Single-Nanoflake Photo-Electrochemistry Reveals Champion and Spectator Flakes in Exfoliated MoSe2 Films

Todt, Michael A.; Isenberg, Allan E.; Nanayakkara, Sanjini U.; Miller, Elisa M.; Sambur, Justin B.

doi:10.1021/acs.jpcc.7b12715

Title: Single-Nanoflake Photo-Electrochemistry Reveals Champion and Spectator Flakes in Exfoliated MoSe₂ Films

Journal Article · Tue Mar 06 00:00:00 EST 2018 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b12715· OSTI ID:1435696

Todt, Michael A. ^[1]; Isenberg, Allan E. ^[1]; Nanayakkara, Sanjini U. ^[2];

^[2];

^[1]

Colorado State Univ., Fort Collins, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Semiconducting transition-metal dichalcogenide (TMD) nanoflake thin films are promising large-area electrodes for photo-electrochemical solar energy conversion applications. However, their energy conversion efficiencies are typically much lower than those of bulk electrodes. It is unclear to what extent this efficiency gap stems from differences among nanoflakes (e.g., area, thickness, and surface structural features). It is also unclear whether individual exfoliated nanoflakes can achieve energy conversion efficiencies similar to those of bulk crystals. Here, we use a single-nanoflake photo-electrochemical approach to show that there are both highly active and completely inactive nanoflakes within a film. For the exfoliated MoSe₂ samples studied herein, 7% of nanoflakes are highly active champions, whose photocurrent efficiency exceeds that of the bulk crystal. However, 66% of nanoflakes are inactive spectators, which are mostly responsible for the overall lower photocurrent efficiency compared to the bulk crystal. The photocurrent collection efficiency increases with nanoflake area and decreases more at perimeter edges than at interior step edges. These observations, which are hidden in ensemble-level measurements, reveal the underlying performance issues of exfoliated TMD electrodes for photo-electrochemical energy conversion applications.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1435696

Report Number(s):: NREL/JA-5900-71132; TRN: US1900084

Journal Information:: Journal of Physical Chemistry. C, Vol. 122, Issue 12; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 17 works

Citation information provided by
Web of Science

References (28)

