Transformation-Optics-Designed Plasmonic Singularities for Efficient Photocatalytic Hydrogen Evolution at Metal/Semiconductor Interfaces

Tingting Lin; Tianyi Yang; Yuhang Cai; Jingwei Li; Guangxiang Lu; Shuangqun Chen; Yi Li; Liang Guo; Stefan A. Maier; Changxu Liu; Jianfeng Huang

doi:10.1021/acs.nanolett.3c01287

Transformation-Optics-Designed Plasmonic Singularities for Efficient Photocatalytic Hydrogen Evolution at Metal/Semiconductor Interfaces

Tingting Lin, Tianyi Yang, Yuhang Cai, Jingwei Li, Guangxiang Lu, Shuangqun Chen, Yi Li, Liang Guo^*, Stefan A. Maier^*, Changxu Liu, Jianfeng Huang^*

^*Corresponding author for this work

Mathematics, Physics and Electrical Engineering

Research output: Contribution to journal › Article › peer-review

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Abstract

Inspired by transformation optics, we propose a new concept for plasmonic photocatalysis by creating a novel hybrid nanostructure with a plasmonic singularity. Our geometry enables broad and strong spectral light harvesting at the active site of a nearby semiconductor where the chemical reaction occurs. A proof-of-concept nanostructure comprising Cu2ZnSnS4 (CZTS) and Au–Au dimer (t-CZTS@Au–Au) is fabricated via a colloidal strategy combining templating and seeded growth. On the basis of numerical and experimental results of different related hybrid nanostructures, we show that both the sharpness of the singular feature and the relative position to the reactive site play a pivotal role in optimizing photocatalytic activity. Compared with bare CZTS, the hybrid nanostructure (t-CZTS@Au–Au) exhibits an enhancement of the photocatalytic hydrogen evolution rate by up to ∼9 times. The insights gained from this work might be beneficial for designing efficient composite plasmonic photocatalysts for diverse photocatalytic reactions.

Original language	English
Pages (from-to)	5288-5296
Number of pages	9
Journal	Nano Letters
Volume	23
Issue number	11
Early online date	26 May 2023
DOIs	https://doi.org/10.1021/acs.nanolett.3c01287
Publication status	Published - 14 Jun 2023

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Cite this

@article{cd954dc95a6d40d78070832f52cb4569,

title = "Transformation-Optics-Designed Plasmonic Singularities for Efficient Photocatalytic Hydrogen Evolution at Metal/Semiconductor Interfaces",

abstract = "Inspired by transformation optics, we propose a new concept for plasmonic photocatalysis by creating a novel hybrid nanostructure with a plasmonic singularity. Our geometry enables broad and strong spectral light harvesting at the active site of a nearby semiconductor where the chemical reaction occurs. A proof-of-concept nanostructure comprising Cu2ZnSnS4 (CZTS) and Au–Au dimer (t-CZTS@Au–Au) is fabricated via a colloidal strategy combining templating and seeded growth. On the basis of numerical and experimental results of different related hybrid nanostructures, we show that both the sharpness of the singular feature and the relative position to the reactive site play a pivotal role in optimizing photocatalytic activity. Compared with bare CZTS, the hybrid nanostructure (t-CZTS@Au–Au) exhibits an enhancement of the photocatalytic hydrogen evolution rate by up to ∼9 times. The insights gained from this work might be beneficial for designing efficient composite plasmonic photocatalysts for diverse photocatalytic reactions.",

author = "Tingting Lin and Tianyi Yang and Yuhang Cai and Jingwei Li and Guangxiang Lu and Shuangqun Chen and Yi Li and Liang Guo and Maier, {Stefan A.} and Changxu Liu and Jianfeng Huang",

note = "Funding information: This work was supported by the Venture and Innovation Support Program for Chongqing Overseas Returnees (cx2020107), the Fundamental Research Funds for the Central Universities (2020CDJQY-A072), the Thousand Talents Program for Distinguished Young Scholars and Natural Science Foundation of Chongqing (cstc2021jcyj-msxmX0945). C.L. acknowledges the funding support from Humboldt Research Fellowship from the Alexander von Humboldt Foundation. S.M. acknowledges the funding support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany{\textquoteright}s Excellence Strategy, EXC 2089/1-390776260, the Solar Energies go Hybrid (SolTech) programme, the EPSRC (EP/W017075/1) and Lee-Lucas Chair in Physics. L G. acknowledges the funding support from the National Natural Science Foundation of China (No. 52176075) and Characteristic Innovation Project of the Department of Education of Guangdong Province (No. 2022KTSCX109). Prof. Tao Yang from the School of Chemistry and Chemical Engineering of Chongqing University is acknowledged for the generous offer of the facility for photocatalytic hydrogen evolution test. Dr. Kai Zhou from the Analytical and Testing Center of Chongqing University is acknowledged for the acquisition of the XPS spectra.",

