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Allying cobalt nanoclusters with carbon nanofibers for selectively electrocatalytic hydrogenation of unsaturated aldehyde with water as hydrogen source 以水为氢源,钴纳米团簇与碳纳米纤维选择性电催化不饱和醛加氢
Materials Today Catalysis Pub Date : 2025-06-01 DOI: 10.1016/j.mtcata.2025.100104
Xinyu Yang , Sheng-Hua Zhou , Xiaofang Li , Xin-Tao Wu , Qi-Long Zhu
{"title":"Allying cobalt nanoclusters with carbon nanofibers for selectively electrocatalytic hydrogenation of unsaturated aldehyde with water as hydrogen source","authors":"Xinyu Yang ,&nbsp;Sheng-Hua Zhou ,&nbsp;Xiaofang Li ,&nbsp;Xin-Tao Wu ,&nbsp;Qi-Long Zhu","doi":"10.1016/j.mtcata.2025.100104","DOIUrl":"10.1016/j.mtcata.2025.100104","url":null,"abstract":"<div><div>The electrocatalytic hydrogenation of α, β-unsaturated aldehydes has attracted significant attention, yet the design of electrocatalysts with selective adsorption over C<img>C or C<img>O bond remaining a challenging task. In this study, the Co nanoclusters anchored onto the nitrogen-doped porous carbon nanofibers were elaborately fabricated for efficient electrocatalytic hydrogenation. A kinetically driven mono-micelle-oriented self-assembly method was applied to synthesize the polymer nanofibers as the accommodation for Co<sup>2 +</sup>. The stepwise pyrolysis of Co<sup>2+</sup>/polymer nanofibers with dicyandiamide yielded the evenly distributed Co nanoclusters with an average size of ∼4 nm over the nitrogen-doped porous carbon nanofibers. Benefited from the high activity of the Co nanoclusters and their rapid electron communication with the nitrogen-doped porous carbon nanofibers, this electrocatalyst demonstrated excellent performance in the selectively electrocatalytic hydrogenation of cinnamaldehyde to hydrocinnamaldehyde, achieving a high selectivity of 90.9 % and a conversion of 68.2 % at 12 mA cm<sup>−2</sup>. The further in-situ spectroscopy analysis and density functional theory calculations revealed the more preferred adsorption of C<img>C bond and easier water dissociation to give the active H atoms over the Co nanoclusters, which shed light on the hydrogenation mechanism over this electrocatalyst. Our study can provide a new insight in catalyst design for electrocatalytic hydrogenation reaction.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100104"},"PeriodicalIF":0.0,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144185726","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Superior reversible hydrogen storage in eutectic LiBH4–KBH4 system via Ni–based catalysts synergized with graphene 镍基催化剂与石墨烯协同作用在LiBH4-KBH4共晶体系中具有优异的可逆储氢性能
Materials Today Catalysis Pub Date : 2025-05-27 DOI: 10.1016/j.mtcata.2025.100105
Shanqing Qu , Yaxiong Yang , Mingxia Gao , Zhenglong Li , Wenping Sun , Chu Liang , Xin Zhang , Xiaoyu Zhang , Lingchao Zhang , Ruizi Wang , Hongge Pan
{"title":"Superior reversible hydrogen storage in eutectic LiBH4–KBH4 system via Ni–based catalysts synergized with graphene","authors":"Shanqing Qu ,&nbsp;Yaxiong Yang ,&nbsp;Mingxia Gao ,&nbsp;Zhenglong Li ,&nbsp;Wenping Sun ,&nbsp;Chu Liang ,&nbsp;Xin Zhang ,&nbsp;Xiaoyu Zhang ,&nbsp;Lingchao Zhang ,&nbsp;Ruizi Wang ,&nbsp;Hongge Pan","doi":"10.1016/j.mtcata.2025.100105","DOIUrl":"10.1016/j.mtcata.2025.100105","url":null,"abstract":"<div><div>Light metal borohydrides are promising candidates for solid–state hydrogen storage due to their high hydrogen storage capacities; however, the reversibility and kinetics of de/hydrogenation still require significant improvement. The present work focuses on the improvement of the hydrogen storage properties of the eutectic borohydride system of LiBH<sub>4</sub>–KBH<sub>4</sub> (Li/KBH<sub>4</sub>). A layered composite of graphene supported with ultrafine Ni<sub>3</sub>B nanoparticles (Ni<sub>3</sub>B/G) is designed and synthesized, which acts as catalyst and confinement carrier for Li/KBH<sub>4</sub>. Assisted with a heating of the mixture of Li/KBH<sub>4</sub> and Ni<sub>3</sub>B/G to 110 °C in the molten state of Li/KBH<sub>4</sub>, an interlayer structure of graphene dispersed with Ni<sub>3</sub>B nanoparticles and sheet–like Li/KBH<sub>4</sub> is constructed. The graphene effectively disperses Ni<sub>3</sub>B nanoparticles and confines the Li/KBH<sub>4</sub> in its interlayers. The confinement of Li/KBH<sub>4</sub> and the catalysis of Ni<sub>3</sub>B nanoparticles, assisted with the