Li Zhongliang, Cao Lili, Yang Ting, He Jinwei, Wang Zelin, He Jinlu, Zhao Yan, Chai Zhanli
School of Chemistry and Chemical Engineering, College of Energy Materials and Chemistry, Inner Mongolia University, Hohhot 010021, P. R. China.
School of Chemistry and Chemical Engineering, College of Energy Materials and Chemistry, Inner Mongolia University, Hohhot 010021, P. R. China; Shandong Electric Power Engineering Consulting Institute Co., Ltd., Jinan 250000, China.
J Colloid Interface Sci. 2025 Jan;677(Pt A):677-686. doi: 10.1016/j.jcis.2024.07.167. Epub 2024 Jul 28.
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 mg) and specific (1.75 mA cm) 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 O 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.
开发用于氧还原反应（ORR）的具有高活性和长耐久性的碳载铂基电催化剂，对于其商业应用而言是一项巨大挑战，因为在高电位下，碳载体在酸性/碱性溶液中会发生腐蚀。在这项工作中，通过原位分子自组装策略合成了一种Janus结构的TaON/类石墨烯碳（GLC），它被用作铂（Pt）的双载体。所制备的Pt/TaON/GLC在0.9 V时具有高半波电位（相对于可逆氢电极（RHE）为0.94 V）、优异的质量活性（1.48 A mg）和比活性（1.75 mA cm），并且在碱性溶液中经过10000次循环后具有优异的长期耐久性，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效应，包括增强的界面电子密度、改善的电荷转移、增强的O吸附和叠加的O-O裂解。这项工作展示了一种通过协同促进界面工程制备高活性和长耐久性铂基电催化剂的潜在策略。
