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Catalysts for Production and Conversion of Syngas

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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 2020) | Viewed by 50404

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Dr. Rufino Navarro Yerga

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Instituto de Catálisis y Petroleoquímica (CSIC), C/Marie Curie 2, Cantoblanco, 28049 Madrid, Spain
Interests: heterogeneous catalysis; catalytic hydrogen production; catalytic steam reforming; catalytic partial oxidation; WGS; SCR-NOx; photocatalytic hydrogen production
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Prof. Dr. José Luis García Fierro

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Instituto de Catálisis y Petroleoquímica (CSIC), C/ Marie Curie 2, Cantoblanco, 28049 Madrid, Spain
Interests: heterogeneous catalysts for the direct and indirect conversion of methane to syngas and methanol, conversion of light alkanes into olefins, hydrodesulfurization and oxidesulfurization of middle distillates, de-NOx of industrial effluents, three-way catalysts for exhaust treatment, reforming of light and heavy hydrocarbons, catalytic combustion reactions, CO2 valorization

Special Issue Information

Dear Colleagues,

Synthesis gas or, briefly, syngas, is a mixture of CO, CO₂, and H₂. Syngas is a crucial platform for the production of a variety of products including synthetic hydrocarbons and oxygenates fuels. This Special Issue compiles and reviews the latest advances in catalytic production from several sources (fossil, biomass) and the conversion of syngas into value-added products. Catalytic processes for Syngas production will be revised including production from natural gas, coal, biomass, or virtually any hydrocarbon feedstock, by reaction with steam or oxygen. with an emphasis on the selective production of low molecular weight alcohols (C_nOH, n = 1 − 5), dimethyl ether (DME), light olefins (C2-C4, which are key building block chemicals), and hydrocarbons (C5+ as liquid fuels). Recent advances in understanding and developing active phases, supports, promoters, and reactor configurations to control the selectivity in the syngas production and conversion are the most challenging subjects for scientific research in syngas conversion. This Special Issue provides insight into the challenges surrounding syngas conversion and the initiatives in catalysis research undertaken to overcome those. Submissions are welcome in the form of original research papers or short reviews that reflect the state-of-the-art of this research area.

Dr. Rufino M. Navarro Yerga
Prof. Dr. Jose Luis García Fierro
Guest Editors

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Keywords

Production of syngas
Syngas to methanol
Syngas to alcohols
Syngas to lower olefins
Syngas to DME
Heterogeneous catalysts
Fischer–Tropsch synthesis

Published Papers (13 papers)

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Editorial

Jump to: Research, Review

4 pages, 178 KiB

Open AccessEditorial

Catalysts for Production and Conversion of Syngas

by Rufino M. Navarro Yerga

Catalysts 2021, 11(6), 752; https://doi.org/10.3390/catal11060752 - 21 Jun 2021

Cited by 10 | Viewed by 2996

Abstract

Synthesis gas, or syngas for short, is a mixture of CO, CO₂, and H₂ [...] Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

2 pages, 715 KiB

Open AccessEditorial

Remembering Professor Jose Luis García Fierro (1948–2020)

by Rufino M. Navarro Yerga

Catalysts 2020, 10(4), 357; https://doi.org/10.3390/catal10040357 - 25 Mar 2020

Cited by 1 | Viewed by 2699

Abstract

On 3 February, Professor Jose Luis Garcia Fierro died in Madrid, Spain, at the age of 71 [...] Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

