Although defects are traditionally perceived as undesired feature, the prevalence of tenacious low‐coordinated defects can instead give rise to desirable functionalities. Here, a spontaneous etching of mesostructured crystal, cyanide‐bridged cobalt‐iron (CN‐CoFe) organometallic hybrid into atomically crafted open framework that is populated with erosion‐tolerant high surface energy defects is presented. Unprecedently, the distinct mechanistic etching pathway dictated by the mesostructured assembly, bulk defects, and strong intercoordinated cyanide‐bridged hybrid mediates not only formation of excess low‐coordinated defects but also more importantly stabilizes them against prevailing dissolution and migration issues. Clearly, the heteropolynuclear cyanide bonded inorganic mesostructured clusters sanction the restructuring of a new breed of stable organometallic polymorph with 3D accessible structure enclosed by electrochemical active atomic stepped edges and high index facets. The exceptional electrocatalysis performance supports the assertion that defective mesostructured polymorph offers a new material paradigm to synthetically tailor the elementary building block constituents toward functional materials.

中文翻译：

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介孔纳米框架的功能性缺陷金属-有机配位网络，用于增强电催化

尽管传统上认为缺陷是不希望有的特征，但顽固的低配位缺陷的普遍存在反而会带来理想的功能。在此，提出了一种介观结构的晶体（氰化物桥联的钴铁（CN-CoFe）有机金属杂化物）自发刻蚀成原子加工的开放骨架的方法，该骨架中填充了耐腐蚀的高表面能缺陷。前所未有的是，由介观结构的组装，整体缺陷和强的配位氰化物桥接杂化所决定的独特的机械蚀刻途径，不仅可以介导形成过多的低配位缺陷，而且还可以使它们稳定地抵抗普遍的溶解和迁移问题。清楚地，异质多核氰化物键合的无机介孔结构团簇可重组具有3D可及结构并被电化学活性原子阶梯状边缘和高折射率刻面包围的新型稳定有机金属多晶型物。出色的电催化性能支持这样的主张，即有缺陷的介孔多晶型物提供了一种新的材料范式，可以根据功能材料合成定制基本的构建基块成分。