Boron nitride quantum dots decorated ultrathin porous g-C3N4: Intensified exciton dissociation and charge transfer for promoting visible-light-driven molecular oxygen activation

[Display omitted] •A novel photocatalyst constructed by BNQDs and UPCN was prepared.•Intensified exciton dissociation and charge transfer across BNQDs/UPCN heterostructure.•Higher photocatalytic efficiency toward molecular oxygen activation under visible light.•Mechanisms of enhanced photocatalytic...

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Published inApplied catalysis. B, Environmental Vol. 245; pp. 87 - 99
Main Authors Yang, Yang, Zhang, Chen, Huang, Danlian, Zeng, Guangming, Huang, Jinhui, Lai, Cui, Zhou, Chengyun, Wang, Wenjun, Guo, Hai, Xue, Wenjing, Deng, Rui, Cheng, Min, Xiong, Weiping
Format Journal Article
LanguageEnglish
Published Amsterdam Elsevier B.V 15.05.2019
Elsevier BV
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Abstract [Display omitted] •A novel photocatalyst constructed by BNQDs and UPCN was prepared.•Intensified exciton dissociation and charge transfer across BNQDs/UPCN heterostructure.•Higher photocatalytic efficiency toward molecular oxygen activation under visible light.•Mechanisms of enhanced photocatalytic activities were proposed. Graphitic carbon nitride (g-C3N4) has enormous potential for photocatalysis, but only possesses moderate activity because of excitonic effects and sluggish charge transfer. Herein, metal-free heterostructure photocatalyst constructed by boron nitride quantum dots (BNQDs) and ultrathin porous g-C3N4 (UPCN) was successfully developed for overcoming these defects. Results showed that the BNQDs loaded UPCN can simultaneously promote the dissociation of excitons and accelerate the transfer of charges owing to the negatively charged functional groups on the surface of BNQDs as well as the ultrathin and porous nanostructure of g-C3N4. Benefiting from the intensified exciton dissociation and charge transfer, the BNQDs/UPCN (BU) photocatalyst presented superior visible-light-driven molecular oxygen activation ability, such as superoxide radical (O2−) generation and hydrogen peroxide (H2O2) production. The average O2− generation rate of the optimal sample (BU-3) was estimated to be 0.25 μmol L−1 min−1, which was about 2.3 and 1.6 times than that of bulk g-C3N4 and UPCN. Moreover, the H2O2 production by BU-3 was also higher than that of bulk g-C3N4 (22.77 μmol L−1) and UPCN (36.13 μmol L−1), and reached 72.30 μmol L−1 over 60 min. This work reveals how rational combination of g-C3N4 with BNQDs can endow it with improved photocatalytic activity for molecular oxygen activation, and provides a novel metal-free and highly efficient photocatalyst for environmental remediation and energy conversion.
AbstractList [Display omitted] •A novel photocatalyst constructed by BNQDs and UPCN was prepared.•Intensified exciton dissociation and charge transfer across BNQDs/UPCN heterostructure.•Higher photocatalytic efficiency toward molecular oxygen activation under visible light.•Mechanisms of enhanced photocatalytic activities were proposed. Graphitic carbon nitride (g-C3N4) has enormous potential for photocatalysis, but only possesses moderate activity because of excitonic effects and sluggish charge transfer. Herein, metal-free heterostructure photocatalyst constructed by boron nitride quantum dots (BNQDs) and ultrathin porous g-C3N4 (UPCN) was successfully developed for overcoming these defects. Results showed that the BNQDs loaded UPCN can simultaneously promote the dissociation of excitons and accelerate the transfer of charges owing to the negatively charged functional groups on the surface of BNQDs as well as the ultrathin and porous nanostructure of g-C3N4. Benefiting from the intensified exciton dissociation and charge transfer, the BNQDs/UPCN (BU) photocatalyst presented superior visible-light-driven molecular oxygen activation ability, such as superoxide radical (O2−) generation and hydrogen peroxide (H2O2) production. The average O2− generation rate of the optimal sample (BU-3) was estimated to be 0.25 μmol L−1 min−1, which was about 2.3 and 1.6 times than that of bulk g-C3N4 and UPCN. Moreover, the H2O2 production by BU-3 was also higher than that of bulk g-C3N4 (22.77 μmol L−1) and UPCN (36.13 μmol L−1), and reached 72.30 μmol L−1 over 60 min. This work reveals how rational combination of g-C3N4 with BNQDs can endow it with improved photocatalytic activity for molecular oxygen activation, and provides a novel metal-free and highly efficient photocatalyst for environmental remediation and energy conversion.
