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Title: Energy transfer-enhanced photocatalytic reduction of protons within quantum dot light-harvesting–catalyst assemblies

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [1]; ORCiD logo [2]; ORCiD logo [2]
  1. Department of Chemistry, Northwestern University, Evanston, IL 60208-3113,
  2. Department of Chemistry, Northwestern University, Evanston, IL 60208-3113,, Center for Bio-Inspired Energy Science, Northwestern University, Chicago, IL 60611-3015

Significance A feature of natural photosynthetic systems is their ability to operate with the low photon flux of sunlight, where the absorption of light and transport of photochemical potential to the catalytic centers is efficiency-limiting. Natural systems overcome this limitation through a process called energy transfer, where quanta of energy are gathered by many weakly coupled light-absorbing centers that pass the energy among themselves to funnel it to a single catalytic reaction center. Prior to this report, this type of energy migration-based approach to light-powered chemistry has not been employed in artificial photocatalytic systems. This work demonstrates the viability of energy-transfer–based sensitization in colloidal photocatalytic assemblies and provides a framework for its incorporation into scalable solar energy conversion systems.

Sponsoring Organization:
USDOE
Grant/Contract Number:
SC0000989
OSTI ID:
1462458
Alternate ID(s):
OSTI ID: 1540299
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 33 Vol. 115; ISSN 0027-8424
Publisher:
Proceedings of the National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

References (40)

Photovoltaic concepts inspired by coherence effects in photosynthetic systems journal December 2016
Semiconductor quantum dot-sensitized rainbow photocathode for effective photoelectrochemical hydrogen generation journal October 2017
Artificial Photosynthesis: Molecular Systems for Catalytic Water Oxidation journal October 2014
Multiscale model of light harvesting by photosystem II in plants journal January 2016
Hydrogen Production by Molecular Photocatalysis journal October 2007
The photoluminescence spectral profiles of water-soluble aggregates of PbS quantum dots assembled through reversible metal coordination journal January 2017
Distance-Dependence of Interparticle Energy Transfer in the Near-Infrared within Electrostatic Assemblies of PbS Quantum Dots journal April 2017
Powering a CO 2 Reduction Catalyst with Visible Light through Multiple Sub-picosecond Electron Transfers from a Quantum Dot journal June 2017
Robust Photogeneration of H2 in Water Using Semiconductor Nanocrystals and a Nickel Catalyst journal November 2012
Working the Other Way Around: Photocatalytic Water Oxidation Triggered by Reductive Quenching of the Photoexcited Chromophore journal January 2015
Charge Carrier Resolved Relaxation of the First Excitonic State in CdSe Quantum Dots Probed with Near-Infrared Transient Absorption Spectroscopy journal November 2010
A Little Coherence in Photosynthetic Light Harvesting journal November 2013
A Place in the Sun for Artificial Photosynthesis? journal May 2016
Fuel from Water: The Photochemical Generation of Hydrogen from Water journal June 2014
Nickel Complexes for Robust Light-Driven and Electrocatalytic Hydrogen Production from Water journal January 2015
Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution journal March 2017
Enhanced Photocatalysis of Rhenium(I) Complex by Light-Harvesting Periodic Mesoporous Organosilica journal May 2010
Efficient and Limiting Reactions in Aqueous Light-Induced Hydrogen Evolution Systems using Molecular Catalysts and Quantum Dots journal May 2014
Architecture of the Photosynthetic Oxygen-Evolving Center journal March 2004
Photocatalytically Active Superstructures of Quantum Dots and Iron Porphyrins for Reduction of CO 2 to CO in Water journal January 2018
Photocatalytic CO 2 Reduction Using Cu(I) Photosensitizers with a Fe(II) Catalyst journal March 2016
Towards non-blinking colloidal quantum dots journal June 2008
WO 3 -based photocatalysts: morphology control, activity enhancement and multifunctional applications journal January 2017
Redox shuttle mechanism enhances photocatalytic H2 generation on Ni-decorated CdS nanorods journal August 2014
The native architecture of a photosynthetic membrane journal August 2004
Carbon dots as photosensitisers for solar-driven catalysis journal January 2017
ZnSe quantum dots modified with a Ni(cyclam) catalyst for efficient visible-light driven CO 2 reduction in water journal January 2018
Visible-Light Induced Water Detoxification Catalyzed by Pt II Dye Sensitized Titania journal September 2008
An Exceptional Artificial Photocatalyst, Ni h -CdSe/CdS Core/Shell Hybrid, Made In Situ from CdSe Quantum Dots and Nickel Salts for Efficient Hydrogen Evolution journal August 2013
Semiconductor-based Photocatalytic Hydrogen Generation journal November 2010
Light Absorption and Energy Transfer in the Antenna Complexes of Photosynthetic Organisms journal March 2016
Selective Photocatalytic CO 2 Reduction in Water through Anchoring of a Molecular Ni Catalyst on CdS Nanocrystals journal May 2017
Chlorophyll Fluorescence: A Probe of Photosynthesis In Vivo journal June 2008
Near-Quantitative Yield for Transfer of Near-Infrared Excitons within Solution-Phase Assemblies of PbS Quantum Dots journal September 2016
Energy Transfer in Aqueous Solutions of Oppositely Charged CdSe/ZnS Core/Shell Quantum Dots and in Quantum Dot−Nanogold Assemblies journal March 2004
The Water Oxidation Bottleneck in Artificial Photosynthesis: How Can We Get Through It? An Alternative Route Involving a Two-Electron Process journal January 2011
Photogeneration of hydrogen from water using CdSe nanocrystals demonstrating the importance of surface exchange journal September 2013
Principles, Efficiency, and Blueprint Character of Solar-Energy Conversion in Photosynthetic Water Oxidation journal December 2009
Light-driven dinitrogen reduction catalyzed by a CdS:nitrogenase MoFe protein biohybrid journal April 2016
Direct-Coupling O 2 Bond Forming a Pathway in Cobalt Oxide Water Oxidation Catalysts journal August 2011