In-situ implantation of plasmonic Ag into metal-organic frameworks for constructing efficient Ag/NH2-MIL-125/TiO2 photoanode
In-situ implantation of plasmonic Ag into metal-organic frameworks for constructing efficient Ag/NH2-MIL-125/TiO2 photoanode
复制标题
将等离子体Ag原位注入金属有机框架中构建高效Ag/NH2-MIL-125/TiO2光电阳极
DOI：
10.1016/j.cej.2020.124206
复制
发表时间：
2020-05-15
影响因子：
15.1
通讯作者：
Shi, Weidong
中科院分区：
文献类型：
--
作者：
Cui, Weicheng;Shang, Jianpeng;Shi, Weidong
由于TiO2光响应能力弱，电导率差，实现高效的光电化学水分解催化活性已成为制备TiO2光阳极的关键挑战。我们首次制备了以NH2-MIL-125薄膜装饰的TiO2纳米棒，并利用胺基的温和还原过程将银纳米粒子（Ag NPs）原位植入到NH2-MIL-125薄膜中。NH2-MIL-125和Ag NPs之间的协同效应旨在有效提高光阳极的光响应和整体电导率。系统地研究了制备的Ag/NH2-MIL-125/TiO2混合光阳极的PEC性能。优化后的Ag/NH2-MIL-125/TiO2在1.23 V （vs. RHE）光照（100 mW/cm(2)）下的光电流密度达到1.06 mA/cm(2)，几乎是原始TiO2的4.42倍。在390 nm处，Ag/NH2-MIL-125/TiO2的入射光子电子转换效率（IPCE）值提高到51.0%。此外，还获得了理想的电荷注入效率（.injection）为96.4%，电荷分离效率（eta）为33.1%。在NH2-MIL-125/TiO2异质结构中原位引入Ag NPs为理解金属和MOF在PEC水分解中的协同效应提供了一个新的模型。
Realizing a highly efficient catalytic activity for photoelectrochemical (PEC) water splitting has been becoming a key challenge for fabricating TiO2 photoanode, due to its weak light-response ability and poor electrical conductivity. For the first time, we prepared the TiO2 nanorods decorated with NH2-MIL-125 film, and subsequently in-situ implanted Ag nanoparticles (Ag NPs) into NH2-MIL-125 film by mild reduction process with the help of amine group. The synergistic effect between NH2-MIL-125 and Ag NPs is aimed at efficiently improving light-response and the overall conductivity of photoanode. The PEC performance of as-prepared Ag/NH2-MIL-125/TiO2 hybrid-photoanode has been systemically investigated. The photocurrent density of optimal Ag/NH2-MIL-125/TiO2 has reached 1.06 mA/cm(2) at 1.23 V (vs. RHE) under illumination (100 mW/cm(2)), which is almost 4.42 times higher than that of pristine TiO2. The incident photon-to-electron conversion efficiency (IPCE) value of Ag/NH2-MIL-125/TiO2 has been increased to 51.0% at 390 nm. Furthermore, the desirable charge injection (.injection) of 96.4% and charge separation (eta(separation)) efficiency of 33.1% have been achieved. The in-situ introduction of Ag NPs into NH2-MIL-125/TiO2 heterostructure provides a novel model for understanding the synergistic effect between metal and MOF over PEC water splitting.