Enhanced Hydrogen Production from Ethanol Photoreforming by Site-Specific Deposition of Au on Cu<sub>2</sub>O/TiO<sub>2</sub> p-n Junction
Hydrogen production by photoreforming of biomass-derived ethanol is a renewable way of obtaining clean fuel. We developed a site-specific deposition strategy to construct supported Au catalysts by rationally constructing Ti<sup>3+</sup> defects inTiO<sub>2</sub> nanorods and...
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doaj-a943762b194845118b2f039ee0972cab2020-11-25T02:33:17ZengMDPI AGCatalysts2073-43442020-05-011053953910.3390/catal10050539Enhanced Hydrogen Production from Ethanol Photoreforming by Site-Specific Deposition of Au on Cu<sub>2</sub>O/TiO<sub>2</sub> p-n JunctionLan Luo0Tingting Zhang1Xin Zhang2Rongping Yun3Yanjun Lin4Bing Zhang5Xu Xiang6State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, 15 Beisanhuan Donglu, Beijing 100029, ChinaState Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, 15 Beisanhuan Donglu, Beijing 100029, ChinaState Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, 15 Beisanhuan Donglu, Beijing 100029, ChinaState Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, 15 Beisanhuan Donglu, Beijing 100029, ChinaState Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, 15 Beisanhuan Donglu, Beijing 100029, ChinaSchool of Chemical Engineering, Zhengzhou University, 100 Science Avenue, Zhengzhou 450001, ChinaState Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, 15 Beisanhuan Donglu, Beijing 100029, ChinaHydrogen production by photoreforming of biomass-derived ethanol is a renewable way of obtaining clean fuel. We developed a site-specific deposition strategy to construct supported Au catalysts by rationally constructing Ti<sup>3+</sup> defects inTiO<sub>2</sub> nanorods and Cu<sub>2</sub>O-TiO<sub>2</sub> p-n junction across the interface of two components. The Au nanoparticles (~2.5 nm) were selectively anchored onto either TiO<sub>2</sub> nanorods (Au@TiO<sub>2</sub>/Cu<sub>2</sub>O) or Cu<sub>2</sub>O nanocubes (Au@Cu<sub>2</sub>O/TiO<sub>2</sub>) or both TiO<sub>2</sub> and Cu<sub>2</sub>O (Au@TiO<sub>2</sub>/Cu<sub>2</sub>O@Au) with the same Au loading. The electronic structure of supported Au species was changed by forming Au@TiO<sub>2</sub> interface due to the adjacent Ti<sup>3+</sup> defects and the associated oxygen vacancies while unchanged in Au@Cu<sub>2</sub>O/TiO<sub>2</sub> catalyst. The p-n junction of TiO<sub>2</sub>/Cu<sub>2</sub>O promoted charge separation and transfer across the junction. During ethanol photoreforming, Au@TiO<sub>2</sub>/Cu<sub>2</sub>O catalyst possessing both the Au@TiO<sub>2</sub> interface and the p-n junction showed the highest H<sub>2</sub> production rate of 8548 μmol g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> under simulated solar light, apparently superior to both Au@TiO<sub>2</sub> and Au@Cu<sub>2</sub>O/TiO<sub>2</sub> catalyst. The acetaldehyde was produced in liquid phase at an almost stoichiometric rate, and C−C cleavage of ethanol molecules to form CH<sub>4</sub> or CO<sub>2</sub> was greatly inhibited. Extensive spectroscopic results support the claim that Au adjacent to surface Ti<sup>3+</sup> defects could be active sites for H<sub>2</sub> production and p-n junction of TiO<sub>2</sub>/Cu<sub>2</sub>O facilitates photo-generated charge transfer and further dehydrogenation of ethanol to acetaldehyde during the photoreforming.https://www.mdpi.com/2073-4344/10/5/539ethanol reforminghydrogen productionAu catalystTi<sup>3+</sup> defectsite-specific deposition |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Lan Luo Tingting Zhang Xin Zhang Rongping Yun Yanjun Lin Bing Zhang Xu Xiang |
