Yijian Song , Chao Han , Weijie Li , Xiufeng Yi , Qing Liao , Ji Zhou , Yaqin Zhou , Yitao Ouyang , Yingping Zhang , Qingqing Zheng , Anqiang Pan
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引用次数: 0
摘要
将单个原子和簇整合到一个统一的催化系统中代表了一种提高催化性能的新策略。与单原子催化剂相比,那些结合单原子和簇的催化剂表现出更好的催化活性。然而,这些系统的共同构建及其催化效果的机制仍然具有挑战性且知之甚少。在这项研究中,我们通过简单的两步烧结法合成了一种具有MnY簇和Mn单原子的Mn - n - c催化剂。Y掺杂通过独特的协同效应促进了Mn簇的形成,优化了Mn的d带中心,从而降低了能垒,提高了反应动力学。此外,Y单原子的给电子能力促进了不饱和Mn-N₃配位结构的形成,从而获得了优异的氧还原反应(ORR)性能。因此,MnY/NC催化剂的半波电位(E₁/ 2)为0.90 V,在0.1 M KOH下保持稳定性,优于Mn/NC和Pt/C。这项工作强调了稀土金属在过渡金属中掺杂的潜力,可以创建稳定的单原子和簇体系,有效地利用它们的协同效应来获得卓越的催化性能,并验证了多相催化中“远程协同效应”的概念。
Engineering bimetallic cluster architectures: Harnessing unique “remote synergy effect” between Mn and Y for enhanced electrocatalytic oxygen reduction reaction
Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance. Compared to single-atom catalysts, those incorporating both single atoms and clusters exhibit superior catalytic activity. However, the co-construction of these systems and the mechanisms of their catalytic efficacy remain challenging and poorly understood. In this study, we synthesized a Mn–N–C catalyst featuring MnY clusters and Mn single atoms via a straightforward two-step sintering method. Y doping facilitated the formation of Mn clusters and optimized the d-band center of Mn through a unique synergy effect, thereby reducing energy barriers and enhancing the reaction kinetics. Additionally, the electron-donating ability of Y single atoms promoted the formation of unsaturated Mn–N₃ coordination structures, resulting in excellent oxygen reduction reaction (ORR) performance. Consequently, the MnY/NC catalyst demonstrated a half-wave potential (E₁/₂) of 0.90 V and maintained stability in 0.1 M KOH, outperforming both Mn/NC and Pt/C. This work underscores the potential of rare earth metal doping in transition metals to create stable single-atom and cluster systems, effectively leveraging their synergy effect for superior catalytic performance and validating the concept of the “remote synergy effect” in heterogeneous catalysis.