Journal
ADVANCED MATERIALS
Volume 32, Issue 33, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202003082
Keywords
benzene oxidation; carbon nitride; charge transfer dynamics; Cu single atoms; hydrogen evolution reactions
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Funding
- National Key RAMP
- D Program of China [2018YFE0201704, 2016YFA0200602, 2018YFA0208702]
- National Natural Science Foundation of China [21631004, 21771061, 21573211, 21633007]
- Training Program of the Major Research Plan of the National Natural Science Foundation of China [91961111]
- Anhui Initiative in Quantum Information Technologies [AHY090200]
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Establishing highly effective charge transfer channels in carbon nitride (C3N4) for enhancing its photocatalytic activity is still a challenging issue. Herein, for the first time, the engineering of C(3)N(4)layers with single-atom Cu bonded with compositional N (Cu-N-x) is demonstrated to address this challenge. The Cu-N(x)is formed by intercalation of chlorophyll sodium copper salt into a melamine-based supramolecular precursor followed by controlled pyrolysis. Two groups of Cu-N(x)are identified: in one group each of Cu atoms is bonded with three in-plane N atoms, while in the other group each of Cu atoms is bonded with four N atoms of two neighboring C(3)N(4)layers, thus forming both in-plane and interlayer charge transfer channels. Importantly, ultrafast spectroscopy has further proved that Cu-N(x)can greatly improve in-plane and interlayer separation/transfer of charge carriers and in turn boost the photocatalytic efficiency. Consequently, the catalyst exhibits a superior visible-light photocatalytic hydrogen production rate (approximate to 212 mu mol h(-1)/0.02 g catalyst), 30 times higher than that of bulk C3N4. Moreover, it leads to an outstanding conversion rate (92.3%) and selectivity (99.9%) for the oxidation of benzene under visible light.
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