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The 2D layered metal hydroxides (LMHs) have been developed for electrooxidation of 5‐hydroxymethylfurfural (HMF). In this work, an effective strategy is proposed to tailor the electronic structure of active sites at the atomic level, which is by introducing defects into the lattice structure. As an example, a series of ultrathin crumpled ternary NiVW‐LMH electrocatalysts with abundant lattice vacancies...
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