Article
Chemistry, Physical
Alexandre Nau, Remy Pointecouteau, Melissandre Richard, Thomas Belin, Fabien Can, Clement Comminges, Nicolas Bion
Summary: Catalytic methane combustion experiments were conducted on YSZ, Pd/YSZ, and Rh/YSZ at temperatures ranging from 200 to 700 degrees Celsius. While Pd/YSZ and Rh/YSZ exhibited similar light-off curves between 200 and 450 degrees Celsius, isotopic exchange experiments using CD4 and 18O2 revealed differences in the activation of reactant molecules for both supported catalysts. The use of C18O2 isotopic gas was found to be more suitable than 18O2 to evaluate the bulk oxygen mobility in YSZ at low temperatures. The exchange of gaseous CO2 with lattice YSZ oxygen atoms, facilitated by surface hydrogen carbonate intermediate species, demonstrated the contribution of YSZ bulk oxygen atoms in Rh/YSZ at low temperatures.
CATALYSIS COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Lingting Ye, Zhibo Shang, Kui Xie
Summary: This study demonstrates a novel method for the selective conversion of methane to ethylene in a solid oxide electrolyser with high selectivity and stability, showing promising potential applications in the chemical field.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Paulina Jagodka, Krzysztof Matus, Michal Sobota, Agata Lamacz
Summary: Dry reforming of methane (DRM) is an important process for transforming two potent greenhouse gases into synthesis gas. However, prompt deactivation of the catalyst due to carbon deposition can be hindered by proper catalyst design.
Article
Chemistry, Physical
Cecile Daniel, David Farrusseng, Yves Schuurman
Summary: The synthesis of dimethyl carbonate (DMC) from carbon dioxide and methanol was investigated. Oxygen-18 labeled ceria-zirconia did not produce labeled DMC or water, while oxygen-18 labeled methanol primarily resulted in the formation of double labeled DMC. These findings provide insights into the reaction mechanisms and identify the rate-controlling step as the nucleophilic attack of gas phase methanol on surface monomethyl carbonate species to form DMC.
CATALYSIS COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Linyi Li, Renjun Tan, Shizhong Luo, Chengfa Jiang, Fangli Jing
Summary: In this study, Fe, Ni, Mn, and Ti were directly doped into the CeO2 lattice by hydrothermal method to form solid solution catalysts. Various techniques were used to study the structural evolution and properties of the catalysts. It was found that the incorporation of metal elements distorted the lattice and resulted in differences in redox, oxygen activity, basicity, and surface properties. The catalytic conversion of ethane with CO2 showed different features depending on the doped metal atoms. The number and activity of lattice oxygen played a dominant role in influencing the activity and selectivity. The solid solution catalysts also exhibited good coke resistance.
APPLIED CATALYSIS A-GENERAL
(2022)
Article
Chemistry, Physical
Rubina Khatun, Rohan Singh Pal, Mohammad Ahmad Shoeb, Deepak Khurana, Shubham Singhl, Nazia Siddiqui, Mukesh Kumar Poddar, Tuhin Suvra Khan, Rajaram Bal
Summary: In this study, a defect-rich Ni-Pt/CeO2 catalyst with oxygen vacancy sites was synthesized using a one-pot complex combustion method. The catalyst exhibited high activity for CO2 dissociation at low temperature. Comparisons with conventionally impregnated catalysts demonstrated superior catalytic properties and stability.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2024)
Article
Chemistry, Physical
Guo-Qing Yang, Xing Ren, Vita A. Kondratenko, Heng-Bo Zhang, Evgenii V. Kondratenko, Zhong-Wen Liu
Summary: This study investigates the effects of SnO2 promoter on the activity and selectivity of Pt/CeO2 catalyst in the oxidative dehydrogenation of propane with CO2. Increasing the Sn/Pt ratio leads to a decrease in propane conversion and an increase in propene selectivity, which can be explained by the increased electron density of Pt through the promoter. The Sn-modified Pt-O-Ce bonds are identified as the active sites for the reaction, occurring via a redox mechanism involving the activation of CO2 over oxygen vacancies at Sn-modified Pt and CeO2 boundaries.
