College of Physics, Henan Normal University, Xinxiang, Henan 453007, China.
Quantum Materials Research Center, College of Physics and Electronic Engineering, Zhengzhou Normal University, Zhengzhou 450044, China.
Phys Chem Chem Phys. 2019 Sep 21;21(35):19651-19659. doi: 10.1039/c9cp04068d. Epub 2019 Aug 30.
Single-atom catalysts (SACs) are highly desired for maximizing the efficiency of metal atoms and can entail high selectivity and activity. Bifunctional catalysts enable higher performance and lower cost than two single-function catalysts. Supported single-atom bifunctional catalysts are therefore of great economic interest and scientific importance. Density functional theory calculations are used to design SACs, isolated transition metal anchored on graphdiyne (TM@GDY), for oxygen reduction (ORR) and oxygen evolution (OER) reactions in alkaline media. A dual-volcano plot is constructed to thoroughly describe and predict the catalytic activity toward ORR and OER processes on TM@GDY materials. The results demonstrate that GDY could provide a unique platform for synthesizing uniform SACs with high catalytic activity toward ORR and OER. The theoretical evaluations show that Ni@GDY and Pt@GDY catalysts possess comparable electrocatalytic activity for ORR and OER in alkaline media. The study not only provides deep insights into the catalytic activity of TM@GDY, but also guides the design of GDY based SACs.
单原子催化剂（SACs）被高度期望能够最大限度地提高金属原子的效率，并具有高选择性和活性。双功能催化剂比两个单功能催化剂具有更高的性能和更低的成本。因此，负载型单原子双功能催化剂具有重要的经济意义和科学重要性。本研究使用密度泛函理论计算设计了 SACs，即孤立的过渡金属锚定在石墨炔（TM@GDY）上，用于碱性介质中的氧还原（ORR）和氧析出（OER）反应。构建了双火山图来全面描述和预测 TM@GDY 材料对 ORR 和 OER 过程的催化活性。结果表明，GDY 可为合成具有高 ORR 和 OER 催化活性的均一单原子催化剂提供独特的平台。理论评估表明，Ni@GDY 和 Pt@GDY 催化剂在碱性介质中对 ORR 和 OER 具有相当的电催化活性。该研究不仅深入了解了 TM@GDY 的催化活性，还指导了基于 GDY 的 SACs 的设计。
