Special Issue "Catalysis and Catalytic Processes for CO2 Conversion"

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

Deadline for manuscript submissions: closed (31 May 2019).

Special Issue Editors

Guest Editor
Dr. Kwang-Deog Jung Website E-Mail
Clean Energy Research Center, Korea Institute of Science and Technology, Seoul, KoreaDivision of Energy Environment Technology, University of Science and Technology, Deajeon, Korea
Phone: +822-958-5218
Fax: +822-958-5219
Interests: CO2 conversion; C1 chemistry; alkane dehydrogenation; hydrogen production
Guest Editor
Prof. Sungho Yoon E-Mail
Department of Applied Chemistry, Kookmin University, Seoul, Korea
Interests: CO2 conversion; C-H activation; hydrogenation and carbonylation

Special Issue Information

Dear Colleagues,

There is still a great deal of controversy over whether CO2 conversion can be considered as a means to massively mitigate CO2. Nonetheless, recent progress in CO2 conversion has shown that the technology has the potential to create new industries in new chemical and energy fields. Catalysis for CO2 conversion have been mainly focused on CO2 hydrogenation and polymer synthesis. The high price of hydrogen is the biggest obstacle to the industrialization of CO2 hydrogenation, but, in recent years, the development of active catalysts at low temperatures and processes have been carried out to overcome these economic limitations. The innovative routes are also explored to prepare environmentally benign polymer from CO2. On the other hand, the advances on the electrochemical CO2 reduction deliver persuasive results that the electrochemical CO2 conversion can be commercialized in near future. Furthermore, enzyme and microbial electrosynthesis are also studied to reduce CO2 into valuable products. The processes using the innovative catalysts are also studied to examine the potential of the commercialization of the CO2 conversion.

Here, this Special Issue aims to cover recent progress and advances on both catalysts and processes in the field of CO2 conversion: (1) CO2 hydrogenation, (2) monomer and polymer synthesis from CO2, (3) Electrochemical CO2 reduction, (4) photoelectrochemical CO2 reduction, and (5) enzyme- and microbial-electrosynthesis from CO2.

Dr. Kwang-Deog Jung
Prof. Sungho Yoon
Guest Editors

Manuscript Submission Information

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Keywords

  • CO2 hydrogenation
  • Organic carbonates
  • Carboxylation
  • Electrochemical CO2 reduction
  • Photoelectrochemical CO2 reduction
  • Electroenzymatic CO2 reduction
  • Microbial electrosynthesis

Published Papers (8 papers)

