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Lanthanum-doped nickel-based composite metal oxide catalyst for hydrogenation of isophthalonitrile to produce meta-xylenediamine†
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-13 DOI: 10.1039/D4CY00802B
Heng Shao, Jing Guo, Rulong Li, Dekun Ji, Long Huang and Haibin Chu
{"title":"Lanthanum-doped nickel-based composite metal oxide catalyst for hydrogenation of isophthalonitrile to produce meta-xylenediamine†","authors":"Heng Shao, Jing Guo, Rulong Li, Dekun Ji, Long Huang and Haibin Chu","doi":"10.1039/D4CY00802B","DOIUrl":"https://doi.org/10.1039/D4CY00802B","url":null,"abstract":"<p >NiMAl (4 : 3 : 1)-LDO (M = Ca, Ba, and Mg) catalysts were prepared by co-precipitation. The optimal Ni<small><sub>4</sub></small>Mg<small><sub>3</sub></small>Al catalyst was selected and further modified with La to create the Ni<small><sub>4</sub></small>Mg<small><sub>3</sub></small>La<small><sub>0.15</sub></small>Al composite metal oxide catalyst. Under optimised reaction conditions, the isophthalonitrile (IPN) conversion reached 100%, and the selectivity to the target product <em>meta</em>-xylenediamine (MXDA) was remarkably high at 98.68%, while the selectivity of the by-product was as low as 0.05%. After ten reaction cycles, no significant decrease in the IPN conversion or MXDA selectivity was observed. The catalyst also exhibited excellent stability in a fixed-bed reactor over 400 hours, with the IPN conversion remaining at above 99% and MXDA selectivity maintained at an average of around 90%. The characterization results of the catalyst revealed that La addition strengthened the interaction between active Ni and the support, increased the content of strong basic sites in the catalyst, reduced the Ni nanoparticle size, and improved dispersion, leading to improved catalytic activity and stability.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7182-7190"},"PeriodicalIF":4.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IBzH (IBenzhydryl): sterically-flexible N-aliphatic N-heterocyclic carbenes (NHCs) for iron-catalyzed C(sp3)–C(sp2) cross-coupling of unactivated haloalkanes† IBzH(IBenzhydryl):立体灵活的 N-脂肪族 N-杂环碳烯 (NHC),用于铁催化未活化卤代烃的 C(sp3)-C(sp2)交叉偶联†。
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-12 DOI: 10.1039/D4CY01315H
Marlena Kardela, Błażej Dziuk, Roman Szostak, Michal Szostak and Elwira Bisz
{"title":"IBzH (IBenzhydryl): sterically-flexible N-aliphatic N-heterocyclic carbenes (NHCs) for iron-catalyzed C(sp3)–C(sp2) cross-coupling of unactivated haloalkanes†","authors":"Marlena Kardela, Błażej Dziuk, Roman Szostak, Michal Szostak and Elwira Bisz","doi":"10.1039/D4CY01315H","DOIUrl":"https://doi.org/10.1039/D4CY01315H","url":null,"abstract":"<p >Iron-catalyzed cross-coupling has emerged as a pivotal concept for the synthesis of valuable products across various facets of chemical research, including pharmaceuticals, organic materials and biological probes. In this respect, the use of <em>N</em>-heterocyclic carbenes (NHCs) as ancillary ligands to iron has been particularly effective. However, the major limitation is that the successful iron-catalytic systems have been almost exclusively limited to <em>N</em>-aryl-<em>N</em>-heterocyclic carbenes, which significantly restricts future developments of this commanding catalysis platform. Herein, we report IBzH (IBenzhydryl), a class of <em>N</em>-heterocyclic carbenes that are based on benzhydryl substitution of the imidazole ring. We demonstrate that this <em>N</em>-alkyl yet sterically-flexible ligand class promote the challenging C(sp<small><sup>3</sup></small>)–C(sp<small><sup>2</sup></small>) iron-catalyzed cross-coupling of unactivated haloalkanes, superseding the performance of other NHC ligands. Alkyl–alkyl cross-coupling is also described. Large scale synthesis and the evaluation of steric and electronic properties is presented. Considering the major advantages of sterically-flexible <em>N</em>-heterocyclic carbenes, we anticipate that this class of <em>N</em>-alkyl NHC ligands will have broad application.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7002-7008"},"PeriodicalIF":4.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798102","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Anthracene-based covalent organic framework supported palladium nanoparticles for visible-light-mediated Suzuki–Miyaura cross-coupling†
