Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 32, Issue 30, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202202571
Keywords
adsorption energy of water; coordination bond connected MOFs; MXene; efficient electrons transfer; PAW method; solar water splitting
Categories
Funding
- National Natural Science Foundation of China [52071171, 22101105]
- Liaoning Revitalization Talents Program -Pan Deng Scholars [XLYC1802005]
- Liaoning BaiQianWan Talents Program [LNBQW2018B0048]
- Natural Science Fund of Liaoning Province for Excellent Young Scholars [2019-YQ-04]
- Key Project of Scientific Research of the Education Department of Liaoning Province [LZD201902]
- Department of Education of Liaoning Province [LQN201903, LQN202008]
- Foundation for Young Scholars of Liaoning University [LDQN2019007]
- Shenyang Science and Technology Project [21-108-904]
- Research Fund for the Doctoral Program of Liaoning Province [2021-BS-086]
- Jinan 5150 Talent Plan,Excellent Young Scientists Fund Program (Oversea) of Shandong Province
- Australian Research Council (ARC) [FT210100298, DP220100603, LP210200504]
- Kick-Start Project
- Victorian Government through Study Melbourne
- University of Calgary's Canada First Research Excellence Fund program
- Global Research Initiative for Sustainable Low-Carbon Unconventional Resources
- CSIRO Energy Centre
- Australian Research Council [LP210200504] Funding Source: Australian Research Council
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Metal organic frameworks (MOFs) are widely used as photocatalysts, but carrier recombination limits their activity. In this study, carboxyl groups on MXene were used to coordinate with UiO-66-NH2(Zr/Ti) (UZT) and create a tightly connected UiO-66-NH2(Zr/Ti)/carboxyl-functionalized MXene (UZT/CFMX) heterostructure. This unique heterostructure showed efficient solar-driven photocatalytic performance for water splitting, with a hydrogen evolution rate much higher than other MOF-based photocatalysts.
Metal organic frameworks (MOFs) have attracted great interest in photocatalysis, but their activity is hampered by the issue of severe carrier recombination. Here, through a carboxyl group assisted coordination route, MXene decorated with carboxyl groups provides chelation sites enabling coordination with UiO-66-NH2(Zr/Ti) (UZT) to fabricate a tightly connected UiO-66-NH2(Zr/Ti)/carboxyl-functionalized MXene (UZT/CFMX) heterostructure. This is the first instance of direct chemical bonding of MOFs-involved heterostructure via a coordination bond. The critical role of decorated carboxyl groups can be determined so that 1) these can help to establish a strong coordination bond between two materials; 2) act as bridge to promote the electrons transfer from MOFs to MXene, thus relieving carrier recombination, and 3) most interestingly, the carbon atom on the carboxyl group forms a bond with the oxygen from water stimulating the water to dissociate into OH* and H*, thus adding additional reaction pathways for promoting photocatalytic water splitting. Accordingly, the resulting UZT/CFMX shows efficient solar-driven photocatalytic performance for water splitting. The H-2 evolution rate is as high as 2187 mu mol g(-1) h(-1), 20 times higher than that of UZT and 4 times higher than that of UiO-66-NH2 (Zr/Ti)/MXene (UZT/MX), also surpassing the majority of reported MOF-based photocatalysts.
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