Universal Approach to Fabricating Graphene-Supported Single-Atom Catalysts from Doped ZnO Solid Solutions.,ACS Central Science

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Universal Approach to Fabricating Graphene-Supported Single-Atom Catalysts from Doped ZnO Solid Solutions.
ACS Central Science ( IF 12.7 ) Pub Date : 2020-07-07 , DOI: 10.1021/acscentsci.0c00458
Jiashen Meng ₁ , Jiantao Li ₁ , Jinshuai Liu ₁ , Xingcai Zhang ₂ , Gengping Jiang ₃ , Lu Ma ₄ , Zhi-Yi Hu ₅ , Shibo Xi ₆ , Yunlong Zhao ₇ , Mengyu Yan ₁ , Peiyao Wang ₈ , Xiong Liu ₁ , Qidong Li ₁ , Jefferson Zhe Liu ₈ , Tianpin Wu ₄ , Liqiang Mai ₁

Affiliation

Single-atom catalysts (SACs) have attracted widespread interest for many catalytic applications because of their distinguishing properties. However, general and scalable synthesis of efficient SACs remains significantly challenging, which limits their applications. Here we report an efficient and universal approach to fabricating a series of high-content metal atoms anchored into hollow nitrogen-doped graphene frameworks (M-N-Grs; M represents Fe, Co, Ni, Cu, etc.) at gram-scale. The highly compatible doped ZnO templates, acting as the dispersants of targeted metal heteroatoms, can react with the incoming gaseous organic ligands to form doped metal–organic framework thin shells, whose composition determines the heteroatom species and contents in M-N-Grs. We achieved over 1.2 atom % (5.85 wt %) metal loading content, superior oxygen reduction activity over commercial Pt/C catalyst, and a very high diffusion-limiting current (6.82 mA cm^–2). Both experimental analyses and theoretical calculations reveal the oxygen reduction activity sequence of M-N-Grs. Additionally, the superior performance in Fe-N-Gr is mainly attributed to its unique electron structure, rich exposed active sites, and robust hollow framework. This synthesis strategy will stimulate the rapid development of SACs for diverse energy-related fields.

中文翻译：

从掺杂的ZnO固溶体制备石墨烯负载的单原子催化剂的通用方法。

单原子催化剂（SAC）由于其独特的性能而吸引了许多催化应用的广泛兴趣。但是，高效SAC的常规且可扩展的合成仍然极具挑战性，这限制了它们的应用。在这里，我们报告了一种有效且通用的方法，以克为单位制造一系列固定在中空氮掺杂石墨烯骨架（MN-Grs； M代表Fe，Co，Ni，Cu等）中的高含量金属原子。高度相容的掺杂ZnO模板充当目标金属杂原子的分散剂，可以与进入的气态有机配体反应形成掺杂的金属有机骨架薄壳，其组成决定了MN-Grs中的杂原子种类和含量。我们实现了超过1.2原子％（5.85重量％）的金属负载量，^–2）。实验分析和理论计算均揭示了MN-Grs的氧还原活性序列。另外，Fe-N-Gr的优异性能主要归因于其独特的电子结构，丰富的暴露活性位点和坚固的中空骨架。这种合成策略将刺激SAC在与能源相关的各种领域中的快速发展。

更新日期：2020-08-26

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