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Catalysts
Special Issues
Catalytic Hydrogenation of CO2
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Catalytic Hydrogenation of CO2

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

Deadline for manuscript submissions: closed (31 March 2023) | Viewed by 33462

Special Issue Editors

Prof. Dr. Hengshan Qiu

E-Mail Website
Guest Editor
Research Center of Heterogeneous Catalysis and Engineering Sciences, School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China
Interests: heterogeneous catalysis; surface chemistry; reaction mechanism
Prof. Dr. Weifeng Tu

E-Mail Website
Guest Editor
Research Center of Heterogeneous Catalysis and Engineering Sciences, School of Chemical Engineering and Energy, Zhengzhou University, Zhengzhou 450001, China
Interests: heterogeneous catalysis; intrinsic kinetics; hydrogenation of CO/CO2/O2

Special Issue Information

Dear colleagues,

We are now announcing a new Special Issue entitled “Catalytic hydrogenation of CO2”.

The consumption level of fossil resources has somewhat become an indication of the economic level of countries around the world since about 150 years ago. Unfortunately, the consumption of fossil resources is always accompanied with the emission of CO2—one of the most important human-made green-house gases. The atmospheric CO2 concentration has increased abruptly since the middle of the last century and reached the highest level nowadays (in the past two million years). We have even noticeably felt the rising impact of worldwide extreme weather on our daily life in the recent years, although the direct correlation with CO2 emissions is still a scientific topic. It is urgent for human beings to keep the CO2 emissions at a safe level. Measures may include the reduction of emissions, capture and storage, conversion to value-added chemicals, and so forth.

For the conversion, the typically utilized way is the catalytic hydrogenation of CO2, which includes thermocatalytic, electrochemical, biochemical, plasma, photocatalytic methods, etc. A growing amount of excellent work has been carried out on CO2 hydrogenation to produce CO, methanol, light olefin, dimethyl ether, methane, etc. However, efficient catalysts with combined high activity, selectivity and stability are still the ultimate aim to pursue. In addition, microscopic insight into the catalytic mechanism on an elemental level may speed up the design and exploitation of novel catalysts.

This Special Issue aims to shed light on the recent fundamental and technological advances of the catalytic hydrogenation of CO2. Contributions based on experimental observation, theoretical simulation, industrial data and other related novel ideas are of great interest.

Prof. Dr. Hengshan Qiu
Prof. Dr. Weifeng Tu
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

  • CO2 hydrogenation
  • heterogeneous catalysis
  • active site
  • mechanism
  • reaction kinetics
  • selectivity
  • theoretical simulation
  • operando spectroscopy
  • synergistic effect
  • single atom catalysts
  • supported catalysts
  • oxide catalysts

Published Papers (6 papers)

