Clément Molinet-Chinaglia, Luis Cardenas, Philippe Vernoux, Laurent Piccolo, Stéphane Loridant
{"title":"Tuning the metal loading of Pt/CeO2 catalysts for the water-gas shift reaction","authors":"Clément Molinet-Chinaglia, Luis Cardenas, Philippe Vernoux, Laurent Piccolo, Stéphane Loridant","doi":"10.1016/j.mtcata.2024.100046","DOIUrl":"https://doi.org/10.1016/j.mtcata.2024.100046","url":null,"abstract":"<div><p>Identifying active platinum species at the surface of Pt/CeO<sub>2</sub> catalysts is still a hot topic in the literature. In this work, an oxidizing pretreatment at 500 °C was applied to generate ultradispersed PtO<sub>x</sub> species before the reaction. It is shown that the molar activity of such catalysts for the water-gas shift reaction is strongly dependent on the platinum content, increasing by a factor of 2.5 from 0.1 to 0.6 wt% and stabilizing from 0.6 to 1.4 wt%. The tracking of Pt species present under reaction conditions (230 °C, H<sub>2</sub>O/CO=4) was performed using <em>operando</em> DRIFT spectroscopy, CO-TPR and STEM in connection with the catalytic activity. A major structural change was found for Pt loadings above 0.6 wt% through the formation of metallic Pt<sup>0</sup> nanoparticles of ca 1.4 nm from oxidized Pt single atoms and clusters. Conversely, for Pt contents below 0.6 wt%, Pt species possess a stronger interaction with CeO<sub>2</sub> as well as a lower nuclearity, limiting their activation under reaction conditions. This strongly suggests that metallic Pt nanoparticles, prevalent at high loading, are more active than oxidic Pt single atoms and small clusters, which are predominantly present at low loading. This study highlights the key role of PtO<sub>x</sub> reducibility and the importance to optimize the Pt loading to obtain active catalysts for the water-gas shift reaction.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"4 ","pages":"Article 100046"},"PeriodicalIF":0.0,"publicationDate":"2024-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000085/pdfft?md5=319b07d75eab863c64c71dfd5a987da5&pid=1-s2.0-S2949754X24000085-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139976049","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":"Recent progress on molecular catalysts integrated photoelectrochemical systems for water oxidation","authors":"Xiaokang Wan , Guanghui Zhu , Zhifu Zhou , Xiangjiu Guan","doi":"10.1016/j.mtcata.2024.100042","DOIUrl":"https://doi.org/10.1016/j.mtcata.2024.100042","url":null,"abstract":"<div><p>The major limitations of photoelectrochemical (PEC) water splitting lies in the currently unsatisfying efficiency and stability of the semiconductor materials-based water splitting systems. By addressing these limitations, the immobilization of the molecular catalysts on semiconductor photoanodes to establish a hybrid inorganic-organic PEC system has attracted an increasing research attention. It is crucial to choose a suitable molecular catalyst and effectively couple it into a hybrid photoelectrode system. In this review, focusing on the water oxidation process, molecular catalysts integrated photoelectrochemical water oxidation systems are highlighted from the perspective of the roles of molecular catalysts and the integration strategies in the hybrid system. The most recent advances are summarized with various case studies presented, based on which perspectives are proposed to provide guidance toward the rational design of an integrated system for future development.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"4 ","pages":"Article 100042"},"PeriodicalIF":0.0,"publicationDate":"2024-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000048/pdfft?md5=a9a8d726ef87d23e9b75222c82b862a3&pid=1-s2.0-S2949754X24000048-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139725779","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":"Electro-oxidation of 5-hydroxymethylfurfural by a catalyst containing copper nanoparticles and single copper atoms","authors":"Yongfang Zhou , Yi Shen , Hongying Li","doi":"10.1016/j.mtcata.2024.100041","DOIUrl":"10.1016/j.mtcata.2024.100041","url":null,"abstract":"<div><p>Atomic-site electrocatalysts are being considered as potential alternative catalysts due to their exceptionally high atom utilization efficiencies, well-defined active sites and high selectivities. However, the presence of nanoparticles in the single-atom catalysts may affect the catalytic performance. Herein, single-copper-atoms and copper nanoparticles co-embedded in nitrogen-doped carbon nanosheets (Cu<sub>NPs</sub>@Cu/NCNSs) were synthesized for 5-hydroxymethylfurfural electro-oxidation. Single copper atoms supported on nitrogen-doped carbon nanosheets (Cu/NCNSs) and copper nanoparticles supported on carbon (Cu<sub>NPs</sub>/C) were also synthesized for comparison. The Cu<sub>NPs</sub>/C exhibited high efficiency in electro-oxidation of HMF to 2,5-furandicarboxylic acid (FDCA) at a low potential of 1.42 V. However, the Cu<sub>NPs</sub>@Cu/NCNSs showed a high 5-formyl-2-furancarboxylic acid (FFCA) selectivity of 86.7%. Oxalic acid (OA) treatment experiments showed that single copper atoms played a major role on the oxidation of HMF to FFCA. Cu(OH)<sub>2</sub> active species generated by electrochemical oxidation were demonstrated as the primary catalytic sites for HMF oxidation on the Cu<sub>NPs</sub>/C. In-situ Raman spectra results demonstrated that HMF oxidation on the Cu<sub>NPs</sub>/C followed the path to 5-hydroxymethyl-2-furancarboxylic acid (HFCA), while on the Cu<sub>NPs</sub>@Cu/NCNSs and Cu/NCNSs, HMF was oxidized along the 5-diformylfuran (DFF) pathway.