Article
Chemistry, Physical
Fan Lin, Kenneth Rappe, Libor Kovarik, Miao Song, Xiaohong Shari Li, Mark Engelhard, Yong Wang
Summary: Research has found that high-temperature pretreatment of CeO2 support can enhance the redox and hydrocarbon oxidation activity of Pt/CeO2 catalyst. Compared to untreated CeO2 support, high-temperature pretreated CeO2 support can enhance the mobility of surface lattice oxygen, thus promoting the oxidation activity of Pt/CeO2 catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Engineering, Chemical
Jason Sun, Doki Yamaguchi, Liangguang Tang, Selvakannan Periasamy, Hongyang Ma, Judy N. Hart, Ken Chiang
Summary: This study investigated the influence of oxygen exchanging capability on the catalytic activity of methane dry reforming. The results showed that a small loading amount of Ru onto ceria-zirconia catalyst increased its oxygen mobility and catalytic activity, leading to high conversions of methane and carbon dioxide.
ADVANCED POWDER TECHNOLOGY
(2022)
Article
Engineering, Chemical
Ashvin L. L. Karemore, Renu Sinha, Parivesh Chugh, Prakash D. D. Vaidya
Summary: In this study, the performance of two Pt-based catalysts in the process of carbon dioxide reforming of methane (CDRM) was investigated. The effects of parameters such as space time, CO2/CH4 ratio, and time-on-stream on the conversion and yield of CH4 and CO2 were analyzed. The kinetics of CDRM were also studied and analyzed using different kinetic models.
CHEMICAL ENGINEERING SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Dewu Lin, Yue Yu, Lanying Li, Mingzhi Zou, Jin Zhang
Summary: The article describes a method for synthesizing high-purity semiconducting single-walled carbon nanotube arrays using a bicomponent catalyst of Au and ZrO2, which creates a localized etching zone to improve the purity and performance of carbon nanotubes.
Article
Chemistry, Physical
Weidong Sun, Ya Gao, Guofeng Zhao, Jiaqi Si, Ye Liu, Yong Lu
Summary: In this study, CexZr1-xO2 solid solutions modified with Mn2O3-Na2WO4 were used as catalysts for OCM. The effects of Ce/Zr ratio and Mn2O3-Na2WO4 doping on catalyst reactivity were investigated, with the catalyst with a Ce/Zr molar ratio of 0.15/0.85 showing promising activity and selectivity. The doped Ce0.15Zr0.85O2 catalyst was found to generate more O-2(-) species, leading to improved activity and selectivity at lower reaction temperatures.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Yu-Shih Lin, Jia-Yun Tu, De-Hao Tsai
Summary: This study demonstrates a facile aerosol-based method to prepare hybrid nanostructures for catalyzing steam-promoted CO2 reforming with methane. The resulting NiPdOx-CeO2 nanoparticles deposited on SiO2 nanoparticle clusters exhibit superior catalytic performance at low temperatures, with high turnover frequency, tunable H2/CO ratio, and long-term operation stability. Incorporating SiO2 nanoparticle clusters as support material helps to enhance the dispersion of active metals and suppress metal sintering.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Engineering, Environmental
Yuanqing Ding, Yanyan Jia, Mingxiang Jiang, Yanglong Guo, Yun Guo, Li Wang, Qingping Ke, Minh Ngoc Ha, Sheng Dai, Wangcheng Zhan
Summary: The structure of CeO2-ZrO2 mixed oxides support significantly affects the catalytic activity of Pd/CZ catalysts in methane combustion, with CZ oxides featuring a two-phase composite structure exhibiting higher oxygen storage capacity and mobility, positively impacting the performance of Pd/CZ catalysts.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Ning Rui, Xiaoshan Zhang, Feng Zhang, Zongyuan Liu, Xinxiang Cao, Zhenhua Xie, Rui Zou, Sanjaya D. Senanayake, Yanhui Yang, Jose A. Rodriguez, Chang-Jun Liu
Summary: The Ni/CeO2 catalyst prepared via gas discharge plasma and hydrogen reduction shows high activity in CO2 methanation at low temperatures, with excellent CH4 formation rate and redox property. The unique interfacial structure and metal-support interaction lead to the formation of rich interfacial Ni-CeO2 sites, improving the catalyst's performance significantly in H-2 splitting and CO2 activation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Alexandre Van Assche, Catherine Especel, Anthony Le Valant, Florence Epron
Summary: Low-loaded Pt-based catalysts supported on gamma-Al2O3, particularly when modified by K, show a decrease in deactivation due to coke deposition without affecting the initial turnover frequencies (TOF). Additionally, the Pt content does not have an impact on the TOF values on K-modified catalysts, indicating that ultradispersed Pt entities maintain the same activity regardless of Pt loading.
