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New Catalytic Systems for Light-driven Hydrogen Evolution

Li, Chuanshuai LU (2020) 1.
Abstract
Solar-driven reduction of water to produce hydrogen is one of the most promising ways to develop sustainable clean
energy for the future. The challenge in photocatalytic hydrogen evolution research is to design inexpensive catalysts
and construct efficient hydrogen production systems. In this thesis, different photocatalytic hydrogen production
systems consisting of catalysts, photosensitizers and sacrificial agents (electron donors and proton source) has been
designed and investigated based on non-precious molecular catalysts based on iron, cobalt, or molybdenum.
[Ru(bpy)3]2+ and CdSe quantum dots were explored as photosensitizers. The photocatalytic hydrogen production of
the studied systems was systematically... (More)
Solar-driven reduction of water to produce hydrogen is one of the most promising ways to develop sustainable clean
energy for the future. The challenge in photocatalytic hydrogen evolution research is to design inexpensive catalysts
and construct efficient hydrogen production systems. In this thesis, different photocatalytic hydrogen production
systems consisting of catalysts, photosensitizers and sacrificial agents (electron donors and proton source) has been
designed and investigated based on non-precious molecular catalysts based on iron, cobalt, or molybdenum.
[Ru(bpy)3]2+ and CdSe quantum dots were explored as photosensitizers. The photocatalytic hydrogen production of
the studied systems was systematically investigated, and the attempts to establish essential steps of the mechanism
of hydrogen evolution were made.
Chapter 1 gives a short introduction about photocatalytic hydrogen evolution, including semiconductor-based and
[Ru(bpy)3]2+-based photocatalytic hydrogen evolution systems. Chapter 2 relates to papers I and II in the thesis,
and describes the study of light-driven hydrogen evolution by CdSe quantum dot/iron carbonyl cluster assemblies
and a related graphitic carbon nitride based quantum dot/iron carbonyl cluster composite. It is shown that hole transfer
from CdSe quantum dots to biomimetic iron complexes dominates the fast charge transfer process and leads to
enhanced hydrogen production. Chapter 3, corresponding to paper III, describes the study of photoinduced hydrogen
evolution using cobalt compounds. The primary photochemical processes of three new Co(II) complexes in the
photocatalytic system have been probed by time-resolved spectroscopic analyses. Chapter 4, corresponding to paper
IV, describes the study of molybdenum-organic sulfides as catalysts for photocatalytic hydrogen evolution. Timeresolved
photoluminescence (TRPL) spectroscopy was used to investigate the charge carrier transfer dynamics for
the photochemical properties of derivatives of [Mo3S13]2-.
The close connection between hydrogen generating activity and charge carrier transfer dynamics in photocatalytic
systems is a key theme of this thesis. Studies on the carrier dynamics can enhance the understanding of key
processes in the mechanism of photocatalytic hydrogen production, and thus facilitate the design of efficient and
robust photocatalytic hydrogen evolution systems. (Less)
Please use this url to cite or link to this publication:
author
supervisor
opponent
  • Professor Philipp Kurz, University of Freiburg, Germany
organization
publishing date
type
Thesis
publication status
published
subject
keywords
photocatalysis, hydrogen evolution, semiconductor, molecular catalyst, charge transfer, mechanism
volume
1
edition
1
pages
190 pages
publisher
Media-Tryck, Lund University, Sweden
defense location
Lecture Hall F, Kemicentrum, Naturvetarvägen 14, Lund Join via zoom: https://lu-se.zoom.us/j/61134555703
defense date
2021-01-29 13:00:00
ISBN
978-91-7422-781-9
978-91-7422-780-2
language
English
LU publication?
yes
id
c137d77a-951b-4cad-80d1-8babc31ab7c0
date added to LUP
2021-01-04 13:51:23
date last changed
2025-04-04 14:25:55
@phdthesis{c137d77a-951b-4cad-80d1-8babc31ab7c0,
  abstract     = {{Solar-driven reduction of water to produce hydrogen is one of the most promising ways to develop sustainable clean<br/>energy for the future. The challenge in photocatalytic hydrogen evolution research is to design inexpensive catalysts<br/>and construct efficient hydrogen production systems. In this thesis, different photocatalytic hydrogen production<br/>systems consisting of catalysts, photosensitizers and sacrificial agents (electron donors and proton source) has been<br/>designed and investigated based on non-precious molecular catalysts based on iron, cobalt, or molybdenum.<br/>[Ru(bpy)3]2+ and CdSe quantum dots were explored as photosensitizers. The photocatalytic hydrogen production of<br/>the studied systems was systematically investigated, and the attempts to establish essential steps of the mechanism<br/>of hydrogen evolution were made.<br/>Chapter 1 gives a short introduction about photocatalytic hydrogen evolution, including semiconductor-based and<br/>[Ru(bpy)3]2+-based photocatalytic hydrogen evolution systems. Chapter 2 relates to papers I and II in the thesis,<br/>and describes the study of light-driven hydrogen evolution by CdSe quantum dot/iron carbonyl cluster assemblies<br/>and a related graphitic carbon nitride based quantum dot/iron carbonyl cluster composite. It is shown that hole transfer<br/>from CdSe quantum dots to biomimetic iron complexes dominates the fast charge transfer process and leads to<br/>enhanced hydrogen production. Chapter 3, corresponding to paper III, describes the study of photoinduced hydrogen<br/>evolution using cobalt compounds. The primary photochemical processes of three new Co(II) complexes in the<br/>photocatalytic system have been probed by time-resolved spectroscopic analyses. Chapter 4, corresponding to paper<br/>IV, describes the study of molybdenum-organic sulfides as catalysts for photocatalytic hydrogen evolution. Timeresolved<br/>photoluminescence (TRPL) spectroscopy was used to investigate the charge carrier transfer dynamics for<br/>the photochemical properties of derivatives of [Mo3S13]2-.<br/>The close connection between hydrogen generating activity and charge carrier transfer dynamics in photocatalytic<br/>systems is a key theme of this thesis. Studies on the carrier dynamics can enhance the understanding of key<br/>processes in the mechanism of photocatalytic hydrogen production, and thus facilitate the design of efficient and<br/>robust photocatalytic hydrogen evolution systems.}},
  author       = {{Li, Chuanshuai}},
  isbn         = {{978-91-7422-781-9}},
  keywords     = {{photocatalysis; hydrogen evolution; semiconductor; molecular catalyst; charge transfer; mechanism}},
  language     = {{eng}},
  month        = {{12}},
  publisher    = {{Media-Tryck, Lund University, Sweden}},
  school       = {{Lund University}},
  title        = {{New Catalytic Systems for Light-driven Hydrogen Evolution}},
  url          = {{https://lup.lub.lu.se/search/files/89204685/Chuanshuai_Li_WEBB.pdf}},
  volume       = {{1}},
  year         = {{2020}},
}