Local spatial charge separation and proton activation induced by surface hydroxylation promoting photocatalytic hydrogen evolution of polymeric carbon nitride

Shen, Yu; Li, Jieyuan; Zhang, Yihe; Li, Min; Dong, Fan; Zhang, Tierui

doi:10.1016/j.nanoen.2018.05.053

Cited by 247 publications

(145 citation statements)

References 45 publications

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“…Moreover, the peak shifts from 400.0 eV to 399.9 or 399.6 eV due to the increased charge density of nitrogen atom, coinciding with the C 1s spectra. The O 1s spectrum from the pristine carbon nitride shows two distinct signals at 530.1 and 532.40 eV, corresponding to −OH and −C=O bonds . As indicated in Figure c, the peak assigned to −C=O increases in UCN‐AB and UCN‐APy, proving the presence of −O=C−N, which is in line with the results of C 1s and N 1s spectra.…”

Section: Resultssupporting

confidence: 85%

Delocalization of π‐Electron in Graphitic Carbon Nitride to Promote its Photocatalytic Activity for Hydrogen Evolution

Guan

Zhang

2019

ChemCatChem

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Polymers with a large π‐electron conjugated system have aroused extensive concern in photocatalysis due to their appropriate bandgap and high stability. In order to overcome such drawbacks as its inadequate visible light absorption and rapid recombination of the photogenerated electron‐hole pairs of graphic carbon nitride (g‐C3N4), a facile strategy is proposed to tune its electronic structure by grafting small molecules. The conjugated photocatalysts were prepared by attaching 3‐Aminobenzoic acid (AB) and 6‐Aminopyridine‐2‐carboxylic acid (APy) to the framework of g‐C3N4 via low‐temperature condensation. The obtained catalysts UCN‐AB and UCN‐APy possess higher visible light absorption that results from the modified band structure by extending π‐electron delocalization. Additionally, AB and APy worked as the electron acceptors which further enhance transport of the photogenerated electrons. The optimal UCN‐AB and UCN‐APy accomplished remarkable photocatalytic hydrogen evolution rates of 104.0 and 133.2 μmol/h, respectively, which are nearly four or five times of that over g‐C3N4. This work provides a simple and feasible modification approach to extend π‐electron delocalization in g‐C3N4 with a stronger visible light response and accelerated charge transfer for high photocatalytic hydrogen evolution.

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Section: Resultssupporting

confidence: 85%

Delocalization of π‐Electron in Graphitic Carbon Nitride to Promote its Photocatalytic Activity for Hydrogen Evolution

Guan

Zhang

2019

ChemCatChem

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“…The surface polarization with graphitic carbon rings on polymeric carbon nitride (g‐C 3 N 4 ) was demonstrated to transport the photoinduced e − and h + in diverse directions, leading to a 21‐times improvement of H 2 evolution rate . Recently, our group reported that the surface hydroxylation, halogenation and oxygen vacancies (OVs) can serve as efficient polarization strategies for advancing surface charge separation, markedly enhancing the photocatalytic activity for H 2 evolution of g‐C 3 N 4 and CO 2 reduction of Bi 2 O 2 (OH)(NO 3 ) and Sr 2 Bi 2 Nb 2 TiO 12 …”

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Macroscopic Spontaneous Polarization and Surface Oxygen Vacancies Collaboratively Boosting CO₂ Photoreduction on BiOIO₃ Single Crystals

et al. 2020

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Prompt recombination of photogenerated electrons and holes in bulk and on the surface of photocatalysts harshly impedes the photocatalytic efficiency. However, the simultaneous manipulation of photocharges in the two locations is challenging. Herein, the synchronous promotion of bulk and surface separation of photoinduced charges for prominent CO2 photoreduction by coupling macroscopic spontaneous polarization and surface oxygen vacancies (OVs) of BiOIO3 single crystals is reported. The oriented growth of BiOIO3 single‐crystal nanostrips along the [001] direction, ensuing substantial well‐aligned IO3 polar units, renders a large enhancement for the macroscopic polarization electric field, which is capable of driving the rapid separation and migration of charges from bulk to surface. Meanwhile the introduction of surface OVs establishes a local electric field for charge migration to catalytic sites on the surface of BiOIO3 nanostrips. Highly polarized BiOIO3 nanostrips with ample OVs demonstrate outstanding CO2 reduction activity for CO production with a rate of 17.33 µmol g−1 h−1 (approximately ten times enhancement) without any sacrificial agents or cocatalysts, being one of the best CO2 reduction photocatalysts in the gas–solid system reported so far. This work provides an integrated solution to governing charge movement behavior on the basis of collaborative polarization from bulk and surface.

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“…( Figure S14). [25] Electrochemical impedance spectra (EIS) indicate that the interfacial charge transfer of eighteen-faceted BiOCl is faster than that of BiOCl square plates ( Figure S15). [24] In contrast to BiOCl-10 with weak SPV response,BiOCl-100 shows very strong SPV signal around 340 nm (Figure 2c), indicating the concentration of charge carriers in eighteenfaceted BiOCl is much higher than that in BiOCl square plates.…”

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Unprecedented Eighteen‐Faceted BiOCl with a Ternary Facet Junction Boosting Cascade Charge Flow and Photo‐redox

et al. 2019

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Local spatial charge separation and proton activation induced by surface hydroxylation promoting photocatalytic hydrogen evolution of polymeric carbon nitride

Cited by 247 publications

References 45 publications

Delocalization of π‐Electron in Graphitic Carbon Nitride to Promote its Photocatalytic Activity for Hydrogen Evolution

Delocalization of π‐Electron in Graphitic Carbon Nitride to Promote its Photocatalytic Activity for Hydrogen Evolution

Macroscopic Spontaneous Polarization and Surface Oxygen Vacancies Collaboratively Boosting CO₂ Photoreduction on BiOIO₃ Single Crystals

Unprecedented Eighteen‐Faceted BiOCl with a Ternary Facet Junction Boosting Cascade Charge Flow and Photo‐redox

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Local spatial charge separation and proton activation induced by surface hydroxylation promoting photocatalytic hydrogen evolution of polymeric carbon nitride

Cited by 247 publications

References 45 publications

Delocalization of π‐Electron in Graphitic Carbon Nitride to Promote its Photocatalytic Activity for Hydrogen Evolution

Delocalization of π‐Electron in Graphitic Carbon Nitride to Promote its Photocatalytic Activity for Hydrogen Evolution

Macroscopic Spontaneous Polarization and Surface Oxygen Vacancies Collaboratively Boosting CO2 Photoreduction on BiOIO3 Single Crystals

Unprecedented Eighteen‐Faceted BiOCl with a Ternary Facet Junction Boosting Cascade Charge Flow and Photo‐redox

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Macroscopic Spontaneous Polarization and Surface Oxygen Vacancies Collaboratively Boosting CO₂ Photoreduction on BiOIO₃ Single Crystals