Performance of Synthetical n-MoSe[sub 2] in Electrochemical Solar Cells Gobrecht, J. Journal of The Electrochemical Society, Vol. 125, Issue 12 https://doi.org/10.1149/1.2131370	journal	January 1978
Semiconductor Electrodes Fan, Fu-Ren F. Journal of The Electrochemical Society, Vol. 127, Issue 2 https://doi.org/10.1149/1.2129700	journal	January 1980
Relationship between surface morphology and solar conversion efficiency of tungsten diselenide photoanodes Lewerenz, H. J.; Heller, A.; DiSalvo, F. J. Journal of the American Chemical Society, Vol. 102, Issue 6 https://doi.org/10.1021/ja00526a019	journal	March 1980
Evaluation and reduction of efficiency losses at tungsten diselenide photoanodes Parkinson, Bruce A.; Furtak, Thomas E.; Canfield, Duane Faraday Discussions of the Chemical Society, Vol. 70 https://doi.org/10.1039/dc9807000233	journal	January 1980
Spontaneous Photoelectrolysis of HBr and HI Levy-Clement, Claude Journal of The Electrochemical Society, Vol. 129, Issue 8, p. 1701-1705 https://doi.org/10.1149/1.2124253	journal	January 1982
Electrochemical characterization of p-type semiconducting tungsten disulfide photocathodes: efficient photoreduction processes at semiconductor/liquid electrolyte interfaces Baglio, Joseph A.; Calabrese, Gary S.; Harrison, D. Jed Journal of the American Chemical Society, Vol. 105, Issue 8 https://doi.org/10.1021/ja00346a024	journal	April 1983
Tungsten disulfide: a novel hydrogen evolution catalyst for water decomposition Sobczynski, Andrzej; Yildiz, Attila; Bard, Allen J. The Journal of Physical Chemistry, Vol. 92, Issue 8 https://doi.org/10.1021/j100319a042	journal	April 1988
Hydrogen Evolution from Pt/Ru-Coated p-Type WSe ₂ Photocathodes McKone, James R.; Pieterick, Adam P.; Gray, Harry B. Journal of the American Chemical Society, Vol. 135, Issue 1 https://doi.org/10.1021/ja308581g	journal	December 2012
Passivation of recombination centers in n ‐WSe ₂ yields high efficiency (>14%) photoelectrochemical cell Tenne, R.; Wold, A. Applied Physics Letters, Vol. 47, Issue 7 https://doi.org/10.1063/1.96066	journal	October 1985
The high-efficiency (17.1%) WSe ₂ photo-electrochemical solar cell Prasad, G.; Srivastava, O. N. Journal of Physics D: Applied Physics, Vol. 21, Issue 6 https://doi.org/10.1088/0022-3727/21/6/029	journal	June 1988
Materials Availability Expands the Opportunity for Large-Scale Photovoltaics Deployment Wadia, Cyrus; Alivisatos, A. Paul; Kammen, Daniel M. Environmental Science & Technology, Vol. 43, Issue 6 https://doi.org/10.1021/es8019534	journal	March 2009
Toward Large-Area Solar Energy Conversion with Semiconducting 2D Transition Metal Dichalcogenides Yu, Xiaoyun; Sivula, Kevin ACS Energy Letters, Vol. 1, Issue 1 https://doi.org/10.1021/acsenergylett.6b00114	journal	June 2016
MoS ₂ /WS ₂ Heterojunction for Photoelectrochemical Water Oxidation Pesci, Federico M.; Sokolikova, Maria S.; Grotta, Chiara ACS Catalysis, Vol. 7, Issue 8 https://doi.org/10.1021/acscatal.7b01517	journal	July 2017
Self-assembled 2D WSe2 thin films for photoelectrochemical hydrogen production Yu, Xiaoyun; Prévot, Mathieu S.; Guijarro, Néstor Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8596	journal	July 2015
Photogenerated Charge Harvesting and Recombination in Photocathodes of Solvent-Exfoliated WSe ₂ Yu, Xiaoyun; Sivula, Kevin Chemistry of Materials, Vol. 29, Issue 16 https://doi.org/10.1021/acs.chemmater.7b02018	journal	August 2017
Photoelectrochemistry of Pristine Mono- and Few-Layer MoS ₂ Velický, Matěj; Bissett, Mark A.; Woods, Colin R. Nano Letters, Vol. 16, Issue 3 https://doi.org/10.1021/acs.nanolett.5b05317	journal	February 2016
The Role of Surface Defects in the Photooxidation of Iodide at n-MoSe2: Evidence for a Local "Autocatalytic" Effect Chaparro, A. M.; Salvador, P.; Peter, L. M. The Journal of Physical Chemistry, Vol. 99, Issue 17 https://doi.org/10.1021/j100017a059	journal	April 1995
Influence of crystal surface orientation on redox reactions at semiconducting MoS2 Ahmed, Syed M.; Gerischer, H. Electrochimica Acta, Vol. 24, Issue 6 https://doi.org/10.1016/0013-4686(79)87055-3	journal	June 1979
Photoelectrochemistry of WSe[sub 2] Electrodes Lewerenz, H. J. Journal of The Electrochemical Society, Vol. 131, Issue 1 https://doi.org/10.1149/1.2115467	journal	January 1984
Imaging the Anisotropic Reactivity of a Tungsten Diselenide Photocathode Eisenberg, David ChemElectroChem, Vol. 2, Issue 9 https://doi.org/10.1002/celc.201500103	journal	June 2015
Reliable Exfoliation of Large-Area High-Quality Flakes of Graphene and Other Two-Dimensional Materials Huang, Yuan; Sutter, Eli; Shi, Norman N. ACS Nano, Vol. 9, Issue 11 https://doi.org/10.1021/acsnano.5b04258	journal	September 2015
The scanning microscope for semiconductor characterization: photocurrent, photovoltage and electrolyte electroreflectance imaging at the n-MoSe2/I− interface Chaparro, A. M.; Salvador, P.; Mir, A. Journal of Electroanalytical Chemistry, Vol. 424, Issue 1-2 https://doi.org/10.1016/s0022-0728(96)04903-0	journal	March 1997
Photoinduced layer phenomenon caused by iodine formation in MoSe2: electrolyte (iodide) junctions Tributsch, H.; Sakata, T.; Kawai, T. Electrochimica Acta, Vol. 26, Issue 1 https://doi.org/10.1016/0013-4686(81)80002-3	journal	January 1981
The application of chronocoulometry to the study of adsorption at the semiconductor/electrolyte interface Turner, John A.; Parkinson, Bruce A. Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 150, Issue 1-2 https://doi.org/10.1016/S0022-0728(83)80240-X	journal	July 1983
Critical analysis of electrical contacts to layered semiconductors for use in (photo)electrochemical studies Etman, Mohamed; Neumann-Spallart, Michael Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 269, Issue 2 https://doi.org/10.1016/0022-0728(89)85148-4	journal	September 1989
Semiconductor Electrodes Fan, Fu-Ren F. Journal of The Electrochemical Society, Vol. 128, Issue 5 https://doi.org/10.1149/1.2127580	journal	January 1981
Electrochemical Solar Cell Based on the d-Band Semiconductor Tungsten-Diselenide Gobrecht, J.; Gerischer, H.; Tributsch, H. Berichte der Bunsengesellschaft für physikalische Chemie, Vol. 82, Issue 12 https://doi.org/10.1002/bbpc.19780821212	journal	December 1978
Digital Imaging of the Effect of Photoetching on the Photoresponse of n-Type Tungsten Diselenide and Molybdenum Diselenide Single Crystal Electrodes Salvador, P.; Chaparro, A. M.; Mir, A. The Journal of Physical Chemistry, Vol. 100, Issue 2 https://doi.org/10.1021/jp952001x	journal	January 1996