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-12 DOI: 10.1039/D4CY01083C
Lei Li, Qiujie Shan, Jiyuan Zang, Lei Yu, David J. Young, Zhi-Gang Ren and Hong-Xi Li
{"title":"Anthracene-based covalent organic framework supported palladium nanoparticles for visible-light-mediated Suzuki–Miyaura cross-coupling†","authors":"Lei Li, Qiujie Shan, Jiyuan Zang, Lei Yu, David J. Young, Zhi-Gang Ren and Hong-Xi Li","doi":"10.1039/D4CY01083C","DOIUrl":"https://doi.org/10.1039/D4CY01083C","url":null,"abstract":"<p >An anthracene-based covalent organic framework (COF) anchoring Pd(0) nanoparticles (Pd/AntCOF) photocatalyzed Suzuki–Miyaura cross-coupling of arylbromides and arylboronic acids in water under blue LED irradiation at ambient temperature. The AntCOF both stabilized the Pd(0) nanoparticles and acted as a visible-light photocatalyst to separate electrons and holes, facilitating oxidative addition and transmetallation of the substrates. Only a trace of product was achieved without blue light irradiation. This protocol exhibited wide functional group tolerance and the heterogeneous photocatalyst could be recycled with negligible loss of activity after four cycles.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7212-7218"},"PeriodicalIF":4.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bifunctional catalysts based on PdZn/ZnO and hierarchical zeolites in the direct synthesis of dimethyl ether from CO-rich syngas: influence of the support and the Zn/Pd molar ratio†
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-11 DOI: 10.1039/D4CY00860J
Bing Wang, Nicola Da Roit, Michael Zimmermann, Markus Boese, Thomas Zevaco and Silke Behrens
{"title":"Bifunctional catalysts based on PdZn/ZnO and hierarchical zeolites in the direct synthesis of dimethyl ether from CO-rich syngas: influence of the support and the Zn/Pd molar ratio†","authors":"Bing Wang, Nicola Da Roit, Michael Zimmermann, Markus Boese, Thomas Zevaco and Silke Behrens","doi":"10.1039/D4CY00860J","DOIUrl":"https://doi.org/10.1039/D4CY00860J","url":null,"abstract":"<p >Following the ‘precursor’ concept, a series of Pd/Zn-based, colloidal nanoparticles (NPs) with different Zn/Pd molar ratios were synthesized by reductive stabilization and used as precursors for the methanol active component in bifunctional catalysts. The bifunctional catalysts for the single-step dimethyl ether synthesis from CO-rich syngas were obtained by immobilizing the NPs on a microporous or hierarchical HZSM-5 zeolite, which were used as dehydration catalysts. The catalysts were characterized, <em>e.g.</em>, by (<em>in situ</em>) powder X-ray diffraction, scanning and transmission electron microscopy with energy-dispersive X-ray analysis, N<small><sub>2</sub></small> physisorption, and NH<small><sub>3</sub></small> temperature programmed desorption. This study demonstrates the influence of the Zn/Pd molar ratio on the size of PdZn particles formed under reaction conditions, which correlates with the catalytic performance in the STD process. The introduction of mesopores in the hierarchical zeolite by desilication of HZSM-5 increased the DME yield while decreasing the selectivity to hydrocarbons.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7152-7162"},"PeriodicalIF":4.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/cy/d4cy00860j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798125","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The O2-stable [FeFe]-hydrogenase CbA5H reveals high resilience against organic solvents†
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-07 DOI: 10.1039/D4CY01018C
Martin Gerbaulet, Anja Hemschemeier and Thomas Happe