spellingShingle |
Lan Luo Tingting Zhang Xin Zhang Rongping Yun Yanjun Lin Bing Zhang Xu Xiang Enhanced Hydrogen Production from Ethanol Photoreforming by Site-Specific Deposition of Au on Cu<sub>2</sub>O/TiO<sub>2</sub> p-n Junction Catalysts ethanol reforming hydrogen production Au catalyst Ti<sup>3+</sup> defect site-specific deposition |
author_facet |
Lan Luo Tingting Zhang Xin Zhang Rongping Yun Yanjun Lin Bing Zhang Xu Xiang |
author_sort |
Lan Luo |
title |
Enhanced Hydrogen Production from Ethanol Photoreforming by Site-Specific Deposition of Au on Cu<sub>2</sub>O/TiO<sub>2</sub> p-n Junction |
title_short |
Enhanced Hydrogen Production from Ethanol Photoreforming by Site-Specific Deposition of Au on Cu<sub>2</sub>O/TiO<sub>2</sub> p-n Junction |
title_full |
Enhanced Hydrogen Production from Ethanol Photoreforming by Site-Specific Deposition of Au on Cu<sub>2</sub>O/TiO<sub>2</sub> p-n Junction |
title_fullStr |
Enhanced Hydrogen Production from Ethanol Photoreforming by Site-Specific Deposition of Au on Cu<sub>2</sub>O/TiO<sub>2</sub> p-n Junction |
title_full_unstemmed |
Enhanced Hydrogen Production from Ethanol Photoreforming by Site-Specific Deposition of Au on Cu<sub>2</sub>O/TiO<sub>2</sub> p-n Junction |
title_sort |
enhanced hydrogen production from ethanol photoreforming by site-specific deposition of au on cu<sub>2</sub>o/tio<sub>2</sub> p-n junction |
publisher |
MDPI AG |
series |
Catalysts |
issn |
2073-4344 |
publishDate |
2020-05-01 |
description |
Hydrogen production by photoreforming of biomass-derived ethanol is a renewable way of obtaining clean fuel. We developed a site-specific deposition strategy to construct supported Au catalysts by rationally constructing Ti<sup>3+</sup> defects inTiO<sub>2</sub> nanorods and Cu<sub>2</sub>O-TiO<sub>2</sub> p-n junction across the interface of two components. The Au nanoparticles (~2.5 nm) were selectively anchored onto either TiO<sub>2</sub> nanorods (Au@TiO<sub>2</sub>/Cu<sub>2</sub>O) or Cu<sub>2</sub>O nanocubes (Au@Cu<sub>2</sub>O/TiO<sub>2</sub>) or both TiO<sub>2</sub> and Cu<sub>2</sub>O (Au@TiO<sub>2</sub>/Cu<sub>2</sub>O@Au) with the same Au loading. The electronic structure of supported Au species was changed by forming Au@TiO<sub>2</sub> interface due to the adjacent Ti<sup>3+</sup> defects and the associated oxygen vacancies while unchanged in Au@Cu<sub>2</sub>O/TiO<sub>2</sub> catalyst. The p-n junction of TiO<sub>2</sub>/Cu<sub>2</sub>O promoted charge separation and transfer across the junction. During ethanol photoreforming, Au@TiO<sub>2</sub>/Cu<sub>2</sub>O catalyst possessing both the Au@TiO<sub>2</sub> interface and the p-n junction showed the highest H<sub>2</sub> production rate of 8548 μmol g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> under simulated solar light, apparently superior to both Au@TiO<sub>2</sub> and Au@Cu<sub>2</sub>O/TiO<sub>2</sub> catalyst. The acetaldehyde was produced in liquid phase at an almost stoichiometric rate, and C−C cleavage of ethanol molecules to form CH<sub>4</sub> or CO<sub>2</sub> was greatly inhibited. Extensive spectroscopic results support the claim that Au adjacent to surface Ti<sup>3+</sup> defects could be active sites for H<sub>2</sub> production and p-n junction of TiO<sub>2</sub>/Cu<sub>2</sub>O facilitates photo-generated charge transfer and further dehydrogenation of ethanol to acetaldehyde during the photoreforming. |
topic |
ethanol reforming hydrogen production Au catalyst Ti<sup>3+</sup> defect site-specific deposition |
url |
https://www.mdpi.com/2073-4344/10/5/539 |
work_keys_str_mv |
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