Cited By (1)

Single nanoparticle photoelectrochemistry: What is next? Wang, Li; Schmid, Merranda; Sambur, Justin B. The Journal of Chemical Physics, Vol. 151, Issue 18 https://doi.org/10.1063/1.5124710	journal	November 2019

Figures / Tables (4)

Similar Records

Single Nanoflake Photoelectrochemistry Reveals Intrananoflake Doping Heterogeneity That Explains Ensemble-Level Photoelectrochemical Behavior

Journal Article · Mon Nov 01 00:00:00 EDT 2021 · ACS Applied Materials and Interfaces · OSTI ID:1435696

Erdewyk, Michael Van; Sambur, Justin B.

Liquid Phase Exfoliation of Chemically Prelithiated Bilayered Vanadium Oxide in Aqueous Media for Li-Ion Batteries

Journal Article · Thu Jan 05 00:00:00 EST 2023 · Journal of Physical Chemistry. C · OSTI ID:1435696

Zhang, Raymond; Averianov, Timofey; Andris, Ryan; +2 more

Semi-monolithic Integration of All-Chalcopyrite Multijunction Solar Conversion Devices via Thin-Film Bonding and Exfoliation

Journal Article · Mon Dec 05 00:00:00 EST 2022 · ACS Applied Materials and Interfaces · OSTI ID:1435696

Outlaw-Spruell, Kai; Crunk, Joshua; Septina, Wilman; +3 more

Related Subjects

14 SOLAR ENERGY
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
transition-metal dichalcogenide
nanoflake thin films
photovoltiacs
solar energy conversion

Title: Single-Nanoflake Photo-Electrochemistry Reveals Champion and Spectator Flakes in Exfoliated MoSe2 Films

Citation Formats