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Oxide-Encapsulated Electrocatalysts For Solar Fuels Production
N. Y. Labrador
Published 2018 · Materials Science
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Oxide-Encapsulated Electrocatalysts for Solar Fuels Production Natalie Labrador As the cost of solar energy continues to drop, the major hurdle limiting the widespread use of intermittent renewable solar energy is the lack of efficient and cost-effective energy storage. Electrochemical technologies, such as electrolyzers, photoelectrochemical cells, and fuel cells, have the potential to compensate for solar energy intermittency on a large scale, by converting excess solar energy into storable solar fuels, such as hydrogen (H2), which can be converted back to electrical energy at a later time. However, improvements in the efficiency and lifetime of these technologies, in particular the electrocatalysts, are necessary for their commercialization. During operation, efficiency losses result from energetic penalties (overpotentials) associated with several processes occurring at or near the electrocatalyst/electrolyte (ohmic resistance, kinetic barriers, and mass transport limitations). These losses can be further exacerbated due to electrocatalyst durability issues such as dissolution, agglomeration, detachment, and poisoning. A major challenge in electrocatalysis field is developing methods to mitigate these losses without adversely affecting the electrocatalytic stability, selectivity, and/or activity. One promising solution is an oxide-encapsulated electrocatalyst architecture, which has been shown to improve electrocatalyst durability and provide mechanisms for controlling reaction pathways. Previous studies on oxide-encapsulated electrocatalysts, in which metal catalysts are fully or partially covered by ultrathin layers of permeable oxide films, have mostly focused on supported nanoparticles because of their high electrochemically active surface area per catalyst loading. However, these nanoparticle-based architectures tend to have poorly defined and/or nonuniform structures which make it difficult to understand and elucidate structure-propertyrelationships. This dissertation investigates well-defined oxide-coated electrocatalysts, which serve as model platforms for gaining a fundamental understanding of kinetic and transport phenomena that underlie their operation. This dissertation presents three studies which highlight the versatile functionalities of oxide-encapsulated electrocatalysts to improve the electrocatalyst stability, selectivity, and activity in different electrochemical systems. This dissertation demonstrates the ability of room temperature synthesized silicon oxide (SiOx)-encapsulated Pt electrocatalysts to: i) stabilize nanoparticles and improve electron transfer, ii) mitigate catalyst poisoning and control reaction pathways through selective transport, and iii) alter reaction energetics associated with catalysis at the buried interface. First, this dissertation establishes the ability of room temperature synthesized SiOx coatings to stabilize nanoparticle electrocatalysts by mitigating electrocatalyst migration, coalescence, and detachment on metal-insulator-semiconductor (MIS) photoelectrodes for solar-driven water splitting. Metallic Pt nanoparticles are inherently unstable on the insulating support due to poor physical adhesion and electronic coupling between Pt and SiO2. To overcome this issue, a room temperature UV ozone synthesis process was used to deposit 2-10 nm thick SiOx overlayers on top of electrodeposited Pt nanoparticles to stabilize Pt on the electrode surface. The photoelectrodes containing oxide-encapsulated electrocatalysts exhibit superior durability and electron transfer (ohmic) properties compared to the photoelectrode that lacked the SiOx encapsulation. While this study demonstrates that the oxide-encapsulated electrocatalyst architecture improves the stability of electrocatalytic nanoparticles deposited on insulating materials, it does not elucidate how reactants and products transport through the SiOx barrier to reach the Pt surface. In order to gain a better understanding of kinetic and transport phenomena that govern performance of oxide-encapsulated electrocatalysts, the following studies investigate model electrodes consisting of continuous SiOx overlayers of uniform thickness deposited onto smooth Pt thin films. This planar electrode geometry allows for simple and unambiguous characterization of structure-property relationships. The next study systematically evaluates the influence of SiOx thickness on the HER performance to understand species transport through SiOx. Through detailed characterization and electroanalytical tests, it is shown that proton and H2 transport occur primarily through the SiOx coating such that the HER occurs at the buried Pt|SiOx interface. Importantly, the SiOx nanomembranes were found to exhibit high selectivity for proton and H2 transport compared to Cu, a model HER poison. Leveraging this property, it is shown that SiOx–encapsulation can enable poison-resistant operation of Pt HER electrocatalysts. This oxide-encapsulated architecture offers a promising approach to enhancing electrocatalyst stability while incorporating advanced catalytic functionalities such as poison resistance or tunable reaction selectivity. The final study demonstrates ability of SiOx overlayers to alter reaction energetics associated with catalysis at the buried interface. Carbon monoxide (CO), methanol, and ethanol oxidation reactions are studied for their relevance in direct alcohol fuel cell applications. Oxidesupported catalysts have been shown to enhance alcohol oxidation by promoting CO oxidation at metal/oxide interfacial regions through the so-called bifunctional mechanism, in which hydroxyls on the oxide facilitate the removal of adsorbed CO−intermediates from active sites. A key advantage of the oxide-encapsulated electrocatalyst design compared to oxide–supported nanoparticles is that the former maximizes the density of metal/oxide interfacial sites. This study shows that the SiOx overlayer provides proximal hydroxyls, in the form of silanol groups, which can enhance CO and alcohol oxidation through unique interactions at the buried Pt|SiOx interface. Overall, this dissertation highlights the potential of using oxide-encapsulated electrocatalysts for stable, selective, and efficient electrochemical production and use of solar fuels.