{"title":"The O2-stable [FeFe]-hydrogenase CbA5H reveals high resilience against organic solvents†","authors":"Martin Gerbaulet, Anja Hemschemeier and Thomas Happe","doi":"10.1039/D4CY01018C","DOIUrl":"https://doi.org/10.1039/D4CY01018C","url":null,"abstract":"<p >[FeFe]-Hydrogenases are highly efficient hydrogen-(H<small><sub>2</sub></small>) converting enzymes which play pivotal roles for H<small><sub>2</sub></small> cycling in natural habitats, but which are also of interest for sustainable approaches to generate or employ H<small><sub>2</sub></small> gas. [FeFe]-Hydrogenases harbor a unique active site metal cofactor, the H-cluster, whose di-iron site by itself is nearly inactive but, as part of the protein, allows high turnover rates. Understanding this essential interplay of protein and co-factor might help to install [FeFe]-hydrogenases in biotechnological applications. The catalytic unit of the H-Cluster can be synthesized chemically and incorporated into [FeFe]-hydrogenase precursors, which allows to introduce non-natural metals or ligands and study their impact on catalytic activity. However, these compounds are often not water-soluble and have to be added to the proteins in solvents known to destabilize polypeptides. The resilience of [FeFe]-hydrogenases against organic solvents has hardly been investigated. To address this knowledge gap, we characterized the stability of the [FeFe]-hydrogenase CbA5H from <em>Clostridium beijerinckii</em> in several organic solvents (dimethylsulfoxide (DMSO), acetone, acetonitrile as well as water-miscible short-chain alcohols). These solvents are required to dissolve co-factor analogues and are also employed in chemical syntheses that might be combined with biocatalysts such as hydrogenases for more sustainable industrial processes. In the medium time-frame, CbA5H is remarkably stable in high concentrations of acetone and acetonitrile and also withstands intermediate concentrations of DMSO, ethanol and methanol. Combined with the unusual O<small><sub>2</sub></small> stability and high temperature and pressure tolerance, this makes CbA5H a candidate for its use in non-aqueous reaction environments.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7093-7106"},"PeriodicalIF":4.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/cy/d4cy01018c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798120","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Insight into the influence of Re and Cl on Ag catalysts in ethylene epoxidation. 深入了解 Re 和 Cl 对乙烯环氧化中银催化剂的影响。
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-06 DOI: 10.1039/d4cy00858h
Claudia J Keijzer, Pim T Weide, Kristiaan H Helfferich, Justyna Zieciak, Marco de Ridder, Remco Dalebout, Tracy L Lohr, John R Lockemeyer, Peter van den Brink, Petra E de Jongh
{"title":"Insight into the influence of Re and Cl on Ag catalysts in ethylene epoxidation.","authors":"Claudia J Keijzer, Pim T Weide, Kristiaan H Helfferich, Justyna Zieciak, Marco de Ridder, Remco Dalebout, Tracy L Lohr, John R Lockemeyer, Peter van den Brink, Petra E de Jongh","doi":"10.1039/d4cy00858h","DOIUrl":"10.1039/d4cy00858h","url":null,"abstract":"<p><p>Commercial ethylene epoxidation catalysts consist of α-alumina supported Ag particles and usually contain a mixture of promoters. High selectivity catalysts typically include a small amount of rhenium species. We studied a series of Ag catalysts promoted with Re loadings up to 4 at% (Re/(Re + Ag)), which is intentionally higher than in optimized commercial catalysts to facilitate characterization and to amplify the influence on catalysis. Sequential impregnation brought Re and Ag in such close contact that they formed a new characterized phase of AgReO<sub>4</sub>. Chemisorption experiments showed that both ReO <sub><i>x</i></sub> and AgReO<sub>4</sub> species act as a reversible reservoir for O<sub>2</sub>. Ethylene epoxidation was performed without and with the industrially crucial ethyl chloride promoter in the feed. Without the chloride (Cl), the ethylene oxide selectivity increased when Re was present, whereas the combination of Re and Cl decreased the ethylene oxide selectivity at higher Re loadings. Systematic ethylene oxide isomerization experiments revealed that Re and Cl individually inhibit the isomerization on the Ag surface. However, Re and Cl combined increased the isomerization, which can be explained by the surface becoming overly electrophilic. This hence shows the importance of studying promoters both individually and combined.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" ","pages":""},"PeriodicalIF":4.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11563198/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646022","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Deciphering the role of chemisorbed CO in CO2 methanation: kinetic and mechanistic investigation over monometallic (Ru) and bimetallic (Ru–Ni) catalysts† 解读化学吸附 CO 在 CO2 甲烷化过程中的作用:单金属(Ru)和双金属(Ru-Ni)催化剂的动力学和机理研究†。
