Materials Today CatalysisPub Date : 2024-09-01Epub Date: 2024-09-12DOI: 10.1016/j.mtcata.2024.100060
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}
Materials Today CatalysisPub Date : 2024-09-01Epub Date: 2024-07-25DOI: 10.1016/j.mtcata.2024.100059
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":"2024-09-01","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}
Materials Today CatalysisPub Date : 2024-09-01Epub Date: 2024-06-23DOI: 10.1016/j.mtcata.2024.100058
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":"2024-09-01","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}
{"title":"Pore size modulation of cobalt-corrole-based porous organic polymers for boosted electrocatalytic oxygen reduction reaction","authors":"Qian Zhao , Qingxin Zhang , Yizhen Wu , Zixuan Xiao , Yuxin Peng , Yuxin Zhou , Wei Zhang , Haitao Lei , Rui Cao","doi":"10.1016/j.mtcata.2024.100050","DOIUrl":"https://doi.org/10.1016/j.mtcata.2024.100050","url":null,"abstract":"<div><p>The highly active and selective oxygen reduction reaction (ORR) is vital to promote the performance of advanced energy conversion systems, such as fuel cells and other electrochemical devices. Porous framework materials have the capability to combine the catalytic performance of catalytic active units with their porous characteristics, making them promising oxygen reduction catalysts. However, due to the difficulty in designing and synthesizing catalytic active units, the pore size modulation of framework materials is primarily achieved by altering the linkers. We herein report the design and synthesis of three cobalt-corrole-based porous organic polymers (<strong>Co-POP-1</strong>, <strong>Co-POP-2</strong> and <strong>Co-POP-3</strong>) with different pore sizes, which were obtained by extending 5,15-<em>meso</em> substituents of Co corroles. Compared to <strong>Co-POP-1</strong> and <strong>Co-POP-2</strong>, <strong>Co-POP-3</strong> has the largest pore size. Benefiting from the enhanced mass transfer and the highly exposed active sites, <strong>Co-POP-3</strong> displayed remarkably boosted activity for the selective four-electron/four-proton (4e<sup>−</sup>/4 H<sup>+</sup>) ORR with a half-wave potential of <em>E</em><sub>1/2</sub> = 0.89 V versus reversible hydrogen electrode (RHE) in 0.1 M KOH solutions. This work not only presents a cobalt-corrole-based porous organic polymer catalyst with high ORR activity and selectivity but also provides a new strategy to moderate the pore size of porous framework materials.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"5 ","pages":"Article 100050"},"PeriodicalIF":0.0,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000127/pdfft?md5=85007b586e2d4239ae805d0523746dc9&pid=1-s2.0-S2949754X24000127-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140646874","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}
Materials Today CatalysisPub Date : 2024-06-01Epub Date: 2024-03-10DOI: 10.1016/j.mtcata.2024.100049
Nidhi Kumari , Supriyo Halder , Srijita Naskar , Sanjib Ganguly , Kausikisankar Pramanik , Farzaneh Yari , Adrian Dorniak , Wolfgang Schöfberger , Soumyajit Roy
{"title":"Coordinatively fluxional diazo-based organo-electrocatalyst for conversion of CO2 to C2 and C3 products","authors":"Nidhi Kumari , Supriyo Halder , Srijita Naskar , Sanjib Ganguly , Kausikisankar Pramanik , Farzaneh Yari , Adrian Dorniak , Wolfgang Schöfberger , Soumyajit Roy","doi":"10.1016/j.mtcata.2024.100049","DOIUrl":"https://doi.org/10.1016/j.mtcata.2024.100049","url":null,"abstract":"<div><p>The conversion of carbon dioxide (CO<sub>2</sub>) into valuable chemicals, specifically C<sub>2</sub> and C<sub>3</sub>, through metal-free electrocatalysis remains a formidable challenge. Breaking away from traditional transition metal complexes, the focus is on designing and selecting efficient organic catalysts. In this pursuit, a diazo-based organic bulky ligand emerges as a promising candidate, offering a solution that is both sustainable and renewable. The key feature of this ligand is its low-lying π* (LUMO), enabling it to readily accept an electron in an electrochemical environment when a potential is applied. The synthesized Diazo-based ligands have been meticulously characterized using various techniques, including <sup>1</sup>H NMR, <sup>13</sup>C NMR, UV-Vis, and IR spectroscopy. This diazo-based ligand serves as an electrocatalyst, undergoing reduction to a triplet diradical that acts as a nucleophile. In an aqueous medium, it forms an adduct with CO<sub>2</sub>, leading to the generation of a formyl radical. This radical further couples to produce acetic acid and acetone with efficiencies of 19.6% and 24.2%, respectively, at pH 5.5. To provide a deeper understanding, we present a proposed mechanism pathway supported by <em>in-situ</em> UV-Vis spectroscopy and a comprehensive Density Functional Theory (DFT) study. These findings mark a significant step forward in the field of metal-free electrocatalysis, offering a sustainable approach to the conversion of CO<sub>2</sub> into valuable chemicals, contributing to the development of renewable and environmentally friendly systems.