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Short-Range Ordered Iridium Single Atoms Integrated into Cobalt Oxide Spinel Structure for Highly Efficient Electrocatalytic Water Oxidation
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-03-25 , DOI: 10.1021/jacs.1c01525
Jieqiong Shan 1, 2 , Chao Ye 1, 2 , Shuangming Chen 3 , Tulai Sun 4 , Yan Jiao 1, 2 , Lingmei Liu 5 , Chongzhi Zhu 4 , Li Song 3 , Yu Han 5 , Mietek Jaroniec 6 , Yihan Zhu 4 , Yao Zheng 1, 2 , Shi-Zhang Qiao 1, 2
Affiliation  

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 Ir0.06Co2.94O4 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 Ir0.06Co2.94O4 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.

中文翻译:

短程有序铱单原子集成到氧化钴尖晶石结构中,可实现高效电催化水氧化

贵金属以其独特的电子结构和在广泛的催化应用中无可替代的活性表现出来,但不幸的是,有限的跨越单个原子,团簇,纳米颗粒和块状晶体的几何结构选择受到限制。在本文中,我们提出了如何通过将贵金属原子整合到过渡金属氧化物的晶格中以创建新型的杂化结构来克服这一限制的方法。这项研究表明,铱单原子可以以短程顺序和与主体晶格相同的空间相关性容纳在钴尖晶石氧化物的阳离子位点中。生成的Ir 0.06 Co 2.94 O 4在酸性条件下,具有挑战性的放氧反应催化剂比母体氧化物具有高出两个数量级的电催化活性。由于铱和氧化钴载体之间的强相互作用,Ir 0.06 Co 2.94 O 4催化剂在酸性条件和氧化电位下显示出显着改善的耐腐蚀性。这项工作消除了贵金属的“密堆积”限制,并提供了有希望的机会来制造具有所需拓扑结构的类似物以用于各种催化应用。
更新日期:2021-04-08
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