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Catalytic Reforming and Hydrogen Production: From the Past to the Future

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

Deadline for manuscript submissions: closed (30 November 2024) | Viewed by 16271

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Dr. Georgios Bampos

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Guest Editor

Department of Chemical Engineering, University of Patras, 26504 Patras, Greece
Interests: catalysis; electrocatalysis; electrochemistry; advanced oxidation processes; hydrocarbon reforming; CO₂ reduction
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Dr. Paraskevi Panagiotopoulou

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Guest Editor

School of Environmental Engineering, Technical University of Crete, GR-73100 Chania, Greece
Interests: methane production; catalyst; synthesis gas; hydrogen production; steam reforming; WGS reaction
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Dr. Eleni A. Kyriakidou

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Guest Editor

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA
Interests: heterogeneous catalysis; nanoparticle synthesis; surface science; catalysts; environmental processes
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The Special Issue is dedicated to the exploration of catalytic reforming and hydrogen production, delving into a journey starting in the past of these processes and ending in their future applications. The catalytic reforming of light hydrocarbons stands out as a prominent technique for generating valuable products like synthesis gas. Syngas, a crucial intermediary substance in the creation of hydrogen, ammonia, methanol, and synthetic hydrocarbon fuels, holds significant potential for fostering a cleaner, more sustainable energy environment. Furthermore, through advancements in catalyst development, reactor designs, and process optimization strategies, hydrogen has emerged as a pivotal player in the global energy shift towards a more efficient and sustainable hydrogen economy.

This Special Issue aims to showcase the most recent research findings in heterogeneous catalysis concerning catalytic reforming and hydrogen production, assuming a future where clean energy takes center stage. We invite submissions in the form of original research papers or reviews that reflect the state of the art of this research area. Topics of interest include, but are not limited to, the following:

Methane conversion.
Dry reforming.
CO₂ methanation.
Hydrogen production processes.
Water–gas shift (WGS) reaction.
Production of syngas.
Fischer–Tropsch synthesis.
Fuel cells.

Dr. Georgios Bampos
Dr. Paraskevi Panagiotopoulou
Dr. Eleni A. Kyriakidou
Guest Editors

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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 2200 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

syngas
hydrogen production
steam reforming
CO₂ methanation
water gas shift (WGS) reaction
fuels
clean energy
hydrocarbons to fuels
fuel cells

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Related Special Issue

Catalytic Reforming and Hydrogen Production: From the Past to the Future, 2nd Edition in Catalysts (1 article)

Published Papers (11 papers)

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Editorial

Jump to: Research, Review

4 pages, 152 KiB

Open AccessEditorial

Catalytic Reforming and Hydrogen Production: From the Past to the Future

by Georgios Bampos, Paraskevi Panagiotopoulou and Eleni A. Kyriakidou

Catalysts 2025, 15(4), 332; https://doi.org/10.3390/catal15040332 - 31 Mar 2025

Viewed by 417

Abstract

Continuously increasing energy demands and the intense environmental pollution caused by the increasing global population and modern lifestyles have driven research interest toward finding alternative sustainable energy sources [...] Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

Research

Jump to: Editorial, Review

16 pages, 3071 KiB

Open AccessArticle

Effect of Calcination-Induced Oxidation on the Photocatalytic H₂ Production Performance of Cubic Cu₂O/CuO Composite Photocatalysts

