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Catalysts
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Heterogeneous Electrocatalysis: Fundamentals and Applications
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Heterogeneous Electrocatalysis: Fundamentals and Applications

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

Deadline for manuscript submissions: closed (30 April 2022) | Viewed by 27967

Special Issue Editors

Dr. Shangqian Zhu

E-Mail Website
Guest Editor
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Hong Kong, China
Interests: electrocatalysis; electrochemistry; in situ infrared spectroscopy; hydrogen oxidation reaction; CO2 reduction reaction; nanomaterials
Dr. Qinglan Zhao

E-Mail Website
Guest Editor
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Hong Kong, China
Interests: electrocatalytic CO2 reduction reaction; electrocatalytic O2 reduction reaction; sodium-ion batteries; organic electrode materials; porous carbon materials
Dr. Yao Yao

E-Mail Website
Guest Editor
Laboratory of Photonics and Interfaces, École polytechnique fédérale de Lausanne, Lausanne, Switzerland
Interests: electrochemical CO2 reduction reaction; electrochemical N2 reduction reaction; surface enhanced IR absorption spectroscopy; membrane electrode assembly based electrolyzer
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Energy conversion and storage techniques based on heterogeneous electrocatalysis are expected to play a substantial role in the sustainable development of human society. The development of advanced electrocatalysts for electrochemical reactions, e.g., CO2 reduction, N2 reduction, H2 evolution/oxidation, ethanol oxidation, etc., constitutes a significant part toward the practical applications of various electrochemical devices, which not only require advances in material engineering techniques but also fundamental understanding of reaction mechanisms.

In the past few years, the community has witnessed rapid and continuous development in the field of heterogeneous electrocatalysis. This Special Issue will cover experimental and theoretical studies in various electrochemical reactions, particularly CO2/N2/nitrate reduction into value-added chemicals, H2 electrocatalysis, and fuel cell reactions. Both fundamental and applied studies are of interest, particularly in the development of new catalysts of high activity/selectivity/stability, fundamental investigations into reaction mechanisms/pathways, impacts of catalyst structure/composition and interfacial environment on the catalytic results, and in situ characterizations of catalysts.  The hope is to compile a set of high-quality manuscripts that convey exciting advances of heterogeneous electrocatalysis.

Dr. Shangqian Zhu
Dr. Qinglan Zhao
Dr. Yao Yao
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Catalysts is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Electrocatalysis
  • Electrocatalysts
  • Reaction mechanisms
  • CO2 reduction reaction
  • N2 reduction reaction
  • Nitrate reduction reaction
  • O2 reduction reaction
  • H2 evolution/oxidation reaction
  • Ethanol/methanol/formic acid oxidation reaction
  • In situ characterizations

Published Papers (7 papers)