MOLECULAR CATALYSIS
(2022)
Review
Chemistry, Physical
Catherine Especel, Gwendoline Lafaye, Florence Epron
Summary: The development of bimetallic catalysts involves selecting appropriate metals and controlling their distribution on the support surface. Redox reactions can be used to deposit a second metal onto monometallic nanoparticles, creating core-shell nanoparticles with strong metal-metal interactions. This minireview describes the fundamentals and recent advances in the preparation of bimetallic catalysts using both direct redox reactions and the reduction of an intermediate reducing agent.
Article
Chemistry, Physical
Charlotte Croise, Khaled Alabd, Sophie Tence, Etienne Gaudin, Antoine Villesuzanne, Xavier Courtois, Nicolas Bion, Fabien Can
Summary: This study investigates the influence of rare-earth (R) element in Ru/RScSi electride-like intermetallic catalysts for ammonia synthesis under mild conditions. The catalytic performances follow the lanthanides series and appear correlated with the formation of the hydride phase. Ru-1.7/CeScSi shows remarkable catalytic activity associated with its reversible hydrogen storage-release properties. It is suggested that NHX formation could be the rate determining step rather than the N-2 cleavage over these catalysts.
Article
Chemistry, Applied
Maxime Delporte, Helena Kaper, Fabien Can, Nicolas Bion, Xavier Courtois
Summary: The use of expensive precious metal based catalysts has shown promise for catalytic treatment of residual refractory methane in the exhaust gas from NGV engines. Recent research has found that combining a perovskite with a Pd/YSZ catalyst improves both oxygen exchange behavior and methane oxidation. This study aims to investigate the concept of this dual catalytic bed system under more realistic conditions, and found that the configuration promoted CH4 abatement in lean mixture but was inhibited by CO2 and H2O.
TOPICS IN CATALYSIS
(2023)
Article
Chemistry, Physical
Charlotte Croise, Khaled Alabd, Antoine Villesuzanne, Fabien Can, Xavier Courtois, Etienne Gaudin, Sophie Tence, Nicolas Bion
Summary: Ru/LaScSi and Ru/CeTiGe were found to be the most active catalysts for ammonia synthesis, with Ru/LaScSi exhibiting electride-like properties and Ru/CeTiGe following an associative mechanism with the assistance of absorbed H. This conclusion was drawn through a combination of DFT calculations and 15N/14N homomolecular exchange experiments.
CATALYSIS COMMUNICATIONS
(2023)
Article
Chemistry, Applied
Olena Vozniuk, Thomas Cacciaguerra, Nathalie Tanchoux, Stefania Albonetti, Lorenzo Stievano, Jean-Marc M. Millet, Nicolas Bion, Francesco Di Renzo, Fabrizio Cavani
Summary: Copper-manganese spinel ferrites were evaluated as solid oxygen carriers for hydrogen production from water. The nature of the oxygen carrier phases greatly affected the amount and purity of hydrogen produced. Cu-rich ferrites were reduced to metallic copper and iron carbides, while Mn-rich ferrites were less deeply reduced to manganowustite. The oxidation reactions of ethanol by Cu-ferrites mainly produced CO and CO2, while Mn-ferrites mainly formed oxydehydrogenation products. The production of CO and CO2 during the reoxidation negatively affected the purity of the hydrogen formed.
Article
Chemistry, Physical
Remy Pointecouteau, Pierre Florian, Vincent Rodriguez, Nicolas Bion, Alain Demourgues
Summary: Cerium-based complex oxides are important materials for various applications in heterogeneous catalysis and electrocatalysis. The influence of structural defects on the thermal stability of the surface is still not fully understood. By using La-139 NMR and Raman spectroscopy, the lanthanum environments and associated defects in cerium-based compounds were analyzed. An unusual isolated La pseudo-cubic site was found to exist, and when thermally stable, it maintains a high specific surface area for catalytic applications at high temperatures.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Victoria Goncalves F. Pereira, Clarissa Perdomo Rodrigues, Fabio Souza Toniolo
Summary: This paper compared three methods of Ni/Al2O3 deposition on cordierite monoliths and evaluated their performance in methane steam reforming. The results showed that Al2O3 coating followed by NiO wet impregnation was the most efficient and suitable deposition method.