by Chi-Jung Chang, Chun-Wen Kang and Arul Pundi

Catalysts 2024, 14(12), 926; https://doi.org/10.3390/catal14120926 - 16 Dec 2024

Viewed by 950

Abstract

This study explores the H₂ production performance of CuO/Cu₂O with different morphology (nanocubes) synthesized by different methods using different sacrificial reagent (lactic acid), compared with the other three reported CuO/Cu₂O photocatalysts used for H₂ production. A cubic Cu₂O photocatalyst was prepared using a hydrothermal method. It was then calcined at a certain temperature to form a cubic Cu₂O/CuO composite photocatalyst. XRD, TEM, and XPS spectra confirmed the successful synthesis of cubic Cu₂O/CuO composite photocatalysts by calcination-induced oxidation at a certain temperature. As the calcination temperature increases, the crystal phase of the photocatalyst changes from Cu₂O to Cu₂O/CuO and then to CuO. The effects of calcination-induced oxidation on morphology, light absorption, the separation of photoexcited carriers, and the H₂ production activity of photocatalysts were studied. EPR spectra were monitored to analyze the oxygen vacancies in different samples. Mott–Schottky and Tauc plots were utilized to establish the band structure of the composite photocatalyst. Cu₂O/CuO is a type II photocatalyst with a heterogeneous structure that helps to improve electron–hole separation efficiency. The H₂ production efficiency of Cu₂O/CuO composite photocatalyst reaches 11,888 μmol h⁻¹g⁻¹, 1.6 times that of Cu₂O. The formation of the Cu₂O/CuO heterojunction leads to enhanced light absorption, charge separation, and hydrogen production activity. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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11 pages, 3582 KiB

Open AccessArticle

Hydrothermal Synthesis of La-MoS₂ and Its Catalytic Activity for Improved Hydrogen Evolution Reaction

by Archana Chaudhary, Rais Ahmad Khan, Sultan Saad Almadhhi, Ali Alsulmi, Khursheed Ahmad and Tae Hwan Oh

Catalysts 2024, 14(12), 893; https://doi.org/10.3390/catal14120893 - 5 Dec 2024

Viewed by 1366

Abstract

Herein, we report the synthesis and characterization of lanthanum-doped MoS₂ (La-MoS₂) via a hydrothermal route. The synthesized La-MoS₂ was characterized using powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), and energy-dispersive X-ray (EDX) techniques. The band gap of La-MoS₂ was observed to be 1.68 eV, compared to 1.80 eV for synthesized MoS₂. In the photoluminescence (PL) spectra, a decrease in the intensity was observed for La-MoS₂ compared to MoS₂, which suggests that due to doping with charged La³⁺, separation increases. The as-synthesized MoS₂ and La-MoS₂ were used for photocatalytic hydrogen evolution reactions (HERs), exhibiting 928 µmol·g⁻¹ evolution of H₂ in five hours for a 10 mg dose of La-MoS₂, compared to 612 µmol·g⁻¹ for MoS₂. A 50 mg mass of the catalyst (La-MoS₂) exhibited enhanced H₂ production of 1670 µmol·g⁻¹ after five hours. The higher rate of the HER for La-MoS₂ is because of doping with La³⁺. The photocatalytic hydrogen evolution performance of La-MoS₂ was also evaluated for different doses of La-MoS₂ exhibiting reusability up to the fourth cycle, showing potential applications of La-MoS₂ in hydrogen evolution reactions. Mechanistic aspects of the HER on the surface of La-MoS₂ have also been discussed. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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16 pages, 7807 KiB

Open AccessArticle

Aqueous Phase Reforming by Platinum Catalysts: Effect of Particle Size and Carbon Support

by Xuan Trung Nguyen, Ella Kitching, Thomas Slater, Emanuela Pitzalis, Jonathan Filippi, Werner Oberhauser and Claudio Evangelisti

Catalysts 2024, 14(11), 798; https://doi.org/10.3390/catal14110798 - 7 Nov 2024

Viewed by 1614

Abstract

Aqueous phase reforming (APR) is a promising method for producing hydrogen from biomass-derived feedstocks. In this study, carbon-supported Pt catalysts containing particles of different sizes (below 3 nm) were deposited on different commercially available carbons (i.e., Vulcan XC72 and Ketjenblack EC-600JD) using the metal vapor synthesis approach, and their catalytic efficiency and stability were evaluated in the aqueous phase reforming of ethylene glycol, the simplest polyol containing both C–C and C–O bonds. High-surface-area carbon supports were found to stabilize Pt nanoparticles with a mean diameter of 1.5 nm, preventing metal sintering. In contrast, Pt single atoms and clusters (below 0.5 nm) were not stable under the reaction conditions, contributing minimally to catalytic activity and promoting particle growth. The most effective catalyst Pt_A/C^K, containing a mean Pt NP size of 1.5 nm and highly dispersed on Ketjenblack carbon, demonstrated high hydrogen site time yield (8.92 min⁻¹ at 220 °C) and high stability under both high-temperature treatment conditions and over several recycling runs. The catalyst was also successfully applied to the APR of polyethylene terephthalate (PET), showing potential for hydrogen production from plastic waste. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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12 pages, 8618 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Hydrogen and CO Over-Equilibria in Catalytic Reactions of Methane Reforming

by Vitaliy R. Trishch, Mykhailo O. Vilboi, Gregory S. Yablonsky and Dmytro O. Kovaliuk