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Research

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Open AccessArticle
CO2 Methanation over Ni/[email protected]2O4 (M = Zn, Mg, or Mn) Catalysts
Catalysts 2019, 9(7), 599; https://doi.org/10.3390/catal9070599 - 11 Jul 2019
Cited by 1
Abstract
In this study, unique core-shell aluminate spinel supports, [email protected]2O4 (M = Zn, Mg, or Mn), were obtained by simple hydrothermal surface oxidation and were applied to the preparation of supported Ni catalysts for CO2 methanation. For comparison, CO methanation [...] Read more.
In this study, unique core-shell aluminate spinel supports, [email protected]2O4 (M = Zn, Mg, or Mn), were obtained by simple hydrothermal surface oxidation and were applied to the preparation of supported Ni catalysts for CO2 methanation. For comparison, CO methanation was also evaluated using the same catalysts. The prepared catalysts were characterized with a variety of techniques, including N2 physisorption, CO2 chemisorption, H2 chemisorption, temperature-programmed reduction with H2, temperature-programmed desorption of CO2, X-ray diffraction, high-resolution transmission electron microscopy, and in-situ diffuse reflectance infrared Fourier transform spectroscopy. The combination of supports with core-shell spinel structures and Ni doping with a deposition–precipitation method created outstanding catalytic performance of the Ni catalysts supported on [email protected]2O4 and [email protected]2O4 due to improved dispersion of Ni nanoparticles and creation of moderate basic sites with suitable strength. Good stability of Ni/[email protected]2O4 catalyst was also confirmed in the study. Full article
(This article belongs to the Special Issue Catalysis and Catalytic Processes for CO2 Conversion)
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Open AccessArticle
Catalytic Activity of Ni1-xLi2xWO4 Particles for Carbon Dioxide Photoreduction
Catalysts 2019, 9(5), 467; https://doi.org/10.3390/catal9050467 - 21 May 2019
Abstract
This study introduces NiWO4 as a main photocatalyst, where the Ni component promotes methanation to generate a WO3-based catalyst, as a new type of catalyst that promotes the photoreduction of carbon dioxide by slowing the recombination of electrons and holes. [...] Read more.
This study introduces NiWO4 as a main photocatalyst, where the Ni component promotes methanation to generate a WO3-based catalyst, as a new type of catalyst that promotes the photoreduction of carbon dioxide by slowing the recombination of electrons and holes. The bandgap of NiWO4 is 2.74 eV, which was expected to improve the initial activity for the photoreduction of carbon dioxide. However, fast recombination between the holes and electrons was also expected. To overcome this problem, attempts were made to induce structural defects by partially replacing the Ni2+ ions in NiWO4 with Li+. The resulting CO2 conversion reaction was greatly enhanced with the Ni1-xLi2xWO4 catalysts containing Li+, compared to that of the pure NiWO4 catalysts. Notably, the total amount of CO and CH4 produced with the Ni0.8Li0.4WO4 catalyst was 411.6 nmol g−1. It is believed that the insertion of Li+ ions into the NiWO4 skeleton results in lattice defects due to charge and structural imbalance, which play a role in the capture of CO2 gas or excited electrons, thereby inhibiting recombination between the electrons and holes in the Ni1-xLi2xWO4 particles. Full article
(This article belongs to the Special Issue Catalysis and Catalytic Processes for CO2 Conversion)
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Open AccessArticle
Electrocatalytic Processes for the Valorization of CO2: Synthesis of Cyanobenzoic Acid Using Eco-Friendly Strategies
Catalysts 2019, 9(5), 413; https://doi.org/10.3390/catal9050413 - 02 May 2019
Cited by 2
Abstract
Carbon dioxide (CO2) is a known greenhouse gas, and is the most important contributor to global warming. Therefore, one of the main challenges is to either eliminate or reuse it through the synthesis of value-added products, such as carboxylated derivatives. One [...] Read more.
Carbon dioxide (CO2) is a known greenhouse gas, and is the most important contributor to global warming. Therefore, one of the main challenges is to either eliminate or reuse it through the synthesis of value-added products, such as carboxylated derivatives. One of the most promising approaches for activating, capturing, and valorizing CO2 is the use of electrochemical techniques. In the current manuscript, we described an electrocarboxylation route for synthesizing 4-cyanobenzoic acid by valorizing CO2 through the synergistic use of electrochemical techniques (“green technology”) and ionic liquids (ILs) (“green solvents”)—two of the major entries in the general green chemistry tool kit. Moreover, the use of silver cathodes and ILs enabled the electrochemical potential applied to be reduced by more than 0.4 V. The “green” synthesis of those derivatives would provide a suitable environmentally friendly process for the design of plasticizers based on phthalate derivatives. Full article
(This article belongs to the Special Issue Catalysis and Catalytic Processes for CO2 Conversion)
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Open AccessArticle
Preparation of Metal Amalgam Electrodes and Their Selective Electrocatalytic CO2 Reduction for Formate Production
Catalysts 2019, 9(4), 367; https://doi.org/10.3390/catal9040367 - 18 Apr 2019
Abstract
Electrochemical CO2 reduction to produce formate ions has studied for the sustainable carbon cycle. Mercury in the liquid state is known to be an active metallic component to selectively convert CO2 to formate ions, but it is not scalable to use [...] Read more.
Electrochemical CO2 reduction to produce formate ions has studied for the sustainable carbon cycle. Mercury in the liquid state is known to be an active metallic component to selectively convert CO2 to formate ions, but it is not scalable to use as an electrode in electrochemical CO2 reduction. Therefore, scalable amalgam electrodes with different base metals are tested to produce formate by an electrochemical CO2 reduction. The amalgam electrodes are prepared by the electrodeposition of Hg on the pre-electrodeposited Pd, Au, Pt and Cu nanoparticles on the glassy carbon. The formate faradaic efficiency with the Pd, Au, Pt and Cu is lower than 25%, while the one with the respective metal amalgams is higher than 50%. Pd amalgam among the tested samples shows the highest formate faradic efficiency and current density. The formate faradaic efficiency is recorded 85% at −2.1 V vs SCE and the formate current density is −6.9 mA cm−2. It is concluded that Pd2Hg5 alloy on the Pd amalgam electrode is an active phase for formate production in the electrochemical CO2 reduction. Full article
(This article belongs to the Special Issue Catalysis and Catalytic Processes for CO2 Conversion)
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Open AccessFeature PaperArticle
Molecular Rh(III) and Ir(III) Catalysts Immobilized on Bipyridine-Based Covalent Triazine Frameworks for the Hydrogenation of CO2 to Formate
Catalysts 2018, 8(7), 295; https://doi.org/10.3390/catal8070295 - 22 Jul 2018
Cited by 5
Abstract
The catalytic reactivity of molecular Rh(III)/Ir(III) catalysts immobilized on two- and three-dimensional Bipyridine-based Covalent Triazine Frameworks (bpy-CTF) for the hydrogenation of CO2 to formate has been described. The heterogenized Ir complex demonstrated superior catalytic efficiency over its Rh counterpart. The Ir catalyst [...] Read more.
The catalytic reactivity of molecular Rh(III)/Ir(III) catalysts immobilized on two- and three-dimensional Bipyridine-based Covalent Triazine Frameworks (bpy-CTF) for the hydrogenation of CO2 to formate has been described. The heterogenized Ir complex demonstrated superior catalytic efficiency over its Rh counterpart. The Ir catalyst immobilized on two-dimensional bpy-CTF showed an improved turnover frequency and turnover number compared to its three-dimensional counterpart. The two-dimensional Ir catalyst produced a maximum formate concentration of 1.8 M and maintained its catalytic efficiency over five consecutive runs with an average of 92% in each cycle. The reduced activity after recycling was studied by density functional theory calculations, and a plausible leaching pathway along with a rational catalyst design guidance have been proposed. Full article
(This article belongs to the Special Issue Catalysis and Catalytic Processes for CO2 Conversion)
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Open AccessArticle
Theoretical Study of the Mechanism for CO2 Hydrogenation to Methanol Catalyzed by trans-RuH2(CO)(dpa)
Catalysts 2018, 8(6), 244; https://doi.org/10.3390/catal8060244 - 11 Jun 2018
Cited by 1
Abstract
In this work, the reaction mechanism for the conversion of CO2 and H2 to methanol has been researched by density functional theory (DFT). The production of methanol from CO2 and H2 is catalyzed by a univocal bifunctional pincer-type complex [...] Read more.
In this work, the reaction mechanism for the conversion of CO2 and H2 to methanol has been researched by density functional theory (DFT). The production of methanol from CO2 and H2 is catalyzed by a univocal bifunctional pincer-type complex trans-RuH2(CO)(dpa) (dpa = bis-(2-diphenylphosphinoethyl)amine). The reaction mechanism includes three continuous catalytic processes: (1) CO2 is converted to formic acid; (2) formic acid is converted to formaldehyde and water; (3) formaldehyde is converted to methanol. By computing the catalytic processes, we have shown that the rate-limiting step in the whole process is the direct cleavage of H2. The calculated largest free energy barrier is 21.6 kcal/mol. However, with the help of water, the free energy barrier can be lowered to 12.7 kcal/mol, which suggests viability of trans-RuH2(CO)(dpa) as a catalyst for the direct conversion of CO2 and H2 to methanol. Full article
(This article belongs to the Special Issue Catalysis and Catalytic Processes for CO2 Conversion)
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Review

