Oxygen reduction reaction catalyzed by carbon composites with ruthenium-doped iron oxide nanoparticles
Oxygen reduction reaction catalyzed by carbon composites with ruthenium-doped iron oxide nanoparticles
复制标题
钌掺杂氧化铁纳米颗粒碳复合材料催化氧还原反应
DOI：
10.1039/d2ma00054g
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发表时间：
2022
影响因子：
5
通讯作者：
Bridges, Frank
中科院分区：
文献类型：
--
作者：
Liu, Qiming;Zhou, Hong Bo;Nichols, Forrest;Kuo, Han-Lin;Mercado, Rene;Lu, Bingzhang;Zhu, Weiya;Liu, Yashu;Lu, Jennifer Q.;Bridges, Frank
基于过渡金属氧化物的碳纳米复合材料作为一种高性价比的氧还原反应催化剂受到了广泛关注。然而，与现有技术的铂催化剂相比，活性仍然低于标准。提高ORR性能的一种方法是将第二种金属掺杂到纳米复合材料中以操纵电子结构，从而操纵与关键反应中间体的相互作用。本文通过控制热解Fe-Ru-Fe三核配合物沿着咪唑骨架-8合成了双金属（Ru和Fe）和氮共掺杂碳（RuFe-NC）纳米复合材料。所得的多孔纳米复合材料由嵌入在碳支架内的Ru掺杂的Fe 2 O3纳米颗粒组成，并且在碱性介质中表现出与商业Pt/C相媲美的ORR活性，这也明显优于那些monoclonal对应物和用单个monoclonal化合物前体的简单混合物制备的纳米复合材料。结构表征表明，三核配合物的使用促进了钌在氧化铁纳米颗粒内的原子分散，并且金属中心之间的电荷转移导致高ORR活性。从这项研究的结果表明，合理设计的杂原子配合物可能是一个独特的战略，在高性能的电催化碳-金属纳米复合材料的结构工程。
Carbon nanocomposites based on transition-metal oxides have been attracting extensive attention as cost-effective catalysts towards the oxygen reduction reaction (ORR). However, the activity remains subpar as compared to state-of-the-art platinum catalysts. One way to enhance the ORR performance is to dope a second metal into the nanocomposite to manipulate the electronic structure and hence the interactions with key reaction intermediates. Herein, dual metal (Ru and Fe) and nitrogen codoped carbon (RuFe-NC) nanocomposites were synthesized by controlled pyrolysis of a Fe–Ru–Fe trinuclear complex along with zeolitic imidazolate framework-8. The obtained porous nanocomposites consisted of Ru-doped Fe2O3 nanoparticles embedded within a carbon scaffold, and exhibited an ORR activity in alkaline media rivaling that of commercial Pt/C, which was also markedly better than those of the monometallic counterparts and nanocomposites prepared with a simple mixture of the individual monometallic compound precursors. Structural characterization suggests that the use of the trinuclear complex facilitated the atomic dispersion of ruthenium within the iron oxide nanoparticles and charge transfer between the metal centers led to a high ORR activity. Results from this study suggest that rational design of heteronuclear complexes may be a unique strategy in the structural engineering of carbon-metal nanocomposites for high-performance electrocatalysis.