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.
| Language | English |
|---|---|
| Pages | 9468-9477 |
| Number of pages | 10 |
| Journal | ACS Applied Materials and Interfaces |
| Volume | 10 |
| Issue number | 11 |
| DOIs | |
| Publication status | Published - 21 Mar 2018 |
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Keywords
- visible-light H₂ production
- C₃N₄ NTs
- Ag−Cu bimetallic nanoparticles
- sacrificial reagents
- monoelectronic oxidation
Cite this
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Bimetallic Ag-Cu supported on graphitic carbon nitride nanotubes for improved visible-light Photocatalytic hydrogen roduction. / Zhu, Yuxiang; Marianov, Aleksei; Xu, Haimei; Lang, Candace; Jiang, Yijiao.
In: ACS Applied Materials and Interfaces, Vol. 10, No. 11, 21.03.2018, p. 9468-9477.Research output: Contribution to journal › Article › Research › peer-review
TY - JOUR
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
UR - http://www.scopus.com/inward/record.url?scp=85044186916&partnerID=8YFLogxK
UR - http://purl.org/au-research/grants/arc/DE120100329
UR - http://purl.org/au-research/grants/arc/DP140102432
U2 - 10.1021/acsami.8b00393
DO - 10.1021/acsami.8b00393
M3 - Article
VL - 10
SP - 9468
EP - 9477
JO - ACS Applied Materials and Interfaces
T2 - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
SN - 1944-8244
IS - 11
ER -