high thermal conductivity of graphene, contribute synergistically the hydrogen storage of Li/KBH<sub>4</sub>. The main dehydrogenation peak temperature of the system is lowered to 278 °C. The system can release 8.5 wt% H<sub>2</sub> within 30 min at 350 °C. The capacity retention achieves 81.2 % after 50 cycles. DFT theoretical analysis shows that there is strong charge transfer interaction between Ni<sub>3</sub>B and LiBH<sub>4</sub>/KBH<sub>4</sub>, which destabilizes the [BH<sub>4</sub>]<sup>–</sup> structure and promotes the dehydrogenation. This work provides a new approach for the design of new structural LiBH<sub>4</sub>–based eutectic system with high capacity, low dehydrogenation temperature, high reversibility and long cycling life.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100105"},"PeriodicalIF":0.0,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144169432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Photocatalytic transformation of organic pollutants and remediation strategies of carbon emissions and nitrogen fixation in inland water 内陆水体有机污染物的光催化转化及碳排放固氮修复策略
Materials Today Catalysis Pub Date : 2025-05-09 DOI: 10.1016/j.mtcata.2025.100103
Masiha Rahman, Saman Shaheen, Tokeer Ahmad
{"title":"Photocatalytic transformation of organic pollutants and remediation strategies of carbon emissions and nitrogen fixation in inland water","authors":"Masiha Rahman,&nbsp;Saman Shaheen,&nbsp;Tokeer Ahmad","doi":"10.1016/j.mtcata.2025.100103","DOIUrl":"10.1016/j.mtcata.2025.100103","url":null,"abstract":"<div><div>Photocatalysis is an environmentally friendly approach and a propitious avenue for addressing water contamination including toxic chemicals, radioactive materials, and nitrate fertilizer. In the past few years, urbanization and industrialization have affected the water quality, causing various environmental hazards. Inland water ecosystems such as lakes, rivers and wetland not only play a vital role in maintaining biodiversity but also provide important sources of GHGs emissions. Despite their significance, the emission from inland water is poorly quantified. This review systematically reveals the sources of carbon and nitrogen emissions, the efficiency and mechanisms of various photocatalysts in degrading a range of organic pollutants, highlighting their potential to reduce environmental toxins significantly. The state-of-the-art and innovative remediation strategies targeting carbon emissions and N<sub>2</sub> fixation have been thoroughly discussed. By consolidating photocatalytic processes with carbon sequestration and N<sub>2</sub> fixation, the review develops a holistic approach to alleviating water quality and mitigating climate change impacts. Finally, the findings concluded with the role of advanced photocatalytic materials and proffering perspectives in promoting sustainable environmental management and ecological health in inland aquatic systems.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100103"},"PeriodicalIF":0.0,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143929593","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
VN/Copper foam self-supporting catalyst for efficient electrocatalytic hydrogen peroxide generation 用于高效电催化过氧化氢生成的VN/铜泡沫自支撑催化剂
Materials Today Catalysis Pub Date : 2025-05-09 DOI: 10.1016/j.mtcata.2025.100102
Jiahao Liu , Zhaorui Zhang , Chenshuai Han, Minghui Yang
{"title":"VN/Copper foam self-supporting catalyst for efficient electrocatalytic hydrogen peroxide generation","authors":"Jiahao Liu ,&nbsp;Zhaorui Zhang ,&nbsp;Chenshuai Han,&nbsp;Minghui Yang","doi":"10.1016/j.mtcata.2025.100102","DOIUrl":"10.1016/j.mtcata.2025.100102","url":null,"abstract":"<div><div>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is a crucial chemical, while its conventional production methods are energy-intensive and environmentally damaging. Electrocatalytic synthesis of H<sub>2</sub>O<sub>2</sub> through 2e<sup>-</sup> oxygen reduction reaction (ORR) presents a sustainable alternative. Here, we introduce a novel VN/Copper foam (VN/CF) self-supporting catalyst, achieving an H<sub>2</sub>O<sub>2</sub> production yield rate of 169.7 mg·h<sup>−1</sup>·cm<sup>−2</sup> with a Faradaic efficiency (FE) of 89.1 %. The self-supporting VN/CF demonstrates remarkable durability, sustaining stable operation at a current density of 300 mA cm<sup>−2</sup> over 110 h. Notably, the capital cost of 70 wt% H<sub>2</sub>O<sub>2</sub> is remarkably low at just $0.25/kg. This work highlights the potential of self-supported metal nitrides as stable and efficient 2e<sup>-</sup> ORR catalysts.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100102"},"PeriodicalIF":0.0,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143948226","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Advances in understanding and manipulating electrode wettability for electrocatalytic performance enhancement 提高电催化性能的电极润湿性研究进展