Research

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10 pages, 2346 KiB

Open AccessArticle

Integrating Syngas Fermentation into a Single-Cell Microbial Electrosynthesis (MES) Reactor

by Vasan Sivalingam, Vafa Ahmadi, Omodara Babafemi and Carlos Dinamarca

Catalysts 2021, 11(1), 40; https://doi.org/10.3390/catal11010040 - 31 Dec 2020

Cited by 12 | Viewed by 2474

Abstract

This study presents a series of experiments to test the integration of syngas fermentation into a single-cell microbial electrosynthesis (MES) process. Minimal gas–liquid mass transfer is the primary bottleneck in such gas-fermentation processes. Therefore, we hypothesized that MES integration could trigger the thermodynamic barrier, resulting in higher gas–liquid mass transfer and product-formation rates. The study was performed in three different phases as batch experiments. The first phase dealt with mixed-culture fermentation at 1 bar H₂ headspace pressure. During the second phase, surface electrodes were integrated into the fermentation medium, and investigations were performed in open-circuit mode. In the third phase, the electrodes were poised with a voltage, and the second phase was extended in closed-circuit mode. Phase 2 demonstrated three times the gas consumption (1021 mmol) and 63% more production of acetic acid (60 mmol/L) than Phase 1. However, Phase 3 failed; at –0.8 V, acetic acid was oxidized to yield hydrogen gas in the headspace. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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17 pages, 4421 KiB

Open AccessFeature PaperArticle

Unravelling the Structural Modification (Meso-Nano-) of Cu/ZnO-Al₂O₃ Catalysts for Methanol Synthesis by the Residual NaNO₃ in Hydroxycarbonate Precursors

by Rut Guil-López, Noelia Mota, Jorge Llorente, Elena Millan, Bárbara G. Pawelec, Jose Luis G. Fierro and Rufino M. Navarro

Catalysts 2020, 10(11), 1346; https://doi.org/10.3390/catal10111346 - 19 Nov 2020

Cited by 4 | Viewed by 2205

Abstract

The effects of residual NaNO₃ on the modification of Cu/ZnO-Al₂O₃ catalysts have been extensively documented, but the modification mechanism is so far unclear. This work studies in detail the influence of the residual sodium nitrate present in the hydroxycarbonate precursors on their decomposition during calcination and how it affects to the formation and configuration of the final active sites of the Cu/ZnO-Al₂O₃ catalysts. Different samples with varying sodium content after washing (from 0.01 to 7.3 wt%) were prepared and studied in detail after calcination and reduction steps. The results of this work demonstrated that NaNO₃ affects the decomposition mechanism of the hydroxycarbonate precursors during calcination and produces its decarbonation at low temperature. The enhancement of the decarbonation by NaNO₃ leads to segregation and crystallization of CuO and ZnO with loss of mesostructure and surface area in the calcined catalysts. The loss of mesostructure in calcined catalysts affects the subsequent reduction step, decreasing the reducibility and damaging the nanostructure of the reduced catalysts forming large Cu particles in poor contact with ZnO_x that results in a significant decrease in the intrinsic activity of the copper active sites for methanol synthesis. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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17 pages, 2772 KiB

Open AccessArticle

Experimental Study on CO₂ Methanation over Ni/Al₂O₃, Ru/Al₂O₃, and Ru-Ni/Al₂O₃ Catalysts

by Rei-Yu Chein and Chih-Chang Wang

Catalysts 2020, 10(10), 1112; https://doi.org/10.3390/catal10101112 - 25 Sep 2020

Cited by 29 | Viewed by 4626

Abstract

CO₂ methanation is recognized as one of the best technologies for storing intermittent renewable energy in the form of CH₄. In this study, CO₂ methanation performance is investigated using Ni/Al₂O₃, Ru/Al₂O₃, and Ru-Ni/Al₂O₃ as the catalysts under conditions of atmospheric pressure, a molar ratio of H₂/CO₂ = 5, and a space velocity of 5835 h⁻¹. For reaction temperatures ranging from 250 to 550 °C, it was found that the optimum reaction temperature is 400 °C for all catalysts studied. At this temperature, the maximum values of CO₂ conversion, H₂ efficiency, and CH₄ yield and lowest CO yield can be obtained. With temperatures higher than 400 °C, reverse CO₂ methanation results in CO₂ conversion and CH₄ yield decreases with increased temperature, while CO is formed due to reverse water-gas shift reaction. The experimental results showed that CO₂ methanation performance at low temperatures can be enhanced greatly using the bimetallic Ru-Ni catalyst compared with the monometallic Ru or Ni catalyst. Under ascending-descending temperature changes between 250 °C and 550 °C, good thermal stability is obtained from Ru-Ni/Al₂O₃ catalyst. About a 3% decrease in CO₂ conversion is found after three continuous cycles (74 h) test. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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22 pages, 6553 KiB

