CdS纳米片与纳米线负载Au<sub>25</sub>纳米团簇光催化苯甲醇无氧脱氢制苯甲醛反应的研究

LI Xing-chi; ZHAO Han; PAN Xiao-li; SU Yang; LI Ren-gui; WANG Hua; KANG Lei-lei; LIU Xiao-yan

doi:10.1016/S1872-5813(23)60373-1

CdS纳米片与纳米线负载Au₂₅纳米团簇光催化苯甲醇无氧脱氢制苯甲醛反应的研究

doi: 10.1016/S1872-5813(23)60373-1

李星池^{1, 2, #,},
赵晗^{1, #,},
潘晓丽^1,,
苏杨^1,,
李仁贵^3,,
王华^1,,
康磊磊^1,,
刘晓艳^1, ,

1.
中国科学院大连化学物理研究所航天催化与新材料研究室, 辽宁大连 116023
2.
中国科学院大学, 北京 100049
3.
中国科学院大连化学物理研究所洁净能源国家重点实验室, 辽宁大连 116023

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中图分类号: O643
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出版历程
- 收稿日期: 2023-02-21
- 修回日期: 2023-03-24
- 录用日期: 2023-03-28
- 网络出版日期: 2023-06-14

Directing the CdS nanosheet and nanowire to high efficiency for photocatalytic anaerobic dehydrogenation of benzyl alcohol to benzaldehyde by depositing Au₂₅ nanoclusters

LI Xing-chi^{1, 2, #
,},
ZHAO Han^{1, #
,},
PAN Xiao-li^1
,,
SU Yang^1
,,
LI Ren-gui^3
,,
WANG Hua^1
,,
KANG Lei-lei^1
,,
LIU Xiao-yan^{1
, ,}

1.
CAS Key Laboratory of Science and Technology on Applied Catalysis, iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

More Information

Corresponding author: E-mail: xyliu2003@dicp.ac.cn

# These authors contributed equally to this work

摘要

摘要: 光催化苯甲醇直接脱氢制苯甲醛，是一种利用太阳能合成精细化学品同时生成氢气的节能途径。半导体CdS负载的催化剂是该反应的一类典型的光催化剂。文献报道CdS的形貌对光催化水分解的性能有明显的影响，但其在光催化苯甲醇无氧脱氢制苯甲醛反应中的形貌效应研究报道极少。本工作合成了纳米片状（NS）和纳米线状（NW）两种不同形貌的CdS，发现CdS-NS表现出比CdS-NW更高的转化苯甲醇的光催化活性，但这两种催化剂对苯甲醛的选择性非常低。通过在CdS-NS和CdS-NW上负载Au₂₅纳米团簇，光催化苯甲醇无氧脱氢制苯甲醛反应的活性和选择性明显提高，并在很大程度上减弱了CdS载体的形貌对催化反应性能的影响。以上结果将为设计合成精细化学品的高效光催化剂提供参考。
- CdS /
- 形貌效应 /
- 苯甲醇脱氢 /
- 无氧 /
- Au₂₅ 纳米团簇
Abstract: The photocatalysis of direct dehydrogenation of benzyl alcohol to benzaldehyde is an energy saving way to synthesize fine chemicals and pure hydrogen by using solar energy. The CdS-based catalysts were one of the typical kinds of photocatalysts for this reaction. The morphology of CdS could be easily tuned, which could greatly influence the photocatalytic performances. However, the morphology effect of CdS on the photocatalytic behaviour of the direct dehydrogenation of benzyl alcohol has not been investigated yet. In this work, we synthesized CdS with two different morphologies (nanosheet (NS) and nanowire (NW)) and found the CdS-NS showed much higher photocatalytic activity for converting the benzyl alcohol than the CdS-NW, but the selectivity to benzaldehyde over the two supports was very low. By depositing Au₂₅ nanoclusters on the CdS-NW and CdS-NS, the morphology effect of the CdS support could be mitigated and their catalytic activity and selectivity could be greatly boosted for the photocatalytic anaerobic dehydrogenation of benzyl alcohol to benzaldehyde and H₂. The results of this work would provide new insight into the design of efficient photocatalysts for synthesizing fine chemicals.
- CdS /
- morphology effect /
- benzyl alcohol dehydrogenation /
- anaerobic /
- Au₂₅ nanoclusters
# These authors contributed equally to this work
注释:

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Figure 1 Representative TEM images with different magnifications of (a-c) CdS-NS and (d-f) CdS-NW. The inset is the corresponding Fourier-transform diffraction patterns of the (b-c) CdS-NS and (e-f) CdS-NW

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Figure 2 XRD patterns of the samples including the CdS-NW, CdS-NS, Au₂₅/CdS-NW and Au₂₅/CdS-NS

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Figure 3 (a, d) STEM images, (b, e) the Au particle size distribution, and (c, f) the HRTEM images and the corresponding Fourier-transform diffraction patterns of Au of the (a-c) Au₂₅/CdS-NS and (d-f) Au₂₅/CdS-NW

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Figure 4 Cd 3d, S 2p and Au4f XPS data of the samples including the CdS-NW, CdS-NS, Au₂₅/CdS-NW and Au₂₅/CdS-NS

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Figure 5 Specific reaction rate of benzyl alcohol, and the formation rate of H₂ and benzaldehyde on the (a) CdS-NW, CdS-NS and (b) Au₂₅/CdS-NW, Au₂₅/CdS-NS with and without light illumination. (c) selectivity for benzaldehyde formation on the CdS-NW, CdS-NS, Au₂₅/CdS-NW and Au₂₅/CdS-NS

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Figure 6 UV-vis absorption spectra of the CdS and Au₂₅/CdS samples as indicated

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Figure 7 Photocatalytic dehydrogenation of BzOH to benzaldehyde by “PhCH₂O• Route” and “•CH(Ph)-OH Route”

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