金属镍广泛应用于析氧反应（OER）催化，其作为预催化剂，经表面重构转化为NiOOH，后者为OER的实际活性物种。因此，OER性能与NiOOH结构密切相关，而NiOOH结构取决于预催化剂的性质。由此可见，调控金属镍以获得高性能NiOOH至关重要。本研究提出了一种界面氧化还原调控策略，利用电化学剥离石墨烯（EG）将泡沫镍（NF）表面氧化为所需的Ni2+物种。采用原位表征技术在阳极电位下对EG氧化NF表面的γ-NiOOH进行了研究，该物种有利于OER进行，研究发现此过程抑制了性能较差的β-NiOOH的生成。还原后，单原子镍及镍团簇被锚定于EG层上。改性后的γ-NiOOH以及单原子镍和镍团簇共同提升了EG氧化NF的OER性能，表现出较低的过电位和增强的稳定性。随后，采用可控的EG与镍基金属验证了该界面氧化还原调控策略的普适性。优化后的EG氧化NiFe体系在10 mA·cm-2电流密度下过电位仅为243 mV，并在500 mA·cm-2高电流密度下实现了100 h的长期稳定运行。

Metallic Ni is widely used for oxygen evolution reaction (OER) catalysis. It acts as a precatalyst and undergoes surface reconstruction into NiOOH, which is the active species used in OER. Consequently, OER performance is highly related to the NiOOH structure, which is determined by the precatalyst. Thus, the modulation of metallic Ni to obtain superior NiOOH is critical. Herein, an interfacial redox modulation strategy is proposed to oxidize a Ni foam (NF) surface into the desired Ni²⁺ species using electrochemically exfoliated graphene (EG). OER-favorable γ-NiOOH on EG-oxidized NF was investigated under anodic potentials by in situ characterization techniques, whereby the formation of inferior β-NiOOH was found to be inhibited. Single Ni atoms and clusters were anchored onto the EG layers after reduction. The altered γ-NiOOH and Ni single atoms and clusters improved the OER performance of the EG-oxidized NF with low overpotential and enhanced stability. Subsequently, controllable EG and Ni-based metals were used to verify the versatility of the proposed interfacial redox modulation strategy. The optimized EG-oxidized NiFe system achieved an overpotential of 243 mV at 10 mA⋅cm⁻² and long-term stability at 500 mA⋅cm⁻² for 100 h.