Graphitic carbon nitride (g-C3N4) has enormous potential for photocatalysis, but only possesses moderate activity because of excitonic effects and sluggish charge transfer. Herein, metal-free heterostructure photocatalyst constructed by boron nitride quantum dots (BNQDs) and ultrathin porous g-C3N4 (UPCN) was successfully developed for overcoming these defects. Results showed that the BNQDs loaded UPCN can simultaneously promote the dissociation of excitons and accelerate the transfer of charges owing to the negatively charged functional groups on the surface of BNQDs as well as the ultrathin and porous nanostructure of g-C3N4. Benefiting from the intensified exciton dissociation and charge transfer, the BNQDs/UPCN (BU) photocatalyst presented superior visible-light-driven molecular oxygen activation ability, such as superoxide radical (O2−) generation and hydrogen peroxide (H2O2) production. The average O2− generation rate of the optimal sample (BU-3) was estimated to be 0.25 μmol L−1 min−1, which was about 2.3 and 1.6 times than that of bulk g-C3N4 and UPCN. Moreover, the H2O2 production by BU-3 was also higher than that of bulk g-C3N4 (22.77 μmol L−1) and UPCN (36.13 μmol L−1), and reached 72.30 μmol L−1 over 60 min. This work reveals how rational combination of g-C3N4 with BNQDs can endow it with improved photocatalytic activity for molecular oxygen activation, and provides a novel metal-free and highly efficient photocatalyst for environmental remediation and energy conversion.
Author Huang, Danlian
Zhang, Chen
Huang, Jinhui
Deng, Rui
Guo, Hai
Wang, Wenjun
Xue, Wenjing
Yang, Yang
Cheng, Min
Xiong, Weiping
Lai, Cui
Zeng, Guangming
Zhou, Chengyun
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  surname: Yang
  fullname: Yang, Yang
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 2
  givenname: Chen
  orcidid: 0000-0002-3579-6980
  surname: Zhang
  fullname: Zhang, Chen
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 3
  givenname: Danlian
  surname: Huang
  fullname: Huang, Danlian
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 4
  givenname: Guangming
  orcidid: 0000-0002-4230-7647
  surname: Zeng
  fullname: Zeng, Guangming
  email: zgming@hnu.edu.cn
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 5
  givenname: Jinhui
  surname: Huang
  fullname: Huang, Jinhui
  email: jinhui@hnu.edu.cn
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 6
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  surname: Lai
  fullname: Lai, Cui
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 7
  givenname: Chengyun
  surname: Zhou
  fullname: Zhou, Chengyun
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 8
  givenname: Wenjun
  surname: Wang
  fullname: Wang, Wenjun
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 9
  givenname: Hai
  surname: Guo
  fullname: Guo, Hai
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 10
  givenname: Wenjing
  surname: Xue
  fullname: Xue, Wenjing
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
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  surname: Deng
  fullname: Deng, Rui
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 12
  givenname: Min
  surname: Cheng
  fullname: Cheng, Min
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
– sequence: 13
  givenname: Weiping
  surname: Xiong
  fullname: Xiong, Weiping
  organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China
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Boron nitride quantum dots
H2O2 production
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SSID ssj0002328
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Snippet [Display omitted] •A novel photocatalyst constructed by BNQDs and UPCN was prepared.•Intensified exciton dissociation and charge transfer across BNQDs/UPCN...
Graphitic carbon nitride (g-C3N4) has enormous potential for photocatalysis, but only possesses moderate activity because of excitonic effects and sluggish...
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StartPage 87
SubjectTerms Activation
Boron
Boron nitride
Boron nitride quantum dots
Carbon nitride
Catalytic activity
Charge transfer
Energy conversion
Environmental cleanup
Exciton dissociation
Excitons
Functional groups
H2O2 production
Heterostructures
Hydrogen peroxide
Oxygen
Photocatalysis
Photocatalysts
Photocatalytic molecular oxygen activation
Quantum dots
Superoxide
Ultrathin porous g-C3N4
Title Boron nitride quantum dots decorated ultrathin porous g-C3N4: Intensified exciton dissociation and charge transfer for promoting visible-light-driven molecular oxygen activation
URI https://dx.doi.org/10.1016/j.apcatb.2018.12.049
https://www.proquest.com/docview/2230286105
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