EES catalysis最新文献

{"title":"Plasma catalysis: what is needed to create synergy?","authors":"Joran Van Turnhout, Kevin Rouwenhorst, Leon Lefferts, Annemie Bogaerts","doi":"10.1039/d5ey00027k","DOIUrl":"https://doi.org/10.1039/d5ey00027k","url":null,"abstract":"<p><p>Plasma catalysis is gaining increasing interest for the synthesis of chemicals and fuels, but the underlying mechanisms are still far from understood. This hampers plasma-catalyst synergy. Indeed, there is not enough insight into the optimal catalyst material tailored to the plasma environment, and <i>vice versa</i>, in the optimal plasma conditions for the catalyst needs. Furthermore, plasma catalysis suffers from energy losses <i>via</i> backward reactions, and probably most importantly, there is a clear need for improved plasma reactor design with better contact between plasma and catalyst. In this paper, we describe these critical limitations and suggest possible solutions. In addition, we stress the importance of correct measurements and consistent reporting, and finally we also propose other promising plasma-material combinations beyond the strict definition of catalysts. We hope this opinion paper can help to make progress in this booming research field.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11976520/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144059790","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":"Correction: Single atom catalysts for water electrolysis: from catalyst-coated substrate to catalyst-coated membrane","authors":"Sol A Lee, Sang Eon Jun, Sun Hwa Park, Ki Chang Kwon, Jong Hun Kang, Min Sang Kwon and Ho Won Jang","doi":"10.1039/D5EY90009C","DOIUrl":"https://doi.org/10.1039/D5EY90009C","url":null,"abstract":"<p >Correction for ‘Single atom catalysts for water electrolysis: from catalyst-coated substrate to catalyst-coated membrane’ by Sol A Lee <em>et al.</em>, <em>EES. Catal.</em>, 2024, <strong>2</strong>, 49–70, https://doi.org/10.1039/D3EY00165B.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 579-579"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey90009c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143925406","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":"Two-step tandem electrochemical conversion of oxalic acid and nitrate to glycine.","authors":"Yuan-Zi Xu, Daniel F Abbott, Lok Nga Poon, Victor Mougel","doi":"10.1039/d5ey00016e","DOIUrl":"https://doi.org/10.1039/d5ey00016e","url":null,"abstract":"<p><p>This study presents a facile tandem strategy for improving the efficiency of glycine electrosynthesis from oxalic acid and nitrate. In this tandem electrocatalytic process, oxalic acid is first reduced to glyoxylic acid, while nitrate is reduced to hydroxylamine. Subsequent coupling of these two precursors results in the formation of a C-N bond, producing the intermediate glyoxylic acid oxime, which is further reduced <i>in situ</i> to glycine. Here we show, using only a simple Pb foil electrode, which maximizes the yield of the first step of the transformation (<i>i.e.</i> the reduction of oxalic acid to glyoxylic acid) prior to the coupling step allows for an unprecedented selectivity and conversion for glycine electrosynthesis to be achieved. Overall, a maximum glycine faradaic efficiency (FE) of 59% is achieved at -300 mA cm^-2 and a high glycine partial current density of -232 mA cm^-2 and a glycine production rate of 0.82 mmol h^-1 cm^-2 are attained at -400 mA cm^-2, thereby paving the way for an energy and economically efficient electrochemical synthesis of glycine.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11973474/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144051860","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":"Identification of catalyst optimization trends for electrocatalytic CO(2) reduction to ethylene†","authors":"Stefan J. Raaijman, Maarten P. Schellekens, Yoon Jun Son, Marc T. M. Koper and Paul J. Corbett","doi":"10.1039/D4EY00287C","DOIUrl":"https://doi.org/10.1039/D4EY00287C","url":null,"abstract":"<p >In this perspective we analyze copper and copper-based electrocatalysts with high ethylene selectivities from the literature to identify global catalyst formulation trends that allow for making catalysts with improved ethylene performance for industrial application. From our analysis, we identified six trends that can aid researchers in creating novel, high selectivity electrocatalysts for the electroreduction of CO<small>₍₂₎</small> to ethylene. These trends were as follows. (i) Tandem-type and (ii) supported-type catalysts perform relatively more poorly than other types of systems. Engineering the nanoenvironment through implementing nanoconfining morphologies (iii) or <em>via</em> the addition of polymeric additives (iv) brings about significant C<small>₂</small>H<small>₄</small> selectivity enhancements. (v) Catalyst heterogeneity is an important driver for improving C<small>₂</small>H<small>₄</small> selectivity. (vi) Both CO<small>₂</small> and CO can serve as feedstock with little impact on maximum achievable C<small>₂</small>H<small>₄</small> selectivity. As we identified during our study that the field lacks reproducibility of catalyst performance and independent reproduction of results, we propose several strategies on how to improve. Finally, we discuss changes that authors can implement to improve the industrial relevancy of their work.