Materials Today Catalysis Pub Date : 2025-05-07 DOI: 10.1016/j.mtcata.2025.100101
Hailing Zhao , Kaijie Ma , Shiqin Gao , Bolun Wang , Yang Wang
{"title":"Advances in understanding and manipulating electrode wettability for electrocatalytic performance enhancement","authors":"Hailing Zhao ,&nbsp;Kaijie Ma ,&nbsp;Shiqin Gao ,&nbsp;Bolun Wang ,&nbsp;Yang Wang","doi":"10.1016/j.mtcata.2025.100101","DOIUrl":"10.1016/j.mtcata.2025.100101","url":null,"abstract":"<div><div>In the realm of heterogeneous catalysis, the wettability of the catalyst significantly impacts the interaction between the catalyst surface and reactants or products, thereby playing a pivotal role in determining catalytic performance. Electrocatalytic reactions predominantly occur at multiphase interfaces. As a result, gas-liquid-solid interface mass transfer is of utmost importance during the reaction process. In the electrocatalysis process, for steps including molecular adsorption, desorption, and surface transfer, the modulation of electrode wettability directly influences the behavior of gas bubbles beneath the solution. This affects the gas-liquid-solid interface mass transfer process during electrocatalysis. Consequently, a comprehensive understanding of the principles governing this interfacial interaction is crucial for fundamentally enhancing the efficiency of electrocatalytic reactions. This review summarizes the basic theory of wettability and its relationship with electrocatalytic reactions. It also accentuates some recent advancements in the impact of electrode wettability in heterogeneous electrocatalytic reactions. Finally, the review offers a perspective on the challenges associated with wettability regulation in influencing the electrocatalytic reaction process.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100101"},"PeriodicalIF":0.0,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143929592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles 研究镍纳米颗粒在苯甲醛还原胺化反应中的尺寸依赖性选择性
Materials Today Catalysis Pub Date : 2025-04-29 DOI: 10.1016/j.mtcata.2025.100100
Yunong Li , Ching Kit Tommy Wun , Tianxiang Chen , Tsz Woon Benedict Lo
{"title":"Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles","authors":"Yunong Li ,&nbsp;Ching Kit Tommy Wun ,&nbsp;Tianxiang Chen ,&nbsp;Tsz Woon Benedict Lo","doi":"10.1016/j.mtcata.2025.100100","DOIUrl":"10.1016/j.mtcata.2025.100100","url":null,"abstract":"<div><div>Selectivity control is a fundamental focus in catalysis chemistry, as it directly reflects the efficiency and efficacy of catalytic processes. While catalysis often involves intricate and cascade reaction steps using nanoparticle (NP) catalysts, the mechanism behind the size effect of nanoparticles on product selectivity has not been fully explored. We herein prepared a series of Ni-containing zeolitic catalysts in which the Ni NPs are uniformly supported on the mesopores and outer surfaces of H-ZSM-5 zeolites. The dynamic formation of Ni NPs from highly dispersed Ni precursors was monitored using transmission electron microscopy, in-situ X-ray pair distribution function, and in-situ X-ray absorption fine structure analysis. The metal nanoparticle size was carefully controlled between 3.72(5) nm and 11.91(7) by controlling the reduction temperature. We evaluated the catalytic performance of Ni NPs using the reductive amination of benzaldehyde in batch reactors at low temperatures. This reaction inherently favors the formation of a series of products, suffering highly from selectivity issues. Our results revealed a size-dependent behavior in reaction efficiency, with the catalyst achieving the highest catalytic activity (93 % selectivity in primary amine) at a particle size of 5.62(3) nm. This optimal performance is attributed to a balanced interplay between hydrogenation and amination capabilities. These findings highlight the intricate relationship between nanoparticle size and catalytic performance, emphasizing the necessity for precise optimization in catalyst design to enhance selectivity and sustainability in industrial applications.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100100"},"PeriodicalIF":0.0,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143895821","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Assessing the photocatalytic activity of visible light active Bi2S3-based nanocomposites for Methylene Blue and Rhodamine B degradation 评价可见光活性bi2s3基纳米复合材料对亚甲基蓝和罗丹明B降解的光催化活性
