摘要
Efficient generation, transport, and utilization of plasmon-induced hot carriers remain fundamental challenges in the development of photoresponsive electrocatalysts. Herein, a hierarchical Au nanoparticle (NP)-decorated NiFe layered double hydroxide/Ni(TCNQ) 2 heterostructure supported on copper foam (Au NPs–NiFe LDH–Ni(TCNQ) 2 /CF) with a rationally designed conductive Ni(TCNQ) 2 interlayer is engineered, and the Au NPs size is systematically optimized to maximize plasmon-enhanced electrocatalytic performance. The conductive Ni(TCNQ) 2 nanorods serve as both electron-transport pathways and structural scaffolds enabling the growth of ultrathin NiFe LDH nanosheets, while plasmonic Au NPs enable light-driven electronic modulation. The integration of these components establishes efficient pathways for charge generation, separation, and transfer, thereby improving the utilization efficiency of plasmon-generated carriers. Notably, a systematic size-dependent investigation identifies 5-nm Au NPs as the optimal plasmonic configuration, exhibiting the strongest localized surface plasmon resonance enhancement. Under light irradiation, the optimized catalyst achieves an additional overpotential reduction of 22 mV at 100 mA cm −2 and a decreased Tafel slope of 60.47 mV dec −1 , highlighting the critical role of NP dimensions in regulating hot-carrier generation and interfacial charge-transfer efficiency. Importantly, the synergistic interaction between plasmon-induced electronic excitation and conductive interlayer engineering effectively promotes charge transport across the heterointerface and enhances the overall electrocatalytic process. This study provides new insights into the rational design of plasmon-enhanced electrocatalysts and offers a versatile strategy for integrating hot-carrier modulation with conductive interface engineering in solar-driven energy conversion systems.
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