Catalytic Transformation of Low-Carbon Resources

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

Deadline for manuscript submissions: closed (15 May 2023) | Viewed by 8308

Special Issue Editors


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Guest Editor
State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China
Interests: methanol synthesis; CO2 conversion; methanol to propylene

E-Mail Website
Guest Editor
State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China
Interests: Fischer–Tropsch synthesis; CO2 activation and catalytic conversion
Special Issues, Collections and Topics in MDPI journals
State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China
Interests: CO2 reduction; heterogeneous catalyst; Fischer–Tropsch synthesis; zeolite
Special Issues, Collections and Topics in MDPI journals

E-Mail
Guest Editor
State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China
Interests: heterogeneous catalyst; catalytic conversion of low carbon resources, zeolite synthesis
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The transformation of COx has entered an era with more efficient and directional features, especially as reducing emitted CO2 becomes more urgent. The catalytic conversion of low-carbon resources to value-added chemicals is desired. On the one hand, the utilization of CO tends to be more selective and has a smaller release of CO2. On the other hand, the valorization of CO2 needs to strengthen to boost its circulation. Additionally, the coupling transformation of small carbon-containing molecules is anticipated to open new horizons over the traditional processes.

This Special Issue focuses on the fundamental understanding of new strategies for syngas conversion, CO2 activation, and oxygenates preparation through thermo-, electro-, and photocatalysis.

This Special Issue collects original research articles and reviews on all aspects of the catalytic conversion of low-carbon resources.

We believe this topic will provide an update on developing novel catalysts and technologies for transforming low-carbon resources.

Prof. Dr. Tian-Sheng Zhao
Dr. Jianli Zhang
Dr. Xinhua Gao
Dr. Kangzhou Wang
Guest Editors

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Keywords

  • advanced COx hydrogenation
  • synergistic catalysis
  • catalysis in surface and interface
  • atomic economic process
  • theoretical chemistry

Published Papers (6 papers)

