EES catalysis最新文献

{"title":"Cation distribution: a descriptor for hydrogen evolution electrocatalysis on transition-metal spinels†","authors":"Aya K. Gomaa, Maram G. Zonkol, Ghada E. Khedr and Nageh K. Allam","doi":"10.1039/D4EY00121D","DOIUrl":"10.1039/D4EY00121D","url":null,"abstract":"<p >Exploring cost-effective and efficient electrocatalysts for the hydrogen evolution reaction (HER) is essential for realizing green energy technologies such as water electrolyzers and fuel cells. To this end, identifying descriptors that determine the activity of the employed catalysts would render the process more efficient and help to design selective catalytic materials. Herein, cation distribution (<em>δ</em>) is presented as the activity descriptor for the HER on CoFe<small>₂</small>O<small>₄</small> spinels. A one-step hydrothermal synthesis method is demonstrated for the fabrication of flower-shaped spinel CoFe<small>₂</small>O<small>₄</small> nanosheets on Ni foam at various pH values with different cation distributions. XPS and Raman analyses revealed the cation distribution of Co and Fe as the main factor determining the catalytic activity of the material. This has been confirmed both experimentally and computationally. The catalyst with the largest <em>δ</em> (0.33) showed as low as 66 mV overpotential at −10 mA cm<small>⁻²</small> with exceptional stability for 44 hours of continuous electrolysis in 1 M KOH. Our study demonstrates cation distribution in spinels as a descriptor of their HER catalytic activity.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00121d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141930324","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":"Uniting activity design principles of anode catalysts for direct liquid fuel cells†","authors":"Daniel J. Zheng, Jiayu Peng, Kaylee McCormack, Hongbin Xu, Jin Soo Kang, Zhenshu Wang, Zhichu Ren, Ju Li, Yuriy Román-Leshkov and Yang Shao-Horn","doi":"10.1039/D4EY00100A","DOIUrl":"10.1039/D4EY00100A","url":null,"abstract":"<p >Direct liquid fuel cells have advantages over hydrogen-based fuel cells and lithium-ion batteries for portable and mobile applications due to their high volumetric energy density and the convenient storage or refueling of liquid fuels. Unfortunately, the electrochemical oxidation of liquid fuels (such as methanol, ethanol, and formic acid) currently corresponds to ∼50% of the energy losses of these devices at operating conditions. Moreover, state-of-the-art catalysts for such critical reactions are generally composed of precious metals such as Pt and Pd, hindering the cost-effective implementation of these technologies. The development of novel catalyst design principles for electrochemical liquid fuel oxidation has been constrained by its complex, structure-sensitive reaction energetics that can involve multiple parallel, competitive reaction intermediates and pathways. In this review, we aim to dissect and bridge the understanding of fundamental energetics and the materials engineering of novel catalysts for the electrochemical oxidation of various liquid fuels. By deconvoluting these reactions into the energetics of different critical elementary steps, we define essential descriptors that govern the activity and selectivity of electrochemical liquid fuel oxidation. Several universal and fundamental design principles are proposed to optimize the catalytic performance of state-to-the-art and emerging electrocatalysts by tuning the chemistry and electronic structure of active sites. This review aims to provide a unique perspective connecting the electro-oxidation energetics of different liquid fuels with mechanistic and materials-centric studies to provide a holistic picture connecting the fundamental surface science with materials engineering for the rational design of electrocatalysts for liquid fuel oxidation.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00100a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141883266","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":"Medium entropy alloy wavy nanowires as highly effective and selective alcohol oxidation reaction catalysts for energy-saving hydrogen production and alcohol upgrade†","authors":"Xiaoyang Fu, Chengzhang Wan, Huaixun Huyan, Sibo Wang, Ao Zhang, Jingxuan Zhou, Hongtu Zhang, Xun Zhao, Jun Chen, Xiaoqing Pan, Yu Huang and Xiangfeng Duan","doi":"10.1039/D4EY00090K","DOIUrl":"10.1039/D4EY00090K","url":null,"abstract":"<p >Alcohol-assisted water electrolysis offers an attractive path for on-demand hydrogen generation while concurrently producing value added carboxylates. However, the anodic alcohol oxidation reaction (AOR) often requires precious metal-based catalysts, yet is still plagued with high overpotential or limited mass activity. Herein we report a facile synthesis of medium entropy Au-doped PtAgRhCu alloy wavy nanowires for highly efficient AORs. The alloy design facilitates hydroxyl adsorption that promotes the conversion of the carbonaceous intermediates (<em>e.g.