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Superatomic Layer of Cubic Mo4S4 Clusters Connected by Cl Cross-Linking
Advanced Materials ( IF 27.4 ) Pub Date : 2024-07-25 , DOI: 10.1002/adma.202404249
Yusuke Nakanishi 1 , Naoyuki Kanda 2 , Motoki Aizaki 2 , Kaito Hirata 3 , Yasufumi Takahashi 3, 4 , Takahiko Endo 1 , Yung-Chang Lin 5 , Ryosuke Senga 5 , Kazu Suenaga 6 , Shinobu Aoyagi 7 , Mina Maruyama 8 , Yanlin Gao 8 , Susumu Okada 8 , Yasumitsu Miyata 1 , Zheng Liu 9
Advanced Materials ( IF 27.4 ) Pub Date : 2024-07-25 , DOI: 10.1002/adma.202404249
Yusuke Nakanishi 1 , Naoyuki Kanda 2 , Motoki Aizaki 2 , Kaito Hirata 3 , Yasufumi Takahashi 3, 4 , Takahiko Endo 1 , Yung-Chang Lin 5 , Ryosuke Senga 5 , Kazu Suenaga 6 , Shinobu Aoyagi 7 , Mina Maruyama 8 , Yanlin Gao 8 , Susumu Okada 8 , Yasumitsu Miyata 1 , Zheng Liu 9
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Superatomic clusters – assemblies of atoms with various sizes, shapes, and compositions – can form hierarchical architectures that exhibit emergent electronic properties not found in their individual units. In particular, cubic M4X4 clusters of chalcogenides (M = transition metal; X = chalcogen) are recognized as versatile building blocks for 3D structures with tunable morphologies and electronic properties. However, tetrahedral M4X4 clusters rarely assemble into 2D architectures, which could offer a distinct class of functional materials from their 3D analogues. Here, this work reports the preparation of 2D Mo8S8Cl11, a superatomic layer with a sandwich structure consisting of Mo4S4 clusters interconnected through Cl cross-linking. The vapor-phase reaction inside nanotubes promotes the selective growth of Mo8S8Cl11 nanoribbons, allowing detailed characterization via transmission electron microscopy. This methodology can be applied to the growth of layered structures containing Mo8S8Cl11 at the micrometer scale. This work has demonstrated that mono- and few-layer Mo8S8Cl11 can be prepared by exfoliation of parent solids. Electronic structure calculations indicate that the 2D monolayer has quasi-flat bands, giving rise to an indirect-to-direct bandgap transition under mechanical strain. Furthermore, scanning electrochemical microscopy reveals the potential of the layered structures as highly efficient catalysts for the hydrogen-evolution reaction.
中文翻译：
通过 Cl 交联连接的立方 Mo4S4 团簇的超原子层
超原子团簇——具有不同尺寸、形状和成分的原子的集合体——可以形成分层结构，这些结构表现出单个单元中未发现的新兴电子特性。特别是，立方 M 4 X 4硫族化物簇（M = 过渡金属；X = 硫族元素）被认为是具有可调节形态和电子特性的 3D 结构的通用构建模块。然而，四面体 M 4 X 4簇很少组装成 2D 结构，而 2D 结构可以提供与其 3D 类似物不同的一类功能材料。在这里，这项工作报告了2D Mo 8 S 8 Cl 11的制备，这是一种具有三明治结构的超原子层，由通过Cl交联互连的Mo 4 S 4簇组成。纳米管内的气相反应促进Mo 8 S 8 Cl 11纳米带的选择性生长，从而可以通过透射电子显微镜进行详细表征。该方法可应用于微米级含有Mo 8 S 8 Cl 11的层状结构的生长。这项工作证明单层和少层Mo 8 S 8 Cl 11可以通过母体固体的剥离来制备。电子结构计算表明，二维单层具有准平坦能带，在机械应变下产生间接带隙到直接带隙的转变。此外，扫描电化学显微镜揭示了层状结构作为析氢反应高效催化剂的潜力。
更新日期：2024-07-25
中文翻译：
通过 Cl 交联连接的立方 Mo4S4 团簇的超原子层
超原子团簇——具有不同尺寸、形状和成分的原子的集合体——可以形成分层结构，这些结构表现出单个单元中未发现的新兴电子特性。特别是，立方 M 4 X 4硫族化物簇（M = 过渡金属；X = 硫族元素）被认为是具有可调节形态和电子特性的 3D 结构的通用构建模块。然而，四面体 M 4 X 4簇很少组装成 2D 结构，而 2D 结构可以提供与其 3D 类似物不同的一类功能材料。在这里，这项工作报告了2D Mo 8 S 8 Cl 11的制备，这是一种具有三明治结构的超原子层，由通过Cl交联互连的Mo 4 S 4簇组成。纳米管内的气相反应促进Mo 8 S 8 Cl 11纳米带的选择性生长，从而可以通过透射电子显微镜进行详细表征。该方法可应用于微米级含有Mo 8 S 8 Cl 11的层状结构的生长。这项工作证明单层和少层Mo 8 S 8 Cl 11可以通过母体固体的剥离来制备。电子结构计算表明，二维单层具有准平坦能带，在机械应变下产生间接带隙到直接带隙的转变。此外，扫描电化学显微镜揭示了层状结构作为析氢反应高效催化剂的潜力。
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