Article
Chemistry, Physical
Eugenio Meloni, Marco Martino, Antonio Ricca, Vincenzo Palma
Summary: Hydrogen as a green energy source can be produced through methane steam reforming, but traditional methods have limitations in terms of efficiency and cost. Microwave heating could overcome these limitations by efficiently transferring heat to the catalyst, resulting in faster reactions and higher energy efficiency. Initial tests showed promising results, with the system reaching high temperatures and methane conversion rates close to thermodynamic equilibrium values. Future studies will focus on optimizing the microwave reactor to further increase energy efficiency and improve CH4 conversion rates for enhanced hydrogen production.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
Tianqing Zheng, Wei Zhou, Xuyang Chu, Yunsong Lian
Summary: This study proposes a method of designing a trapezoidal cavity in an auto-thermal methanol steam reforming micro-reactor (ATMSRM) to enhance its reforming temperature performance and hydrogen production. The numerical simulation model of ATMSRM is used to investigate the influence of different geometric sizes of the trapezoidal cavity. The results show that using a specific size of trapezoidal cavity can improve the reforming temperature performance and hydrogen production performance.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Inorganic & Nuclear
Xiaomin Hu, Chenyu Ding, Qiao Wang, Hui Chen, Xuanyi Jia, Lihong Huang
Summary: Co-Ce-O oxides catalysts were successfully fabricated using different hydrothermal methods, and the characterization results showed that the structure and properties of the catalysts varied with different synthesis methods. The catalyst with nanorod morphology exhibited promising catalytic performance in auto-thermal reforming of acetic acid, with high conversion and yield of hydrogen, as well as negligible by-products, demonstrating its potential for hydrogen production.
INORGANIC CHEMISTRY COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Yuxuan Zeng, Guoxing Chen, Qianyun Bai, Li Wang, Renbing Wu, Xin Tu
Summary: This study investigates the plasma-enhanced catalytic biogas reforming process for hydrogen-rich syngas production using a Ni-K/Al2O3 catalyst in a tabular dielectric barrier discharge non-thermal plasma reactor. Different reaction modes, including plasma catalysis, plasma alone, and catalysis alone, are compared to understand the synergy at elevated temperatures. The combination of Ni-K/Al2O3 and plasma shows temperature-dependent and varied synergistic effects. The results demonstrate that the plasma catalysis achieves the maximum conversions of CH4 and CO2 at 160 degrees C, while increasing the temperature enhances the H2/CO ratio.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Review
Chemistry, Physical
Robinson L. Manfro, Mariana M. V. M. Souza
Summary: This review presents the recent advances in Ni-based catalysts for biogas reforming, discussing the effects of supports and promoters on catalyst performance and analyzing the influence of synthesis method, metal-support interaction, acid/base sites, and oxygen mobility on catalytic activity. It also highlights the development of core-shell structure catalysts and bimetallic catalysts of Ni with other transition metals and noble metals.
Article
Chemistry, Physical
Concetta Ruocco, Vincenzo Palma, Gianmario Picciotti, Antonio Coppola
Summary: The study comprehensively investigates the kinetics of ethanol oxidative reforming over a Pt-Ni/CeO2-Al2O3 catalyst in the presence of fuel grade bioethanol, and develops a kinetic model that includes the formation of solid carbon. The results show a satisfactory fitting of the experimental data for the reaction scheme involving ethylene and acetaldehyde formation, their subsequent decomposition, methane oxidation, and steam reforming and water gas shift reaction. Furthermore, the catalyst exhibits high stability and near-zero carbon emission during long-term testing.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Applied
Pilar Tarifa, Nicola Schiaroli, Phuoc Hoang Ho, Fernando Canaza, Francesca Ospitali, Giancosimo Sanghez de Luna, Carlo Lucarelli, Giuseppe Fornasari, Angelo Vaccari, Antonio Monzon, Patricia Benito
Summary: The valorisation of clean biogas by steam reforming over metal open-cell foam-based structured catalysts was studied, showing that Rh-based catalysts exhibit superior activity and stability compared to Ru catalysts, leading to reduced carbon deposition and increased biogas valorisation and productivity.
Article
Energy & Fuels
Dan Zhou, Zhiyuan Li, Yaoqi Deng, Chengxiong Dang, Weiquan Cai
Summary: Sorption-enhanced biogas steam reforming with a Pb-modified Ni-CaO catalyst shows excellent stability and can continuously produce high-purity hydrogen.
