Shan Jieqiong, Ye Chao, Chen Shuangming, Sun Tulai, Jiao Yan, Liu Lingmei, Zhu Chongzhi, Song Li, Han Yu, Jaroniec Mietek, Zhu Yihan, Zheng Yao, Qiao Shi-Zhang
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide SA5005, Australia.
Centre for Materials in Energy and Catalysis, The University of Adelaide, Adelaide SA 5005, Australia.
J Am Chem Soc. 2021 Apr 7;143(13):5201-5211. doi: 10.1021/jacs.1c01525. Epub 2021 Mar 25.
Noble metals manifest themselves with unique electronic structures and irreplaceable activity toward a wide range of catalytic applications but are unfortunately restricted by limited choice of geometric structures spanning single atoms, clusters, nanoparticles, and bulk crystals. Herein, we propose how to overcome this limitation by integrating noble metal atoms into the lattice of transition metal oxides to create a new type of hybrid structure. This study shows that iridium single atoms can be accommodated into the cationic sites of cobalt spinel oxide with short-range order and an identical spatial correlation as the host lattice. The resultant IrCoO catalyst exhibits much higher electrocatalytic activity than the parent oxide by 2 orders of magnitude toward the challenging oxygen evolution reaction under acidic conditions. Because of the strong interaction between iridium and cobalt oxide support, the IrCoO catalyst shows significantly improved corrosion resistance under acidic conditions and oxidative potentials. This work eliminates the "close-packing" limitation of noble metals and offers promising opportunity to create analogues with desired topologies for various catalytic applications.
贵金属具有独特的电子结构，在广泛的催化应用中展现出不可替代的活性，但遗憾的是，其几何结构选择有限，仅涵盖单原子、团簇、纳米颗粒和块状晶体。在此，我们提出如何通过将贵金属原子整合到过渡金属氧化物晶格中以创造新型杂化结构来克服这一限制。本研究表明，铱单原子能够以短程有序且与主体晶格相同的空间相关性容纳于钴尖晶石氧化物的阳离子位点。所得的IrCoO催化剂在酸性条件下对具有挑战性的析氧反应表现出比母体氧化物高2个数量级的电催化活性。由于铱与氧化钴载体之间的强相互作用，IrCoO催化剂在酸性条件和氧化电位下表现出显著提高的耐腐蚀性。这项工作消除了贵金属的“紧密堆积”限制，并为创造具有所需拓扑结构的类似物用于各种催化应用提供了广阔前景。