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Catalytic Activity of Highly Durable Pt/CNT Catalysts Covered with Hydrophobic Silica Layers for the Oxygen Reduction Reaction in PEFCs
S. Takenaka (2014)
Real‐space observation of strong metal‐support interaction: state‐of‐the‐art and what's the next
X. Shi (2016)
Record high efficiency single-walled carbon nanotube/silicon p-n junction solar cells.
Y. Jung (2013)
Preparation of Carbon Nanotube-Supported Pt Metal Particles Covered with Silica Layers and Their Application to Electrocatalysts for PEMFC
S. Takenaka (2009)
Highly durable silica coated Pt/Cs with different surfactant types for proton exchange membrane fuel cell applications
Wattanachai Yaowarat (2015)
Impact of oxidation on nanoparticle adhesion to carbon substrates
Qianping He (2013)
Highly durable carbon nanotube-supported Pd catalysts covered with silica layers for the oxygen reduction reaction
S. Takenaka (2011)
Highly Durable and Active PtFe Nanocatalyst for Electrochemical Oxygen Reduction Reaction.
D. Chung (2015)
Electrochemical determination of activation energies for methanol oxidation on polycrystalline platinum in acidic and alkaline electrolytes.
J. Cohen (2007)
Extend Poison Resistance Chapter 4 provided an example of poison resistance against a model poison species
Nitrogen: unraveling the secret to stable carbon-supported Pt-alloy electrocatalysts
S. Pylypenko (2013)
Dissolution of Platinum: Limits for the Deployment of Electrochemical Energy Conversion?**
A. Topalov (2012)
Carbon-Supported Pt and PtRu Nanoparticles as Catalysts for a Direct Methanol Fuel Cell
Z. Liu (2004)
A sinter-resistant catalytic system based on platinum nanoparticles supported on TiO2 nanofibers and covered by porous silica.
Y. Dai (2010)
Effect of carbon black support corrosion on the durability of Pt/C catalyst
Jiajun Wang (2007)
The CO Poisoning Effect in PEMFCs Operational at Temperatures up to 200°C
Q. Li (2003)
Surface-oxide growth at platinum electrodes in aqueous H2SO4 ☆: Reexamination of its mechanism through combined cyclic-voltammetry, electrochemical quartz-crystal nanobalance, and Auger electron spectroscopy measurements
G. Jerkiewicz (2004)
Core/shell Au/CuPt nanoparticles and their dual electrocatalysis for both reduction and oxidation reactions.
X. Sun (2014)
Photoelectrocatalysis and electrocatalysis on p-silicon
M. Szklarczyk (1984)
Design principles for maximizing photovoltage in metal-oxide-protected water-splitting photoanodes.