</em> CH<small>₃</small>CO*) to carboxylate products and weakens the adsorption of carboxylate products, resulting in greatly enhanced mass activity for four-electron AORs and highly selective upgrade of ethanol and ethylene glycol into value added acetate and glycolate. Furthermore, we constructed an alcohol assisted water electrolyser that delivers a current density of 100 mA cm<small>⁻²</small> at a cell voltage lower than 0.6 V and a current density of 1 A cm<small>⁻²</small> at a cell voltage of 1.2 V.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00090k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141782338","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":"Revolutionizing ORR catalyst design through computational methodologies and materials informatics†","authors":"Lanna E. B. Lucchetti, James M. de Almeida and Samira Siahrostami","doi":"10.1039/D4EY00104D","DOIUrl":"10.1039/D4EY00104D","url":null,"abstract":"<p >Computational approaches, such as density functional theory (DFT) in conjunction with descriptor-based analysis and computational hydrogen electrode, have enabled exploring the intricate interactions between catalyst surfaces and oxygen species allowing for the rational design of materials with optimized electronic structure and reactivity for oxygen reduction reaction (ORR). The identification of active sites and the tuning of catalyst compositions at the atomic scale have been facilitated by computational simulations, accelerating the discovery of promising ORR catalysts. In this contribution, the insights provided by the computational analysis to understand the fundamental reasons behind inherent ORR overpotentials in the experimental reported catalysts are discussed. Various strategies to overcome the limitations in ORR catalysis using computational design are discussed. Several alternative earth-abundant and cost-effective materials suggested by computational guidance to replace platinum-based catalysts are reviewed. The accuracy of DFT and the role of solvent and electrolyte pH are outlined based on the understanding provided by the computational insight. Finally, an overview of recent achievements in employing materials informatics to accelerate catalyst material discovery for ORR is provided. These computational advancements hold great promise for the development of efficient and cost-effective ORR catalysts, bringing us closer to realizing the full potential of fuel cells as efficient electrochemical energy conversion technologies.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00104d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141782339","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":"Shining light on hybrid perovskites for photoelectrochemical solar to fuel conversion","authors":"Sudhanshu Shukla, Vishal Jose and Nripan Mathews","doi":"10.1039/D4EY00091A","DOIUrl":"10.1039/D4EY00091A","url":null,"abstract":"<p >Hybrid halide perovskites (HaPs) represent a class of material with excellent optoelectronic properties providing distinct avenues for disruptive photo(-electro) catalytic technologies. However, their photocatalytic activity, selectivity and stability remains a scientific and technological hurdle. In this perspective, we discuss fundamental aspects of perovskite based photocatalytic systems, specifically for CO<small>₂</small> conversion and high value oxidation reactions, and highlight critical limiting factors and on-going challenges in the field. We critically assess the recent advances in designing halide perovskite hetero-interfaces and characterization methodologies which are often used to define the performance metrics. Furthermore, we outline important questions and identify emerging trends in relation to the remediation strategy towards improved photocatalytic performance and stability from halide perovskite semiconductors.