Open AccessFeature PaperArticle

Direct Synthesis of Dimethyl Ether from Syngas on Bifunctional Hybrid Catalysts Based on Supported H₃PW₁₂O₄₀ and Cu-ZnO(Al): Effect of Heteropolyacid Loading on Hybrid Structure and Catalytic Activity

by Elena Millán, Noelia Mota, Rut Guil-López, Bárbara Pawelec, José L. García Fierro and Rufino M. Navarro

Catalysts 2020, 10(9), 1071; https://doi.org/10.3390/catal10091071 - 17 Sep 2020

Cited by 12 | Viewed by 4672

Abstract

The performance of bifunctional hybrid catalysts based on phosphotungstic acid (H₃PW₁₂O₄₀, HPW) supported on TiO₂ combined with Cu-ZnO(Al) catalyst in the direct synthesis of dimethyl ether (DME) from syngas has been investigated. We studied the effect of the HPW loading on TiO₂ (from 1.4 to 2.7 monolayers) on the dispersion and acid characteristics of the HPW clusters. When the concentration of the heteropoliacid is slightly higher than the monolayer (1.4 monolayers) the acidity of the clusters is perturbed by the surface of titania, while for concentration higher than 1.7 monolayers results in the formation of three-dimensional HPW nanocrystals with acidity similar to the bulk heteropolyacid. Physical hybridization of supported heteropolyacids with the Cu-ZnO(Al) catalyst modifies both the acid characteristics of the supported heteropolyacids and the copper surface area of the Cu-ZnO(Al) catalyst. Hybridization gives rise to a decrease in the copper surface area and the disappearance of the strong acidic sites typical of HPW nanocrystals, showing all hybrids similar acid sites of weak or medium strength. The activity of the hybrids was tested for direct DME synthesis from syngas at 30 bar and 250 °C; only the hybrids with HPW loading higher than 1.4 monolayers showed activity for the direct synthesis of DME, showing that the sample loaded with 2.7 monolayers of heteropolyacid had higher activity than the reference hybrid representative of the most widely applied catalysts based on the combination of Cu-ZnO(Al) with HZSM-5. In spite of the high activity of the hybrids, they show a moderate loss in the DME production with TOS that denotes some kind of deactivation of the acidity function under reaction conditions. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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17 pages, 4347 KiB

Open AccessArticle

Significance of C₃ Olefin to Paraffin Ratio in Cobalt Fischer–Tropsch Synthesis

by Erling Rytter, Jia Yang, Øyvind Borg and Anders Holmen

Catalysts 2020, 10(9), 967; https://doi.org/10.3390/catal10090967 - 24 Aug 2020

Cited by 4 | Viewed by 2954

Abstract

The ratio between propene and propane (C₃ o/p) during Fischer–Tropsch synthesis (FTS) has been analyzed based on both literature reports and experiments for five catalysts. The latter comprise four cobalt catalysts on γ-alumina with variations in pore sizes, and one catalyst on α-alumina. Overall variations include H₂/CO feed ratio, residence time, water addition, transients between test conditions, CO conversion, cobalt particle size, promoter (Re), and support material. It was possible to rationalize all data based on secondary hydrogenation of olefins. In fact, it was deduced that olefins are dominating termination products in FTS, estimated to ca. 90% for C₃, but that some paraffins most likely are also produced directly. Increased residence time and high H2/CO feed ratio favors olefin hydrogenation, while added water presumably displaces hydrogen on cobalt giving enhanced C₃ o/p. High cobalt dispersion favors hydrogenation, as also promoted by Re. Effect of intraparticle diffusion is seen in transient periods; for example, as water is added or depleted. There is frequently positive correlation between C₃ o/p and selectivity to longer chains; the latter expressed as C₅₊ selectivity, as both are sensitive to hydrogen activity. Some modifications, however, are needed due to the accepted volcano plot for C₅₊ selectivity with cobalt crystallite size. Titania as support shows unexpectedly low C₃ o/p; probably due to SMSI (strong-metal-support-interaction). Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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21 pages, 5049 KiB

