Non-bonding-type dual-metal atom sites have emerged as a frontier for bifunctional electrocatalysis, however, respectively customizing the local electronic states of two metal sites remains elusive. Herein, by fabricating FeN₄ and NiN₄ single atoms that Janus-distributed on the inner and outer of sulfur-doped carbon hollow spheres, namely FeN₄-SC-NiN₄, we demonstrate the sulfur-induced anisotropic electronic regulation for Fe/Ni dual-atom sites and build “one stone two birds” bidirectional facilitation mechanism for reversible oxygen electrocatalysis. For the separated FeN₄ and NiN₄ sites, the ambient sulfur reduces the charges of FeN₄ sites while downshifts the d-band center of NiN₄ sites. Such enlarged difference in electronic structure respectively promotes OH* desorption at FeN₄ sites but accelerates O₂ * stripping at NiN₄ sites, enabling the FeN₄-SC-NiN₄ dual-atom sites to feature simultaneously enhanced oxygen reduction (E_1/2 =0.844 V) and oxygen evolution (η₁₀ =246 mV_iR-free) activity, together with a small potential gap (0.632 V) and superior long-term cycling stability for Zn-air battery.

非键合型双金属原子位点已成为双功能电催化的前沿，然而，分别定制两个金属位点的局部电子态仍然难以实现。在此，通过制造 FeN ₄和 NiN ₄单原子，Janus 分布在硫掺杂碳空心球的内外，即 FeN ₄ -SC-NiN ₄，我们证明了硫诱导的 Fe/Ni 各向异性电子调节双原子位点构建“一石二鸟”双向促进可逆氧电催化机制。对于分离的 FeN ₄和 NiN _{4位点，环境中的硫减少了 FeN 4}的电荷站点，同时下移NiN _4站点的d波段中心。这种电子结构差异的扩大分别促进了 FeN _{4 位}点的 OH* 脱附和加速了NiN _{4位点的 O 2} * 剥离，使得 FeN ₄ -SC-NiN ₄双原子位点同时增强了氧还原（E _1/2 =0.844 V) 和析氧 ( η ₁₀ =246 mV _iR-free ) 活动，以及锌空气电池的小电位差 (0.632 V) 和出色的长期循环稳定性。