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Novel stable metal–organic framework photocatalyst for light-driven hydrogen production†
CrystEngComm ( IF 2.6 ) Pub Date : 2018-05-11 00:00:00 , DOI: 10.1039/c8ce00386f Qi Yu 1, 2, 3, 4, 5 , Hong Dong 1, 2, 3, 4, 5 , Xin Zhang 1, 2, 3, 4, 5 , Ya-Xin Zhu 1, 2, 3, 4, 5 , Jian-Hui Wang 1, 2, 3, 4, 5 , Feng-Ming Zhang 1, 2, 3, 4, 5 , Xiao-Jun Sun 1, 2, 3, 4, 5
CrystEngComm ( IF 2.6 ) Pub Date : 2018-05-11 00:00:00 , DOI: 10.1039/c8ce00386f Qi Yu 1, 2, 3, 4, 5 , Hong Dong 1, 2, 3, 4, 5 , Xin Zhang 1, 2, 3, 4, 5 , Ya-Xin Zhu 1, 2, 3, 4, 5 , Jian-Hui Wang 1, 2, 3, 4, 5 , Feng-Ming Zhang 1, 2, 3, 4, 5 , Xiao-Jun Sun 1, 2, 3, 4, 5
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A novel MOF formulated as [Dy2(abtc)(H2O)2(OH)2]·2H2O (H4abtc = 3,3′,5,5′-azobenzene tetracarboxylic acid) was successfully synthesized, in which a dye-like ligand was integrated as a photosensitizer into MOFs by the reaction with Dy3+ ions (dye-based Dy-MOF). The ultra-stable dye-based Dy-MOF possesses a HOMO–LUMO gap of 2.17 eV as determined by UV-vis spectrum with absorbed edge at 570 nm. The dye-based Dy-MOF shows high catalytic activity for the UV-vis light driven hydrogen production, attributed to the porous structure and light harvesting from the dye-like ligand. The band-edge positions of the crystals of the dye-based Dy-MOF were studied via cyclic voltammetry (CV) to further verify the principle of photocatalytic hydrogen production. Furthermore, the exceptional thermal and pH stability of the dye-based Dy-MOF makes it possible to use them as photocatalysts in water. On using Pt cocatalyst, the UV-vis light photocatalytic hydrogen evolution rate of the dye-based Dy-MOF reaches 21.53 μmol h−1 g−1. In addition, the as-prepared dye-based Dy-MOF materials also exhibited good stability and recycling performance.
中文翻译：
新型稳定的金属-有机骨架光催化剂，用于光驱动制氢†
成功地合成了一种新型的MOF，其配方为[Dy 2（abtc）（H 2 O）2（OH）2 ]·2H 2 O（H 4 abtc = 3,3'，5,5'-偶氮苯四羧酸），通过与Dy 3+离子（基于染料的Dy-MOF）反应，将染料样配体作为光敏剂整合到MOF中。超稳定染料基Dy-MOF的HOMO-LUMO间隙为2.17 eV，这是由紫外可见光谱确定的，吸收边在570 nm。染料基Dy-MOF对紫外可见光驱动的氢气生产显示出高催化活性，这归因于多孔结构和从染料样配体收集的光。研究了染料基Dy-MOF晶体的带边位置通过循环伏安法（CV）进一步验证了光催化制氢的原理。此外，基于染料的Dy-MOF具有出色的热稳定性和pH稳定性，因此可以将它们用作水中的光催化剂。在使用Pt助催化剂时，染料基Dy-MOF的UV-可见光光催化氢释放速率达到21.53μmolh -1 g -1。另外，所制备的基于染料的Dy-MOF材料还表现出良好的稳定性和再循环性能。
更新日期：2018-05-11
中文翻译：
新型稳定的金属-有机骨架光催化剂，用于光驱动制氢†
成功地合成了一种新型的MOF，其配方为[Dy 2（abtc）（H 2 O）2（OH）2 ]·2H 2 O（H 4 abtc = 3,3'，5,5'-偶氮苯四羧酸），通过与Dy 3+离子（基于染料的Dy-MOF）反应，将染料样配体作为光敏剂整合到MOF中。超稳定染料基Dy-MOF的HOMO-LUMO间隙为2.17 eV，这是由紫外可见光谱确定的，吸收边在570 nm。染料基Dy-MOF对紫外可见光驱动的氢气生产显示出高催化活性，这归因于多孔结构和从染料样配体收集的光。研究了染料基Dy-MOF晶体的带边位置通过循环伏安法（CV）进一步验证了光催化制氢的原理。此外，基于染料的Dy-MOF具有出色的热稳定性和pH稳定性，因此可以将它们用作水中的光催化剂。在使用Pt助催化剂时，染料基Dy-MOF的UV-可见光光催化氢释放速率达到21.53μmolh -1 g -1。另外，所制备的基于染料的Dy-MOF材料还表现出良好的稳定性和再循环性能。
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