Charlotte Croisé, Xavier Courtois, Stéphane Célérier, Lola Loupias, Christine Canaff, Julie Rousseau, Nicolas Bion, Fabien Can
{"title":"(Ru-)Mo2C (MXene) catalysts for ammonia synthesis: From Haber-Bosch to chemical looping processes","authors":"Charlotte Croisé, Xavier Courtois, Stéphane Célérier, Lola Loupias, Christine Canaff, Julie Rousseau, Nicolas Bion, Fabien Can","doi":"10.1016/j.mtcata.2024.100066","DOIUrl":"10.1016/j.mtcata.2024.100066","url":null,"abstract":"<div><div>This study investigated (Ru-)Mo<sub>2</sub>C (MXene) materials for ammonia thermo-catalytic synthesis under atmospheric or moderate pressure. Under a H<sub>2</sub>-N<sub>2</sub> (3:1) flow, the Mo<sub>2</sub>C MXene phase showed limited activity in ammonia synthesis at atmospheric pressure at 400 °C (0.01 mmol h⁻¹ g⁻¹), which increased significantly with temperature and pressure, reaching 2.07 mmol h⁻¹ g⁻¹ at 500°C and under 5 bar. Interestingly, Mo-based MXene was able to generate an appreciable quantity of ammonia without promoters such as ruthenium, the most active metal for the ammonia synthesis reaction. Unexpectedly, the addition of Ru to Mo<sub>2</sub>C did not enhance its activity. The nitriding of the MXene under NH<sub>3</sub> or N<sub>2</sub> was then performed and characterized. A thermal treatment under NH<sub>3</sub> (600 °C, 5 bar) was efficient and, interestingly, nitriding also occurred in a lower extent under N<sub>2</sub> (600 °C, 5 bar) for the sample containing ruthenium. The N-containing MXene produced ammonia under pure H<sub>2</sub> flow from temperatures lower than 250 °C. Consecutive nitriding treatments and ammonia production under pure H<sub>2</sub> were successfully achieved and demonstrated for 5 cycles. This result is promising for chemical looping ammonia production process. This work highlights essential aspects that should be explored for future advances to consider using Mo<sub>2</sub>CT<sub>x</sub> MXene for the efficient thermal production of ammonia.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100066"},"PeriodicalIF":0.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142320116","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Youcai Meng , Junyang Ding , Yifan Liu , Guangzhi Hu , Yanhong Feng , Yinghong Wu , Xijun Liu
{"title":"Advancements in Amorphous Oxides For Electrocatalytic Carbon Dioxide Reduction","authors":"Youcai Meng , Junyang Ding , Yifan Liu , Guangzhi Hu , Yanhong Feng , Yinghong Wu , Xijun Liu","doi":"10.1016/j.mtcata.2024.100065","DOIUrl":"10.1016/j.mtcata.2024.100065","url":null,"abstract":"<div><div>Electrocatalytic CO<sub>2</sub> reduction (ECR) is a crucial energy conversion technology that transforms CO<sub>2</sub> into value-added chemicals, reducing reliance on fossil fuels and advancing energy transitions. Designing high-performance catalysts is pivotal for widespread adoption of CO<sub>2</sub> reduction reactions, aiming for high activity, selectivity, and stability. Amorphous oxides represent a burgeoning frontier in this field, attracting attention due to their abundant active sites that refine the catalyst structure-performance relationship. This paper aims to provide an overview of recent advances in using amorphous oxides for ECR. We begin by introducing the basic theory of electrocatalytic CO<sub>2</sub> reduction, followed by discussing current synthesis approaches for amorphous oxides in CO<sub>2</sub> reduction, focusing on optimization strategies for these catalysts. Finally, we address challenges and future perspectives of amorphous oxides in ECR, aiming to foster the development of more efficient catalyst designs.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100065"},"PeriodicalIF":0.0,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142320117","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Haixin Sun , Yingying Gao , Mengyuan Chen , Ming Li , Qinqin Xia , Yongzhuang Liu , Juan Meng , Shuo Dou , Haipeng Yu