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"4 ","pages":"Article 100041"},"PeriodicalIF":0.0,"publicationDate":"2024-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000036/pdfft?md5=5f10506b80a4c815c4026a4d17601254&pid=1-s2.0-S2949754X24000036-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139635002","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":"Synergy of visible-light responsive photocatalytic materials and device engineering for energy and environment: Minireview on hydrogen production and water decontamination","authors":"Pablo Jiménez-Calvo","doi":"10.1016/j.mtcata.2024.100040","DOIUrl":"10.1016/j.mtcata.2024.100040","url":null,"abstract":"<div><p>Accelerated advances in photocatalysis demand alignment with a well-defined Technology Readiness Levels (TRLs) roadmap to overcome bottlenecks and attain TRLs of 3 or beyond. This minireview highlights the key components for the development of device technology for photocatalytic hydrogen production, focusing on visible-light responsive catalysts and lab-scale setups. Two main aspects are critically discussed: modifications in semiconductor-based materials and progress in device engineering design. In the first section, the emphasis is on two specific energy materials: visible-light active carbon nitrides (CN) and the established benchmark titanium dioxide (TiO<sub>2</sub>). Examples of both CN and TiO<sub>2</sub> modified by heteroatom doping, semiconductor heterojunction, metal Schottky junction, pre- and post-thermal treatments are showcased. Furthermore, Imogolite nanotubes are introduced as evolving 1D nanostructured nanoreactors for energetic photoelectrocatalysis. In the second section, the emphasis is on two types of laboratory batch photoreactors tailored for hydrogen production. Their main features are critically discussed in terms of their impact on the overall photonic, heat, and mass profiles. Moreover, a continuous flow water disinfection system is introduced as promising environmental technology. The objective to showcase these devices is to underscore the significance of advancing TRLs from 3 to 4–6. A few perspectives, routes, and challenges on visible-light absorbers and photoreactors devices are stated. Research trends are included to stay update with the latest advances in engineering and materials, specifically polyheptazine imides, computational modeling, machine learning, biomass conversion, single-atom catalysis, operando characterization, and the use of sea and wastewater for solar liquid fuels. This mini-review succinctly updates experts and non-experts on the author's recent works.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"4 ","pages":"Article 100040"},"PeriodicalIF":0.0,"publicationDate":"2024-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000024/pdfft?md5=eb0bb930f451ba4befd93269f39e56fe&pid=1-s2.0-S2949754X24000024-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139638934","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":"High-entropy oxides for energy-related electrocatalysis","authors":"Han Cai, Peikun Zhang, Bowen Li, Yinlong Zhu, Zhuhua Zhang, Wanlin Guo","doi":"10.1016/j.mtcata.2024.100039","DOIUrl":"https://doi.org/10.1016/j.mtcata.2024.100039","url":null,"abstract":"<div><p>Electrocatalysis plays a crucial role in the conversion and storage of renewable energy, offering significant potential for addressing the energy crisis and environmental concerns. High-entropy oxides (HEOs), a class of emerging functional materials, have gained increasing attention in electrocatalysis due to their stable crystal structure, exceptional geometric compatibility, unique electronic balance factors, and abundant active sites. In this comprehensive review, we present recent advancements in utilizing HEOs as catalysts for various energy-based electrocatalytic reactions. We begin with an overview of HEOs that includes definitions, fundamental properties, and theoretical investigations. Subsequently, we describe different synthetic methods for HEOs while highlighting two newly-developed techniques. Furthermore, we extensively discuss recent developments in HEO-based electrocatalysts with diverse crystal structures such as rock-salt-type, rutile-type, spinel-type, perovskite-type, and other specially-structured HEOs. Special emphasis is placed on designed strategies aimed at enhancing performance and exploring correlations between structure/ composition and electrocatalytic performance. Finally, we provide concluding remarks along with perspectives on future opportunities in this exciting field.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"4 ","pages":"Article 100039"},"PeriodicalIF":0.0,"publicationDate":"2024-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000012/pdfft?md5=11e664a61eb536774de857281b78177b&pid=1-s2.0-S2949754X24000012-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139504057","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}
He Sun , Houssein Awada , Haitato Lei , Abdalaziz Aljabour , Luyang Song , Simon Offenthaler , Rui Cao , Wolfgang Schöfberger
