期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 24, 页码 7681-7686出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b03472
关键词
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资金
- National Science Foundation [DMR-1263006, NSF- SEP-1229089]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, through Argonne National Laboratory [DE-AC02-06CH11357]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1229089, 1263006, 1230217] Funding Source: National Science Foundation
Developing highly efficient photocatalyts for water splitting is one of the grand challenges in solar energy conversion. Here, we report the rational design and synthesis of porous conjugated polymer (PCP) that photocatalytically generates hydrogen from water splitting. The design mimics natural photosynthetics systems with conjugated polymer component to harvest photons and the transition metal part to facilitate catalytic activities. A series of PCPs have been synthesized with different light harvesting chromophores and transition metal binding bipyridyl (bpy) sites. The photocatalytic activity of these bpy-containing PCPs can be greatly enhanced due to the improved light absorption, better wettability, local ordering structure, and the improved charge separation process. The PCP made of strong and fully conjugated donor chromophore DBD (M-4) shows the highest hydrogen production rate at similar to 33 itmol/h. The results indicate that copolymerization between a strong electron donor and weak electron acceptor into the same polymer chain is a useful strategy for developing efficient photocatalysts. This study also reveals that the residual palladium in the PCP networks plays a key role for the catalytic performance. The hydrogen generation activity of PCP photocatalyst can be further enhanced to 164 mu mol/h with an apparent quantum yield of 1.8% at 350 nm by loading 2 wt % of extra platinum co catalyst.
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