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Title: Bandgap- and local field-dependent photoactivity of Ag/black phosphorus nanohybrids

Abstract

Black phosphorus (BP) is the most exciting post-graphene layered nanomaterial that serendipitously bridges the 2D materials gap between semimetallic graphene and large bandgap transition-metal dichalcogenides in terms of high charge-carrier mobility and tunable direct bandgap, yet research into BP-based solar to chemical energy conversion is still in its infancy. Herein, a novel hybrid photocatalyst with Ag nanoparticles supported on BP nanosheets is prepared using a chemical reduction approach. Spin-polarized density functional theory (DFT) calculations show that Ag nanoparticles are stabilized on BP by covalent bonds at the Ag/BP interface and Ag–Ag interactions. In the visible-light photocatalysis of rhodamine B by Ag/BP plasmonic nanohybrids, a significant rise in photoactivity compared with pristine BP nanosheets is observed either by decreasing BP layer thickness or increasing Ag particle size, with the greatest enhancement being up to ~20-fold. By virtue of finite-difference time domain (FDTD) simulations and photocurrent measurements, we give insights into the enhanced photocatalytic performance of Ag/BP nanohybrids, including the effects of BP layer thickness and Ag particle size. In comparison with BP, Ag/BP nanohybrids present intense local field amplification at the perimeter of Ag NPs, which is increased by either decreasing the BP layer thickness from multiple to few layers ormore » increasing the Ag particle size from 20 to 40 nm. Additionally, when the BP layer thickness is decreased from multiple to few layers, the bandgap becomes favorable to generate more strongly oxidative holes in the proximity of the Ag/BP interface to enhance photoactivity. Our findings illustrate a synergy between locally enhanced electric fields and BP bandgap, in which BP layer thickness and Ag particle size can be independently tuned to enhance photoactivity. Lastly, this study may open a new avenue for further exploiting BP-based plasmonic nanostructures in photocatalysis, photodetectors, and photovoltaics.« less

Authors:
 [1];  [2];  [3];  [3];  [2];  [2]
  1. National Center for Nanoscience and Technology, Beijing (People's Republic of China); Peking Univ., Beijing (People's Republic of China); Univ. of Chinese Academy of Sciences, Beijing (People's Republic of China)
  2. National Center for Nanoscience and Technology, Beijing (People's Republic of China)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1345735
Report Number(s):
BNL-113575-2017-JA
Journal ID: ISSN 2155-5435; R&D Project: CO040; KC0302010; TRN: US1701364
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 12; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ag nanoparticles; black phosphorus; density functional theory; localized surface plasmon resonance; photocatalysis

Citation Formats

Lei, Wanying, Zhang, Tingting, Liu, Ping, Rodriguez, Jose A., Liu, Gang, and Liu, Minghua. Bandgap- and local field-dependent photoactivity of Ag/black phosphorus nanohybrids. United States: N. p., 2016. Web. doi:10.1021/acscatal.6b02520.
Lei, Wanying, Zhang, Tingting, Liu, Ping, Rodriguez, Jose A., Liu, Gang, & Liu, Minghua. Bandgap- and local field-dependent photoactivity of Ag/black phosphorus nanohybrids. United States. https://doi.org/10.1021/acscatal.6b02520
Lei, Wanying, Zhang, Tingting, Liu, Ping, Rodriguez, Jose A., Liu, Gang, and Liu, Minghua. Tue . "Bandgap- and local field-dependent photoactivity of Ag/black phosphorus nanohybrids". United States. https://doi.org/10.1021/acscatal.6b02520. https://www.osti.gov/servlets/purl/1345735.
@article{osti_1345735,
title = {Bandgap- and local field-dependent photoactivity of Ag/black phosphorus nanohybrids},
author = {Lei, Wanying and Zhang, Tingting and Liu, Ping and Rodriguez, Jose A. and Liu, Gang and Liu, Minghua},
abstractNote = {Black phosphorus (BP) is the most exciting post-graphene layered nanomaterial that serendipitously bridges the 2D materials gap between semimetallic graphene and large bandgap transition-metal dichalcogenides in terms of high charge-carrier mobility and tunable direct bandgap, yet research into BP-based solar to chemical energy conversion is still in its infancy. Herein, a novel hybrid photocatalyst with Ag nanoparticles supported on BP nanosheets is prepared using a chemical reduction approach. Spin-polarized density functional theory (DFT) calculations show that Ag nanoparticles are stabilized on BP by covalent bonds at the Ag/BP interface and Ag–Ag interactions. In the visible-light photocatalysis of rhodamine B by Ag/BP plasmonic nanohybrids, a significant rise in photoactivity compared with pristine BP nanosheets is observed either by decreasing BP layer thickness or increasing Ag particle size, with the greatest enhancement being up to ~20-fold. By virtue of finite-difference time domain (FDTD) simulations and photocurrent measurements, we give insights into the enhanced photocatalytic performance of Ag/BP nanohybrids, including the effects of BP layer thickness and Ag particle size. In comparison with BP, Ag/BP nanohybrids present intense local field amplification at the perimeter of Ag NPs, which is increased by either decreasing the BP layer thickness from multiple to few layers or increasing the Ag particle size from 20 to 40 nm. Additionally, when the BP layer thickness is decreased from multiple to few layers, the bandgap becomes favorable to generate more strongly oxidative holes in the proximity of the Ag/BP interface to enhance photoactivity. Our findings illustrate a synergy between locally enhanced electric fields and BP bandgap, in which BP layer thickness and Ag particle size can be independently tuned to enhance photoactivity. Lastly, this study may open a new avenue for further exploiting BP-based plasmonic nanostructures in photocatalysis, photodetectors, and photovoltaics.},
doi = {10.1021/acscatal.6b02520},
journal = {ACS Catalysis},
number = 12,
volume = 6,
place = {United States},
year = {Tue Oct 18 00:00:00 EDT 2016},
month = {Tue Oct 18 00:00:00 EDT 2016}
}

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