由于碳载体在高电位的酸/碱溶液中的腐蚀,开发用于氧还原反应(ORR)的具有高活性和长期耐久性的碳负载的Pt基电催化剂对于它们的商业应用是巨大的挑战。在这项工作中,通过原位分子自组装策略合成了Janus结构TaON/石墨烯状碳(GLC),用作铂(Pt)的双载体。获得的Pt/TaON/GLC呈现高半波电位(0.94Vvs.RHE),在0.9V时具有出色的质量(1.48AmgPt-1)和比(1.75mAcmPt-2)活性,和卓越的长期耐久性,在碱性溶液中10,000次循环后质量活性损失最小(8.0%),优于Pt/C和其他催化剂。结构表征和密度泛函理论(DFT)计算表明,Pt/TaON/GLC催化剂表现出最大的协同作用,包括增强的界面电子密度,改进的电荷转移,增强O2吸附,并叠加OO卵裂。这项工作显示了通过协同促进的界面工程制备高活性和长期耐用的Pt基电催化剂的潜在策略。
Developing carbon-supported Pt-based electrocatalysts with high activity and long-durability for the oxygen reduction reaction (ORR) is an enormous challenge for their commercial applications due to the corrosion of carbon supports in acid/alkaline solution at high potential. In this work, a Janus structural TaON/graphene-like carbon (GLC) was synthesized via an in-situ molecular selfassembly strategy, which was used as a dual-carrier for platinum (Pt). The as-obtained Pt/TaON/GLC presents high half-wave potential (0.94 V vs. RHE), excellent mass (1.48 A mgPt-1) and specific (1.75 mA cmPt-2) activities at 0.9 V, and superior long-term durability with a minimal loss (8.0 %) of mass activity after 10,000 cycles in alkaline solution, outperforming those of Pt/C and other catalysts. The structural characterizations and density functional theory (DFT) calculations indicate that the Pt/TaON/GLC catalyst exhibits the maximum synergies, including enhanced interfacial electron density, improved charge transfer, enhanced O2 adsorption, andsuperimposed OO cleavage. This work shows a potential strategy for preparing the high-active and long-durable Pt-based
electrocatalyst by synergism-promoted interface engineering.