2D Metal Organic Framework Nanosheet: A Universal Platform Promoting Highly Efficient Visible-Light-Induced Hydrogen Production
2D Metal Organic Framework Nanosheet: A Universal Platform Promoting Highly Efficient Visible-Light-Induced Hydrogen Production
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DOI：
10.1002/aenm.201803402
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发表时间：
2019-03-01
影响因子：
27.8
通讯作者：
Qiao, Shi-Zhang
中科院分区：
文献类型：
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作者：
Ran, Jingrun;Qu, Jiangtao;Qiao, Shi-Zhang
二维金属有机骨架（MOF）由于其有机-无机杂化性质、大表面积、高暴露活性位点和超薄厚度而受到广泛关注。然而，二维MOF在光-氢（H-2）转化中的应用鲜有报道。在这里，一种新的二维MOF [Ni(phen)(oba)](n)中心点0.5nH(2)O （phen = 1,10-菲罗啉，oba = 4,4 '-氧双（苯甲酸盐））首次被用作支持CdS或Zn0.8Cd0.2S的一般、高性能和地球丰富的平台，以实现大大提高可见光诱导的h- 2生成活性。特别是，负载cd的2D MOF表现出良好的h -2生成活性，为45 201 mu mol h(-1) g(-1)，甚至比负载pt的cd高出185%。先进的表征，例如基于同步加速器的x射线吸收近边结构和理论计算表明，二维MOF和CdS之间的相互作用性质，加上二维MOF的高表面积，丰富的反应中心和良好的波段结构，协同促成了这种杰出的光催化性能。这项工作不仅证明了地球上丰富的2D MOF可以作为一个多功能和有效的平台，支持金属硫化物在没有贵金属共催化剂的情况下提高其光催化h- 2生产性能，而且为设计和合成基于2D MOF的异质结构铺平了道路，用于催化和电子应用。
2D metal organic frameworks (MOF) have received tremendous attention due to their organic-inorganic hybrid nature, large surface area, highly exposed active sites, and ultrathin thickness. However, the application of 2D MOF in light-to-hydrogen (H-2) conversion is rarely reported. Here, a novel 2D MOF [Ni(phen)(oba)](n)center dot 0.5nH(2)O (phen = 1,10-phenanthroline, oba = 4,4 '-oxybis(benzoate)) is for the first time employed as a general, high-performance, and earth-abundant platform to support CdS or Zn0.8Cd0.2S for achieving tremendously improved visible-light-induced H-2-production activity. Particularly, the CdS-loaded 2D MOF exhibits an excellent H-2-production activity of 45 201 mu mol h(-1) g(-1), even exceeding that of Pt-loaded CdS by 185%. Advanced characterizations, e.g., synchrotron-based X-ray absorption near edge structure, and theoretical calculations disclose that the interactive nature between 2D MOF and CdS, combined with the high surface area, abundant reactive centers, and favorable band structure of 2D MOFs, synergistically contribute to this distinguished photocatalytic performance. The work not only demonstrates that the earth-abundant 2D MOF can serve as a versatile and effective platform supporting metal sulfides to boost their photocatalytic H-2-production performance without noble-metal co-catalysts, but also paves avenues to the design and synthesis of 2D-MOF-based heterostructures for catalysis and electronics applications.