Catalysts 2024, 14(11), 773; https://doi.org/10.3390/catal14110773 - 31 Oct 2024

Cited by 1 | Viewed by 941

Abstract

Hydrogen and carbon monoxide over-equilibria have been found computationally in kinetic dependencies of methane-reforming catalytic reactions (steam and dry reforming) using the conditions of the conservatively perturbed equilibrium (CPE) phenomenon, i.e., at the initial equilibrium concentration of hydrogen or carbon monoxide. The influence of the pressure, temperature, flow rate and composition of the initial mixture on the position of the CPE point (the extremum point) was investigated over a wide domain of parameters. The CPE phenomenon significantly increases the product concentration (H₂ and CO) at the reactor length, which is significantly less than the reactor length required to reach equilibrium. The CPE point is interpreted as the “turning point” in kinetic behaviour. Recommendations on temperature and pressure regimes are different from the traditional ones related to Le Chatelier’s law. The obtained results provide valuable information on optimal reaction conditions for complex reversible chemical transformations, offering potential applications in chemical engineering processes. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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18 pages, 4765 KiB

Open AccessArticle

Kinetic Characterization of Pt/Al₂O₃ Catalyst for Hydrogen Production via Methanol Aqueous-Phase Reforming

by José Sousa, Paranjeet Lakhtaria, Paulo Ribeirinha, Werneri Huhtinen, Johan Tallgren and Adélio Mendes

Catalysts 2024, 14(10), 741; https://doi.org/10.3390/catal14100741 - 21 Oct 2024

Cited by 1 | Viewed by 1614

Abstract

Compared to steam reforming, methanol aqueous-phase reforming (APR) converts methanol to hydrogen and carbon dioxide at lower temperatures, but also displays lower conversion rates. Herein, methanol APR is studied over the active Pt/Al₂O₃ catalyst under different operating conditions. Studies were conducted at different temperatures, pressures, methanol mass fractions, and residence times. APR performance was evaluated in terms of methanol conversion, hydrogen production rate, hydrogen selectivity, and by-product formation. The results revealed that an increase in operating pressure and methanol mass fraction had an adverse effect on the APR performance. Conversely, it was found that hydrogen selectivity was unaffected by the operating pressure and residence time for the methanol feed mass fraction of 5%. For the methanol feed mass fraction of 55%, hydrogen selectivity was improved by operating pressure and residence time. The alumina support phase change to boehmite as well as sintering and leaching of the catalytic particles were observed during catalyst stability experiments. Additionally, a comparison between methanol steam reforming (MSR) and APR was also performed. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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20 pages, 5958 KiB

Open AccessArticle

Dry Reforming of Methane (DRM) over Hydrotalcite-Based Ni-Ga/(Mg, Al)O_x Catalysts: Tailoring Ga Content for Improved Stability

by Ahmed Y. Elnour, Ahmed E. Abasaeed, Anis H. Fakeeha, Ahmed A. Ibrahim, Salwa B. Alreshaidan and Ahmed S. Al-Fatesh

