Branched In2O3 Mesocrystal of Ordered Architecture Derived from the Oriented Alignment of a Metal–Organic Framework for Accelerated Hydrogen Evolution over In2O3–ZnIn2S4,ACS Applied Materials & Interfaces

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Branched In2O3 Mesocrystal of Ordered Architecture Derived from the Oriented Alignment of a Metal–Organic Framework for Accelerated Hydrogen Evolution over In2O3–ZnIn2S4
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-02-18 , DOI: 10.1021/acsami.0c19806
Guoxin Zhuang _{1,

2} , Qihui Fang _{1,

2} , Jinxin Wei _{1,

2} , Chengkai Yang _{1,

2,

3} , Muqing Chen _{1,

2} , Zikun Lyu _{1,

2} , Zanyong Zhuang _{1,

2} , Yan Yu _{1,

2}

Affiliation

It is fascinating yet challenging to assemble anisotropic nanowires into ordered architectures of high complexity and intriguing functions. We exploited a facile strategy involving oriented etching of a metal–organic fragment (MOF) to advance the rational design of highly ordered nanostructures. As a proof of concept, a microscale MIL-68(In) single crystal was etched with a K₃[Co(CN)₆] solution to give a microtube composed of aligned MIL-68(In) nanorods. Annealing such a MIL-68(In) microtube readily created an unprecedented branched In₂O₃ mesocrystal by assembly of In₂O₃ nanorods aligned in order. The derived ordered-In₂O₃–ZnIn₂S₄ is more efficient in catalyzing visible-light-driven H₂ evolution (8753 μmol h^–1 g^–1) outperforming the disordered-In₂O₃–ZnIn₂S₄ counterpart (2700 μmol h^–1 g^–1) as well as many other state-of-the-art ZnIn₂S₄-based photocatalysts. The ordered architecture significantly boosts the short-range electron transfer in an In₂O₃–ZnIn₂S₄ heterojunction but has a negligible impact on the long-range electron transfer among In₂O₃ mesocrystals. The density functional theory (DFT) calculation reveals that the oriented etching is achieved by the selective binding of the [Co(CN)₆]^3– etchant on the (110) plane of MIL-68(In), which can drag the In atoms out of the framework in order. Our findings could broaden the technical sense toward advanced photocatalyst design and impose scientific impacts on unveiling how ordered photosystems operate.

中文翻译：

支链在₂ ö ₃从金属-有机骨架的面向对准衍生为加速氢有序建筑非晶演进超过在₂ ö ₃ -ZnIn ₂小号₄

将各向异性纳米线组装成具有高度复杂性和有趣功能的有序体系结构既有趣又具有挑战性。我们开发了一种简便的策略，包括对金属-有机碎片（MOF）进行定向刻蚀，以推进高度有序的纳米结构的合理设计。作为概念的证明，用K ₃ [Co（CN）₆ ]溶液蚀刻了微型MIL-68（In）单晶，得到了由对准的MIL-68（In）纳米棒组成的微管。通过按顺序排列的In ₂ O ₃纳米棒的组装，对这样的MIL-68（In）微管进行退火很容易创建了前所未有的分支In ₂ O ₃中间晶体。导出有序-In ₂ O ₃ -ZnIn₂小号₄是在催化可见光驱动H以下高效的₂演进（8753微摩尔ħ ^-1克^-1）表现好于无序-在₂ ö ₃ -ZnIn ₂ š ₄对方（2700微摩尔ħ ^-1克^-1）以及许多其他最先进的ZnIn ₂ S ₄基光催化剂。有序体系结构显着提高了In ₂ O ₃ –ZnIn ₂ S ₄中的短程电子转移异质结，但对In ₂ O ₃中间晶体之间的远程电子转移影响微不足道。密度泛函理论（DFT）计算表明，定向刻蚀是通过在MIL-68（In）的（110）平面上选择性结合[Co（CN）₆ ] ^3–刻蚀剂实现的，这会拖延In原子按顺序脱离框架。我们的发现可以将技术意义扩展到高级光催化剂设计，并对揭示有序光系统的工作方式产生科学影响。

更新日期：2021-03-03

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