Unleashing the power of zero-valent platinum single atoms for enhancing low-temperature oxygen activation

Developing efficient catalysts for low-temperature O2 activation is critical for energy-efficient heterogeneous catalysis, yet designing highly active and accessible active sites remains a formidable challenge. Here, we construct a new type of zero-valent platinum single atoms (Pt0 SAs) on two-dimensional Co3O4 through a feasible low-temperature reduction strategy. By eliminating oxygen coordination, we induce strong Pt−Co electronic interactions and optimize the Pt 5 d band center, promoting electron donation that strengthens O2 activation. In contrast, conventional high-valent Pt4+ SAs, which rely on oxygen vacancy formation, exhibits weaker O2 activation. Consequently, Pt0 SAs achieves a 9.3-fold higher turnover frequency in toluene oxidation than does the Pt4+ SAs at 140 °C (the temperature at which a toluene conversion efficiency of 90% is achieved). This work highlights electronic modulation in optimizing O2 activation and affords a strategy for designing highly efficient zero-valent single atom catalysts. Efficient low temperature oxygen activation is essential but hard to achieve with accessible metal sites. This work shows that zero-valent single Pt atoms on cobalt oxide donate electrons to oxygen, enabling low-temperature toluene oxidation.