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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
Published on: April 12, 2019
Coupling heterointerface engineering with morphological design for high-performance water-splitting electrocatalysts
Zhijie Feng1, Lili Bo2, Chengzhuo Li3
1College of Science, Gansu Agricultural University, Lanzhou 730070, China.
None:
This study tackles critical challenges in non-noble-metal bifunctional electrocatalysts for the HER and OER, including insufficient intrinsic activity, inefficient mass transport, and limited long-term stability. By synergistically integrating heterointerface engineering with morphological engineering, NiO/NiS2 heterostructured catalysts featuring a hydrangea-like hierarchical porous architecture are fabricated on textile biomass-derived N-doped carbon. The NiO/NiS2 heterointerface induces pronounced interfacial electronic redistribution, effectively optimizing the electronic structure of Ni active sites and enhancing intrinsic catalytic activity. Simultaneously, the multidimensional micro-nanochannel architecture endows the catalyst with exceptional superhydrophilic and superaerophobic properties, substantially improving mass-transfer efficiency. Moreover, the heterostructure undergoes controlled dynamic surface reconstruction under operating conditions, forming stable and highly active interfacial phases. As a result, the catalyst delivers excellent overall water-splitting performance, achieving 10 mA·cm-2at 1.52 V with less than 5 % performance decay after 100 h in alkaline electrolyte, surpassing noble-metal benchmarks (Pt/C || RuO2). This work establishes general design principles and mechanistic insights for the rational development of efficient and durable non-noble-metal electrocatalysts.
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