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 386-406"},"PeriodicalIF":0.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00287c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143925352","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":"Above 2 W cm−2 direct liquid fuel cells enabled by mitigating cathode polarization†","authors":"Yu Guo, Fukang Gui, Yangkai Han, Yingjian Cao, Zijun Hu, Yongkang Han, Qinggang Tan, Yong Che, Cunman Zhang, Yun Zhao and Qiangfeng Xiao","doi":"10.1039/D5EY00005J","DOIUrl":"https://doi.org/10.1039/D5EY00005J","url":null,"abstract":"<p >Among direct liquid fuel cells, the direct borohydride fuel cells (DBFCs) are considered as attractive portable or mobile power sources due to their high theoretical voltage and high energy density. However, the development of DBFCs has been greatly hindered by the borohydride crossover and oxidation at the cathode. Here we have developed DBFCs featuring a borohydride-tolerant Mn–Co–C spinel cathode catalyst and a microscale bipolar interface constituting a poly(arylene piperidinium) anion exchange membrane and Nafion®-based cathode that can achieve breakthroughs in performance and scalability. The areal peak power density surpasses 2 W cm<small>⁻²</small> at 80 °C with a platinum loading less than 1 mg cm<small>⁻²</small>. The three-electrode and crossover studies elucidate that the cathode polarization is significantly mitigated by the suppressed parasitic borohydride oxidation as compared with conventional configurations. The success of transforming the performance from a single cell of 1.5 × 1.5 to 5 × 5 cm<small>²</small> paves the way for practical applications.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 566-578"},"PeriodicalIF":0.0,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00005j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143925405","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":"The dark side of metal exsolution: a combined in situ surface spectroscopic and electrochemical study on perovskite-type cathodes for high-temperature CO2 electrolysis†","authors":"Christian Melcher, Andreas Nenning, Florian Schrenk, Kirsten Rath, Christoph Rameshan and Alexander Karl Opitz","doi":"10.1039/D5EY00013K","DOIUrl":"10.1039/D5EY00013K","url":null,"abstract":"<p >In solid oxide CO<small>₂</small> electrolysis cells, moderate activity and coking of the cathode are major issues that hinder commercialization of this important technology. It has been already shown that cathodes based on a mixed conducting oxide decorated with well-dispersed metal nanoparticles, which were grown <em>via</em> an exsolution process, are highly resilient to carbon deposition. Using perovskite-type oxides that contain reducible transition metals, such nanoparticles can be obtained <em>in situ</em> under sufficiently reducing conditions. However, the direct catalytic effect of exsolved metal nanoparticles on the CO<small>₂</small> splitting reaction has not yet been explored thoroughly (<em>e.g.</em> by employing well-defined model systems), thus, an in-depth understanding is still lacking. In this study, we aim at providing a crucial piece of insight into high-temperature electrochemical CO<small>₂</small> splitting on exsolution-decorated electrodes: we present the results of combined Near Ambient Pressure X-ray Photoelectron Spectroscopy (NAP-XPS) and electrochemical measurements on three different ferrite perovskites, which were employed as thin film model electrodes. The investigated materials are: La<small>_0.6</small>Ca<small>_0.4</small>FeO<small>_{3−<em>δ</em>}</small> (LCF), Nd<small>_0.6</small>Ca<small>_0.4</small>FeO<small>_{3−<em>δ</em>}</small> (NCF), and Pr<small>_0.6</small>Ca<small>_0.4</small>FeO<small>_{3−<em>δ</em>}</small> (PCF). The results obtained allow us to directly link the electrode's CO<small>₂</small> splitting activity to their surface chemistry. Especially, the electro-catalytic activity of the materials decorated with and without metallic iron nanoparticles was in focus. Our experiments reveal that in contrast to their beneficial role in H<small>₂</small>O electrolysis, exsolved Fe<small>⁰</small> metal particles deteriorate CO<small>₂</small> electrolysis activity. This behavior contrasts with expectations derived from earlier reports on porous samples, and is likely a consequence of the differences between the CO<small>₂</small> splitting and H<small>₂</small>O splitting mechanism.