Elucidating Charge Separation Dynamics in a Hybrid Metal-Organic Framework Photocatalyst for Light-Driven H2 Evolution

被引：54
作者：
Yang, Sizhuo [1 ]
Fan, Donghua [2 ]
Hu, Wenhui [1 ]
Pattengale, Brian [1 ]
Liu, Cunming [3 ]
Zhang, Xiaoyi [3 ]
Huang, Jier [1 ]
机构：
[1] Marquette Univ, Dept Chem, Milwaukee, WI 53201 USA
[2] Wuyi Univ, Sch Appl Phys & Mat, Jiangmen 529020, Peoples R China
[3] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60349 USA
来源：
JOURNAL OF PHYSICAL CHEMISTRY C | 2018年 / 122卷 / 06期
基金：
美国国家科学基金会;
关键词：
POROUS COORDINATION POLYMERS; CARBON-DIOXIDE REDUCTION; VISIBLE-LIGHT; HYDROGEN-PRODUCTION; ENERGY-TRANSFER; ARTIFICIAL PHOTOSYNTHESIS; WATER; CATALYST; NANOCRYSTALS; GENERATION;
D O I：
10.1021/acs.jpcc.8b00471
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
Metal organic frameworks (MOFs) have emerged as novel scaffolds for artificial photosynthesis due to their unique capability in incorporating homogeneous photosensitizer and catalyst to their robust heterogeneous matrix. In this work, we report the charge separation dynamics between molecular Ru-photosensitizer and Pt-catalyst, both of which were successfully incorporated into a Zr-MOF that demonstrates excellent activity and stability for light-driven H2 generation from water. Using optical transient absorption (OTA) spectroscopy, we show that charge separation in this hybrid MOF occurs via electron transfer (ET) from Ru-photosensitizer to Pt-catalyst. Using Pt L-3-edge X-ray transient absorption (XTA) spectroscopy, we observed the intermediate reduced Pt site, directly confirming the formation of charge separated state due to ET from Ru-photosensitizer and unraveling their key roles in photocatalysis.
引用
收藏
页码：3305 / 3311
页数：7
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