Materials Today Catalysis Pub Date : 2025-04-05 DOI: 10.1016/j.mtcata.2025.100099
Bachir Yaou Balarabe , Yerkanat N. Kanafin , Kuralay Rustembekkyzy , Imanzhussip Serkul , Meruert A. Nauryzbaeva , Timur Sh. Atabaev
{"title":"Assessing the photocatalytic activity of visible light active Bi2S3-based nanocomposites for Methylene Blue and Rhodamine B degradation","authors":"Bachir Yaou Balarabe ,&nbsp;Yerkanat N. Kanafin ,&nbsp;Kuralay Rustembekkyzy ,&nbsp;Imanzhussip Serkul ,&nbsp;Meruert A. Nauryzbaeva ,&nbsp;Timur Sh. Atabaev","doi":"10.1016/j.mtcata.2025.100099","DOIUrl":"10.1016/j.mtcata.2025.100099","url":null,"abstract":"<div><div>High levels of organic compounds, notably synthetic dyes like Methylene blue (MB) and Rhodamine B (RhB), in untreated effluents have become a major environmental concern, endangering human health and ecosystems. These dyes are difficult to remove due to their non-biodegradable nature, prompting extensive research in this area. Photocatalysis has emerged as a promising, environmentally friendly method that only requires a light source and a photocatalyst for pollutant degradation. Bismuth sulfide (Bi<sub>2</sub>S<sub>3</sub>) stands out among other photocatalytic materials due to its narrow band gap, strong light absorption in the visible range, and nontoxicity, making it a good candidate to improve the overall photocatalytic efficiency. Therefore, this review article focuses on recent advances in Bi<sub>2</sub>S<sub>3</sub>-based nanocomposites and their role in the effective degradation of organic pollutants, particularly MB and RhB, through enhanced photocatalytic mechanisms.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100099"},"PeriodicalIF":0.0,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143839610","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Constructing electron transport channel of SnO2/BaSO4 on g-C3N4 for enhanced visible-light-driven photocatalytic H2 production 在g-C3N4上构建SnO2/BaSO4的电子传递通道以增强可见光驱动光催化制氢
Materials Today Catalysis Pub Date : 2025-03-24 DOI: 10.1016/j.mtcata.2025.100098
Gongyue Dong , Xiaojuan Guo , Cheng Cheng , Feng Chen , Jinfeng Zhang , Yanping Du , Wei Meng , Maochang Liu , Jinwen Shi
{"title":"Constructing electron transport channel of SnO2/BaSO4 on g-C3N4 for enhanced visible-light-driven photocatalytic H2 production","authors":"Gongyue Dong ,&nbsp;Xiaojuan Guo ,&nbsp;Cheng Cheng ,&nbsp;Feng Chen ,&nbsp;Jinfeng Zhang ,&nbsp;Yanping Du ,&nbsp;Wei Meng ,&nbsp;Maochang Liu ,&nbsp;Jinwen Shi","doi":"10.1016/j.mtcata.2025.100098","DOIUrl":"10.1016/j.mtcata.2025.100098","url":null,"abstract":"<div><div>Graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) is confronted with the issue of poor utilization of photogenerated charge carriers, thereby leading to limited performance of photocatalytic hydrogen (H<sub>2</sub>) production, which restricts its potential application. Herein, the electron transport material SnO<sub>2</sub>/BaSO<sub>4</sub> was synthesized to integrate with g-C<sub>3</sub>N<sub>4</sub> for addressing the above problem. Various characterizations were conducted to investigate the g-C<sub>3</sub>N<sub>4</sub>-SnO<sub>2</sub>/BaSO<sub>4</sub> photocatalyst, and it demonstrated that photogenerated electrons from g-C<sub>3</sub>N<sub>4</sub> expeditiously migrate to SnO<sub>2</sub>/BaSO<sub>4</sub> nanoparticles, which markedly hindered photogenerated carriers’ recombination. Subsequently, the g-C<sub>3</sub>N<sub>4</sub>-SnO<sub>2</sub>/BaSO<sub>4</sub> photocatalyst demonstrated promoted photocatalytic H<sub>2</sub> production at a rate of 14.2 μmol h<sup>−1</sup> under visible-light illumination, which was 2.5 times higher than that of pristine g-C<sub>3</sub>N<sub>4</sub>.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100098"},"PeriodicalIF":0.0,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143725196","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}