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 550-565"},"PeriodicalIF":0.0,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11894520/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143626876","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":"CO2/NOx storage and reduction (CNSR) technology—a new concept for flue gas treatment†","authors":"Jiaqi Wei, Yanshan Gao, Cheng Zhang and Qiang Wang","doi":"10.1039/D4EY00235K","DOIUrl":"https://doi.org/10.1039/D4EY00235K","url":null,"abstract":"<p >The emission of CO<small>₂</small> and NO<small>_<em>x</em></small> from industrial factories poses significant challenges to human health and contributes to extreme climate change. NO<small>_<em>x</em></small> storage and reduction (NSR) and integrated CO<small>₂</small> capture and methanation (ICCM) technology are some of the effective technologies used to deal with NO<small>_<em>x</em></small> and CO<small>₂</small>, respectively. However, there is currently no relevant technology available for the simultaneous removal of both NO<small>_<em>x</em></small> and CO<small>₂</small> gases co-existing in flue gas. This paper proposes a new concept named CO<small>₂</small>/NO<small>_<em>x</em></small> storage and reduction (CNSR) for the first time. This approach utilizes a K–Pt/Ni<small>₃</small>Al<small>₁</small>O<small>_<em>x</em></small> dual functional material (DFM) to achieve co-storage of CO<small>₂</small> and NO<small>_<em>x</em></small>, followed by their reduction to CH<small>₄</small> and N<small>₂</small>, respectively. The CNSR tests demonstrate the feasibility of this technology. At 350 °C, the conversion for CO<small>₂</small> and NO<small>_<em>x</em></small> was 60.8% and 99.5%, with CH<small>₄</small> and N<small>₂</small> selectivity of 98.9% and 90.3%, respectively. After 10 cycles, the sample exhibited a relatively stable CO<small>₂</small> conversion of around 66%, with CH<small>₄</small> selectivity remaining above 90%. The conversion of NO<small>_<em>x</em></small> remained essentially unchanged at close to 100%. Furthermore, a possible mechanism for the CNSR process is proposed in this study. We believe that this work will provide a novel strategy for the treatment of multi-component gaseous pollutants in flue gas.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 535-549"},"PeriodicalIF":0.0,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00235k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143925404","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":"Tailoring the electronic structure of an exfoliated layered double hydroxide using a lanthanide for chloride-ion blocking in seawater splitting†","authors":"Ashish Gaur, Jiseok Kwon, Jatin Sharma, Ghulam Ali, Enkhtuvshin Enkhbayar, Chan-Yeup Chung, HyukSu Han and Taeseup Song","doi":"10.1039/D4EY00278D","DOIUrl":"https://doi.org/10.1039/D4EY00278D","url":null,"abstract":"<p >Seawater is one of the most abundant sources of hydrogen in our environment, and it has great potential for the production of hydrogen <em>via</em> water electrolysis. However, seawater electrolysis is challenging as chloride ions could obstruct catalytic active sites, reducing *OH adsorption. Therefore, it is crucial to prevent chloride ions from accessing the active sites. Herein, we modulated the Lewis acidity of electrocatalysts to solve this problem. In particular, the Lewis acidity of Ni<small>²⁺</small> and Fe<small>³⁺</small> ions in a layered double hydroxide (LDH) was enhanced by incorporating the lanthanide dopant Ce, thereby tuning the surface electronic configurations to prefer OH* adsorption over Cl* adsorption. Further, the Ce-doped Ni–Fe LDH (CNF-LDH) was exfoliated <em>via</em> the O<small>₂</small> plasma process to improve the accessibility of active sites for intermediates. The resultant CNF-LDH-E exhibited an overpotential of 230 and 169 mV at 100 mA cm<small>⁻²</small> for OER and HER, respectively, in alkaline freshwater (1 M KOH) and 290 and 285 mV, respectively, in simulated seawater (1 M KOH + 0.1 M NaCl) electrolytes. The impact of Lewis acidity on blocking the chloride ions was further investigated using density functional theory (DFT) calculations.