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Research

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13 pages, 3384 KiB  
Article
The Role of Steps on Silver Nanoparticles in Electrocatalytic Oxygen Reduction
by Jack Jon Hinsch, Junxian Liu, Jessica Jein White and Yun Wang
Catalysts 2022, 12(6), 576; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12060576 - 24 May 2022
Cited by 8 | Viewed by 2227
Abstract
Hydrogen fuel cell technology is an essential component of a green economy. However, it is limited in practicality and affordability by the oxygen reduction reaction (ORR). Nanoscale silver particles have been proposed as a cost-effective solution to this problem. However, previous computational studies [...] Read more.
Hydrogen fuel cell technology is an essential component of a green economy. However, it is limited in practicality and affordability by the oxygen reduction reaction (ORR). Nanoscale silver particles have been proposed as a cost-effective solution to this problem. However, previous computational studies focused on clean and flat surfaces. High-index surfaces can be used to model active steps presented in nanoparticles. Here, we used the stable stepped Ag(322) surface as a model to understand the ORR performance of steps on Ag nanoparticles. Our density functional theory (DFT) results demonstrate a small dissociation energy barrier for O2 molecules on the Ag(322) surface, which can be ascribed to the existence of low-coordination number surface atoms. Consequently, the adsorption of OOH* led to the associative pathway becoming ineffective. Alternatively, the unusual dissociative mechanism is energetically favored on Ag(322) for ORR. Our findings reveal the importance of the coordination numbers of active sites for catalytic performance, which can further guide electrocatalysts’ design. Full article
(This article belongs to the Special Issue Heterogeneous Electrocatalysis: Fundamentals and Applications)
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11 pages, 2497 KiB  
Article
Cobalt-Containing Nitrogen-Doped Carbon Materials Derived from Saccharides as Efficient Electrocatalysts for Oxygen Reduction Reaction
by Kaidi Veske, Ave Sarapuu, Maike Käärik, Arvo Kikas, Vambola Kisand, Helle-Mai Piirsoo, Alexey Treshchalov, Jaan Leis, Aile Tamm and Kaido Tammeveski
Catalysts 2022, 12(5), 568; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12050568 - 20 May 2022
Cited by 3 | Viewed by 2887
Abstract
The development of non-precious metal electrocatalysts towards oxygen reduction reaction (ORR) is crucial for the commercialisation of polymer electrolyte fuel cells. In this work, cobalt-containing nitrogen-doped porous carbon materials were prepared by a pyrolysis of mixtures of saccharides, cobalt nitrate and dicyandiamide, which [...] Read more.
The development of non-precious metal electrocatalysts towards oxygen reduction reaction (ORR) is crucial for the commercialisation of polymer electrolyte fuel cells. In this work, cobalt-containing nitrogen-doped porous carbon materials were prepared by a pyrolysis of mixtures of saccharides, cobalt nitrate and dicyandiamide, which acts as a precursor for reactive carbon nitride template and a nitrogen source. The rotating disk electrode (RDE) experiments in 0.1 M KOH solution showed that the glucose-derived material with optimised cobalt content had excellent ORR activity, which was comparable to that of 20 wt% Pt/C catalyst. In addition, the catalyst exhibited high tolerance to methanol, good stability in short-time potential cycling test and low peroxide yield. The materials derived from xylan, xylose and cyclodextrin displayed similar activities, indicating that various saccharides can be used as inexpensive and sustainable precursors to synthesise active catalyst materials for anion exchange membrane fuel cells. Full article
(This article belongs to the Special Issue Heterogeneous Electrocatalysis: Fundamentals and Applications)
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14 pages, 4029 KiB  
Article
High-Performance of Electrocatalytic CO2 Reduction on Defective Graphene-Supported Cu4S2 Cluster
by Qiyan Zhang, Yawei Li, Haiyan Zhu and Bingbing Suo
Catalysts 2022, 12(5), 454; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12050454 - 19 Apr 2022
Cited by 4 | Viewed by 2116
Abstract
Electrochemical CO2 reduction reaction (CO2RR) to high-value chemicals is one of the most splendid approaches to mitigating environmental threats and energy shortage. In this study, the catalytic performance of CO2RR on defective graphene-supported Cu4S2 clusters [...] Read more.