Catalysts 2024, 14(10), 721; https://doi.org/10.3390/catal14100721 - 16 Oct 2024

Cited by 1 | Viewed by 1780

Abstract

Dry reforming of methane (DRM) is a promising way to convert methane and carbon dioxide into syngas, which can be further utilized to synthesize value-added chemicals. One of the main challenges for the DRM process is finding catalysts that are highly active and stable. This study explores the potential use of Ni-based catalysts modified by Ga. Different Ni-Ga/(Mg, Al)O_x catalysts, with various Ga/Ni molar ratios (0, 0.1, 0.3, 0.5, and 1), were synthesized by the co-precipitation method. The catalysts were tested for the DRM reaction to evaluate their activity and stability. The Ni/(Mg, Al)O_x and its Ga-modified Ni-Ga/(Mg, Al)O_x were characterized by N₂ adsorption–desorption, Fourier Transform Infrared Spectroscopy (FTIR), H₂-temperature-programmed reduction (TPR), X-ray diffraction (XRD), thermogravimetric analysis (TGA) and Raman techniques. The test of catalytic activity, at 700 °C, 1 atm, GHSV of 42,000 mL/h/g, and a CH₄: CO₂ ratio of 1, revealed that Ga incorporation effectively enhanced the catalyst stability. Particularly, the Ni-Ga/(Mg, Al)O_x catalyst with Ga/Ni ratio of 0.3 exhibited the best catalytic performance, with CH₄ and CO₂ conversions of 66% and 74%, respectively, and an H₂/CO ratio of 0.92. Furthermore, the CH₄ and CO₂ conversions increased from 34% and 46%, respectively, when testing at 600 °C, to 94% and 96% when the catalytic activity was operated at 850 °C. The best catalyst’s 20 h stream performance demonstrated its great stability. DFT analysis revealed an alteration in the electronic properties of nickel upon Ga incorporation, the d-band center of the Ga modified catalyst (Ga/Ni ratio of 0.3) shifted closer to the Fermi level, and a charge transfer from Ga to Ni atoms was observed. This research provides valuable insights into the development of Ga-modified catalysts and emphasizes their potential for efficient conversion of greenhouse gases into syngas. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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18 pages, 2811 KiB

Open AccessFeature PaperArticle

Are Rh Catalysts a Suitable Choice for Bio-Oil Reforming? The Case of a Commercial Rh Catalyst in the Combined H₂O and CO₂ Reforming of Bio-Oil

by José Valecillos, Leire Landa, Gorka Elordi, Aingeru Remiro, Javier Bilbao and Ana Guadalupe Gayubo

Catalysts 2024, 14(9), 571; https://doi.org/10.3390/catal14090571 - 29 Aug 2024

Cited by 1 | Viewed by 1018

Abstract

Bio-oil combined steam/dry reforming (CSDR) with H₂O and CO₂ as reactants is an attractive route for the joint valorization of CO₂ and biomass towards the sustainable production of syngas (H₂ + CO). The technological development of the process requires the use of an active and stable catalyst, but also special attention should be paid to its regeneration capacity due to the unavoidable and quite rapid catalyst deactivation in the reforming of bio-oil. In this work, a commercial Rh/ZDC (zirconium-doped ceria) catalyst was tested for reaction–regeneration cycles in the bio-oil CSDR in a fluidized bed reactor, which is beneficial for attaining an isothermal operation and, moreover, minimizes catalyst deactivation by coke deposition compared to a fixed-bed reactor. The fresh, spent, and regenerated catalysts were characterized using either N₂ physisorption, H₂-TPR, TPO, SEM, TEM, or XRD. The Rh/ZDC catalyst is initially highly active for the syngas production (yield of 77% and H₂/CO ratio of 1.2) and for valorizing CO₂ (conversion of 22%) at 700 °C, with space time of 0.125 g_catalyst h (g_oxygenates)⁻¹ and CO₂/H₂O/C ratio of 0.6/0.5/1. The catalyst activity evolves in different periods that evidence a selective deactivation of the catalyst for the reforming reactions of the different compounds, with the CH₄ reforming reactions (with both steam and CO₂) being more rapidly affected by catalyst deactivation than the reforming of hydrocarbons or oxygenates. After regeneration, the catalyst’s textural properties are not completely restored and there is a change in the Rh–support interaction that irreversibly deactivates the catalyst for the CH₄ reforming reactions (both SR and DR). As a result, the coke formed over the regenerated catalyst is different from that over the fresh catalyst, being an amorphous mass (of probably turbostractic nature) that encapsulates the catalyst and causes rapid deactivation. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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19 pages, 5418 KiB