Open AccessArticle

Hydrogen Production via the Oxy-Steam Reforming of LNG or Methane on Ni Catalysts

by Pawel Mierczynski, Natalia Stępińska, Magdalena Mosinska, Karolina Chalupka, Jadwiga Albinska, Waldemar Maniukiewicz, Jacek Rogowski, Magdalena Nowosielska and Malgorzata I. Szynkowska

Catalysts 2020, 10(3), 346; https://doi.org/10.3390/catal10030346 - 20 Mar 2020

Cited by 10 | Viewed by 2740

Abstract

Ni catalysts supported on ZrO₂, 5%CeO₂-ZrO₂, and 5%La₂O₃-ZrO₂ were prepared via the impregnation method and tested in the oxy-steam reforming of methane and liquified natural gas (LNG). All tested catalysts exhibited high catalytic activity in the studied process at 700 and 900 °C. The improvement of the stability of Ni catalysts after the addition of CeO₂ oxide in the studied oxy-steam reforming of LNG process was confirmed. In addition, high activity and selectivity towards hydrogen was proven in the oxy-steam reforming process at 900 °C over a 20%Ni/5%CeO₂-ZrO₂ catalyst. It was also proved that the addition of CeO₂ onto a ZrO₂ carrier leads to a decrease in the NiO and metallic Ni crystallite sizes that were detected by the X-Ray diffraction (XRD) technique. The solid solution formation between NiO and ZrO₂ and/or NiO and CeO₂ was proved. Superior reactivity in the oxy-steam reforming of CH₄ and the LNG process exhibited a 20%Ni/ZrO₂ catalyst, which showed the highest methane conversions at 500 and 600 °C, equal to 63% and 89%, respectively. In addition, also in the case of the LNG reforming reaction, the most active catalyst was the 20%Ni/ZrO₂ system, which demonstrated 46.3% and 76.9% of the methane conversion value at 500 and 600 °C and the total conversion of others hydrocarbons (ethane, propane and butane). In addition, this catalytic system exhibited the highest selectivity towards hydrogen formation in the oxy-steam reforming of the LNG reaction equal to 71.2% and 71.3% at 500 and 600 °C, respectively. The highest activity of this system can be explained by the uniform distributions of Ni species and their highest concentration compared to the rest of the monometallic Ni catalysts. Time-of-flight secondary ion mass spectrometry (ToF-SIMS) results also confirmed a strong interaction of NiO with ZrO₂ in the case of the 20%Ni/ZrO₂ catalysts. The presence of selected NiZrO⁺ ions emitted from the investigated surface of the 20%Ni/ZrO₂ system was detected. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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11 pages, 2486 KiB

Open AccessCommunication

The Effects of the Crystalline Phase of Zirconia on C–O Activation and C–C Coupling in Converting Syngas into Aromatics

