The precise self‐assembly of building blocks at atomic level provides the opportunity to achieve clusters with advanced catalytic properties. However, most of the current self‐assembled materials are fabricated by 1/2D assembly of blocks. High dimensional (that is, 3D) assembly is widely believed to improve the performance of cluster. Herein, the effect of 3D assembly on the activity for electrocatalytic CO2 reduction reaction (CO2RR) is investigated by using a range of clusters (Au8Ag55, Au8Ag57, Au12Ag60) based on 3D assembly of M13 unit as models. Although three clusters have almost the same sizes and geometric structures, Au8Ag55 exhibits the best CO2RR performance due to the strong CO2 adsorption capacity and effective inhibition of H2 evolution competition reaction. The deep insight into the superior activity of Au8Ag55 is the unique electronic structure attributed to the charge segregation. This study not only demonstrates that the assembly mode greatly affects the catalytic activity, but also offers an idea for rational designing and precisely constructing catalysts with controllable activities.
Developing non‐noble metal catalysts with high efficiency and stability is critical for the industrial application of electrocatalytic water splitting. Herein, FeNi nanoalloys‐layered porous N‐doped carbon nanosheets (FeNi‐NCS) were large‐scale synthesized by simple formamide pyrolysis method. The framework of FeNi‐NCS was a micro‐flowerlike structure composed of mesoporous N‐doped carbon nanosheets as petals, on which FeNi nanoalloy particles were uniformly dispersed. Benefiting from the unique N doping electronic modification, hierarchically porous structure, and the synergetic effect between Fe and Ni, the FeNi‐NCS exhibited high intrinsic activity and robust structure which can improve catalytic performance significantly. By tuning the pyrolysis temperature and the molar ratio of Fe and Ni, the Fe1Ni1‐NCS‐900 displayed optimal activity and stability for electrocatalytic hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) and required 261 and 310 mV overpotential to achieve 10 mA cm−2 respectively. This work presented a simple and effective way to fabricate high‐performance and stable non‐noble metal electrocatalysts for water splitting.
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