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Research

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17 pages, 6125 KiB  
Article
Influence of Cu/Al Ratio on the Performance of Carbon-Supported Cu/ZnO/Al2O3 Catalysts for CO2 Hydrogenation to Methanol
by Zhong Xie, Jinpei Hei, Lei Cheng, Jing Li, Xiaojie Yin and Sugang Meng
Catalysts 2023, 13(5), 800; https://doi.org/10.3390/catal13050800 - 25 Apr 2023
Viewed by 2300
Abstract
CO2 hydrogenation to methanol was conducted using a set of activated carbon-supported Cu/ZnO/Al2O3 catalysts (CCZA) prepared by an incipient wetness impregnation approach. The effect of the Cu/Al ratio on the physicochemical properties of the catalysts, as well as their [...] Read more.
CO2 hydrogenation to methanol was conducted using a set of activated carbon-supported Cu/ZnO/Al2O3 catalysts (CCZA) prepared by an incipient wetness impregnation approach. The effect of the Cu/Al ratio on the physicochemical properties of the catalysts, as well as their catalytic performance, were investigated. As Cu/Al ratio increased, the metallic Cu surface area displayed a reducing trend from 6.88 to 4.18 m2∙gcat−1, while the CO2 adsorption capacity exhibited an increasing trend. Meanwhile, aluminum content will have an important effect on the catalysts’ reducibility and, thus, on their catalytic performance. The CCZA-2.7-de catalyst demonstrated the highest selectivity to methanol at 83.75% due to the excellent distribution and synergistic effect of copper and zinc. Although the CO2 conversion of CCZA-2.2-de and CCZA-3.5-de exceeded 10%, the CH3OH selectivity was less than 60%, which may be attributed to the larger particle sizes of ZnO and poor interactions in Cu–Zn. The present study offers a novel approach to increase the number of active sites, optimize the activated carbon-aided Cu/ZnO/Al2O3 catalyst’s composition, and finally elucidate the mechanism for CO2 hydrogenation to methanol. Full article
(This article belongs to the Special Issue Catalytic Hydrogenation of CO2)
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15 pages, 7217 KiB  
Article
Preparation of C3N4 Thin Films for Photo-/Electrocatalytic CO2 Reduction to Produce Liquid Hydrocarbons
by Jin You Zheng, Amol Uttam Pawar and Young Soo Kang
Catalysts 2022, 12(11), 1399; https://doi.org/10.3390/catal12111399 - 09 Nov 2022
Cited by 4 | Viewed by 2151
Abstract
Thermal vapor condensation of melamine at various temperatures was used to fabricate thin graphitic carbon nitride (g-C3N4) films on fluorine-doped tin oxide (FTO) coated glass substrates. Photoanodic (n-type) and photocathodic (p-type) responses were observed simultaneously in the g-C3 [...] Read more.
Thermal vapor condensation of melamine at various temperatures was used to fabricate thin graphitic carbon nitride (g-C3N4) films on fluorine-doped tin oxide (FTO) coated glass substrates. Photoanodic (n-type) and photocathodic (p-type) responses were observed simultaneously in the g-C3N4 films. The g-C3N4 film formed at 520 °C with the longest average lifetime of the photo-excited electrons shows the best cathodic photocurrent performance, which was then chosen for electrochemical and photoelectrochemical reduction of CO2. When the basic electrolyte (CO2-saturated 0.5 M KHCO3, pH = 7.6) was adopted, CO2 was electrochemically converted into formaldehyde ((54.6 μM/h)) in the liquid product. When the acidic electrolyte (CO2-saturated 0.5 M KCl, pH = 4.1) was adopted, formaldehyde (39.5 μM/h) and ethanol (15.7 μM/h) were generated through photoelectrochemical reduction, stimulated by the presence of sufficient protons from the electrolyte in the reduction process. Therefore, the pure g-C3N4 film has a great potential for CO2 reduction to value-added liquid hydrocarbons products via electrochemical or photoelectrochemical ways. Full article
(This article belongs to the Special Issue Catalytic Hydrogenation of CO2)
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17 pages, 895 KiB  
Article
Detailed Kinetic Modeling of CO2-Based Fischer–Tropsch Synthesis
by Lucas Brübach, Daniel Hodonj, Linus Biffar and Peter Pfeifer
Catalysts 2022, 12(6), 630; https://doi.org/10.3390/catal12060630 - 09 Jun 2022
Cited by 5 | Viewed by 2895
Abstract
The direct hydrogenation of CO2 to long-chain hydrocarbons, so called CO2-based Fischer–Tropsch synthesis (FTS), is a viable future production route for various hydrocarbons used in the chemical industry or fuel applications. The detailed modeling of the reactant consumption and product [...] Read more.
The direct hydrogenation of CO2 to long-chain hydrocarbons, so called CO2-based Fischer–Tropsch synthesis (FTS), is a viable future production route for various hydrocarbons used in the chemical industry or fuel applications. The detailed modeling of the reactant consumption and product distribution is very important for further process improvements but has gained only limited attention so far. We adapted proven modeling approaches from the traditional FTS and developed a detailed kinetic model for the CO2-FTS based on experiments with an Fe based catalyst in a lab-scale tubular reactor. The model is based on a direct CO2 dissociation mechanism for the reverse water gas shift and the alkyl mechanism with an H-assisted CO dissociation step for the FTS. The model is able to predict the reactant consumption, as well as the hydrocarbon distribution, reliably within the experimental range studied (10 bar, 280–320 °C, 900–120,000 mLN h−1 g−1 and H2/CO2 molar inlet ratios of 2–4) and demonstrates the applicability of traditional FTS models for the CO2-based synthesis. Peculiarities of the fractions of individual hydrocarbon classes (1-alkenes, n-alkanes, and iso-alkenes) are accounted for with chain-length-dependent kinetic parameters for branching and dissociative desorption. However, the reliable modeling of class fractions for high carbon number products (>C12) remains a challenge not only from a modeling perspective but also from product collection and analysis. Full article
(This article belongs to the Special Issue Catalytic Hydrogenation of CO2)
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Review