Andrew G. Scheuermann (2016)
Long-term durable silicon photocathode protected by a thin Al2O3/SiOx layer for photoelectrochemical hydrogen evolution
M. Choi (2014)
Hollow and porous titanium nitride nanotubes as high-performance catalyst supports for oxygen reduction reaction
Zhanchang Pan (2014)
Highly durable Pt cathode catalysts for polymer electrolyte fuel cells; coverage of carbon black-supported Pt catalysts with silica layers
S. Takenaka (2011)
Ellipsometric study of the change in the porosity of silica xerogels after chemical modification of the surface with hexamethyldisilazane
C. Himcinschi (2002)
Characterization of Vulcan Electrochemically Oxidized under Simulated PEM Fuel Cell Conditions
K. Kangasniemi (2004)
Methanol oxidation and direct methanol fuel cells: a selective review 1 In honour of Professor W. Vi
S. Wasmus (1999)
Engineering metal organic frameworks for heterogeneous catalysis.
A. Corma (2010)
Electrocatalytic Activity and Stability of Pt clusters on State-of-the-Art Supports: A Review
S. Shrestha (2011)
Tungsten carbide as supports for Pt electrocatalysts with improved CO tolerance in methanol oxidatio
G. Cui (2011)
Conversion of Some Siloxane Polymers to Silicon Oxide by UV/Ozone Photochemical Processes
M. Ouyang (2000)
Novel catalyst support materials for PEM fuel cells : current status and future prospects
Yuyan Shao (2009)
Inorganic core-shell assemblies for closing the artificial photosynthetic cycle.
G. Yuan (2014)
Deconvoluting the influences of 3D structure on the performance of photoelectrodes for solar-driven water splitting
D. Esposito (2017)
A comparative study of photoconductivity and carrier transport in a-Si:H p–i–n solar cells with different back contacts
R. Kaplan (2010)
Pt–Ru catalyzed hydrogen oxidation in alkaline media: oxophilic effect or electronic effect?
Y. Wang (2015)
High Content Niobium in Rutile Titania as Catalyst Support to Promote Methanol Electro-Oxidation
L. Yan (2014)
Comparative DEMS study on the electrochemical oxidation of carbon blacks
S. Ashton (2012)
Review of conductor-insulator-semiconductor (CIS) solar cells
R. Singh (1981)
Solar water splitting cells.
Michael G Walter (2010)
Technical and economic feasibility of centralized facilities for solar hydrogen production via photocatalysis and photoelectrochemistry
B. Pinaud (2013)
Renewable hydrogen production
J. Turner (2008)
Handbook of chemical vapor deposition (CVD) : principles, technology, and applications
Hugh O. Pierson (1992)
Rapid Microwave-Assisted Polyol Reduction for the Preparation of Highly Active PtNi/CNT Electrocatalysts for Methanol Oxidation
A. A. Nassr (2014)
Sulfur-doped graphene as a potential alternative metal-free electrocatalyst and Pt-catalyst supporting material for oxygen reduction reaction.
Ji-Eun Park (2014)
Hydrogen Oxidation and Evolution Reaction Kinetics on Platinum: Acid vs Alkaline Electrolytes
Wenchao Sheng (2010)
THE ROLE OF BURIED OH SITES IN THE RESPONSE MECHANISM OF INORGANIC-GATE pH-SENSITIVE ISFETs
LUC BOUSSW (2001)
Size-dependent electrical behavior of spatially inhomogeneous barrier height regions on silicon
R. Rossi (2000)
Electrochemical investigation of the influence of thin SiOx films deposited on gold on charge transfer characteristics
S. Szunerits (2008)
UV–ozone induced growth of a SiOx surface layer on a cross-linked polysiloxane film: characterization and gas separation properties
M. Ouyang (2000)
Membraneless Electrolyzers for Low-Cost Hydrogen Production in a Renewable Energy Future
Daniel V Esposito (2017)
Electrochemical deposition of metals onto silicon
G. Oskam (1998)
Determination of the platinum and ruthenium surface areas in platinum-ruthenium alloy electrocatalysts by underpotential deposition of copper. I. Unsupported catalysts
Clare L. Green and (2002)
Visible Light Induced Hole Transport from Sensitizer to Co3O4 Water Oxidation Catalyst across Nanoscale Silica Barrier with Embedded Molecular Wires
A. Ağıral (2013)
Site-specific self-assembly of Si/SiOx nanoparticles on micropatterned poly(dimethylsiloxane) thin films
T. Phely-Bobin (2001)
DVE and NYL acknowledge Columbia University (start-up funds) and the National Science Foundation (NSF) (CBET-1752340)
Semimetallic TiO 2 Nanotubes. Angew. Chemie Int
R Hahn (2009)
A reactive molecular dynamics simulation of the silica-water interface.