Electrochemical CO2 reduction reaction (CO2RR) to high-value chemicals is one of the most splendid approaches to mitigating environmental threats and energy shortage. In this study, the catalytic performance of CO2RR on defective graphene-supported Cu4S2 clusters as well as isolated Cu4Xn (X = O, S, Se; n = 2, 4) was systematically investigated based on density functional theory (DFT) computations. Calculation results revealed that the most thermodynamically feasible product is CH3OH among the C1 products on Cu4X2 clusters, in which the Cu4S2 cluster has the best activity concerning CH3OH synthesis with a limiting potential of −0.48 V. When the Cu4S2 cluster was further supported on defective graphene, the strong interaction between cluster and substrate could greatly improve the performance via tuning the electronic structure and improving the stability of the Cu4S2 cluster. The calculated free energy diagram indicated that it is also more energetically preferable for CH3OH production with a low limiting potential of −0.35 V. Besides, the defective graphene support has a significant ability to suppress the competing reactions, such as the hydrogen evolution reaction (HER) and CO and HCOOH production. Geometric structures, limiting potentials, and reduction pathways were also discussed to gain insight into the reaction mechanism and to find the minimum-energy pathway for C1 products. We hope this work will provide theoretical reference for designing and developing advanced supported Cu-based electrocatalysts for CO2 reduction. Full article
(This article belongs to the Special Issue Heterogeneous Electrocatalysis: Fundamentals and Applications)
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12 pages, 2025 KiB  
Article
A Membrane Reactor with Microchannels for Carbon Dioxide Reduction in Extraterrestrial Space
by Deqiang Feng, Wenjun Jiang, Ce Zhang, Long Li, Botao Hu, Jian Song and Wei Yao
Catalysts 2022, 12(1), 3; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12010003 - 21 Dec 2021
Cited by 8 | Viewed by 2804
Abstract
Long-term continuous oxygen supply is of vital importance during the process of space exploration. Considering the cost and feasibility, in situ resource utilization (ISRU) may be a promising solution. The conversion of CO2 to O2 is a key point for ISRU. [...] Read more.
Long-term continuous oxygen supply is of vital importance during the process of space exploration. Considering the cost and feasibility, in situ resource utilization (ISRU) may be a promising solution. The conversion of CO2 to O2 is a key point for ISRU. In addition, the utilization of the abundant CO2 resources in the atmosphere of Mars is an important topic in the field of manned deep space exploration. The Sabatier reaction, Bosch reaction, and solid oxide electrolysis (SOE) are well-known techniques for the reduction of CO2. However, all the above techniques need great energy consumption. In this article, we designed an electrochemical membrane reactor at room temperature based on microfluidic control for the reduction of CO2 in extraterrestrial space. In this system, H2O was oxidized to O2 on the anode, while CO2 was reduced to C2H4 on the cathode. The highest Faraday efficiency (FE) for C2H4 was 72.7%, with a single-pass carbon efficiency toward C2H4 (SPCE-C2H4) of 4.64%. In addition, a microfluidic control technique was adopted to overcome the influence of the microgravity environment. The study may provide a solution for the long-term continuous oxygen supply during the process of space exploration. Full article
(This article belongs to the Special Issue Heterogeneous Electrocatalysis: Fundamentals and Applications)
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11 pages, 1626 KiB  
Communication
Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates
by Guihua Li, Yonghui Zhao, Jerry Pui Ho Li, Wei Chen, Shoujie Li, Xiao Dong, Yanfang Song, Yong Yang, Wei Wei and Yuhan Sun
Catalysts 2021, 11(12), 1502; https://0-doi-org.brum.beds.ac.uk/10.3390/catal11121502 - 10 Dec 2021
Cited by 4 | Viewed by 3377
Abstract
Conversion of CO2 to valuable chemicals driven by renewable electricity via electrocatalytic reduction processes is of great significance for achieving carbon neutrality. Copper-based materials distinguish themselves from other electrocatalysts for their unique capability to produce multicarbon compounds in CO2 electroreduction. However, [...] Read more.
Conversion of CO2 to valuable chemicals driven by renewable electricity via electrocatalytic reduction processes is of great significance for achieving carbon neutrality. Copper-based materials distinguish themselves from other electrocatalysts for their unique capability to produce multicarbon compounds in CO2 electroreduction. However, the intrinsic active composition and C–C coupling mechanism of copper-based catalysts are still ambiguous. This is largely due to the absence of appropriate in situ approaches to monitor the complicated processes of CO2 electroreduction. Here, we adopted operando spectroscopy techniques, including Raman and infrared, to investigate the evolution of compositions and intermediates during gas-phase CO2 electroreduction on Cu foam, Cu2O nanowire and CuO nanowire catalysts. Although all the three copper-based catalysts possessed the activity of electroreducing gas-phase CO2 to multicarbon oxygenates, Cu2O nanowires showed the much superior performance with a 71.9% Faradaic efficiency of acetaldehyde. Operando Raman spectra manifested that the cuprous oxide remained stable during the whole gas-phase CO2 electroreduction, and operando diffuse reflectance infrared Fourier transform spectroscopy (DRFITS) results provide direct evidences of key intermediates and their evolutions for producing multicarbon oxygenates, in consistence with the density functional theory calculations. Full article
(This article belongs to the Special Issue Heterogeneous Electrocatalysis: Fundamentals and Applications)
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Review