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"5 ","pages":"Article 100049"},"PeriodicalIF":0.0,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000115/pdfft?md5=94dc782f0ba3555c82d1b17231c8d404&pid=1-s2.0-S2949754X24000115-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140122974","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}
Materials Today CatalysisPub Date : 2024-06-01Epub Date: 2024-05-24DOI: 10.1016/j.mtcata.2024.100055
Songqing Zhang , Jiarui Lou , Chenhui Wang , Qian Li , Yufeng Li , Linfeng Jin , Changfa Guo
{"title":"Modification strategies and applications of Mn–Cd–S solid solution-based photocatalysts","authors":"Songqing Zhang , Jiarui Lou , Chenhui Wang , Qian Li , Yufeng Li , Linfeng Jin , Changfa Guo","doi":"10.1016/j.mtcata.2024.100055","DOIUrl":"10.1016/j.mtcata.2024.100055","url":null,"abstract":"<div><p>Semiconductor photocatalyzed energy production and environment treatment have received a lot of attention. Mn–Cd–S solid solutions (Mn<sub><em>x</em></sub>Cd<sub>1−<em>x</em></sub>S) with tunable band structure, suitable redox capacity, and visible light response is recognized as one of the most promising photocatalysts for practical applications. However, low separation efficiency of photogenerated carriers and sluggish reaction kinetics restricts its photocatalytic activity. This review discusses the advantages and drawbacks of Mn<sub><em>x</em></sub>Cd<sub>1−<em>x</em></sub>S for photocatalysis in terms of electronic band structure and surveys the modification strategies of photocatalytic activity, including modulation of Mn/Cd ratio, morphology/structure regulation, defect engineering, construction of heterojunction, loading cocatalysts, and integration of multiple strategies. Then, the progress in photocatalytic water splitting to hydrogen, carbon dioxide reduction, and pollutant degradation using Mn<sub><em>x</em></sub>Cd<sub>1−<em>x</em></sub>S-based materials are summarized. Finally, it is concluded by outlining the challenges and opportunities for developing efficient photocatalysts based on Mn<sub><em>x</em></sub>Cd<sub>1−<em>x</em></sub>S.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"5 ","pages":"Article 100055"},"PeriodicalIF":0.0,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000176/pdfft?md5=572fb71d5bec835bd4b23bb2b40c2d37&pid=1-s2.0-S2949754X24000176-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141136771","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}
Materials Today CatalysisPub Date : 2024-06-01Epub Date: 2023-11-17DOI: 10.1016/j.mtcata.2023.100033
Adrian Chun Minh Loy, Wei Lin Ng, Sankar Bhattacharya
{"title":"Advanced characterization techniques for the development of Subatomic scale catalysts: One step closer to industrial scale fabrication","authors":"Adrian Chun Minh Loy, Wei Lin Ng, Sankar Bhattacharya","doi":"10.1016/j.mtcata.2023.100033","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100033","url":null,"abstract":"<div><p>To date, the large-scale fabrication of subatomic scale catalysts (SSCs) remains a formidable challenge despite their tremendous potential to drive future clean energy conversion and decarbonization technologies. The primary hurdle lies in understanding the physicochemical relationship at the multi-scale interface (i.e., nanoscale, sub-nano, clusters, atomic) in constructing the heterogeneous catalysts. Conversely, high throughput advanced characterizations offer efficient and accelerated analysis of catalysts' chemical properties, bridging the gap between laboratory-to-industrial scale catalyst development for various engineering applications. The implementation of advanced characterizations is paramount in reducing uncertainties in bulk production, particularly during pre-screening assessments of a diverse range of SSCs compositions and configurations. Overall, this review aims to provide an illuminating overview of the streamlined SSCs development process, propelling us one step closer to achieving bulk-scale fabrication.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"4 ","pages":"Article 100033"},"PeriodicalIF":0.0,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X23000339/pdfft?md5=95c8706239a036bf057c1c2b885fc375&pid=1-s2.0-S2949754X23000339-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138436367","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}