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 435-445"},"PeriodicalIF":0.0,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00278d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143925355","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":"On the growth and water oxidation stability of hydrous iridium oxide†","authors":"Matej Zlatar, Xianxian Xie, Carlo Franke, Tomáš Hrbek, Zdeněk Krtouš, Tong Li, Ivan Khalakhan and Serhiy Cherevko","doi":"10.1039/D4EY00268G","DOIUrl":"https://doi.org/10.1039/D4EY00268G","url":null,"abstract":"<p >Hydrous iridium oxide (HIROF) is a highly active catalyst for the oxygen evolution reaction (OER) with broad application in pH sensing and charge storage devices. However, the mechanisms driving its growth, as well as the associated iridium dissolution, remain incompletely understood. To address this knowledge gap, we employ online inductively coupled plasma mass spectrometry (ICP-MS) to monitor iridium dissolution from sputtered thin films of varying thicknesses during electrochemical cycling. Complementary techniques, including atom probe tomography (APT), ellipsometry, and X-ray photoelectron spectroscopy (XPS), are used to study oxidation states and interface composition. Our findings reveal a tri-phase interface consisting of metallic iridium, compact anhydrous oxide, and hydrous oxide, where dissolution predominantly occurs at the metal–compact oxide interface, driven by transient processes during cycling. HIROF growth strongly depends on iridium grain size, with smaller grains inhibiting growth due to the accumulation of an inner compact IrO<small>₂</small> layer. This effect is linked to increased oxophilicity, which lowers the reducibility of compact oxide. These insights advance understanding of HIROF growth mechanisms, offering strategies to optimize its performance and stability, particularly in proton exchange membrane water electrolyzers (PEMWEs), where iridium scarcity is critical. Broader implications extend to hydrous oxide formation on other noble and non-noble metals, potentially further advancing other electrochemical applications.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 521-534"},"PeriodicalIF":0.0,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00268g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143925403","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":"Kinetic and process modeling of Guerbet coupling chemistry over Cu–Mg–Al mixed oxides†","authors":"Javier E. Chavarrio, Christoph Markowitsch, Erick Votava, Markus Lehner and George W. Huber","doi":"10.1039/D5EY00045A","DOIUrl":"https://doi.org/10.1039/D5EY00045A","url":null,"abstract":"<p >Guerbet coupling chemistry is a route to oligomerize ethanol into C<small>₄₊</small> alcohols. Long chain ethers can be obtained through bimolecular dehydration of these alcohols. Ethers generated from the dehydration of C<small>₆₊</small> alcohols produce a fuel that satisfies diesel engine requirements, therefore selective production of C<small>₆₊</small> alcohols is of particular interest. The desired hexanol is synthesized through ethanol and butanol coupling, accompanied by the formation of undesired products through several reaction pathways. In this work the coupling of ethanol and butanol has been studied over Cu<small>_0.01</small>Mg<small>_2.99</small>AlO<small>_<em>x</em></small> to produce C<small>₆₊</small> alcohols through Guerbet coupling reactions. Two series of catalytic tests were performed at 325 °C and 300 psig by using either pure ethanol feed or a cofeed ethanol–butanol 70–30 mole%. A kinetic model was developed to predict the product distribution over a wide range of contact times. Kinetic parameters were regressed by coding a routine that included a solution of differential mole balances embedded in an optimization problem. The herein developed kinetic model was integrated in a process simulation flowsheet that models the upgrading of ethanol into C<small>₆₊</small> oxygenates. The butanol cofeeding strategy in the simulations was approached by recycling the produced butanol into the coupling reactor. The simulation results reveal that cofeeding butanol into the Guerbet reactor enhances initial production rates of C<small>₆₊</small> alcohols, at the expense of fostering production of byproducts from butanol self-coupling. A maximum carbon yield of 82.2% for C<small>₆₊</small> diesel fuel precursors can be obtained by minimizing the byproduct production after introduction of a hydrogenation reactor.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 459-474"},"PeriodicalIF":0.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00045a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143925400","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}