Functional Defective Metal‐Organic Coordinated Network of Mesostructured Nanoframes for Enhanced Electrocatalysis
Functional Defective Metal‐Organic Coordinated Network of Mesostructured Nanoframes for Enhanced Electrocatalysis
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DOI：
10.1002/adfm.201704177
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发表时间：
2018
影响因子：
19
通讯作者：
G. Yilmaz;Chuan Fu Tan;M. Hong;G. Ho
中科院分区：
文献类型：
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作者：
G. Yilmaz;Chuan Fu Tan;M. Hong;G. Ho
尽管缺陷传统上被认为是不受欢迎的特征，但顽固的低协调缺陷的普遍存在反而可以带来理想的功能。在这里，提出了将介观结构晶体、氰化物桥联钴铁（CN-CoFe）有机金属杂化物自发蚀刻成原子制作的开放框架，该框架充满耐腐蚀的高表面能缺陷。前所未有的是，由介观结构组装、体缺陷和强相互配位的氰化物桥杂化物决定的独特的机械蚀刻途径不仅介导了过量的低配位缺陷的形成，而且更重要的是使它们稳定下来，以应对普遍存在的溶解和迁移问题。显然，杂多核氰化物键合的无机介观结构簇支持重组新型稳定的有机金属多晶型物，其具有由电化学活性原子阶梯边缘和高折射率面包围的3D可接近结构。卓越的电催化性能支持这样的论点，即有缺陷的介观结构多晶型物提供了一种新的材料范式，可以综合定制功能材料的基本构建块成分。
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.