Bimetallic Ag-Cu supported on graphitic carbon nitride nanotubes for improved visible-light Photocatalytic hydrogen roduction

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Abstract

This work, for the first time, reports visible-light active bare graphitic carbon nitride nanotubes (C3N4 NTs) for photocatalytic hydrogen generation, even in the absence of any cocatalyst. Upon uniform dispersion of the cocatalysts, Ag-Cu nanoparticles, on the well-ordered bare C3N4 NTs, they exhibit twice the H2 evolution rate of the bare C3N4 NTs. The improved activity is attributed to their unique tubular nanostructure, strong metal-support interaction, and efficient photoinduced electron-hole separation compared to their bare and monometallic counterparts, evidenced by complementary characterization techniques. This work reveals that the H2 production rates correlate well with the oxidation potentials of the sacrificial reagents used. Triethylamine (TEA) outperforms other sacrificial reagents, including triethanolamine (TEOA) and methanol. Mechanistic studies on the role of various sacrificial reagents in photocatalytic H2 generation demonstrate that irreversible photodegradation of TEA into diethylamine and acetaldehyde via monoelectronic oxidation contributes to the improved H2 yield. Similarly, TEOA is oxidized to diethanolamine and glycolaldehyde, whereas methanol is unable to quickly capture the photoinduced holes and remains intact due to the low oxidation potential.

LanguageEnglish
Pages9468-9477
Number of pages10
JournalACS Applied Materials and Interfaces
Volume10
Issue number11
DOIs
Publication statusPublished - 21 Mar 2018

Fingerprint

Carbon nitride
Nanotubes
Triethanolamine
Hydrogen
diethanolamine
Oxidation
Methanol
Acetaldehyde
Photodegradation
Nanostructures
Metals
Nanoparticles
Electrons
cyanogen
triethylamine
triethanolamine

Keywords

  • visible-light H₂ production
  • C₃N₄ NTs
  • Ag−Cu bimetallic nanoparticles
  • sacrificial reagents
  • monoelectronic oxidation

Cite this

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title = "Bimetallic Ag-Cu supported on graphitic carbon nitride nanotubes for improved visible-light Photocatalytic hydrogen roduction",
abstract = "This work, for the first time, reports visible-light active bare graphitic carbon nitride nanotubes (C3N4 NTs) for photocatalytic hydrogen generation, even in the absence of any cocatalyst. Upon uniform dispersion of the cocatalysts, Ag-Cu nanoparticles, on the well-ordered bare C3N4 NTs, they exhibit twice the H2 evolution rate of the bare C3N4 NTs. The improved activity is attributed to their unique tubular nanostructure, strong metal-support interaction, and efficient photoinduced electron-hole separation compared to their bare and monometallic counterparts, evidenced by complementary characterization techniques. This work reveals that the H2 production rates correlate well with the oxidation potentials of the sacrificial reagents used. Triethylamine (TEA) outperforms other sacrificial reagents, including triethanolamine (TEOA) and methanol. Mechanistic studies on the role of various sacrificial reagents in photocatalytic H2 generation demonstrate that irreversible photodegradation of TEA into diethylamine and acetaldehyde via monoelectronic oxidation contributes to the improved H2 yield. Similarly, TEOA is oxidized to diethanolamine and glycolaldehyde, whereas methanol is unable to quickly capture the photoinduced holes and remains intact due to the low oxidation potential.",
keywords = "visible-light H₂ production, C₃N₄ NTs, Ag−Cu bimetallic nanoparticles, sacrificial reagents, monoelectronic oxidation",
author = "Yuxiang Zhu and Aleksei Marianov and Haimei Xu and Candace Lang and Yijiao Jiang",
year = "2018",
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doi = "10.1021/acsami.8b00393",
language = "English",
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T1 - Bimetallic Ag-Cu supported on graphitic carbon nitride nanotubes for improved visible-light Photocatalytic hydrogen roduction

AU - Zhu, Yuxiang

AU - Marianov, Aleksei

AU - Xu, Haimei

AU - Lang, Candace

AU - Jiang, Yijiao

PY - 2018/3/21

Y1 - 2018/3/21

N2 - This work, for the first time, reports visible-light active bare graphitic carbon nitride nanotubes (C3N4 NTs) for photocatalytic hydrogen generation, even in the absence of any cocatalyst. Upon uniform dispersion of the cocatalysts, Ag-Cu nanoparticles, on the well-ordered bare C3N4 NTs, they exhibit twice the H2 evolution rate of the bare C3N4 NTs. The improved activity is attributed to their unique tubular nanostructure, strong metal-support interaction, and efficient photoinduced electron-hole separation compared to their bare and monometallic counterparts, evidenced by complementary characterization techniques. This work reveals that the H2 production rates correlate well with the oxidation potentials of the sacrificial reagents used. Triethylamine (TEA) outperforms other sacrificial reagents, including triethanolamine (TEOA) and methanol. Mechanistic studies on the role of various sacrificial reagents in photocatalytic H2 generation demonstrate that irreversible photodegradation of TEA into diethylamine and acetaldehyde via monoelectronic oxidation contributes to the improved H2 yield. Similarly, TEOA is oxidized to diethanolamine and glycolaldehyde, whereas methanol is unable to quickly capture the photoinduced holes and remains intact due to the low oxidation potential.

AB - This work, for the first time, reports visible-light active bare graphitic carbon nitride nanotubes (C3N4 NTs) for photocatalytic hydrogen generation, even in the absence of any cocatalyst. Upon uniform dispersion of the cocatalysts, Ag-Cu nanoparticles, on the well-ordered bare C3N4 NTs, they exhibit twice the H2 evolution rate of the bare C3N4 NTs. The improved activity is attributed to their unique tubular nanostructure, strong metal-support interaction, and efficient photoinduced electron-hole separation compared to their bare and monometallic counterparts, evidenced by complementary characterization techniques. This work reveals that the H2 production rates correlate well with the oxidation potentials of the sacrificial reagents used. Triethylamine (TEA) outperforms other sacrificial reagents, including triethanolamine (TEOA) and methanol. Mechanistic studies on the role of various sacrificial reagents in photocatalytic H2 generation demonstrate that irreversible photodegradation of TEA into diethylamine and acetaldehyde via monoelectronic oxidation contributes to the improved H2 yield. Similarly, TEOA is oxidized to diethanolamine and glycolaldehyde, whereas methanol is unable to quickly capture the photoinduced holes and remains intact due to the low oxidation potential.

KW - visible-light H₂ production

KW - C₃N₄ NTs

KW - Ag−Cu bimetallic nanoparticles

KW - sacrificial reagents

KW - monoelectronic oxidation

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