引用次数: 0
Improved low-temperature CO oxidation using heterogeneous nanofibrous structures decorated with Pd atoms and nanocrystals 用Pd原子和纳米晶体修饰的非均相纳米纤维结构改进低温CO氧化
Materials Today Catalysis Pub Date : 2025-03-08 DOI: 10.1016/j.mtcata.2025.100093
M.A. Rodriguez-Olguin , D. Cazac , F. Ruiz-Zepeda , S. Bartling , M. Bosco , H. Atia , R. Eckelt , A. Manzo-Robledo , M. Vandichel , A. Aguirre , J.G.E. Gardeniers , A. Susarrey-Arce
{"title":"Improved low-temperature CO oxidation using heterogeneous nanofibrous structures decorated with Pd atoms and nanocrystals","authors":"M.A. Rodriguez-Olguin ,&nbsp;D. Cazac ,&nbsp;F. Ruiz-Zepeda ,&nbsp;S. Bartling ,&nbsp;M. Bosco ,&nbsp;H. Atia ,&nbsp;R. Eckelt ,&nbsp;A. Manzo-Robledo ,&nbsp;M. Vandichel ,&nbsp;A. Aguirre ,&nbsp;J.G.E. Gardeniers ,&nbsp;A. Susarrey-Arce","doi":"10.1016/j.mtcata.2025.100093","DOIUrl":"10.1016/j.mtcata.2025.100093","url":null,"abstract":"<div><div>Amorphous alumina shaped as nanofibers forming a non-woven network, functioning as a heterogeneous dispersion for palladium (Pd) atoms and nanocrystals, is unique yet unstudied for low-temperature CO oxidation. This work demonstrates that nanometric-size alumina fibers (ANFs) with a surface area of ⁓230 m<sup>2</sup>/g can host Pd species that remain nearly intact after CO oxidation. The ANFs contain various Pd (Pd-ANFs) loadings, ranging from 1 %wt. (Pd1-ANFs), 3 %wt. (Pd3-ANFs), to 5 %wt. (Pd5-ANFs). Among them, Pd3-ANFs show the highest CO chemisorption. Hence, the chemical environment of the Pd3-ANFs is assessed using NAP-XPS under various CO and O<sub>2</sub> mixtures. NAP-XPS shows the presence of metallic and oxidized Pd species. The results are correlated with DRIFT spectroscopy, which unveils the CO species adsorbed over Pd. Furthermore, a computational-based kinetic model for CO oxidation shows that Pd single atoms start the CO-oxidation, followed by larger Pd crystals during light-off. Our results demonstrate that the Pd-ANFs have higher activity when compared with the Pd alumina nanoparticles (Pd-ANP) counterpart that lacks a fibrous structure, highlighting the benefits of the ANF's structural network in stabilizing atomic and nanometric scale metal catalysts for low-temperature CO oxidation.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100093"},"PeriodicalIF":0.0,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629486","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}
引用次数: 0
Ambient urea synthesis via electrocatalytic C–N coupling 电催化C-N偶联合成环境尿素
Materials Today Catalysis Pub Date : 2025-03-01 DOI: 10.1016/j.mtcata.2025.100092
Chen Chen
{"title":"Ambient urea synthesis via electrocatalytic C–N coupling","authors":"Chen Chen","doi":"10.1016/j.mtcata.2025.100092","DOIUrl":"10.1016/j.mtcata.2025.100092","url":null,"abstract":"<div><div>The construction of C–N bond and synthesis of N-containing compounds directly from N<sub>2</sub> is an extremely attractive subject. The co-electrolysis system coupled with renewable electricity provides one of the potential options for the green and controllable C–N bond construction under ambient conditions, bypassing the intermediate process of ammonia synthesis. In this review, we have summarized the recent progress in ambient urea synthesis via electrocatalytic C–N coupling from CO<sub>2</sub> and nitrogenous species. The reaction mechanisms studies of N<sub>2</sub> and CO<sub>2</sub> coupling has been mainly highlighted, and the coupling enhancement strategies are emphasized for the coupling of nitrate and CO<sub>2</sub>, including intermediate adsorption regulation, functional synergy, site reconstitution and local-environment construction. Moreover, promising directions and remaining challenges are outlined, encompassing the mechanism study combining theory and experiment, reactant source and product application, optimization of urea synthesis evaluation system and the development of devices aiming to coupling system. This review aims to guide further advancements in electrocatalytic C–N coupling, facilitating the efficient and sustainable synthesis of urea for a broad spectrum of applications.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100092"},"PeriodicalIF":0.0,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143509791","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}
引用次数: 0
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