{"title":"Tuning ORR selectivity of π-conjugated cobalt corroles from 2e- to 4e-","authors":"He Sun , Houssein Awada , Haitato Lei , Abdalaziz Aljabour , Luyang Song , Simon Offenthaler , Rui Cao , Wolfgang Schöfberger","doi":"10.1016/j.mtcata.2023.100038","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100038","url":null,"abstract":"<div><p>Efficient oxygen reduction reaction (ORR) is crucial for the performance of fuel cells and other electrochemical devices. Seeking for stable and electrochemically selective 2e<sup>-</sup> and 4e<sup>-</sup> ORR electrocatalyst is yet a challenge, making the design extremely important and outmost of interest. In this study, we demonstrate a method to tune ORR selectivity by adjusting the local cobalt density through oligo-/polymerization of π-conjugated cobalt(III) A<sub>2</sub>B and A<sub>3</sub>-corroles to linear and two-dimensional matrix structures. These heterogeneous catalysts exhibit remarkable physicochemical properties, fast charge transfer kinetics, electrochemical reversibility, and high durability. Unselective three-electron transfer kinetics with n = 2.5–2.9 in between −0.20 V and +0.40 V vs. RHE are detected with the π-conjugated cobalt(III) A<sub>2</sub>B- corrole polymers. Highly selective four-electron kinetics with n = 3.7 in between −0.20 V and +0.40 V vs. RHE are detected by employing the cobalt A<sub>3</sub>-corrole oligomers during the ORR catalysis.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"4 ","pages":"Article 100038"},"PeriodicalIF":0.0,"publicationDate":"2023-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X23000388/pdfft?md5=c57114cb9d4809f18732ffa32a10b97e&pid=1-s2.0-S2949754X23000388-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138838919","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}
Guanyu Chen , Ning Zhao , Yanpeng Chen , Jiuhu Zhao , Rongshu Zhu , Mei Hong
{"title":"Recent advances in synthetic strategies and physicochemical modifications of SSZ-13 zeolites: A review","authors":"Guanyu Chen , Ning Zhao , Yanpeng Chen , Jiuhu Zhao , Rongshu Zhu , Mei Hong","doi":"10.1016/j.mtcata.2023.100037","DOIUrl":"10.1016/j.mtcata.2023.100037","url":null,"abstract":"<div><p>Aluminosilicate zeolites are widely recognized as an industrially important crystalline microporous material. Among them, small-pore SSZ-13 stands out as an artificial aluminosilicate zeolite with CHA topology. Since its invention in 1985, SSZ-13 zeolite has garnered significant attention in both academia and industry due to its exceptional performance in heterogeneous catalysis, gas adsorption and separation. Modification of its physicochemical properties to meet the diverse requirements of various application scenarios has become a prominent topic in zeolite research. Considerable efforts have been devoted to alleviating the diffusion limitations inherent in micropores by downsizing crystal size or introducing additional mesopores and/or macropores to construct hierarchical structures. Regulating framework Al atoms in isolation or pairing introduces remarkable catalytic or adsorptive diversity into compositionally similar SSZ-13 zeolites. The conventional synthesis of SSZ-13 zeolite, which involves the use of expensive and toxic <em>N</em>,<em>N</em>,<em>N</em>-trimethyl-1-adamantylammonium hydroxide (TMAdaOH) as an organic structure-directing agent (OSDA) and a hydrothermal crystallization process lasting typically more than four days, severely hinders its cost-effective utilization. In response, extensive research endeavors have been dedicated to developing innovative synthetic approaches for SSZ-13 zeolites aimed at greener, more efficient, and economically viable production. This article presents a comprehensive overview of recent research developments in the field of SSZ-13 zeolites, encompassing novel synthetic methods, hierarchical engineering, nanocrystal technology, Al distribution, fast synthesis, and cost reduction techniques, aiming to provide valuable insights and guidance to relevant researchers.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"4 ","pages":"Article 100037"},"PeriodicalIF":0.0,"publicationDate":"2023-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X23000376/pdfft?md5=286cac8cb85d22296b84455e19b82f69&pid=1-s2.0-S2949754X23000376-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138616215","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}
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":"2023-11-17","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}
{"title":"Lithium-mediated nitrogen reduction for electrochemical ammonia synthesis: From batch to flow reactor","authors":"Xianbiao Fu","doi":"10.1016/j.mtcata.2023.100031","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100031","url":null,"abstract":"<div><p>The electrochemical synthesis of ammonia has emerged as a sustainable alternative to the traditional Haber-Bosch process. This review provides a comprehensive examination of the transition from batch reactors to flow reactors in the context of lithium-mediated nitrogen reduction for electrochemical ammonia synthesis. It underscores the advances made in mechanistic understanding, reactor design, and the exploration of key variables such as pressure, Li salts, proton shuttles, and additives. The advantages and disadvantages of both reactor types are critically assessed, offering insights into their suitability for scaling up production. Moreover, this review elucidates the role of various factors in enhancing Faradaic efficiency and energy efficiency, thus contributing to the development of more efficient, sustainable, and economically viable electrochemical ammonia synthesis methods. The synergy between fundamental research and engineering advancements in this field is highlighted, providing a roadmap for future research endeavors and industrial applications.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"3 ","pages":"Article 100031"},"PeriodicalIF":0.0,"publicationDate":"2023-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X23000315/pdfft?md5=1f7851e2018e504687d6ba4536283e7a&pid=1-s2.0-S2949754X23000315-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"92039844","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}