by Sheng Wang, Yue Fang, Zhen Huang, Hualong Xu and Wei Shen

Catalysts 2020, 10(2), 262; https://doi.org/10.3390/catal10020262 - 21 Feb 2020

Cited by 13 | Viewed by 3248

Abstract

Zirconia has recently been used as an efficient catalyst in the conversion of syngas. The crystalline phases of ZrO₂ in ZrO₂/HZSM-5 bi-functional catalysts have important effects on C–O activation and C–C coupling in converting syngas into aromatics and been investigated in this work. Monoclinic ZrO₂ (m-ZrO₂) and tetragonal ZrO₂ (t-ZrO₂) were synthesized by hydrothermal and chemical precipitation methods, respectively. The results of in situ diffuse reflection infrared Fourier transform spectroscopy (DRIFTs) revealed that there were more active hydroxyl groups existing on the surface of m-ZrO₂, and CO temperature programmed desorption (CO-TPD) results indicated that the CO adsorption capacity of m-ZrO₂ was higher than that of t-ZrO₂, which can facilitate the C–O activation of m-ZrO₂ for syngas conversion compared to that of t-ZrO₂. And the CO conversion on the m-ZrO₂ catalyst was about 50% more than that on the t-ZrO₂ catalyst. ³¹P and ¹³C magic angle spinning nuclear magnetic resonance (MAS NMR) analysis revealed a higher acid and base density of m-ZrO₂ than that of t-ZrO₂, which enhanced the C–C coupling. The selectivity to CH₄ on the m-ZrO₂ catalyst was about 1/5 of that on the t-ZrO₂ catalyst in syngas conversion. The selectivity to C₂₊ hydrocarbons over m-ZrO₂ or t-ZrO₂ as well as the proximity of the ZrO₂ sample and HZSM-5 greatly affected the further aromatization in converting syngas into aromatics. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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9 pages, 1613 KiB

Open AccessArticle

Adsorption Characteristics of Gas Molecules (H₂O, CO₂, CO, CH₄, and H₂) on CaO-Based Catalysts during Biomass Thermal Conversion with in Situ CO₂ Capture

by Baofeng Zhao, Jingwei Wang, Di Zhu, Ge Song, Huajian Yang, Lei Chen, Laizhi Sun, Shuangxia Yang, Haibin Guan and Xinping Xie

Catalysts 2019, 9(9), 757; https://doi.org/10.3390/catal9090757 - 09 Sep 2019

Cited by 17 | Viewed by 3535

Abstract

Biomass thermochemical conversion with in situ CO₂ capture is a promising technology in the production of high-quality gas. The adsorption competition mechanism of gas molecules (H₂O, CO₂, CO, CH₄, and H₂) on CaO-based catalyst surfaces was studied using density functional theory (DFT) and experimental methods. The adsorption characteristics of CO₂ on CaO and 10 wt % Ni/CaO (100) surfaces were investigated in a temperature range of 550–700 °C. The adsorption energies were increased and then weakened, reaching their maximum at 650 °C. The simulation results were verified by CO₂ temperature-programmed desorption (CO₂-TPD) experiments. By the density of states and Mulliken population analysis, CaO doped with Ni caused a change in the electronic structure of the O_surf atom and decreased the C–O bond stability. The molecular competition mechanism on the CaO-based catalyst surface was identified by DFT simulation. As a result, the adsorption energies decreased in the following order: H₂O > CO₂ > CO > CH₄ > H₂. The increase of CO₂ adsorption energy on the 10 wt % Ni/CaO surface, compared with the CaO surface, was the largest among those of the studied molecules, and its value increased from 1.45 eV to 1.81 eV. Therefore, the 10 wt % Ni/CaO catalyst is conducive to in situ CO₂ capture in biomass pyrolysis. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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13 pages, 4070 KiB

Open AccessCommunication

In Situ Encapsulated Pt Nanoparticles Dispersed in Low Temperature Oxygen for Partial Oxidation of Methane to Syngas

by Junwen Wang, Lichao Ma, Chuanmin Ding, Yanan Xue, Yongkang Zhang and Zhiting Gao

Catalysts 2019, 9(9), 720; https://doi.org/10.3390/catal9090720 - 27 Aug 2019

Cited by 7 | Viewed by 3362

Abstract

Highly dispersed ultra-small Pt nanoparticles limited in nanosized silicalite-1 zeolite were prepared by in situ encapsulation strategy using H₂PtCl₆·6H₂O as a precursor and tetrapropylammonium hydroxide as a template. The prepared Pt@S-1 catalyst was characterized by X-ray diffraction (XRD), inductively coupled plasma (ICP), transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), N₂ adsorption-desorption, CO adsorption, and TGA techniques and exhibited unmatched catalytic activity and sintering resistance in the partial oxidation of methane to syngas. Strikingly, Pt@S-1 catalyst with further reduced size and increased dispersibility of Pt nanoparticles showed enhanced catalytic activity after low-temperature oxygen calcination. However, for Pt/S-1 catalyst, low-temperature oxygen calcination did not improve its catalytic activity. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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12 pages, 3595 KiB