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-05 DOI: 10.1039/D4CY01004C
Pavan Dongapure, Jyoti Tekawadia, V. Satyam Naidu and R. Nandini Devi
{"title":"Deciphering the role of chemisorbed CO in CO2 methanation: kinetic and mechanistic investigation over monometallic (Ru) and bimetallic (Ru–Ni) catalysts†","authors":"Pavan Dongapure, Jyoti Tekawadia, V. Satyam Naidu and R. Nandini Devi","doi":"10.1039/D4CY01004C","DOIUrl":"https://doi.org/10.1039/D4CY01004C","url":null,"abstract":"<p >Supported metal catalysts have made prominent contributions to CO<small><sub>2</sub></small> mitigation through conversion into useful chemicals. However, intermediates and mechanisms involved in this process remain ambiguous. Herein, we present the kinetics, mechanistic route and impact of chemisorbed CO in CO<small><sub>2</sub></small> methanation on Ru/γ-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> and Ru–Ni/γ-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> catalysts. Both the catalysts show minimal variation in adsorbed species on changing the duration of reduction, as confirmed through <em>in situ</em> IR spectroscopy. A notable observation is that the adsorbed CO exhibits a red shift at a longer reduction time and a more reactive nature on the Ru/γ-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> surface. Conversely, stable bridged CO mode is detected on Ru–Ni/γ-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> under similar conditions, leading to catalyst poisoning in all instances. This indicates that pre-reduction duration does not have much effect on the surface but interference of CO has more effect at lower concentrations of reactant gases. <em>In situ</em> XRD analysis reveals limited changes in the metallic or mixed oxide species during these conditions. Reaction kinetic analysis showed that Ru–Ni/γ-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> has better rate performance at higher concentrations of CO<small><sub>2</sub></small>, whereas Ru/γ-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> exhibits better rate performance at lower concentrations. The activation energy was found to be 74.07 kJ per mole for Ru/γ-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> and 89.38 kJ per mole for Ru–Ni/γ-Al<small><sub>2</sub></small>O<small><sub>3</sub></small>. The turnover frequency (TOF) is directly proportional to the rate of formation of methane.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7124-7133"},"PeriodicalIF":4.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798122","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effects of zeolite porosity and acidity on catalytic conversion of carbohydrates to bio-based chemicals: a review
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-05 DOI: 10.1039/D4CY01070A
Deyu Chu, Jinjing Ma, Qishun Liu, Jie Fu and Heng Yin
{"title":"Effects of zeolite porosity and acidity on catalytic conversion of carbohydrates to bio-based chemicals: a review","authors":"Deyu Chu, Jinjing Ma, Qishun Liu, Jie Fu and Heng Yin","doi":"10.1039/D4CY01070A","DOIUrl":"https://doi.org/10.1039/D4CY01070A","url":null,"abstract":"<p >Optimizing the production process of high value-added chemicals derived from renewable biomass holds immense promise for clean energy utilization and environmental sustainability. The abundant acidic sites and distinctive pore structures of zeolites serve as critical catalysts in improving the effectiveness of carbohydrates conversion and enabling the selective preparation of bio-based chemicals. This approach not only maximizes the utilization of renewable resources but also aligns with the imperative of environmental protection. This review presents an extensive overview of the latest advancements in utilizing zeolites as catalysts for converting carbohydrate biomass into bio-based chemicals. Emphasis is placed on elucidating the acidic properties and pore structures of zeolites and their profound impact on the carbohydrates conversion process. Furthermore, the review evaluates future directions for developing zeolite-catalyzed biomass conversion, aiming to offer insights into achieving sustainable and efficient utilization of biomass resources.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 6980-7001"},"PeriodicalIF":4.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798101","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanistic study of DETA-modified CdS for carbon dioxide reduction† DETA 改性 CdS 用于二氧化碳还原的机理研究†。
