Electronic structure engineering lies at the heart of efficient catalyst design. Most previous studies, however, utilize only one technique to modulate the electronic structure, and therefore optimal electronic states are hard to be achieved. In this work, we incorporate both Fe dopants and Co vacancies into atomically thin CoSe₂ nanobelts for /coxygen evolution catalysis, and the resulted CoSe₂-D_Fe–V_Co exhibits much higher catalytic activity than other defect-activated CoSe₂ and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co₂ site that is adjacent to the V_Co-nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co₂ to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔE_OH) without changing ΔE_O, and consequently lowering the catalytic overpotential. The proper combination of multiple defect structures is promising to unlock the catalytic power of different catalysts for various electrochemical reactions.

电子结构工程是高效催化剂设计的核心。然而，大多数先前的研究仅利用一种技术来调制电子结构，因此难以实现最佳的电子状态。在这项工作中，我们将Fe掺杂剂和Co空位都掺入了原子薄的CoSe ₂纳米带中以进行/氧演化催化，并且所得CoSe ₂ -D _Fe -V _Co的催化活性比其他缺陷激活的CoSe _2高，并且先前已有报道FeCo化合物。深入的表征和理论计算可确定与V _Co相邻的Co ₂位置最活跃的中心-最近的表面铁部位。的Fe掺杂和Co空位协同调Co的电子态₂到接近最佳值，从而显着降低OH *（ΔE的结合能_OH而不改变ΔE）_ø，并因此降低了催化剂的超电势。多种缺陷结构的正确组合有望为各种电化学反应释放不同催化剂的催化能力。