2017
DOI: 10.1021/acs.jpca.7b04594
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Mechanism of Photocatalytic Water Splitting with Graphitic Carbon Nitride: Photochemistry of the Heptazine–Water Complex

Abstract: Impressive progress has recently been achieved in photocatalytic hydrogen evolution with polymeric carbon nitride materials consisting of heptazine building blocks. However, the fundamental mechanistic principles of the catalytic cycle are as yet poorly understood. Here, we provide first-principles computational evidence that water splitting with heptazine-based materials can be understood as a molecular excited-state reaction taking place in hydrogen-bonded heptazine-water complexes. The oxidation of water oc… Show more

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Cited by 92 publications
(198 citation statements)
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“…The low‐lying 2 ππ*, 2 nπ* and 2 πσ* excited states have very small oscillator strengths, but can borrow intensity from higher‐lying bright states by vibronic coupling. The bright 2 ππ* excited states of the radicals are slightly higher in energy than the corresponding bright 1 ππ* states of pyridine, triazine and heptazine ,,…”
Section: Photodissociation Of Heterocyclic Radicalsmentioning
confidence: 85%
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“…The low‐lying 2 ππ*, 2 nπ* and 2 πσ* excited states have very small oscillator strengths, but can borrow intensity from higher‐lying bright states by vibronic coupling. The bright 2 ππ* excited states of the radicals are slightly higher in energy than the corresponding bright 1 ππ* states of pyridine, triazine and heptazine ,,…”
Section: Photodissociation Of Heterocyclic Radicalsmentioning
confidence: 85%
“…In pyridinyl and triazinyl, the reactive 2 πσ* state is the second lowest state, while it is the third lowest state in heptazinyl. The vertical excitation energies of the 2 πσ* state are 2.05 eV, 2.85 eV and 3.21 eV for pyridinyl, triazinyl and heptazinyl, respectively, at the UADC(2)/aug‐cc‐pVDZ level ,,. All three radicals exhibit a dense spectrum of 2 ππ* and 2 nπ* excited states above 3.0 eV.…”
Section: Photodissociation Of Heterocyclic Radicalsmentioning
confidence: 97%
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