Multifunctional catalysts that integrate high efficiency hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) catalytic activity in a single material are attractive for unitized regenerative fuel cells and overall water splitting technologies. As the best-known HER and ORR electrocatalysts, Pt and its alloys have only moderate OER activity. Ruthenium and iridium oxides exhibit the highest OER activities but not as active as Pt for HER and ORR. Here, we proposed a general principle for achieving trifunctional electrocatalysis for three reactions in a single material. Using the newly-synthesized pyrazine-modified graphdiyne (PR-GDY) as an example, we demonstrated that the synergistic effect of the pyridinic nitrogen and anchored transition-metal (TM) single atoms renders highly-efficient HER/OER/ORR trifunctional electrocatalytic activity. For the Ni-doped PR-GDY, the overpotentials for HER, OER and ORR can be respectively as low as −0.05, 0.29 and 0.38 V, which are comparable or even superior to the best-known single-functional and bi-functional precious electrocatalysts. These computational results offer not only a promising trifunctional electrocatalyst but also a strategy for the design of multifunctional electrocatalysts.

将高效析氢反应 (HER)、析氧反应 (OER) 和氧还原反应 (ORR) 催化活性集成在单一材料中的多功能催化剂对于单元化再生燃料电池和整体水分解技术具有吸引力。作为最著名的 HER 和 ORR 电催化剂，Pt 及其合金仅具有中等的 OER 活性。钌和铱的氧化物表现出最高的 OER 活性，但在 HER 和 ORR 方面不如铂。在这里，我们提出了在单一材料中实现三个反应的三功能电催化的一般原则。以新合成的吡嗪修饰石墨二炔（PR-GDY）为例，我们证明了吡啶氮和锚定过渡金属 (TM) 单原子的协同效应具有高效的 HER/OER/ORR 三功能电催化活性。对于 Ni 掺杂的 PR-GDY，HER、OER 和 ORR 的过电势可分别低至 -0.05、0.29 和 0.38 V，与最著名的单功能和双功能贵金属相当甚至优于电催化剂。这些计算结果不仅提供了一种有前途的三功能电催化剂，而且为设计多功能电催化剂提供了策略。与最著名的单功能和双功能贵金属电催化剂相当甚至更好。这些计算结果不仅提供了一种有前途的三功能电催化剂，而且为设计多功能电催化剂提供了策略。与最著名的单功能和双功能贵金属电催化剂相当甚至更好。这些计算结果不仅提供了一种有前途的三功能电催化剂，而且为设计多功能电催化剂提供了策略。