Electrocatalytic performance depends on the surface characteristics of catalysts. Understanding the determinants for adsorption of the reactants and desorption of the products is essential for efficient electrocatalyst design. Electrochemical nitrogen reduction (eNRR) is initiated by nitrogen adsorption and is progressed by hydrogenation to produce ammonia. Despite the intensive development of eNRR catalysts, optimum catalyst design for eNRR is barely understood. Here, we report a designer approach study for investigating the relationship between catalyst surface features (surface geometry and composition) and eNRR performances. To test our idea, facet-controlled copper sulfide hexagonal nanoprisms which only expose two types of facets, {100} and {010}, were deliberately prepared. We studied exposed facet density-dependent eNRR performances by controlling aspect ratios of the Cu_1.81S nanoprisms. Thereafter, we tested surface dopant effects on eNRR activity and stability by introducing heteroatoms on the Cu_1.81S nanoprisms. Physical and electrochemical properties of the catalysts were investigated by TEM, CV, and DFT analyses and it is discovered that protruded surfaces are active for the eNRR and dopant enhances the eNRR performances.

References

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