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12 pages, 3499 KiB  
Review
Catalytic Materials by 3D Printing: A Mini Review
by Lina Chen, Shiqiang Zhou, Mengrui Li, Funian Mo, Suzhu Yu and Jun Wei
Catalysts 2022, 12(10), 1081; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12101081 - 20 Sep 2022
Cited by 9 | Viewed by 3143
Abstract
Catalytic processes are the dominant driving force in the chemical industry, proper design and fabrication of three-dimensional (3D) catalysts monoliths helps to keep the active species from scattering in the reaction flow, improve high mass loading, expose abundant active catalytic sites and even [...] Read more.
Catalytic processes are the dominant driving force in the chemical industry, proper design and fabrication of three-dimensional (3D) catalysts monoliths helps to keep the active species from scattering in the reaction flow, improve high mass loading, expose abundant active catalytic sites and even realize turbulent gas flow, greatly improving the catalytic performance. Three-dimensional printing technology, also known as additive manufacturing, provides free design and accurate fabrication of complex 3D structures in an efficient and economic way. This disruptive technology brings light to optimizing and promoting the development of existing catalysts. In this mini review, we firstly introduce various printing techniques which are applicable for fabricating catalysts. Then, the recent developments in 3D printing catalysts are scrutinized. Finally, challenges and possible research directions in this field are proposed, with the expectation of providing guidance for the promotion of 3D printed catalysts. Full article
(This article belongs to the Special Issue Heterogeneous Electrocatalysis: Fundamentals and Applications)
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24 pages, 2945 KiB  
Review
Recent Advances in Seawater Electrolysis
by Siqi Jiang, Hongli Suo, Teng Zhang, Caizhi Liao, Yunxiao Wang, Qinglan Zhao and Weihong Lai
Catalysts 2022, 12(2), 123; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12020123 - 20 Jan 2022
Cited by 30 | Viewed by 10042
Abstract
Hydrogen energy, as a clean and renewable energy, has attracted much attention in recent years. Water electrolysis via the hydrogen evolution reaction at the cathode coupled with the oxygen evolution reaction at the anode is a promising method to produce hydrogen. Given the [...] Read more.
Hydrogen energy, as a clean and renewable energy, has attracted much attention in recent years. Water electrolysis via the hydrogen evolution reaction at the cathode coupled with the oxygen evolution reaction at the anode is a promising method to produce hydrogen. Given the shortage of freshwater resources on the planet, the direct use of seawater as an electrolyte for hydrogen production has become a hot research topic. Direct use of seawater as the electrolyte for water electrolysis can reduce the cost of hydrogen production due to the great abundance and wide availability. In recent years, various high-efficiency electrocatalysts have made great progress in seawater splitting and have shown great potential. This review introduces the mechanisms and challenges of seawater splitting and summarizes the recent progress of various electrocatalysts used for hydrogen and oxygen evolution reaction in seawater electrolysis in recent years. Finally, the challenges and future opportunities of seawater electrolysis for hydrogen and oxygen production are presented. Full article
(This article belongs to the Special Issue Heterogeneous Electrocatalysis: Fundamentals and Applications)
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