It is of great significance to synergistically modulate -band centers (ε) of multiple transition metals (TMs) for designing and developing highly efficient hybridized-electrocatalysts. Herein, the downshift in Co ε is realized by synthesizing Co single atoms with low nitrogen-coordination number (CoN) at high during the pyrolysis step while upshifting Ru ε is achieved decreasing Ru precursor mass to anchor Ru nanoclusters instead of nanoparticles on CoN−containing carbon substrates (CoN/Ru−NC). In our strategy, the downshift in Co ε leads to a favorable affinity between Co sites of CoN/Ru−NC and H* for desorption of H; additionally, upshifting Ru ε helps the adsorption of OH* intermediates on Ru nanoclusters for CoN/Ru−NC to promote water dissociation toward accelerating alkaline producing H. In consequence, CoN/Ru−NC demonstrates an outstanding activity with an ultralow overpotential of ∼ 9.0 mV at 10.0 mA cm, which suppresses activities of Pt/C (24.0 mV) and most previously-reported Ru-based electrocatalysts.

中文翻译：

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协同调节双金属元素的 d 带中心以激活钴原子并促进水解离以加速碱性析氢

协同调节多种过渡金属（TM）的能带中心（ε）对于设计和开发高效杂化电催化剂具有重要意义。在此，Co ε 的下移是通过在热解步骤中合成具有低氮配位数 (CoN) 的 Co 单原子来实现的，而 Ru ε 的上移是通过减少 Ru 前体质量来实现的，以锚定 Ru 纳米团簇而不是在含 CoN 上的纳米颗粒。碳底物 (CoN/Ru−NC)。在我们的策略中，Co ε 的下调导致 CoN/Ru−NC 的 Co 位点与 H* 之间有利于 H 解吸的亲和力；此外，Ru ε 的上移有助于 CoN/Ru−NC 在 Ru 纳米团簇上吸附 OH* 中间体，从而促进水解离，从而加速碱性生成 H。因此，CoN/Ru−NC 表现出出色的活性，超低过电势约为 9.0 mV 在 10.0 mA cm 下，可抑制 Pt/C (24.0 mV) 和大多数先前报道的 Ru 基电催化剂的活性。