Plasmonic Control of Multi-Electron Transfer and C-C Coupling in Visible-Light-Driven CO2 Reduction on Au Nanoparticles

Sungju Yu, Andrew J. Wilson, Jaeyoung Heo, Prashant Jain

Research output: Contribution to journalArticle

Abstract

Artificial photosynthesis relies on the availability of synthetic photocatalysts that can drive CO2 reduction in the presence of water and light. From the standpoint of solar fuel production, it is desirable that these photocatalysts perform under visible light and produce energy-rich hydrocarbons from CO2 reduction. However, the multistep nature of CO2-to-hydrocarbon conversion poses a significant kinetic bottleneck when compared to CO production and H2 evolution. Here, we show that plasmonic Au nanoparticle photocatalysts can harvest visible light for multielectron, multiproton reduction of CO2 to yield C1 (methane) and C2 (ethane) hydrocarbons. The light-excitation attributes influence the C2 and C1 selectivity. The observed trends in activity and selectivity follow Poisson statistics of electron harvesting. Higher photon energies and flux favor simultaneous harvesting of more than one electron from the photocharged Au nanoparticle catalyst, inducing the C-C coupling required for C2 production. These findings elucidate the nature of plasmonic photocatalysis, which involves strong light-matter coupling, and set the stage for the controlled chemical bond formation by light excitation.

Original languageEnglish (US)
Pages (from-to)2189-2194
Number of pages6
JournalNano Letters
Volume18
Issue number4
DOIs
StatePublished - Apr 11 2018

Fingerprint

electron transfer
Nanoparticles
nanoparticles
Electrons
Photocatalysts
Hydrocarbons
hydrocarbons
fuel production
selectivity
Ethane
photosynthesis
Photosynthesis
Photocatalysis
Chemical bonds
Methane
Carbon Monoxide
chemical bonds
ethane
excitation
availability

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

Cite this

Plasmonic Control of Multi-Electron Transfer and C-C Coupling in Visible-Light-Driven CO2 Reduction on Au Nanoparticles. / Yu, Sungju; Wilson, Andrew J.; Heo, Jaeyoung; Jain, Prashant.

In: Nano Letters, Vol. 18, No. 4, 11.04.2018, p. 2189-2194.

Research output: Contribution to journalArticle

@article{5ae98437fcbe4376a4e17548198f7bf7,
title = "Plasmonic Control of Multi-Electron Transfer and C-C Coupling in Visible-Light-Driven CO2 Reduction on Au Nanoparticles",
abstract = "Artificial photosynthesis relies on the availability of synthetic photocatalysts that can drive CO2 reduction in the presence of water and light. From the standpoint of solar fuel production, it is desirable that these photocatalysts perform under visible light and produce energy-rich hydrocarbons from CO2 reduction. However, the multistep nature of CO2-to-hydrocarbon conversion poses a significant kinetic bottleneck when compared to CO production and H2 evolution. Here, we show that plasmonic Au nanoparticle photocatalysts can harvest visible light for multielectron, multiproton reduction of CO2 to yield C1 (methane) and C2 (ethane) hydrocarbons. The light-excitation attributes influence the C2 and C1 selectivity. The observed trends in activity and selectivity follow Poisson statistics of electron harvesting. Higher photon energies and flux favor simultaneous harvesting of more than one electron from the photocharged Au nanoparticle catalyst, inducing the C-C coupling required for C2 production. These findings elucidate the nature of plasmonic photocatalysis, which involves strong light-matter coupling, and set the stage for the controlled chemical bond formation by light excitation.",
author = "Sungju Yu and Wilson, {Andrew J.} and Jaeyoung Heo and Prashant Jain",
year = "2018",
month = "4",
day = "11",
doi = "10.1021/acs.nanolett.7b05410",
language = "English (US)",
volume = "18",
pages = "2189--2194",
journal = "Nano Letters",
issn = "1530-6984",
publisher = "American Chemical Society",
number = "4",

}

TY - JOUR

T1 - Plasmonic Control of Multi-Electron Transfer and C-C Coupling in Visible-Light-Driven CO2 Reduction on Au Nanoparticles

AU - Yu, Sungju

AU - Wilson, Andrew J.

AU - Heo, Jaeyoung

AU - Jain, Prashant

PY - 2018/4/11

Y1 - 2018/4/11

N2 - Artificial photosynthesis relies on the availability of synthetic photocatalysts that can drive CO2 reduction in the presence of water and light. From the standpoint of solar fuel production, it is desirable that these photocatalysts perform under visible light and produce energy-rich hydrocarbons from CO2 reduction. However, the multistep nature of CO2-to-hydrocarbon conversion poses a significant kinetic bottleneck when compared to CO production and H2 evolution. Here, we show that plasmonic Au nanoparticle photocatalysts can harvest visible light for multielectron, multiproton reduction of CO2 to yield C1 (methane) and C2 (ethane) hydrocarbons. The light-excitation attributes influence the C2 and C1 selectivity. The observed trends in activity and selectivity follow Poisson statistics of electron harvesting. Higher photon energies and flux favor simultaneous harvesting of more than one electron from the photocharged Au nanoparticle catalyst, inducing the C-C coupling required for C2 production. These findings elucidate the nature of plasmonic photocatalysis, which involves strong light-matter coupling, and set the stage for the controlled chemical bond formation by light excitation.

AB - Artificial photosynthesis relies on the availability of synthetic photocatalysts that can drive CO2 reduction in the presence of water and light. From the standpoint of solar fuel production, it is desirable that these photocatalysts perform under visible light and produce energy-rich hydrocarbons from CO2 reduction. However, the multistep nature of CO2-to-hydrocarbon conversion poses a significant kinetic bottleneck when compared to CO production and H2 evolution. Here, we show that plasmonic Au nanoparticle photocatalysts can harvest visible light for multielectron, multiproton reduction of CO2 to yield C1 (methane) and C2 (ethane) hydrocarbons. The light-excitation attributes influence the C2 and C1 selectivity. The observed trends in activity and selectivity follow Poisson statistics of electron harvesting. Higher photon energies and flux favor simultaneous harvesting of more than one electron from the photocharged Au nanoparticle catalyst, inducing the C-C coupling required for C2 production. These findings elucidate the nature of plasmonic photocatalysis, which involves strong light-matter coupling, and set the stage for the controlled chemical bond formation by light excitation.

UR - http://www.scopus.com/inward/record.url?scp=85045182218&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85045182218&partnerID=8YFLogxK

U2 - 10.1021/acs.nanolett.7b05410

DO - 10.1021/acs.nanolett.7b05410

M3 - Article

C2 - 29405717

AN - SCOPUS:85045182218

VL - 18

SP - 2189

EP - 2194

JO - Nano Letters

JF - Nano Letters

SN - 1530-6984

IS - 4

ER -