Two types of cooperative nitrogen vacancies in polymeric carbon nitride for efficient solar-driven H2O2 evolution

Xie, You; Li, Yunxiang; Huang, Zhaohui; Zhang, Junying; Jia, Xiaofang; Wang, Xu‐Sheng; Ye, Jinhua

doi:10.1016/j.apcatb.2019.118581

Cited by 128 publications

(66 citation statements)

References 38 publications

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“…Then CN(V1 + V2) was prepared by introducing the third MS into CN(V1), which also has three MSs in CKCN-0.03 with the same content. By comparing the properties of CKCN-0.03, CN (V1) and CN(V1 + V2) experimentally, the speci c role of each site was con rmed, respectively 15 . Similarly, Dong and his co-workers also used the controlled variable method to study the role of each MS experimentally 17 .…”

Section: Introductionmentioning

confidence: 99%

“…Photocatalytic H 2 O 2 production through the O 2 two-electron reduction process (O 2 + 2H + + 2e − → H 2 O 2 ) has attracted wide attention 4,5 . With the continuous efforts of researchers, a large number of photocatalysts for H 2 O 2 evolution have been developed [6][7][8][9][10][11][12][13][14][15][16][17][18] . Among them, photocatalysts with multiple modi cation sites (MSs) exhibited more superior performance as compared to their catalytically inaccessible counterparts of single sites materials [14][15][16][17] .…”

Section: Introductionmentioning

confidence: 99%

“…With the continuous efforts of researchers, a large number of photocatalysts for H 2 O 2 evolution have been developed [6][7][8][9][10][11][12][13][14][15][16][17][18] . Among them, photocatalysts with multiple modi cation sites (MSs) exhibited more superior performance as compared to their catalytically inaccessible counterparts of single sites materials [14][15][16][17] . Nevertheless, it is worth noting that the same kind of MS exhibited diametrically opposite effects when the other MSs are different in the same primitive material [15][16][17]19 .…”

Section: Introductionmentioning

confidence: 99%

“…Among them, photocatalysts with multiple modi cation sites (MSs) exhibited more superior performance as compared to their catalytically inaccessible counterparts of single sites materials [14][15][16][17] . Nevertheless, it is worth noting that the same kind of MS exhibited diametrically opposite effects when the other MSs are different in the same primitive material [15][16][17]19 . For instance, Shiraishi et al reported that amino group reduced the selectivity of H 2 O 2 in mesoporous graphitic carbon nitride (CN) 19 .…”

Section: Introductionmentioning

confidence: 99%

“…Besides, Zhu et al reported that the cyano group acted as an electron acceptor to promote the photocatalytic H 2 O 2 evolution under the synergistic effect of nitrogen vacancy 16 . However, Xie et al proposed that in the defect CN containing three kinds of MSs, the cyano group has no effect on the formation of H 2 O 2 15 . Different preparation methods led to different coordination environments at the same kind of MS.…”

Section: Introductionmentioning

confidence: 99%

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Unveiling real active site for photocatalytic H2O2 evolution: A combined experimental and DFT-TDDFT study

Luo¹,

Liu²,

Fan³

et al. 2020

Preprint

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Photocatalyst with multiple modification sites (MSs) exhibited better performance than single site in photocatalytic H2O2 evolution, while the corresponding reaction mechanism is more complicated. However, neither experiment nor density functional theory (DFT) based on ground state wavefunction cannot precisely confirm the role of each site in photocatalyst with multiple MSs. Here, we propose a universal method that flexibly combines experiments, DFT and time-dependent DFT (TDDFT) calculations to reveal the photocatalytic mechanism and active site of nitrogen deficiency g-C3N4 (NDCN) containing two MSs (bicoordinated nitrogen vacancy and cyano group). Characterization techniques and control experiments prove that generation of H2O2 on NDCN is a two-step single electron transfer process, and NDCN exhibits enhanced charge separation efficiency and higher selectivity for two-electron oxygen reduction. DFT-TDDFT calculations further indicate that nitrogen vacancy is the real catalytic site for activating O2, which promotes O2 adsorption and continuously formation of •O2−, thus inhibiting electron-hole recombination.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Unveiling real active site for photocatalytic H2O2 evolution: A combined experimental and DFT-TDDFT study

Luo¹,

Liu²,

Fan³

et al. 2020

Preprint

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Synthesis of Leaf‐Vein‐Like g‐C₃N₄ with Tunable Band Structures and Charge Transfer Properties for Selective Photocatalytic H₂O₂ Evolution