Article
Chemistry, Applied
Simona Renda, Marta Cortese, Giuseppina Iervolino, Marco Martino, Eugenio Meloni, Vincenzo Palma
Summary: This study investigated the electrification of reforming processes by using commercial silicon carbide (SiC) heating elements as catalyst carriers to provide heat directly for the reaction. The experiments demonstrated the possibility of realizing a process by reversing the flow of heat, achieving higher methane conversion rates in both steam and dry reforming reactions.
Article
Chemistry, Applied
Morgana Rosset, Liliana Amaral Feris, Oscar W. Perez-Lopez
Summary: Ni-M-Al (M = K, Na, Li) LDH-derived catalysts were evaluated for biogas dry reforming, showing differences in acidity and sintering resistance among the catalysts. The NiLi catalyst exhibited higher resistance to sintering and deactivation mainly due to carbon deposition, while NiK and NiNa catalysts were mainly deactivated by sintering during reactions. Different carbon species were produced by the catalysts depending on the reaction conditions.
Article
Energy & Fuels
Cao-Minh Vo, Anh Ngoc T. Cao, Amjad Saleh Qazaq, Cham Q. Pham, Dang Le Tri Nguyen, Mabkhoot Alsaiari, Tuan V. Vu, Ajit Sharma, Pham T. T. Phuong, Thuan Tran Van, Moustafa A. Rizk, Tung M. Nguyen, Dai-Viet N. Vo
Summary: This work investigated the upgrading of simulated biogas through dry reforming using calcium-promoted cobalt-based catalysts. The study found that the loading of calcium is critical in the catalyst performance, with low dosages resulting in smaller cobalt crystalline size and enhanced reducibility and basicity. The optimal catalyst showed high CH4 and CO2 conversions, as well as suppressed coke formation, leading to improved activity and stability. These findings offer new opportunities to enhance the performance of dry reforming using abundant catalysts.
Article
Chemistry, Physical
Morgana Rosset, Liliana Amaral Feris, Oscar W. Perez-Lopez
Summary: Incorporating Mg or Zn into NiAl-LDH for reconstruction using a memory effect improved the catalytic activity and stability in the dry reforming of Biogas. The washing step significantly affected LDH reconstruction, with different metals influencing the properties of the materials. Ni-Zn alloy formation in Zn-reconstructed catalysts led to the best performance in methane and carbon dioxide conversion with a H-2/CO ratio of approximately 2.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Energy & Fuels
Galina Xanthopoulou, Savvas Varitis, Manapkhan Zhumabek, Konstantinos Karanasios, George Vekinis, Svetlana A. Tungatarova, Tolkyn S. Baizhumanova
Summary: The world of energy is undergoing a profound transformation with hydrogen and hydrogen-containing fuel mixtures as efficient carriers of clean energy. Carbon dioxide conversion of methane using Ni/Mn-based catalysts shows promising results in reducing greenhouse gas emissions and city pollution, while also decreasing reliance on oil-based fuels. Characterization and investigation of catalyst composition on activity, selectivity, and product yield have been conducted.
Article
Green & Sustainable Science & Technology
Eugenio Meloni, Emilia Saraceno, Marco Martino, Antonio Corrado, Giuseppina Iervolino, Vincenzo Palma
Summary: The dry reforming of methane (DRM) process converts methane and carbon dioxide into syngas, but it has a significant CO2 footprint due to the fossil fuel combustion required for heat. The process also faces challenges in heat transfer to the catalytic volume. This study proposes the electrified DRM process using two Ni-based structured catalysts, Silicon carbide (SiC) honeycomb monolith and Si-SiC open-cell foam, to enhance heat and mass transport phenomena.
Article
Materials Science, Ceramics
Yingchun Xu, Yuxin Song, Hui Chen, Fuxia Liao, Jia Huang, Lihong Huang
Summary: In this study, a series of Co-Al-Ba composite oxide catalysts with different Ba dopings were synthesized and evaluated for hydrogen production via ATR of acetic acid (HAc). The results showed that the CAB50 catalyst with 50 wt% of BaO exhibited superior activity and stability, which can be attributed to the replacement of Co by Ba in the CoAl2O4 spinel and the promotion of HAc adsorption and activation.
JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
(2023)
Article
Chemistry, Applied
Frederic C. Meunier
Summary: The hydrogenation of CO and especially that of CO2 has gained increasing attention for the production of base chemicals and fuels. This contribution discusses the insights that can be obtained through in situ and operando FT-IR studies on CO and CO2 hydrogenations. It emphasizes the importance of quantitative IR studies for drawing relevant conclusions and discusses the limitations and pitfalls of diffuse reflectance spectroscopy. The potential of IR spectroscopy in unraveling the properties of CO2 trapping-methanation materials is briefly discussed.
Article
Thermodynamics
Malte Doentgen, Sven Eckart, Chris Fritsche, Hartmut Krause, K. Alexander Heufer
Summary: The combustion behavior of trimethoxy methane (TMM), a branched version of oxymethylene ethers (OMEs), was studied and a detailed chemical kinetic model for TMM combustion was provided. The model was validated against experimental data, showing good agreement. The results indicated that TMM exhibits higher reactivity compared to OME2 at high temperatures. This study lays the foundation for future kinetic modeling of TMM and other branched OME-like compounds.
PROCEEDINGS OF THE COMBUSTION INSTITUTE
(2023)
Article
Energy & Fuels
Lea Eggemann, Florian Rau, Detlef Stolten
Summary: This study evaluates the environmental impact of manure treatment in different types of small-scale biogas applications. It found that utilizing manure to produce biogas and subsequent combustion in a combined heat and power plant can reduce emissions by 173 kg CO2 eq. per m3 of manure, while the direct usage of biogas leads to emissions of 20.9 kg CO2 eq. per m3 of manure.
Article
Chemistry, Physical
Sven Eckart, Felix Zijie Rong, Christian Hasse, Hartmut Krause, Arne Scholtissek
Summary: Chemical reaction mechanisms with detailed kinetics are crucial for accurately modeling reactive flows in combustors, and well-defined experimental observables such as laminar burning velocity and ignition delay time are commonly used for their development. However, the extinction strain rate (ESR) of non-premixed flames in the counterflow configuration, which is an important experimental observable, often receives less attention. This study investigates the ESR for different fuel mixtures and oxygen contents, and suggests that ESR could be a useful optimization target for improving chemical reaction mechanisms.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Thermodynamics
Wei Li, Jianguo Zhang, Sven Eckart, Jingxian Xia, Hartmut Krause, Yuyang Li
Summary: This study investigated the laminar flame propagation characteristics of three C(5)H(10)O(2) esters (methyl butanoate, methyl isobutanoate, and ethyl propanoate) and explored the effects of isomeric fuel structures. Experimental measurements and modeling analyses revealed that the laminar burning velocity decreases with increasing pressure and the methyl isobutanoate has the fastest propagation velocity among the three esters. The differences in radical pools of the ester isomers were found to be responsible for the observed fuel isomeric effects on laminar flame propagation.
PROCEEDINGS OF THE COMBUSTION INSTITUTE
(2023)
Article
Chemistry, Multidisciplinary
Frederic C. Meunier, Isaac Dansette, Anaelle Paredes-Nunez, Yves Schuurman
Summary: Cu/ZrO2 is a promising catalyst for CO2 hydrogenation to methanol. Three different types of formates were observed under reaction conditions, with one bound to metallic Cu and the other two bound to ZrO2. The Cu-bound formate, representing only about 7% of surface formates, was found to be highly reactive and the sole source of methanol production. This study highlights the importance of quantitative IR analysis and transient methods in understanding the role of surface species.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Partha Samanta, Albert Sole-Daura, Remy Rajapaksha, Florian M. Wisser, Frederic Meunier, Yves Schuurman, Capucine Sassoye, Caroline Mellot-Draznieks, Jerome Canivet
Summary: Molecularly defined organometallic rhodium phosphine complexes were immobilized within a MOF structure without losing their molecular nature and catalytic behavior. These MOF-based catalysts showed high activity for ethylene hydroformylation and successfully catalyzed the hydroformylation of longer and bulkier alkenes. The combination of experimental and computational methods allowed for a better understanding of the active species and molecular mechanisms involved in the catalytic reactions. The use of MOF-808 as a solid ligand offers advantages such as molecular-scale understanding, site isolation, and recycling ability.