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Research

13 pages, 2888 KiB  
Article
Probing the Roles of Residual Sodium in Physicochemical Properties and Performance of FeAlNa Catalyst for Fischer–Tropsch Synthesis
by Wenlong Song, Qiqi Zhu, Kangzhou Wang, Rui Zhu, Qingxiang Ma, Tiansheng Zhao, Qingjie Guo, Xinhua Gao and Jianli Zhang
Catalysts 2023, 13(7), 1081; https://doi.org/10.3390/catal13071081 - 9 Jul 2023
Viewed by 847
Abstract
Although Fe-based catalysts have made significant progress in Fischer–Tropsch synthesis, the effect of residual sodium on the structural properties and catalytic performance of Fe-based catalysts has been controversial. Herein, we report the positive role of residual sodium in the structural properties and performance [...] Read more.
Although Fe-based catalysts have made significant progress in Fischer–Tropsch synthesis, the effect of residual sodium on the structural properties and catalytic performance of Fe-based catalysts has been controversial. Herein, we report the positive role of residual sodium in the structural properties and performance of FeAlNa catalysts for olefins synthesis from syngas. Meanwhile, the as-prepared catalysts were characterized by the multiple characterization technique to reveal the positive role of residual sodium on the structural properties. The characterization results revealed that the residual sodium improved the reduction behavior of Fe species and adsorption ability of CO, and inhibited the secondary hydrogenation due to its weak adsorption ability of H2. Moreover, the residual sodium inhibited the interaction between Fe and Al. Importantly, a high olefins/paraffins ratio of 6.19 and low CH4 selectivity of 12.8% were achieved on the residual sodium modified FeAlNa catalyst. An in-depth understanding of the structural properties and catalytic performance of residual sodium on FeAl-based catalysts can provide a theoretical basis for the development of novel efficient catalysts and large-scale applications for olefins synthesis from syngas. Full article
(This article belongs to the Special Issue Catalytic Transformation of Low-Carbon Resources)
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15 pages, 4954 KiB  
Article
Highly Selective Transformation of CO2 + H2 into Para-Xylene via a Bifunctional Catalyst Composed of Cr2O3 and Twin-Structured ZSM-5 Zeolite
by Shiyuan Lin, Ruosong He, Wenhang Wang, Yang Wang, Yongqiang Gu, Qiang Liu and Mingbo Wu
Catalysts 2023, 13(7), 1080; https://doi.org/10.3390/catal13071080 - 8 Jul 2023
Cited by 3 | Viewed by 1272
Abstract
The abundant C1 source CO2 can be utilized to produce value-added chemicals through hydrogenation technology. A bifunctional catalyst consisting of reducible metal oxide Cr2O3 and acidic zeolite ZSM-5 was designed for the direct conversion of CO2 + H [...] Read more.
The abundant C1 source CO2 can be utilized to produce value-added chemicals through hydrogenation technology. A bifunctional catalyst consisting of reducible metal oxide Cr2O3 and acidic zeolite ZSM-5 was designed for the direct conversion of CO2 + H2 into valuable aromatics, especially para-xylene (PX), via the methanol-mediated pathway. The twin structure of ZSM-5 (ZSM-5T), with sinusoidal channels that are predominantly exposed to the external surface, enhances the possibility of the transformation of methanol into PX due to the favorable diffusion dynamic of PX in the sinusoidal channels. Via the bifunctional catalyst Cr2O3&ZSM-5T, a PX selectivity of 28.7% and PX space-time yield (STY) of 2.5 gCH2 h−1 kgcat−1 are achieved at a CO2 conversion rate of 16.5%. Furthermore, we rationally modify the ZSM-5T zeolite via Cu species doping and amorphous SiO2 shell coating (Cu-ZSM-5T@SiO2). After combining with the Cr2O3 catalytic component, the CO2 conversion (18.4%) and PX selectivity (33.8%) are increased to some extent, which systematically increases the STY of PX to 3.0 gCH2 h−1 kgcat−1. The physicochemical property of the acidic zeolite and the corresponding structure-function relationship in enhancing the PX productivity are discovered. Our work provides a novel catalyst design idea to boost PX synthesis performance from CO2 hydrogenation. Full article
(This article belongs to the Special Issue Catalytic Transformation of Low-Carbon Resources)
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17 pages, 6298 KiB  
Article
A Cu-SiO2 Catalyst for Highly Efficient Hydrogenation of Methyl Formate to Methanol
by Jincheng Wu, Guoguo Liu, Qin Liu, Yajing Zhang, Fu Ding and Kangjun Wang
Catalysts 2023, 13(7), 1038; https://doi.org/10.3390/catal13071038 - 26 Jun 2023
Cited by 1 | Viewed by 1386
Abstract
The hydrogenation of methyl formate to methanol is considered one of the most effective methods for recycling methyl formate products. We recently developed a highly efficient and cost-effective Cu-SiO2 catalyst using the ammonia-evaporation (AE) method. The Cu-SiO2-AE catalyst demonstrated superior [...] Read more.
The hydrogenation of methyl formate to methanol is considered one of the most effective methods for recycling methyl formate products. We recently developed a highly efficient and cost-effective Cu-SiO2 catalyst using the ammonia-evaporation (AE) method. The Cu-SiO2-AE catalyst demonstrated superior performance, achieving a methyl formate conversion of 94.2% and a methanol selectivity of 99.9% in the liquid product. The catalyst also displayed excellent stability over a durability test of 250 h. Compared to the commonly used Cu-Cr catalyst in the industry, the Cu-SiO2-AE catalyst exhibited higher conversion of methyl formate and methanol yield under the same reaction conditions. Characterization results revealed a significant presence of Si-OH groups in the Cu-SiO2-AE catalyst. These groups enhanced the hydrogen spillover effect and improved hydrogenation efficiency by preventing sintering during the reaction to stabilize the Cu species. The strategy employed in this study is applicable to the rational design of highly efficient catalysts for industrial applications. Full article
(This article belongs to the Special Issue Catalytic Transformation of Low-Carbon Resources)
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24 pages, 7121 KiB  
Article
Hydrogenation of CO2 to Valuable C2-C5 Hydrocarbons on Mn-Promoted High-Surface-Area Iron Catalysts
by Trino A. Zepeda, Sandra Aguirre, Yunuen I. Galindo-Ortega, Alfredo Solís-Garcia, Rufino M. Navarro Yerga, Barbara Pawelec, Juan C. Fierro-Gonzalez and Sergio Fuentes