Joseph C. Fogarty (2010)
Electrocatalytic activity and stability of niobium-doped titanium oxide supported platinum catalyst for polymer electrolyte membrane fuel cells
S. Huang (2010)
Charge Transfer Stabilization of Late Transition Metal Oxide Nanoparticles on a Layered Niobate Support.
Megan E. Strayer (2015)
Proton Diffusion in Amorphous SiO2 and Hafnium Silicate by Ab Initio Molecular Dynamics
J. Godet (2007)
MoS2-an integrated protective and active layer on n(+)p-Si for solar H2 evolution.
A. B. Laursen (2013)
Semiconductor-based photocatalytic hydrogen generation.
X. Chen (2010)
Semiconductor Material and Device Characterization, 3rd Edition
D. Schroder (2005)
Electrochemical stability of nanometer-scale Pt particles in acidic environments.
L. Tang (2010)
Advances in photoelectrocatalysis with nanotopographical photoelectrodes.
A. Muñoz (2010)
Ruthenium–Platinum Catalysts and Direct Methanol Fuel Cells (DMFC): A Review of Theoretical and Experimental Breakthroughs
A. S. Moura (2017)
Hydrogen Bonding Studies. II.1 The Acidity and Basicity of Silanols Compared to Alcohols2
R. West (1959)
Stabilizing Ni Catalysts by Molecular Layer Deposition for Harsh, Dry Reforming Conditions
Troy D. Gould (2014)
Sulfur poisoning of emergent and current electrocatalysts: vulnerability of MoS2, and direct correlation to Pt hydrogen evolution reaction kinetics.
Shu Min Tan (2015)
Understanding the electrocatalysis of oxygen reduction on platinum and its alloys
I. Stephens (2012)
Powering the planet: Chemical challenges in solar energy utilization
N. Lewis (2006)
Perspective on Liquid Solar Fuels
acknowledge Columbia University Columbia Nano Initiative and City University of New York Advanced Science Research Center for use of the physical vapor deposition and SEM equipment
Dielectric breakdown induced epitaxy in ultrathin gate oxide - a reliability concern
K. L. Pey (2002)
Facile synthesis of continuous Pt island networks and their electrochemical properties for methanol electrooxidation.
J. N. Tiwari (2008)
Scalable water splitting on particulate photocatalyst sheets with a solar-to-hydrogen energy conversion efficiency exceeding 1.
Q. Wang (2016)
Advances in interactive supported electrocatalysts for hydrogen and oxygen electrode reactions
N. Krstajić (2007)
Single-Molecule Electrochemistry on a Porous Silica-Coated Electrode.
Jin Lu (2017)
A titanosilicate molecular sieve with adjustable pores for size-selective adsorption of molecules
S. M. Kuznicki (2001)
Hydrogen-Evolving Solar Cells
Adam Heller (1984)
Addressing the terawatt challenge: scalability in the supply of chemical elements for renewable energy
P. C. K. Vesborg (2012)
Practical Approach to Zeolitic Membranes and Coatings: State of the Art, Opportunities, Barriers, and Future Perspectives
J. Gascón (2012)
Instability of Pt ∕ C Electrocatalysts in Proton Exchange Membrane Fuel Cells A Mechanistic Investigation
P. Ferreira (2005)
Toward highly stable electrocatalysts via nanoparticle pore confinement.
Carolina Galeano (2012)
The influence of chloride impurities on Pt/C fuel cell catalyst corrosion.
A. Pavlišič (2014)
Interfacial bonding stabilizes rhodium and rhodium oxide nanoparticles on layered Nb oxide and Ta oxide supports.
Megan E. Strayer (2014)
Noble‐Metal/Cr2O3 Core/Shell Nanoparticles as a Cocatalyst for Photocatalytic Overall Water Splitting
K. Maeda (2006)
The influence of Ferric ion contamination on the solid polymer electrolyte water electrolysis performance
Xunying Wang (2015)
A Review of Graphene‐Based Nanostructural Materials for Both Catalyst Supports and Metal‐Free Catalysts in PEM Fuel Cell Oxygen Reduction Reactions
Xue‐jun Zhou (2014)