Feng

Tang

Deng

et al. 2020

Adv Funct Materials

349

112

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Photocatalytic H 2 O 2 evolution through two-electron oxygen reduction has attracted wide attention as an environmentally friendly strategy compared with the traditional anthraquinone or electrocatalytic method. Herein, a biomimetic leaf-vein-like g-C 3 N 4 as an efficient photocatalyst for H 2 O 2 evolution is reported, which owns tenable band structure, optimized charge transfer, and selective two-electron O 2 reduction. The mechanism for the regulation of band structure and charge transfer is well studied by combining experiments and theoretical calculations. The H 2 O 2 yield of CN4 (287 µmol h −1) is about 3.3 times higher than that of pristine CN (87 µmol h −1), and the apparent quantum yield for H 2 O 2 evolution over CN4 reaches 27.8% at 420 nm, which is much higher than that for many other current photocatalysts. This work not only provides a novel strategy for the design of photocatalyst with excellent H 2 O 2 evolution efficiency, but also promotes deep understanding for the role of defect and doping sites on photocatalytic activity.

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Unraveling the Mechanism on Ultrahigh Efficiency Photocatalytic H₂O₂ Generation for Dual‐Heteroatom Incorporated Polymeric Carbon Nitride

Liu

Wang

Chen

et al. 2022

Adv Funct Materials

128

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Photocatalytic hydrogen peroxide (H 2 O 2 ) production from dioxygen and water is regarded as a promising technology since it can achieve sustainable and green solar-to-chemical energy conversion. Herein, oxygen and potassium dual-heteroatom incorporated polymeric carbon nitride (O/KCN) is rationally designed for H 2 O 2 generation with an ultrahigh rate of 309.44 µM h −1 mg −1 , which surpasses that of other C 3 N 4 -based photocatalysts. The enhanced performance can be ascribed to the effective light absorption, fast charge transfer/separation, strong oxygen adsorption, and highly selective twoelectron oxygen reduction reaction (ORR). Density functional theory calculations further confirm that the obtained O/KCN is more favorable than others for electrons migrating from β spin-orbital to π* orbitals of O 2 molecule, thus optimizing O 2 molecule activation to promote the formation of intermediate species *OOH and decrease the energy barrier of H 2 O 2 production. This work not only provides in-depth insights for the photocatalytic H 2 O 2 generation mechanism, but also lays the foundation for further development of highly active photocatalysts for environmental remediation and energy conversion.

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Two types of cooperative nitrogen vacancies in polymeric carbon nitride for efficient solar-driven H2O2 evolution

Cited by 128 publications

References 38 publications

Unveiling real active site for photocatalytic H2O2 evolution: A combined experimental and DFT-TDDFT study

Unveiling real active site for photocatalytic H2O2 evolution: A combined experimental and DFT-TDDFT study

Synthesis of Leaf‐Vein‐Like g‐C₃N₄ with Tunable Band Structures and Charge Transfer Properties for Selective Photocatalytic H₂O₂ Evolution

Unraveling the Mechanism on Ultrahigh Efficiency Photocatalytic H₂O₂ Generation for Dual‐Heteroatom Incorporated Polymeric Carbon Nitride

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Two types of cooperative nitrogen vacancies in polymeric carbon nitride for efficient solar-driven H2O2 evolution

Cited by 128 publications

References 38 publications

Unveiling real active site for photocatalytic H2O2 evolution: A combined experimental and DFT-TDDFT study

Unveiling real active site for photocatalytic H2O2 evolution: A combined experimental and DFT-TDDFT study

Synthesis of Leaf‐Vein‐Like g‐C3N4 with Tunable Band Structures and Charge Transfer Properties for Selective Photocatalytic H2O2 Evolution

Unraveling the Mechanism on Ultrahigh Efficiency Photocatalytic H2O2 Generation for Dual‐Heteroatom Incorporated Polymeric Carbon Nitride

Contact Info

Product

Resources

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Synthesis of Leaf‐Vein‐Like g‐C₃N₄ with Tunable Band Structures and Charge Transfer Properties for Selective Photocatalytic H₂O₂ Evolution

Unraveling the Mechanism on Ultrahigh Efficiency Photocatalytic H₂O₂ Generation for Dual‐Heteroatom Incorporated Polymeric Carbon Nitride