{"title":"Synergistic boosting the electrooxidation of biomass-based 5-hydroxymethylfurfural on cellulose-derived Co3O4/N-doped carbon catalysts","authors":"Haixin Sun , Yingying Gao , Mengyuan Chen , Ming Li , Qinqin Xia , Yongzhuang Liu , Juan Meng , Shuo Dou , Haipeng Yu","doi":"10.1016/j.mtcata.2024.100062","DOIUrl":"10.1016/j.mtcata.2024.100062","url":null,"abstract":"<div><div>Catalysts play a pivotal role in the efficient conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) through electrochemical oxidation. In this work, a cost-effective and highly efficient cobalt-based electrocatalyst for the synthesis of bio-based carboxylic acids was reported. By the employment of cellulose, which was dissolved in the alkaline-urea with cobalt ion, as the precursor, it derived a carbon-coated Co<sub>3</sub>O<sub>4</sub> (Co<sub>3</sub>O<sub>4</sub>@NC) catalyst with a high specific surface area and rich porous structure. When utilized in the electrocatalytic conversion of HMF to FDCA, the catalyst exhibited exceptional yields and Faradaic efficiency which surpassed 95 %. In-situ Raman spectra unveiled that a dual-pathway process occurred on this catalyst, with part of Co<sub>3</sub>O<sub>4</sub> serving as active sites for HMF adsorption, while other Co<sub>3</sub>O<sub>4</sub> transformed into CoOOH during the reaction. This dual-pathway electrocatalysis facilitated the highly efficient conversion of HMF. Additionally, using bio-based alcohols/aldehydes as the feedstocks, eight carboxylic acids were successfully synthesized with yields ranging from 91.5 % to 99 %. This study presents a highly efficient electrocatalyst derived from biomass, enabling diverse bio-based carboxylic acid production with significant potential for sustainable chemical synthesis.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100062"},"PeriodicalIF":0.0,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142320114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ifeanyi Michael Smarte Anekwe , Stephen Okiemute Akpasi , Emeka Michael Enemuo , Darlington Ashiegbu , Sherif Ishola Mustapha , Yusuf Makarfi Isa
{"title":"Innovations in catalytic understanding: A journey through advanced characterization","authors":"Ifeanyi Michael Smarte Anekwe , Stephen Okiemute Akpasi , Emeka Michael Enemuo , Darlington Ashiegbu , Sherif Ishola Mustapha , Yusuf Makarfi Isa","doi":"10.1016/j.mtcata.2024.100061","DOIUrl":"10.1016/j.mtcata.2024.100061","url":null,"abstract":"<div><div>This work provides a comprehensive overview of advanced characterisation techniques to unravel the molecular intricacies of catalytic processes. It begins with an introduction to catalytic processes and emphasises the importance of innovations in characterisation techniques, including SEM, XRD, UV-Vis, FTIR, RAMAN, XPS, NMR, TEM, AFM and the combined application of these techniques for improved catalytic investigation. The review of the development of catalytic processes provides a historical overview of progress and examines paradigm shifts in catalytic mechanisms and catalyst categories. Conventional microscopic and spectroscopic tools are revisited, highlighting the improvements in these techniques that provide insight into catalytic structures through surface analysis. Significant advances, including the application of computational techniques, in the study of catalysts are also discussed, focusing on state-of-the-art techniques that provide unprecedented detail on catalyst properties, mechanisms and processes. Comparative evaluations highlight the advantages and limitations of these techniques. The study concludes by identifying and overcoming challenges, anticipating prospects and emphasising the constant quest for innovation in understanding catalysts. By integrating developments in microscopic and spectroscopic methods, the study provides a comprehensive insight into how these tools improve the precision and depth of catalyst characterisation, driving innovation and future directions in catalysis research.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100061"},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000231/pdfft?md5=eda9c71863431be2bd77dc1b0173f6ef&pid=1-s2.0-S2949754X24000231-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142312189","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ziyang Gan , Rayantan Sadhukhan , Christof Neumann , Nandita Mohandas , Emad Najafidehaghani , Manuel Mundszinger , Johannes Biskupek , Ute Kaiser , Tharangattu N. Narayanan , Antony George , Andrey Turchanin
