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Visible‐Light‐Responsive 2D Cadmium–Organic Framework Single Crystals with Dual Functions of Water Reduction and Oxidation
Advanced Materials ( IF 27.4 ) Pub Date : 2018-09-17 , DOI: 10.1002/adma.201803401
Yejun Xiao 1, 2 , Yu Qi 1 , Xiuli Wang 1 , Xiaoyu Wang 3 , Fuxiang Zhang 1 , Can Li 1
Affiliation  

The development of new metal–organic frameworks (MOFs) with dual functions of both water reduction and oxidation under visible‐light irradiation is highly desirable for promising solar water splitting, but is not yet reported. Herein, a cadmium‐based MOF (denoted as “Cd‐TBAPy”) single crystal with a 2D layered framework by employing 1,3,6,8‐tetrakis(p‐benzoic acid)pyrene (H4TBAPy) as an organic linker is reported, which exhibits good visible‐light absorption with edge of ≈600 nm. The Mott–Schottky (M–S) measurement and UV–vis analysis integrally reveal that the Cd‐TBAPy is an n‐type semiconductor with a bandgap of ≈2.15 eV whose conduction and valence band are estimated to be −0.05 and 2.10 eV, respectively. Together with loading of Pt or CoPi cocatalyst, the Cd‐TBAPy is active for both water reduction and oxidation in the presence of scavengers under visible‐light irradiation. Especially, the optimized apparent quantum efficiency for O2 evolution reaches 5.6% at 420 nm, much higher than that of previous MOF‐based photocatalysts reported so far. This is thought to be the first MOF that functions as a photocatalyst for both water reduction and oxidation under visible light, demonstrating the intriguing future of MOF materials in solar‐to‐chemical energy conversion.

中文翻译:

具有减水和氧化双重功能的可见光响应二维镉有机骨架单晶

新型的有机金属框架(MOF)具有可见光照射下的减水和氧化双重功能,这对于有希望的太阳能水分解是非常需要的,但尚未见报道。在此,通过使用1,3,6,8-四(对苯甲酸)py(H 4TBAPy)作为有机连接物,据报道它具有良好的可见光吸收,边缘约为600 nm。莫特-肖特基(M-S)测量和紫外可见分析表明,Cd-TBAPy是一种n型半导体,带隙约为2.15 eV,其导带和价带估计为-0.05和2.10 eV,分别。与负载Pt或CoPi助催化剂一起,Cd-TBAPy在可见光照射下,在存在清除剂的情况下,既能减少水分,又能氧化。特别是O 2的最佳表观量子效率在420 nm处演化达到5.6%,远高于迄今为止报道的基于MOF的光催化剂。这被认为是第一个在可见光下同时用作水还原和氧化的光催化剂的MOF,这证明了MOF材料在太阳能转化为化学能方面的迷人前景。
更新日期:2018-09-17
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