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Current Trends in Dry (CO2) Reforming Catalysis
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Current Trends in Dry (CO2) Reforming Catalysis

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

Deadline for manuscript submissions: closed (20 February 2022) | Viewed by 18772

Special Issue Editors

Prof. Dr. Bernhard Klötzer

E-Mail Website
Guest Editor
Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, A-6020 Innsbruck, Austria
Interests: Dynamics and Kinetics of chemical processes at surfaces Catalysis Bimetallic Catalysts Metal-Support-Interactions Corrosion Reconstruction and Phase Transformations at Metal Surfaces Catalytic Nanotechnology Reforming- and (Electro)Oxidation Catalysis on Complex Perovskites in-situ Spectroscopic Characterization of Catalysts using Ambient Pressure-XPS and Synchrotron Radiation
Dr. Simon Penner

E-Mail Website
Guest Editor
Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, A-6020 Innsbruck, Austria
Interests: high-resolution analytical electron microscopy in catalysis; structure-activity correlations in pure and complex oxide catalysts; interfacial engineering of the metal-oxide phase boundary; reactive activation of intermetallic compounds in catalysis; mechanism of methanol and methane steam reforming reactions; preparation and characterization of complex oxide, bi- and multimetallic thin film catalyst systems; operando and in situ structural and spectroscopic studies of catalysts
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Special Issue Information

Dear Colleagues,

In order to develop effective strategies to counteract man-made climate change, almost 200 countries decided to reduce greenhouse gas (GHG) emissions by adopting the “Paris Agreement”. The mitigation and cost-efficient utilization of the major GHGs carbon dioxide and methane represent two of the most important challenges in the area of green energy research. It is well-established that CO2 reforming of methane (in absence of steam: “dry” reforming of methane, DRM), or—more generally—of natural gas, represents a viable process to generate useful synthesis gas (H2 and CO). Beside the industrially ubiquitous steam reforming process, DRM thus represents an additional, effectively CO2-utilizing route toward added-value products and synfuels.

In order to become industrially relevant, the development of cost-effective DRM catalysts with both high activity and pronounced long-term sintering- and coking stability is mandatory. Ongoing catalyst design focuses on the optimization of equally active and coking-resistant (bi)metal components, on the suppression of nucleation and growth of unreactive graphitic species, as well as on the efficient formation and conversion of reactive carbonaceous intermediates. Development of supports and promoters focusses on efficient CO2 activation, on promotional (bi)metal-support interactions, and on optimization of (bi)metallic dispersion and particle size. Acid-base properties, oxygen storage capacity, reducibility, porosity, and surface area of the supporting (mixed) oxides represent further key optimization factors.

The current Special Issue is dedicated to the representation of contemporary trends of DRM catalyst design.

Prof. Dr. Bernhard Klötzer
Dr. Simon Penner
Guest Editors

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Keywords

  • metal support interactions
  • CO2 activation
  • (bi)metal particle size
  • graphite nucleation- and growth
  • carbon clean-off
  • carbon bulk diffusion
  • methane adsorption kinetics
  • acid-base properties
  • oxygen storage capacity
  • oxide reducibility

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Published Papers (3 papers)

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Research

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23 pages, 3729 KiB  
Article
Dry Reforming of Methane on NiCu and NiPd Model Systems: Optimization of Carbon Chemistry
by Philipp Zambaldi, Leander Haug, Simon Penner and Bernhard Klötzer
Catalysts 2022, 12(3), 311; https://doi.org/10.3390/catal12030311 - 9 Mar 2022
Cited by 13 | Viewed by 4325
Abstract
A series of ultra-clean, unsupported Cu-doped and Pd-doped Ni model catalysts was investigated to develop the fundamental concept of metal doping impact on the carbon tolerance and catalytic activity in the dry reforming of methane (DRM). Wet etching with concentrated HNO3 and [...] Read more.
A series of ultra-clean, unsupported Cu-doped and Pd-doped Ni model catalysts was investigated to develop the fundamental concept of metal doping impact on the carbon tolerance and catalytic activity in the dry reforming of methane (DRM). Wet etching with concentrated HNO3 and a subsequent single sputter–anneal cycle resulted in the full removal of an already existing oxidic passivation layer and segregated and/or ambient-deposited surface and bulk impurities to yield ultra-clean Ni substrates. Carbon solubility, support effects, segregation processes, cyclic operation temperatures, and electronic and ensemble effects were all found to play a crucial role in the catalytic activity and stability of these systems, as verified by X-ray photoelectron spectroscopy (XPS) surface and bulk characterization. Minor Cu promotion showed the almost complete suppression of coking with a moderate reduction in catalytic activity, while high Cu loadings facilitated carbon growth alongside severe catalytic deactivation. The improved carbon resistance stems from an increased CH4 dissociation barrier, decreased carbon solubility in the bulk, good prevailing CO2 activation properties and enhanced CO desorption. Cyclic DRM operation on surfaces with Cu content that is too high leads to impaired carbon oxidation kinetics by CO2 and causes irreversible carbon deposition. Thus, an optimal and stable NiCu composition was found in the region of 70–90 atomic % Ni, which allows an appropriate high syngas production rate to be retained alongside a total coking suppression during DRM. In contrast, the more Cu-rich NiCu systems showed a limited stability under reaction conditions, leading to undesired surface and bulk segregation processes of Cu. The much higher carbon deposition rate and solubility of unsupported NiPd and Pd model catalysts results in severe carbon deposition and catalytic deactivation. To achieve enhanced carbon conversion and de-coking, an active metal oxide boundary is required, allowing for the increased clean-off of re-segregated carbon via the inverse Boudouard reaction. The carbon bulk diffusion on the investigated systems depends strongly on the composition and decreases in the following order: Pd > NiPd > Ni > NiCu > Cu. Full article
(This article belongs to the Special Issue Current Trends in Dry (CO2) Reforming Catalysis)
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Review