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-11-01 DOI: 10.1039/D4CY01140F
Meiyan Guo, Wanxiang Yang, Yi Li, Yongfan Zhang and Wei Lin
{"title":"Mechanistic study of DETA-modified CdS for carbon dioxide reduction†","authors":"Meiyan Guo, Wanxiang Yang, Yi Li, Yongfan Zhang and Wei Lin","doi":"10.1039/D4CY01140F","DOIUrl":"https://doi.org/10.1039/D4CY01140F","url":null,"abstract":"<p >Cadmium sulfide (CdS) exhibits remarkable light absorption capabilities and is widely employed in photocatalytic reduction of CO<small><sub>2</sub></small>. Nevertheless, the crystal facet effects on the micro-scale mechanisms governing CO<small><sub>2</sub></small> conversion on CdS remain elusive. This study theoretically investigates the electronic properties of hexagonal-phase (101), (001), and cubic-phase (111) CdS surfaces modified with diethylenetriamine (DETA). From a microscopic viewpoint, it elucidates the unique bonding characteristics of CO<small><sub>2</sub></small> on different exposed facets of DETA/CdS and the formation mechanisms leading to products such as CO, HCOOH, CH<small><sub>2</sub></small>O, CH<small><sub>3</sub></small>OH, and CH<small><sub>4</sub></small>. Our findings reveal that the DETA/CdS(101) surface is the most stable, effectively adsorbing hydrogen and CO<small><sub>2</sub></small> at varied Cd sites with a high selectivity towards CO production, thereby showing promise for syngas generation, albeit with potential yields of formic acid and methane. Conversely, DETA/CdS(001) and (111) primarily facilitate the reduction of CO<small><sub>2</sub></small> to CH<small><sub>4</sub></small>. These discoveries offer theoretical insights into photochemical experiments involving CO<small><sub>2</sub></small> reduction on CdS, shedding light on the influence of crystal facets on reaction pathways.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7172-7181"},"PeriodicalIF":4.4,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhancing the HER rate over Pt–TiO2 nanoparticles under controlled periodic illumination: role of light modulation†
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2024-10-31 DOI: 10.1039/D4CY00775A
Ettore Bianco, Fabrizio Sordello, Francesco Pellegrino and Valter Maurino
{"title":"Enhancing the HER rate over Pt–TiO2 nanoparticles under controlled periodic illumination: role of light modulation†","authors":"Ettore Bianco, Fabrizio Sordello, Francesco Pellegrino and Valter Maurino","doi":"10.1039/D4CY00775A","DOIUrl":"https://doi.org/10.1039/D4CY00775A","url":null,"abstract":"<p >In hydrogen production through water splitting, two reactions are involved: the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), both with efficiency issues. In previous works, our group demonstrated the possibility of enhancing H<small><sub>2</sub></small> production by conducting HCOOH photocatalytic reforming on metal–TiO<small><sub>2</sub></small> nanoparticles under controlled periodic illumination (CPI) rather than continuous illumination performed at the same average incident photon flux. The enhancement was observed only over specific metals, including Pt, Pd and Rh, due to their low Tafel slopes. Hydrogen adsorption and desorption energies are strongly dependent on the potential at the metal nanoparticles, and we demonstrated the ability to use CPI to induce oscillations in the potential of the catalyst. In this work, by modulating the duty cycle and the frequency of the CPI, we observed both of these playing a key role in boosting HER. Experimental evidence suggest that the relaxation of the photopotential during the dark period is the key factor for increasing the photonic efficiency of the reaction.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7205-7211"},"PeriodicalIF":4.4,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/cy/d4cy00775a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798142","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","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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