Towards Single-Site and Single-Atom Photo- and Electrocatalysis

A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Catalytic Materials".

Deadline for manuscript submissions: closed (30 September 2023) | Viewed by 8148

Special Issue Editors


E-Mail Website1 Website2
Guest Editor
Institute of Materials Chemistry, Vienna University of Technology, Getreidemarkt 9/BC/02/A18 1060 Vienna, Austria
Interests: heterogeneous photocatalysis; molecular photocatalysis; polyoxometalates; co-catalysts; materials chemistry; mesoporous materials; metal–organic frameworks

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Guest Editor
1. Department of Physical Chemistry, Fritz Haber institute, Max Planck Society, 14195 Berlin, Germany
2. Faculty of Physics, University of Duisburg-Essen, 47057 Duisburg, Germany
Interests: spectro-electrochemistry; electrocatalysis; fundamental electrochemistry

Special Issue Information

Dear Colleagues, 

The reactions of water splitting (to generate H2) and CO2 reduction (to produce high-value chemicals) have been recognized as potential game-changers in the ongoing economic transition to sustainable development. Both processes can be accessed through photo- and electrocatalysis, however—as they involve highly demanding multielectron redox reactions—a delicate design of the catalytic systems is necessary to achieve satisfactory performance. Besides, given the challenging selectivity issues posed by the CO2 reduction reaction, special attention need to be paid to the structure and location of the active sites responsible for a particular conversion.

Here—in light of the general difficulty to identify active surface sites of common heterogeneous catalysts and co-catalysts – recent years saw the infiltration of the concepts of “single-site” and “single-atom” catalysis into the fields of heterogeneous photo- and electrocatalysis. Not only do such systems allow for better atom-utilization efficiency, but they also enable access to better-defined catalytic sites, which ultimately helps to unravel synthesis-structure-performance space and allows for the development of advanced photo- and electrocatalysts by design.

In order to facilitate the development of this approach and assist in knowledge transfer from thermal heterogeneous catalysis to photo- and electrocatalytic systems, we would like to announce this special issue. Its focus lies in recent advances in preparation, characterization, and theoretical description of single-site and single-atom (co-)catalysts for their use in photocatalytic, electrocatalytic, and photoelectrocatalytic applications.

Preferred contributions:

This Special Issue will embrace any high-quality work that is devoted to:

  • synthesis approaches that aim to facilitate the formation of single-sites or explore strategies of their stabilization;
  • characterization methods that help to unravel the structure of the surface sites or provide insights into their formation, stability, and dynamic nature;
  • theoretical calculations that either provide insights into the performance of the catalytic systems or shed light on some of the experimental data.

We would like to encourage the authors to discuss the obtained characterization and performance data in light of the single-site or single-atom concept so that ideally a link between synthesis/structure and activity of these sites can be made by for example comparing the performance with reference systems where, for example, common bulky (co-)catalysts are used.

Besides, we welcome reviews. These are supposed to provide a background for the topic and talk about the concept of single-site and singe-atom catalysis and its conceptual extension to photocatalytic and electrocatalytic applications. A review can also cover the recent and most prominent literature on the topic.

Dr. Alexey Cherevan
Dr. Yujin Tong
Guest Editors

Manuscript Submission Information

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Keywords

  • photocatalysis
  • photoelectrocatalysis
  • electrocatalysis
  • single-site
  • single-atom
  • homogeneous
  • heterogeneous
  • hydrogen
  • solar fuel
  • CO2­ reduction
  • hydrogen evolution reaction
  • oxidative photocatalysis
  • water splitting

Published Papers (2 papers)

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Research

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18 pages, 4191 KiB  
Article
Isolation Strategy towards Earth-Abundant Single-Site Co-Catalysts for Photocatalytic Hydrogen Evolution Reaction
by Pablo Ayala, Ariane Giesriegl, Sreejith P. Nandan, Stephen Nagaraju Myakala, Peter Wobrauschek and Alexey Cherevan
Catalysts 2021, 11(4), 417; https://doi.org/10.3390/catal11040417 - 25 Mar 2021
Cited by 12 | Viewed by 3422
Abstract
Achieving efficient photocatalytic water splitting remains one of the most vital challenges in the photocatalysis field, as the performance of contemporary heterogeneous catalysts is still limited by their insufficient activity and low predictability. To address this challenge, this work takes inspiration from the [...] Read more.
Achieving efficient photocatalytic water splitting remains one of the most vital challenges in the photocatalysis field, as the performance of contemporary heterogeneous catalysts is still limited by their insufficient activity and low predictability. To address this challenge, this work takes inspiration from the concept of heterogeneous single-metal-site catalysts (HSMSCs) and follows the idea of site-isolation, aiming towards single-site co-catalyst species and a higher atom-utilization efficiency. We synthesized a set of photocatalysts through an adsorption-limited wet impregnation process using bare and phosphate-modified TiO2 as model supports and earth-abundant metals (Cu and Ni) with various loadings (0.008–5 wt.%) as co-catalyst species. The catalysts are characterized by TXRF for the determination of the real co-catalyst loadings, UV-vis and FTIR spectroscopes for semi-quantitative analysis of the metal state and binding modes to the substrate, and HRTEM for resolving the morphology of the sample’s surface. All samples were then evaluated towards the photocatalytic hydrogen evolution reaction (HER). We show that much higher turnover frequencies (TOFs) are obtained for both Cu- and Ni-based systems when lower co-catalyst loadings are used, which indicates an improved atom-utilization efficiency that reaches performances comparable to the noble Au co-catalyst. We also introduce a structural model to explain the observed TOF trends, which confirms that both earth-abundant systems undergo a strong structural reconstruction upon site-isolation towards smaller, perhaps even single-site-like species. Full article
(This article belongs to the Special Issue Towards Single-Site and Single-Atom Photo- and Electrocatalysis)
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Review

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40 pages, 62987 KiB  
Review
Single-Atom Co-Catalysts Employed in Titanium Dioxide Photocatalysis
by Ujjaval Kerketta, Alexander B. Tesler and Patrik Schmuki
Catalysts 2022, 12(10), 1223; https://doi.org/10.3390/catal12101223 - 12 Oct 2022
Cited by 16 | Viewed by 3828
Abstract
With a distinct electronic structure and unsaturated coordination centers, supported single-atoms (SAs) have shown great potential in heterogeneous catalysis due to their superior activity, stability, and selectivity. Over the last few years, the fascination of SA-use spread also over photocatalysis, i.e., a particular [...] Read more.
With a distinct electronic structure and unsaturated coordination centers, supported single-atoms (SAs) have shown great potential in heterogeneous catalysis due to their superior activity, stability, and selectivity. Over the last few years, the fascination of SA-use spread also over photocatalysis, i.e., a particular case of heterogeneous catalysis in which chemical reactions are activated by charge transfer from an illuminated semiconductor. Titanium dioxide (TiO2) is one of the most studied photocatalytic materials. It is widely used as a light absorbing semiconductor decorated with metallic (nanoparticles and single-atom) co-catalysts. In the current review, we emphasize the role of SAs as a co-catalyst in photocatalysis, and clearly set it apart from the use of single atoms in classic heterogeneous catalysis. The review first briefly describes the principal features of SAs, and gives an overview of most important examples of single-atom co-catalysts. Then, we discuss photocatalysis and key examples of single-atom co-catalysts used on TiO2 photocatalysts and their applications. At last, we provide an outlook for further exploring TiO2-based single-atom photocatalytic systems. Full article
(This article belongs to the Special Issue Towards Single-Site and Single-Atom Photo- and Electrocatalysis)
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