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24 pages, 3717 KiB  
Review
Hydrogenation of CO2 to Olefins over Iron-Based Catalysts: A Review
by Wenqi Liu, Sifan Cheng, Haripal Singh Malhi, Xinhua Gao, Zhenzhou Zhang and Weifeng Tu
Catalysts 2022, 12(11), 1432; https://doi.org/10.3390/catal12111432 - 14 Nov 2022
Cited by 7 | Viewed by 3958
Abstract
The widespread use of fossil fuels has caused high CO2 concentrations in the atmosphere, which have had a great impact on climate and the environment. Methods for efficiently utilizing CO2 to produce high value-added chemicals have received increasing attention. Among the [...] Read more.
The widespread use of fossil fuels has caused high CO2 concentrations in the atmosphere, which have had a great impact on climate and the environment. Methods for efficiently utilizing CO2 to produce high value-added chemicals have received increasing attention. Among the products of CO2 hydrogenation, olefins, an important petrochemical feedstock, are one of the essential target products. Therefore, CO2 hydrogenation to olefins has been extensively studied, especially for the development of high-performance catalysts. Iron-based catalysts, which are widely used in Fischer–Tropsch synthesis reactions, have also been considered attractive for use in the CO2 hydrogenation to olefins due to their excellent performance in catalytic activity and reaction stability. Most studies have focused on the modulation of morphology; reduction and adsorption properties by tuning the methods of catalyst syntheses; pretreatment conditions and the composition of catalysts, in order to improve hydrogenation activity and olefin yield. In this review, we briefly discuss a thermodynamic overview of the CO2 hydrogenation to olefins reaction, the optimization of catalyst modifications, and current insights into the reaction mechanism; moreover, we summarize current challenges and future trends in the CO2 hydrogenation to olefins. Full article
(This article belongs to the Special Issue Catalytic Hydrogenation of CO2)
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33 pages, 3775 KiB  
Review
Catalytic Hydrogenation of CO2 to Methanol: A Review
by Menghao Ren, Yanmin Zhang, Xuan Wang and Hengshan Qiu
Catalysts 2022, 12(4), 403; https://doi.org/10.3390/catal12040403 - 06 Apr 2022
Cited by 44 | Viewed by 15785
Abstract
High-efficiency utilization of CO2 facilitates the reduction of CO2 concentration in the global atmosphere and hence the alleviation of the greenhouse effect. The catalytic hydrogenation of CO2 to produce value-added chemicals exhibits attractive prospects by potentially building energy recycling loops. [...] Read more.
High-efficiency utilization of CO2 facilitates the reduction of CO2 concentration in the global atmosphere and hence the alleviation of the greenhouse effect. The catalytic hydrogenation of CO2 to produce value-added chemicals exhibits attractive prospects by potentially building energy recycling loops. Particularly, methanol is one of the practically important objective products, and the catalytic hydrogenation of CO2 to synthesize methanol has been extensively studied. In this review, we focus on some basic concepts on CO2 activation, the recent research advances in the catalytic hydrogenation of CO2 to methanol, the development of high-performance catalysts, and microscopic insight into the reaction mechanisms. Finally, some thinking on the present research and possible future trend is presented. Full article
(This article belongs to the Special Issue Catalytic Hydrogenation of CO2)
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19 pages, 7109 KiB  
Review
Activation of Small Molecules and Hydrogenation of CO2 Catalyzed by Frustrated Lewis Pairs
by Ranita Pal, Manas Ghara and Pratim Kumar Chattaraj
Catalysts 2022, 12(2), 201; https://doi.org/10.3390/catal12020201 - 07 Feb 2022
Cited by 18 | Viewed by 4717
Abstract
The chemistry of frustrated Lewis pair (FLP) is widely explored in the activation of small molecules, the hydrogenation of CO2, and unsaturated organic species. A survey of several experimental works on the activation of small molecules by FLPs and the related [...] Read more.
The chemistry of frustrated Lewis pair (FLP) is widely explored in the activation of small molecules, the hydrogenation of CO2, and unsaturated organic species. A survey of several experimental works on the activation of small molecules by FLPs and the related mechanistic insights into their reactivity from electronic structure theory calculation are provided in the present review, along with the catalytic hydrogenation of CO2. The mechanistic insight into H2 activation is thoroughly discussed, which may provide a guideline to design more efficient FLP for H2 activation. FLPs can activate other small molecules like, CO, NO, CO2, SO2, N2O, alkenes, alkynes, etc. by cooperative action of the Lewis centers of FLPs, as revealed by several computational analyses. The activation barrier of H2 and other small molecules by the FLP can be decreased by utilizing the aromaticity criterion in the FLP as demonstrated by the nucleus independent chemical shift (NICS) analysis. The term boron-ligand cooperation (BLC), which is analogous to the metal-ligand cooperation (MLC), is invoked to describe a distinct class of reactivity of some specific FLPs towards H2 activation. Full article
(This article belongs to the Special Issue Catalytic Hydrogenation of CO2)
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