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64 pages, 18001 KiB  
Review
Quo Vadis Dry Reforming of Methane?—A Review on Its Chemical, Environmental, and Industrial Prospects
by Luis E. Sandoval-Diaz, Robert Schlögl and Thomas Lunkenbein
Catalysts 2022, 12(5), 465; https://doi.org/10.3390/catal12050465 - 22 Apr 2022
Cited by 17 | Viewed by 5412
Abstract
In recent years, the catalytic dry reforming of methane (DRM) has increasingly come into academic focus. The interesting aspect of this reaction is seemingly the conversion of CO2 and methane, two greenhouse gases, into a valuable synthesis gas (syngas) mixture with an [...] Read more.
In recent years, the catalytic dry reforming of methane (DRM) has increasingly come into academic focus. The interesting aspect of this reaction is seemingly the conversion of CO2 and methane, two greenhouse gases, into a valuable synthesis gas (syngas) mixture with an otherwise unachievable but industrially relevant H2/CO ratio of one. In a possible scenario, the chemical conversion of CO2 and CH4 to syngas could be used in consecutive reactions to produce synthetic fuels, with combustion to harness the stored energy. Although the educts of DRM suggest a superior impact of this reaction to mitigate global warming, its potential as a chemical energy converter and greenhouse gas absorber has still to be elucidated. In this review article, we will provide insights into the industrial maturity of this reaction and critically discuss its applicability as a cornerstone in the energy transition. We derive these insights from assessing the current state of research and knowledge on DRM. We conclude that the entire industrial process of syngas production from two greenhouse gases, including heating with current technologies, releases at least 1.23 moles of CO2 per mol of CO2 converted in the catalytic reaction. Furthermore, we show that synthetic fuels derived from this reaction exhibit a negative carbon dioxide capturing efficiency which is similar to burning methane directly in the air. We also outline potential applications and introduce prospective technologies toward a net-zero CO2 strategy based on DRM. Full article
(This article belongs to the Special Issue Current Trends in Dry (CO2) Reforming Catalysis)
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30 pages, 31819 KiB  
Review
Prospects and Technical Challenges in Hydrogen Production through Dry Reforming of Methane
by Fábio Gonçalves Macêdo de Medeiros, Francisco Wendell Bezerra Lopes and Bruna Rego de Vasconcelos
Catalysts 2022, 12(4), 363; https://doi.org/10.3390/catal12040363 - 23 Mar 2022
Cited by 24 | Viewed by 7955
Abstract
Environmental issues related to greenhouse gases (GHG) emissions have pushed the development of new technologies that will allow the economic production of low-carbon energy vectors, such as hydrogen (H2), methane (CH4) and liquid fuels. Dry reforming of methane (DRM) [...] Read more.
Environmental issues related to greenhouse gases (GHG) emissions have pushed the development of new technologies that will allow the economic production of low-carbon energy vectors, such as hydrogen (H2), methane (CH4) and liquid fuels. Dry reforming of methane (DRM) has gained increased attention since it uses CH4 and carbon dioxide (CO2), which are two main greenhouse gases (GHG), as feedstock for the production of syngas, which is a mixture of H2 and carbon monoxide (CO) and can be used as a building block for the production of fuels. Since H2 has been identified as a key enabler of the energy transition, a lot of studies have aimed to benefit from the environmental advantages of DRM and to use it as a pathway for a sustainable H2 production. However, there are several challenges related to this process and to its use for H2 production, such as catalyst deactivation and the low H2/CO ratio of the syngas produced, which is usually below 1.0. This paper presents the recent advances in the catalyst development for H2 production via DRM, the processes that could be combined with DRM to overcome these challenges and the current industrial processes using DRM. The objective is to assess in which conditions DRM could be used for H2 production and the gaps in literature data preventing better evaluation of the environmental and economic potential of this process. Full article
(This article belongs to the Special Issue Current Trends in Dry (CO2) Reforming Catalysis)
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