Catalysts 2023, 13(6), 954; https://doi.org/10.3390/catal13060954 - 31 May 2023
Cited by 3 | Viewed by 1398
Abstract
Mn-promoted bulk iron catalysts with a high specific surface area (82–211 m2·g−1) were synthesized by coprecipitation followed by drying under supercritical conditions. The catalysts were tested in the CO2 hydrogenation to valuable C2-C5 hydrocarbons. The [...] Read more.
Mn-promoted bulk iron catalysts with a high specific surface area (82–211 m2·g−1) were synthesized by coprecipitation followed by drying under supercritical conditions. The catalysts were tested in the CO2 hydrogenation to valuable C2-C5 hydrocarbons. The Mn-promoted iron catalysts exhibited better textural properties than the bare Fe2O3 catalyst, allowing better dispersion of the active phase, easier reduction and carburization of iron oxides and, consequently, resulting in higher catalytic activity than the bare Fe2O3 catalyst. The best activity results were obtained by catalyst promotion with a very low amount of Mn (Mn/Fe atomic ratio of 0.05). Upon steady state conditions (T = 340 °C, total pressure of 20 bar and H2/CO2 = 3), this catalyst exhibited high CO2 conversion (44.2%) and selectivity to C2-C4 hydrocarbons (68%, olefin to paraffin ratio of 0.54), while the selectivity to C5+ hydrocarbons, CH4 and CO was about 3.2, 38.5 and 5%, respectively. A close correlation was found between catalyst textural properties and CO2 conversion. The most active MnFe-0.05 catalyst exhibited high stability during 72 h of reaction related to a low amount of soft coke formation and catalyst activation through the formation of the χ-Fe5C2 phase during the on-stream reaction. Full article
(This article belongs to the Special Issue Catalytic Transformation of Low-Carbon Resources)
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16 pages, 8475 KiB  
Article
Effect of Ce Content on the Chemical Looping Oxidative Dehydrogenation of Propane to Propylene over a VOx-CeO2/γ-Al2O3 Oxygen Carrier
by Fangyuan Qiang, Tuo Guo, Mengdong Nie, Yongzhuo Liu, Man Wu and Qingjie Guo
Catalysts 2023, 13(5), 797; https://doi.org/10.3390/catal13050797 - 24 Apr 2023
Viewed by 1277
Abstract
The chemical looping oxidative dehydrogenation of propane to propylene (CL-ODHP) replaces molecular oxygen with lattice oxygen (Olatt) in oxygen carriers. This method boosts propylene selectivity by avoiding the deep oxidation of propane. Herein, a series of 10V-XCe/Al oxygen carriers with different [...] Read more.
The chemical looping oxidative dehydrogenation of propane to propylene (CL-ODHP) replaces molecular oxygen with lattice oxygen (Olatt) in oxygen carriers. This method boosts propylene selectivity by avoiding the deep oxidation of propane. Herein, a series of 10V-XCe/Al oxygen carriers with different Ce contents were prepared to realize different VOx-CeOy interactions. The effect of the Ce content in 10V-XCe/Al oxygen carriers on the CL-ODHP reaction was studied and the optimal Ce content was determined. CeO2 prevents the outward diffusion and evolution of Olatt in VOx carriers to the adsorbed electrophilic oxygen species (Oelec), effectively inhibiting the loss of Olatt, improving the selectivity of propylene, and extending the lifetime and activity of the oxygen carriers. After characterizing and analyzing the oxygen carriers, it was found that 10V-3Ce/Al has the highest specific surface area, highest oxygen capacity, and lowest reducibility. The 10V-3Ce/Al also delivers the highest oxidative dehydrogenation performance. At 550 °C, the average propylene and COx selectivity values of 10V-3Ce/Al were 81.87% and 7.28%, respectively (vs. 62.79% and 25.64% respectively, for 10V/Al). It is demonstrated that 10V-3Ce/Al exhibits good cycle stability with no significant decrease in catalytic performance after 15 cycles. In situ diffuse-reflectance infrared Fourier-transform spectroscopy indicates that CL-ODHP on 10V-3Ce/Al undergoes the Mars-van Krevelen mechanism. The migration and evolution of Olatt in oxygen carriers is controlled by reasonably modifying the metal oxide interactions to improve propylene yield. This work will thus guide the subsequent development of novel and efficient CL-ODHP oxygen carriers. Full article
(This article belongs to the Special Issue Catalytic Transformation of Low-Carbon Resources)
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10 pages, 1789 KiB  
Article
A One-Pot Hydrothermal Preparation of High Loading Ni/La2O3 Catalyst for Efficient Hydrogenation of Cinnamaldehyde
by Haoting Yan, Yongwang Ren, Renkun Zhang, Feixiang Chang, Qinhong Wei and Jing Xu
Catalysts 2023, 13(2), 298; https://doi.org/10.3390/catal13020298 - 28 Jan 2023
Cited by 1 | Viewed by 1526
Abstract
It is a challenging task for selective hydrogenation of cinnamaldehyde (CAL) to hydrocinnamaldehyde (HCAL) without additional by-product formation. In this work, a La2O3 supported high Ni content nanoparticle catalyst was prepared for CAL selective hydrogenation. Meanwhile, Co-La2O3 [...] Read more.
It is a challenging task for selective hydrogenation of cinnamaldehyde (CAL) to hydrocinnamaldehyde (HCAL) without additional by-product formation. In this work, a La2O3 supported high Ni content nanoparticle catalyst was prepared for CAL selective hydrogenation. Meanwhile, Co-La2O3 catalysts were used as a reference catalyst. XRD, TEM, STEM-HAADF, XPS, and H2-TPR measurements were used to investigate the physicochemical properties of Ni-La2O3 catalysts. The experimental results confirmed that the CAL conversion and HCAL selectivity were effectively promoted with the increase of Ni loading amounts. At a Ni/La molar ratio of four, a high HCAL selectivity of 87.4% was obtained at a CAL conversion of 88.1% under mild reaction conditions. The catalyst was recycled five times without activity loss. Combined with various characterizations, it could be inferred that the good hydrogen adsorption and dissociation capacity of Ni and the presence of a certain amount of oxygen vacancies on the La2O3 support have a positive effect on the improvement of HCAL selectivity. This work provided an effective path to design transition-metal-based supported oxide catalyst for the cinnamaldehyde hydrogenation to hydrocinnamaldehyde. Full article
(This article belongs to the Special Issue Catalytic Transformation of Low-Carbon Resources)
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