Open AccessArticle

Direct Conversion of CO₂ into Dimethyl Ether over Al₂O₃/Cu/ZnO Catalysts Prepared by Sequential Precipitation

by Cheonwoo Jeong, Jinsung Kim, Ji-Hyeon Kim, Sunghoon Lee, Jong Wook Bae and Young-Woong Suh

Catalysts 2019, 9(6), 524; https://doi.org/10.3390/catal9060524 - 12 Jun 2019

Cited by 9 | Viewed by 4194

Abstract

Bifunctional Al₂O₃/Cu/ZnO catalysts with Al composition of between 30 mol% and 80 mol% were prepared by sequential precipitation (SP) for the conversion of CO₂ into dimethyl ether (DME). In the SP synthesis, the concentration of a precipitation agent managed to be high enough to induce the complete precipitation of Al³⁺. The prepared precipitates were composed of zincian malachite and amorphous AlO(OH). Furthermore, the calcined mixed metal oxide materials of 60% and 80% Al exhibited a higher acidity than commercial Al₂O₃ and the H₂-reduced catalysts showed the similar Cu dispersion of 6%–7% at all Cu loadings. In the activity test at 573 K and 50 bar, the SP-derived catalyst of 80% Al (SP-80) displayed the best performance corresponding to CO₂ conversion of 25% and DME selectivity of 75% that are close to equilibrium values. In order to overcome the thermodynamic limitation, a dual-bed catalyst system was made up of SP-80 in the first layer and zeolite ferrierite in the next. This approach enabled DME selectivity to be enhanced to 90% while CO₂ conversion increased a little. Consequently, the studied catalyst system based on the SP-derived catalysts can contribute greatly to selective DME production from CO₂. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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Review

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34 pages, 6186 KiB

Open AccessFeature PaperEditor’s ChoiceReview

Direct Synthesis of Dimethyl Ether from CO₂: Recent Advances in Bifunctional/Hybrid Catalytic Systems

by Noelia Mota, Elena Millán Ordoñez, Bárbara Pawelec, José Luis G. Fierro and Rufino M. Navarro

Catalysts 2021, 11(4), 411; https://doi.org/10.3390/catal11040411 - 24 Mar 2021

Cited by 51 | Viewed by 9773

Abstract

Dimethyl ether (DME) is a versatile raw material and an interesting alternative fuel that can be produced by the catalytic direct hydrogenation of CO₂. Recently, this process has attracted the attention of the industry due to the environmental benefits of CO₂ elimination from the atmosphere and its lower operating costs with respect to the classical, two-step synthesis of DME from syngas (CO + H₂). However, due to kinetics and thermodynamic limits, the direct use of CO₂ as raw material for DME production requires the development of more effective catalysts. In this context, the objective of this review is to present the latest progress achieved in the synthesis of bifunctional/hybrid catalytic systems for the CO₂-to-DME process. For catalyst design, this process is challenging because it should combine metal and acid functionalities in the same catalyst, in a correct ratio and with controlled interaction. The metal catalyst is needed for the activation and transformation of the stable CO₂ molecules into methanol, whereas the acid catalyst is needed to dehydrate the methanol into DME. Recent developments in the catalyst design have been discussed and analyzed in this review, presenting the different strategies employed for the preparation of novel bifunctional catalysts (physical/mechanical mixing) and hybrid catalysts (co-precipitation, impregnation, etc.) with improved efficiency toward DME formation. Finally, an outline of future prospects for the research and development of efficient bi-functional/hybrid catalytic systems will be presented. Full article

(This article belongs to the Special Issue Catalysts for Production and Conversion of Syngas)

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