Open AccessArticle

Ni-Ag Catalysts for Hydrogen Production through Dry Reforming of Methane: Characterization and Performance Evaluation

by Hayat Henni, Rafik Benrabaa, Pascal Roussel and Axel Löfberg

Catalysts 2024, 14(7), 400; https://doi.org/10.3390/catal14070400 - 25 Jun 2024

Cited by 4 | Viewed by 1706

Abstract

To investigate the influence of Ag and the loading of Ni species, Ni-Ag type catalysts were synthesized with varying Ni/Ag ratios (1, 1.5 and 2) using the coprecipitation method. The catalysts were extensively characterized using various techniques such as TG-DSC-SM, XRD, ICP, BET, SEM-EDX and TPR and subsequently tested in the CH₄/CO₂ reaction without any pretreatment. Regardless of the ratio employed, a phase mixture containing NiO and Ag was observed after calcination under air between 600 °C and 1200 °C. SEM analysis confirmed the presence of a close interface between Ag and NiO. The specific surface area was found to be significantly higher for the catalyst with lower Ni content (R = 1). TPR analysis demonstrated that the inclusion of Ag facilitated the reduction of Ni at lower temperatures. XRD analyses of the spent catalyst confirmed catalyst reduction during the reaction. Among the samples, a catalyst with Ni/Ag = 1 exhibited superior catalytic activity without any pretreatment under a reduction atmosphere, in which case the conversions of methane and CO₂ at 650 °C amounted to 38 and 45 mol%, respectively, with H₂/CO = 0.7 and 71 mol% of H₂. The presence of Ag species enhances the stability of the Ni catalyst and improves catalytic performance in the dry reforming of methane. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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Review

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37 pages, 5272 KiB

Open AccessFeature PaperReview

Review on Synthesis and Catalytic Properties of Cobalt Manganese Oxide Spinels (Co_xMn_3−xO₄, 0 < x < 3)

by Kende Attila Béres, Zoltán Homonnay and László Kótai

Catalysts 2025, 15(1), 82; https://doi.org/10.3390/catal15010082 - 16 Jan 2025

Viewed by 1375

Abstract

The cobalt manganese oxides, especially the spinels and related (multiphase) materials described with the formula Co_xMn_3−xO₄ (0 < x < 3), are widely used catalysts in a range of processes in significant industrial and environmental areas. The great diversity in the phase relations, composition, and metal ion valences, together with ion and vacancy site distribution variations, results in great variety and activity as catalysts in various industrially important redox processes such as the removal of CO or volatile organic substances (VOCs) from the air and oxidative destruction of pollutants such as dyes and pharmaceuticals from wastewater using peroxides. These mixed oxides can gain application in the selective oxidation of organic molecules like 5-hydroxyfurfural or aromatic alcohols such as vanillyl alcohol or in the production of fuels and other valuable chemicals (alcohols, esters) with the Fischer–Tropsch method. In this review, we summarize these redox-based reactions in light of the chemical and phase composition of the catalysts with the formula Co_xMn_3−xO₄ with 0 < x < 3. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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35 pages, 4170 KiB

Open AccessFeature PaperReview

Recent Advances in Methanol Steam Reforming Catalysts for Hydrogen Production

by Mengyuan Zhang, Diru Liu, Yiying Wang, Lin Zhao, Guangyan Xu, Yunbo Yu and Hong He

Catalysts 2025, 15(1), 36; https://doi.org/10.3390/catal15010036 - 3 Jan 2025

Cited by 2 | Viewed by 2264

Abstract

The pursuit of carbon neutrality has accelerated advancements in sustainable hydrogen production and storage methods, increasing the importance of methanol steam reforming (MSR) technology. Catalysts are central to MSR technology and are primarily classified into copper-based and noble metal-based catalysts. This review begins with an examination of the active components of these catalysts, tracing the evolution of the understanding of active sites over the past four decades. It then explores the roles of various supports and promoters, along with mechanisms of catalyst deactivation. To address the diverse perspectives on the MSR reaction mechanism, the existing research is systematically organized and synthesized, providing a detailed account of the reaction mechanisms associated with both catalyst types. The discussion concludes with a forward-looking perspective on MSR catalyst development, emphasizing strategies such as anti-sintering methods for copper-based catalysts, approaches to reduce byproduct formation in palladium-based catalysts, comprehensive research methodologies for MSR mechanisms, and efforts to enhance atomic utilization efficiency. Full article

(This article belongs to the Special Issue Catalytic Reforming and Hydrogen Production: From the Past to the Future)

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