Revealing the Mechanism of sp‐N Doping in Graphdiyne for Developing Site‐Defined Metal‐Free Catalysts

• DOI: 10.1002/adma.202206450
• Publication Date: 2022-10-11T07:53:31Z
• Authors: Baokun Liu; Shuhui Zhan; Jiang Du; Xin Yang; Yasong Zhao; Lulu Li; Jiawei Wan; Zhi‐Jian Zhao; Jinlong Gong; Nailiang Yang; Ranbo Yu; Dan Wang
• Keywords: Carbon fibers

Abstract Due to the limited reserves of metals, scientists are devoted exploring high‐performance metal‐free catalysts based on carbon materials solve environment‐related issues. Doping would build up inhomogeneous charge distribution surface, which is an efficient approach for boosting catalytic performance. However, doping sites difficult control in traditional materials, thus hindering their development. Taking advantage unique sp‐C graphdiyne (GDY), a new N configuration sp‐hybridized nitrogen (sp‐N), bringing Pt‐comparable activity oxygen reduction reaction site‐defined introduced. intermediate this process never captured, understanding mechanism and precise synthesis catalysts. After four‐year study, fabrication intermediate‐like molecule realized, finally sp‐N doped GDY via pericyclic obtained. Compared with other configurations, designed shows much higher electroreduction CO 2 toward CH 4 production, owing electronic structure introduced by sp‐N, more favorable stabilizing intermediate. Thus, besides opening black‐box doping, work reveals relationship between products reduction.