Framework Templates

The precise control of active site spatial structure is a central challenge in high-performance catalyst development and is particularly formidable in long-range disordered amorphous materials where inherent disorder prevents any deliberate engineering. Herein, we develop a DNA framework templated approach to program the fine structure of amorphous Cu nanomaterials, enabling tailorable electrocatalytic performance. Various Cu nanosheets were fabricated with effective modulation of electrocatalytic activity through control of the spatial arrangement of metal-binding sequences. We observed that Cu nanomaterials synthesized with different dimensionalities through the modulation of DNA nanostructures exhibit distinct electrocatalytic performance. Using the single-atom structural characteristics of Cu nanosheets, we performed density functional theory calculations to reveal that two-dimensional Cu nanomaterials possess the smallest energy gap and optimal glucose adsorption characteristics, which exhibit superior catalytic activity (3.65-fold and 2.70-fold) to other lower-dimensional counterparts. This work establishes a general methodology that uses prescriptive DNA blueprints to achieve programmable control over material structure and functionality, thereby providing a novel paradigm for crafting amorphous electrocatalysts and informing precision design in fields ranging from energy to biosensing.