利用吡咯氮位点促进双电子氧还原用于电化学过氧化氢生产,Nature Communications

通过双电子氧还原反应生产电催化过氧化氢（H 2 O 2 ）是能源密集型和高污染的蒽醌氧化过程的一种有前途的替代方法。然而，开发具有高H 2 O 2产率、选择性和耐久性的先进电催化剂仍然具有挑战性，因为典型的含金属催化剂上的活性位点数量有限且容易钝化，特别是对于最先进的单一催化剂- 原子。为了解决这个问题，我们报告了一种用于高速率和高效2e-氧还原催化的石墨烯/介孔碳复合材料。吡咯-N位点的配位调节*OOH物质的吸附构型，为H 2 O 2的产生提供动力学上有利的途径。因此，H 2 O 2产量接近30 mol g -1 h -1，法拉第效率为80%，并且耐久性优异，产生7.2 g L -1的高H 2 O 2浓度。这种利用多个非金属活性位点操纵反应物吸附构型的策略为设计用于 2e -氧还原的高效且耐用的无金属电催化剂提供了一种策略。

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Electrocatalytic hydrogen peroxide (H2O2) production via the two-electron oxygen reduction reaction is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H2O2 yield, selectivity, and durability is still challenging, because of the limited quantity and easy passivation of active sites on typical metal-containing catalysts, especially for the state-of-the-art single-atom ones. To address this, we report a graphene/mesoporous carbon composite for high-rate and high-efficiency 2e− oxygen reduction catalysis. The coordination of pyrrolic-N sites -modulates the adsorption configuration of the *OOH species to provide a kinetically favorable pathway for H2O2 production. Consequently, the H2O2 yield approaches 30 mol g−1 h−1 with a Faradaic efficiency of 80% and excellent durability, yielding a high H2O2 concentration of 7.2 g L−1. This strategy of manipulating the adsorption configuration of reactants with multiple non-metal active sites provides a strategy to design efficient and durable metal-free electrocatalyst for 2e− oxygen reduction.