{"title":"Wafer scale and substrate-agnostic growth of MoS2 nanowalls for efficient electrocatalytic hydrogen generation in acidic and alkaline media","authors":"Ziyang Gan , Rayantan Sadhukhan , Christof Neumann , Nandita Mohandas , Emad Najafidehaghani , Manuel Mundszinger , Johannes Biskupek , Ute Kaiser , Tharangattu N. Narayanan , Antony George , Andrey Turchanin","doi":"10.1016/j.mtcata.2024.100060","DOIUrl":"10.1016/j.mtcata.2024.100060","url":null,"abstract":"<div><p>Emerging as a promising alternative to expensive platinum-based catalysts for electrocatalytic hydrogen evolution reaction (HER), molybdenum disulfide (MoS<sub>2</sub>) stands out for its favourable thermodynamic properties. However, the catalytic activity of MoS<sub>2</sub> is mostly confined to its edges while the basal plane remains inactive, limiting practical applicability. Fabrication of stable MoS<sub>2</sub> structures with enhanced active sites on a given surface area still remains a complex task. Here we introduce a substrate-agnostic, metal-organic chemical vapour deposition (MOCVD) method for large-area 3D dendritic nanostructures of 2D MoS<sub>2</sub>, termed as “MoS<sub>2</sub> nanowalls”. Using scanning and transmission electron microscopy (SEM/TEM), we elucidate the growth mechanism of the MoS<sub>2</sub> nanowalls and their branched dendritic structure. Even subjected to extreme pH environments (0 and 14) during the HER, the grown MoS<sub>2</sub> nanowalls show remarkable stability even after >170 hours of continuous operation and exhibit excellent catalytic activity with 10 mAcm<sup>−2</sup> current density achievable by applying low overpotentials (309±2 mV at pH = 0 and 272±2 mV at pH = 14). The presented large-area growth method for inexpensive MoS<sub>2</sub> nanowall based catalyst can pave the way for practical applications of water electrolysis cells operating at low voltages (≤1.5 V).</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"6 ","pages":"Article 100060"},"PeriodicalIF":0.0,"publicationDate":"2024-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X2400022X/pdfft?md5=3786ea9c0af59ae7ea78710e2288582f&pid=1-s2.0-S2949754X2400022X-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142239346","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Marcos G. Farpón, Enrique Torregrosa, Gonzalo Prieto
{"title":"“Heating where it hurts”: Electromagnetic induction remote energy transfer to a solid catalyst enables waste polymer upcycling","authors":"Marcos G. Farpón, Enrique Torregrosa, Gonzalo Prieto","doi":"10.1016/j.mtcata.2024.100059","DOIUrl":"10.1016/j.mtcata.2024.100059","url":null,"abstract":"<div><p>Electromagnetic induction heating currently attracts significant attention as a means to electrify catalytic processes and leverage a highly specific and localized energy supply. This Comment article features the application of this unconventional energy input for waste polymer conversion to fuel hydrocarbons.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"6 ","pages":"Article 100059"},"PeriodicalIF":0.0,"publicationDate":"2024-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000218/pdfft?md5=acf4c1c41b42a8ebdc0b279f0e689320&pid=1-s2.0-S2949754X24000218-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141848684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sarah Bimmermann , Daniel Siegmund , Kallol Ray , Ulf-Peter Apfel
{"title":"Investigation of m- and p-xylene linked bimetallic Ni-cyclam-complexes as potential electrocatalysts for the CO2 reduction","authors":"Sarah Bimmermann , Daniel Siegmund , Kallol Ray , Ulf-Peter Apfel","doi":"10.1016/j.mtcata.2024.100058","DOIUrl":"https://doi.org/10.1016/j.mtcata.2024.100058","url":null,"abstract":"<div><p>Among the various molecular CO<sub>2</sub> reduction catalysts, the [Ni(cyclam)]<sup>2+</sup> (<strong>Ni-{N<sub>4</sub>})</strong> complex with its earth-abundant metal center and macrocyclic ligand proved to be efficient for the selective electrochemical conversion of CO<sub>2</sub> to CO. In the present study we now connected the two Ni-cyclam units by using <em>para</em>- and <em>meta</em>-xylene as organic linkers attached to the amines of the macrocycle to form the <em><strong>p</strong></em><strong>-{Ni<sub>2</sub>} and</strong> <em><strong>m</strong></em><strong>-{Ni<sub>2</sub>}</strong> complexes, respectively, and test them as catalysts for the electrochemical CO<sub>2</sub> reduction reactions. Notably, the <em><strong>p</strong></em><strong>-{Ni<sub>2</sub>}</strong> complex demonstrates a higher faraday efficiency in the electrochemical reduction of CO<sub>2</sub> to CO compared to the <em><strong>m</strong></em><strong>-{Ni<sub>2</sub>}</strong> complex. This finding highlights the significant role played by the M-M distance in influencing this catalytic process.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"6 ","pages":"Article 100058"},"PeriodicalIF":0.0,"publicationDate":"2024-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000206/pdfft?md5=b643e202f5402da26a8e5f551eaf7f0d&pid=1-s2.0-S2949754X24000206-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141479384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}