CATALYSIS COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Alexandre Nau, Remy Pointecouteau, Melissandre Richard, Thomas Belin, Fabien Can, Clement Comminges, Nicolas Bion
Summary: Catalytic methane combustion experiments were conducted on YSZ, Pd/YSZ, and Rh/YSZ at temperatures ranging from 200 to 700 degrees Celsius. While Pd/YSZ and Rh/YSZ exhibited similar light-off curves between 200 and 450 degrees Celsius, isotopic exchange experiments using CD4 and 18O2 revealed differences in the activation of reactant molecules for both supported catalysts. The use of C18O2 isotopic gas was found to be more suitable than 18O2 to evaluate the bulk oxygen mobility in YSZ at low temperatures. The exchange of gaseous CO2 with lattice YSZ oxygen atoms, facilitated by surface hydrogen carbonate intermediate species, demonstrated the contribution of YSZ bulk oxygen atoms in Rh/YSZ at low temperatures.
CATALYSIS COMMUNICATIONS
(2023)
Article
Engineering, Chemical
Vitor Duarte Lage, Anthony Le Valant, Nicolas Bion, Fabio Souza Toniolo
Summary: The catalytic conversion of CO2 and H2 into valuable chemicals is a promising alternative to address energy and environmental challenges. In this study, a facile K-Co-Cu-Al catalyst was developed for the selective conversion of CO2 into higher alcohols. By adjusting the Co:Cu ratio, reduction temperature, and reaction conditions, the selectivity and yield of higher alcohols were greatly enhanced.
CHEMICAL ENGINEERING SCIENCE
(2023)
Review
Energy & Fuels
Victor Hugo Souza de Abreu, Victoria Goncalves Ferreira Pereira, Lais Ferreira Crispino Proenca, Fabio Souza Toniolo, Andrea Souza Santos
Summary: This paper presents a systematic review of techno-economic evaluation studies on hydrogen production, using a bibliometric approach. The results show that water electrolysis is the most researched process, followed by gasification and steam reforming. In the biological category, both photo fermentation and dark fermentation have received attention. However, the literature highlights several gaps, such as a lack of comprehensive studies, emphasis on commercial viability, sensitivity analysis, and comparative analyses between production technologies.
Article
Chemistry, Multidisciplinary
Barbara B. Cazula, Renata O. da Fonseca, Andre Luiz A. Marinho, Fabio B. Noronha, Pedro Augusto Arroyo, Carlos I. Yamamoto, Rodrigo Brackmann, Helton Jose Alves
Summary: The present study focused on the physicochemical characteristics of two Si-MCM-41-type supports synthesized from different silica precursors, TEOS and RHS, with nickel dispersed on their surfaces. The dispersion of the active phase was found to have a direct influence on coke formation and the performance of methane dry reforming (DRM). Catalysts with 5%, 10%, and 20% Ni were prepared by wet impregnation and characterized using various techniques. The DRM reactions were carried out at 800 °C for 24 h, and the gaseous products were analyzed by gas chromatography. The results showed that catalysts with 20% Ni exhibited the best reaction performance, and the DRM results were similar for both TEOS and RHS catalysts at this Ni loading. However, the catalysts supported on RHS showed significantly lower coke formation, which can be considered negligible in a 24 h reaction.
JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Andre L. A. Marinho, Clement Comminges, Aurelien Habrioux, Stephane Celerier, Nicolas Bion, Claudia Morais
Summary: The electrochemical nitrogen reduction reaction (NRR) is an efficient, eco-friendly, and cost-effective alternative to the Haber-Bosch process for NH3 production. The Ti3C2 MXene has emerged as a promising electrocatalyst for NRR, and the addition of Zif-8 to MXene sheets can control the rate of hydrogen evolution reaction (HER). However, the ammonia produced using Zif-8@Ti3C2 as a cathode material is found to originate from nitrogen atoms in the Zif-8 structure, rather than N-2. These results highlight the importance of understanding the N-2 electroreduction process over N-containing electrocatalysts.
CHEMICAL COMMUNICATIONS
(2023)