Editorial Material
Chemistry, Physical
Frederic C. Meunier, Canio Scarfiello
Summary: The IR work in Jo et al.'s paper is critically re-analyzed and alternative interpretations are proposed, challenging some of the conclusions made by the authors.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Frederic C. Meunier, Xianwei Wang, Thomas Buergi
Summary: The presence of negatively charged gold species on Au surfaces or supported Au nanoparticles has been widely reported based on the appearance of IR bands of adsorbed CO below 2090 cm-1. However, some researchers have suggested that these bands may be solely attributed to the presence of Ni-CO species contaminating the sample surfaces. In this study, CO adsorption was monitored using a CO supply, DRIFTS reaction cell, and lines that excluded nickel contamination. The results show that a band at 2067 cm-1 appeared without the involvement of Ni carbonyls, supporting the idea of CO adsorption on negatively charged Au surfaces. © 2023 Elsevier Inc. All rights reserved.
JOURNAL OF CATALYSIS
(2023)
Article
Engineering, Chemical
Chunkan Yu, Sven Eckart, Stefan Essmann, Detlev Markus, Agustin Valera-Medina, Robert Schiessl, Bo Shu, Hartmut Krause, Ulrich Maas
Summary: This study investigates the ignition process of ammonia/hydrogen mixtures through numerical simulations, revealing the influence of system parameters such as strain rate, hydrogen content, pressure, and initial temperature on the minimum ignition energy. Important findings include the quasi-linear correlation between the transition strain rate and characteristic reaction rate, as well as the less pronounced decay of minimum ignition energy with increasing hydrogen content at higher pressures. The analysis of these results provides a knowledge-based approach for fail-proof ignition devices and reliable prevention of hazards.
JOURNAL OF LOSS PREVENTION IN THE PROCESS INDUSTRIES
(2023)
Article
Electrochemistry
Mohammad Reza Bilesan, Meghdad Yazdani, Mathilde Luneau, Gerard Montserrat-Siso, Bjoern Wickman, Eveliina Repo
Summary: In this study, a noble-metal-free 3D printed Ti-6Al-4V electrode is introduced as an alternative anode in alkaline electrochemical processes. The electrode provides a larger projected surface area and facilitates anodic reactions under controlled electrolyte conditions. The 3D scaffold structure enables improved charge transfer and replaces the non-conductive passivation on a flat plate anode with unstable passivation. The results show that the electrochemical active surface area of the 3D Ti-6Al-4V electrode is 42 times higher than a flat plate anode, making it a promising and affordable alternative for alkaline electrochemical applications.
Article
Chemistry, Applied
Pauline Bredy, Ludovic Fine, David Farrusseng, Yves Schuurman, Frederic C. Meunier
Summary: In situ and operando diffuse reflectance FT-IR (DRIFTS) studies often require consideration of changes in optical properties. This study investigated the variation of IR optical pathlength of Fe and Co-based Fischer-Tropsch catalysts by using an internal standard CaCO3 mixed with the catalyst. The results showed the importance of considering changes in optical pathlength for quantitative DRIFTS analysis.
Article
Chemistry, Physical
Mathilde Luneau, Linnea Strandberg, Gerard Montserrat-Siso, Victor Shokhen, Roopathy Mohan, Henrik Gronbeck, Bjorn Wickman
Summary: This study provides new insights into the enhanced activity of palladium supported on ceria (Pd/CeO2) in the hydrogen oxidation reaction (HOR) in alkaline media. Using model thin films, it is shown that Pd/CeO2 thin films have higher activity in HOR compared to pure Pd thin films. In situ characterization using electrochemical quartz crystal microbalance reveals the role of CeO2 in enhancing the activity of Pd/CeO2 in HOR.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Partha Samanta, Albert Sole-Daura, Remy Rajapaksha, Florian M. Wisser, Frederic Meunier, Yves Schuurman, Capucine Sassoye, Caroline Mellot-Draznieks, Jerome Canivet
Summary: Molecularly defined organometallic rhodium phosphine complexes were efficiently immobilized within a MOF structure, maintaining their molecular nature and catalytic behavior. The resulting MOF-heterogenized catalysts showed high activity in ethylene hydroformylation and successfully catalyzed the hydroformylation of longer and bulkier alkenes. The study also provided insights into the structure, evolution, and mechanisms of the active species within the MOF under catalytic conditions.
Article
Chemistry, Multidisciplinary
Loren Acher, Tristan Laredo, Thierry Caillot, Akim Kaddouri, Frederic C. Meunier
Summary: This study investigated CO2 capture and methanation using solid adsorbents, microwave absorbers, and a methane catalyst. The research demonstrated the potential of using inexpensive microwave technology to convert trapped CO2 into valuable products.
APPLIED SCIENCES-BASEL
(2023)