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Open AccessReview
Molecular Catalysis for Utilizing CO2 in Fuel Electro-Generation and in Chemical Feedstock
Catalysts 2019, 9(9), 760; https://doi.org/10.3390/catal9090760 - 10 Sep 2019
Abstract
Processes for the conversion of CO2 to valuable chemicals are highly desired as a result of the increasing CO2 levels in the atmosphere and the subsequent elevating global temperature. However, CO2 is thermodynamically and kinetically inert to transformation and, therefore, [...] Read more.
Processes for the conversion of CO2 to valuable chemicals are highly desired as a result of the increasing CO2 levels in the atmosphere and the subsequent elevating global temperature. However, CO2 is thermodynamically and kinetically inert to transformation and, therefore, many efforts were made in the last few decades. Reformation/hydrogenation of CO2 is widely used as a means to access valuable products such as acetic acids, CH4, CH3OH, and CO. The electrochemical reduction of CO2 using hetero- and homogeneous catalysts recently attracted much attention. In particular, molecular CO2 reduction catalysts were widely studied using transition-metal complexes modified with various ligands to understand the relationship between various catalytic properties and the coordination spheres above the metal centers. Concurrently, the coupling of CO2 with various electrophiles under homogeneous conditions is also considered an important approach for recycling CO2 as a renewable C-1 substrate in the chemical industry. This review summarizes some recent advances in the conversion of CO2 into valuable chemicals with particular focus on the metal-catalyzed reductive conversion and functionalization of CO2. Full article
(This article belongs to the Special Issue Catalysis and Catalytic Processes for CO2 Conversion)
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Open AccessReview
Towards Higher Rate Electrochemical CO2 Conversion: From Liquid-Phase to Gas-Phase Systems
Catalysts 2019, 9(3), 224; https://doi.org/10.3390/catal9030224 - 01 Mar 2019
Abstract
Electrochemical CO2 conversion offers a promising route for value-added products such as formate, carbon monoxide, and hydrocarbons. As a result of the highly required overpotential for CO2 reduction, researchers have extensively studied the development of catalyst materials in a typical H-type [...] Read more.
Electrochemical CO2 conversion offers a promising route for value-added products such as formate, carbon monoxide, and hydrocarbons. As a result of the highly required overpotential for CO2 reduction, researchers have extensively studied the development of catalyst materials in a typical H-type cell, utilizing a dissolved CO2 reactant in the liquid phase. However, the low CO2 solubility in an aqueous solution has critically limited productivity, thereby hindering its practical application. In efforts to realize commercially available CO2 conversion, gas-phase reactor systems have recently attracted considerable attention. Although the achieved performance to date reflects a high feasibility, further development is still required in order for a well-established technology. Accordingly, this review aims to promote the further study of gas-phase systems for CO2 reduction, by generally examining some previous approaches from liquid-phase to gas-phase systems. Finally, we outline major challenges, with significant lessons for practical CO2 conversion systems. Full article
(This article belongs to the Special Issue Catalysis and Catalytic Processes for CO2 Conversion)
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