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Conformal coating of ultrathin metal-organic framework on semiconductor electrode for boosted photoelectrochemical water oxidation
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2018-05-21 , DOI: 10.1016/j.apcatb.2018.05.059
Yu-Jie Dong , Jin-Feng Liao , Zi-Cheng Kong , Yang-Fan Xu , Ze-Jie Chen , Hong-Yan Chen , Dai-Bin Kuang , Dieter Fenske , Cheng-Yong Su

Exploring efficient photocatalysts for water oxidation is highly demanded because of their significant role in artificial photosynthesis. The research of metal-organic frameworks (MOFs) based photoelectrochemical (PEC) water splitting is promising but still in its infancy due to the challenge to fabricate high-quality MOFs photoelectrode. Here an Fe2O3/Fe-based MOF core/shell nanorod is prepared for efficient PEC water oxidation via a facile surfactant-assisted solvothermal method. With polyvinylpyrrolidone (PVP) molecules as intermedia, an ultrathin MOF shell of several nanometers thick can be controllably grown on the surface of Fe2O3 nanorod. Charge dynamical behaviors study by ultrafast transient absorption spectroscopy (TAS) and photoelectrochemical impedance spectroscopy (PEIS), reveal that the ultrathin MOF shell is crucial to promote the charge separation by providing a cascade band level, but also accelerate the hole injection efficiency via exposing more accessible Fe-oxo cluster active sites. Accompanied with good visible-light response, the Ti-doped Fe2O3/NH2-MIL-101(Fe) photoanode delivers a boosted photocurrent density of 2.27 mA cm−2 at 1.23 V vs. RHE, which is about 2.3 folds of that of pristine Fe2O3. This study provides new insights into the rational design of semiconductor/MOFs hybrid materials for photo/photoelectrochemical catalysis.



中文翻译:

半导体电极上超薄金属有机骨架的共形涂层,用于促进光电化学水氧化

由于其在人工光合作用中的重要作用,因此迫切需要探索有效的水氧化光催化剂。基于金属有机骨架(MOFs)的光电化学(PEC)水分解的研究是有前途的,但由于制造高质量MOFs光电极的挑战,该研究仍处于起步阶段。在此,通过一种简便的表面活性剂辅助溶剂热法制备了基于Fe 2 O 3 / Fe的MOF核/壳纳米棒,用于高效PEC水氧化。以聚乙烯吡咯烷酮(PVP)分子为中介,可以在Fe 2 O 3的表面上可控地生长几纳米厚的超薄MOF壳。纳米棒。通过超快速瞬态吸收光谱(TAS)和光电化学阻抗谱(PEIS)进行的电荷动力学行为研究表明,超薄MOF壳对于通过提供级联能级来促进电荷分离至关重要,而且通过暴露更多的电荷来提高空穴注入效率可访问的Fe-oxo群集活动站点。具有良好的可见光响应的陪同下,钛掺杂的Fe 2 ö 3 / NH 2 -MIL-101(Fe)的光电阳极提供的2.27毫安厘米升压光电流密度-2在的1.23V相对于RHE,这大约是2.3倍原始Fe 2 O 3的。这项研究为光/光电化学催化的半导体/ MOFs混合材料的合理设计提供了新的见识。

更新日期:2018-05-21
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