year = "2023",

month = jun,

day = "14",

doi = "10.1021/acs.nanolett.3c01287",

language = "English",

volume = "23",

pages = "5288--5296",

journal = "Nano Letters",

issn = "1530-6984",

publisher = "American Chemical Society",

number = "11",

}

TY - JOUR

T1 - Transformation-Optics-Designed Plasmonic Singularities for Efficient Photocatalytic Hydrogen Evolution at Metal/Semiconductor Interfaces

AU - Lin, Tingting

AU - Yang, Tianyi

AU - Cai, Yuhang

AU - Li, Jingwei

AU - Lu, Guangxiang

AU - Chen, Shuangqun

AU - Li, Yi

AU - Guo, Liang

AU - Maier, Stefan A.

AU - Liu, Changxu

AU - Huang, Jianfeng

N1 - Funding information: This work was supported by the Venture and Innovation Support Program for Chongqing Overseas Returnees (cx2020107), the Fundamental Research Funds for the Central Universities (2020CDJQY-A072), the Thousand Talents Program for Distinguished Young Scholars and Natural Science Foundation of Chongqing (cstc2021jcyj-msxmX0945). C.L. acknowledges the funding support from Humboldt Research Fellowship from the Alexander von Humboldt Foundation. S.M. acknowledges the funding support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy, EXC 2089/1-390776260, the Solar Energies go Hybrid (SolTech) programme, the EPSRC (EP/W017075/1) and Lee-Lucas Chair in Physics. L G. acknowledges the funding support from the National Natural Science Foundation of China (No. 52176075) and Characteristic Innovation Project of the Department of Education of Guangdong Province (No. 2022KTSCX109). Prof. Tao Yang from the School of Chemistry and Chemical Engineering of Chongqing University is acknowledged for the generous offer of the facility for photocatalytic hydrogen evolution test. Dr. Kai Zhou from the Analytical and Testing Center of Chongqing University is acknowledged for the acquisition of the XPS spectra.

PY - 2023/6/14

Y1 - 2023/6/14

N2 - Inspired by transformation optics, we propose a new concept for plasmonic photocatalysis by creating a novel hybrid nanostructure with a plasmonic singularity. Our geometry enables broad and strong spectral light harvesting at the active site of a nearby semiconductor where the chemical reaction occurs. A proof-of-concept nanostructure comprising Cu2ZnSnS4 (CZTS) and Au–Au dimer (t-CZTS@Au–Au) is fabricated via a colloidal strategy combining templating and seeded growth. On the basis of numerical and experimental results of different related hybrid nanostructures, we show that both the sharpness of the singular feature and the relative position to the reactive site play a pivotal role in optimizing photocatalytic activity. Compared with bare CZTS, the hybrid nanostructure (t-CZTS@Au–Au) exhibits an enhancement of the photocatalytic hydrogen evolution rate by up to ∼9 times. The insights gained from this work might be beneficial for designing efficient composite plasmonic photocatalysts for diverse photocatalytic reactions.

AB - Inspired by transformation optics, we propose a new concept for plasmonic photocatalysis by creating a novel hybrid nanostructure with a plasmonic singularity. Our geometry enables broad and strong spectral light harvesting at the active site of a nearby semiconductor where the chemical reaction occurs. A proof-of-concept nanostructure comprising Cu2ZnSnS4 (CZTS) and Au–Au dimer (t-CZTS@Au–Au) is fabricated via a colloidal strategy combining templating and seeded growth. On the basis of numerical and experimental results of different related hybrid nanostructures, we show that both the sharpness of the singular feature and the relative position to the reactive site play a pivotal role in optimizing photocatalytic activity. Compared with bare CZTS, the hybrid nanostructure (t-CZTS@Au–Au) exhibits an enhancement of the photocatalytic hydrogen evolution rate by up to ∼9 times. The insights gained from this work might be beneficial for designing efficient composite plasmonic photocatalysts for diverse photocatalytic reactions.

U2 - 10.1021/acs.nanolett.3c01287

DO - 10.1021/acs.nanolett.3c01287

M3 - Article

SN - 1530-6984

VL - 23

SP - 5288

EP - 5296

JO - Nano Letters

JF - Nano Letters

IS - 11

ER -