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00091a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141719371","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":"Exploring opportunities in operando DRIFTS and complementary techniques for advancing plasma catalysis†","authors":"Stefano Dell’Orco, Noemi Leick, Jeffrey L. Alleman, Susan E. Habas and Calvin Mukarakate","doi":"10.1039/D4EY00088A","DOIUrl":"10.1039/D4EY00088A","url":null,"abstract":"<p >Exploring the dynamic interaction of non-thermal plasma (NTP) with catalytic processes is critical to unravelling elusive catalyst structure–function relationships under NTP conditions, specifically dielectric barrier discharges (DBD). This study investigates the efficacy of <em>operando</em> diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) as a tool for characterizing intermediates created by NTP on catalyst surfaces. Leveraging insights from traditional DRIFTS in thermochemical catalysis, we explore the complexities of plasma-induced catalytic reactions, discussing both opportunities and limitations of DRIFTS to study these reaction mechanisms. By summarizing findings from literature and addressing existing knowledge gaps, this perspective highlights how different DRIFTS configurations can affect results, stressing the importance of establishing best practices for studying DBD-driven reactions with DRIFTS. The intended outcomes of this work are to provide guidance on how to effectively use DRIFTS, share fundamental insights into DBD-assisted catalysis, and emphasize the need for complementary techniques to develop catalysts suited for NTP environments.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00088a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141719303","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":"Outstanding Reviewers for EES Catalysis in 2023","authors":"","doi":"10.1039/D4EY90015D","DOIUrl":"10.1039/D4EY90015D","url":null,"abstract":"<p >We would like to take this opportunity to thank all of <em>EES Catalysis</em>'s reviewers for helping to preserve quality and integrity in chemical science literature. We would also like to highlight the Outstanding Reviewers for <em>EES Catalysis</em> in 2023.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey90015d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141512535","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 photocatalytic yield in the non-oxidative coupling of methane using a Pd–TiO2 nanomembrane gas flow-through reactor†","authors":"Victor Longo, Luana De Pasquale, Francesco Tavella, Mariam Barawi, Miguel Gomez-Mendoza, Víctor de la Peña O’Shea, Claudio Ampelli, Siglinda Perathoner, Gabriele Centi and Chiara Genovese","doi":"10.1039/D4EY00112E","DOIUrl":"10.1039/D4EY00112E","url":null,"abstract":"<p >The photocatalytic non-oxidative coupling of methane (NOCM) is a highly challenging and sustainable reaction to produce H<small>₂</small> and C<small>₂₊</small> hydrocarbons under ambient conditions using sunlight. However, there is a lack of knowledge, particularly on how to achieve high photocatalytic yield in continuous-flow reactors. To address this, we have developed a novel flow-through photocatalytic reactor for NOCM as an alternative to the conventionally used batch reactors. Me/TiO<small>₂</small> photocatalysts, where Me = Au, Ag and Pd, are developed, but only those based on Pd are active. Interestingly, the preparation method significantly impacts performance, going from inactive samples (prepared by wet impregnation) to highly active samples (prepared by strong electrostatic adsorption – SEA). These photocatalysts are deposited on a nanomembrane, and the loading effect, which determines productivity, selectivity, and stability, is also analysed. Transient absorption spectroscopy (TAS) analysis reveals the involvement of holes and photoelectrons after charge separation on Pd/TiO<small>₂</small> (SEA) and their interaction with methane in ethane formation, reaching a production rate of about 1000 μmol g<small>⁻¹</small> h<small>⁻¹</small> and a selectivity of almost 95% after 5 hours of reaction. Stability tests involving 24 h of continuous irradiation are performed, showing changes in productivity and selectivity to ethane, ethylene and CO<small>₂</small>. The effect of a mild oxidative treatment (80 °C) to extend the catalyst's lifetime is also reported.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00112e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141512536","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":"Designing bifunctional perovskite catalysts for the oxygen reduction and evolution reactions†","authors":"Casey E. Beall, Emiliana Fabbri, Adam H. Clark, Vivian Meier, Nur Sena Yüzbasi, Thomas Graule, Sayaka Takahashi, Yuto Shirase, Makoto Uchida and Thomas J. Schmidt","doi":"10.1039/D4EY00084F","DOIUrl":"10.1039/D4EY00084F","url":null,"abstract":"<p >The development of unified regenerative fuel cells (URFCs) necessitates an active and stable bifunctional oxygen electrocatalyst. The unique challenge of possessing high activity for both the oxygen reduction (ORR) and oxygen evolution (OER) reactions, while maintaining stability over a wide potential window impedes the design of bifunctional oxygen electrocatalysts. Herein, two design strategies are explored to optimize their performance. The first incorporates active sites for the ORR and OER, Mn and Co, into a single perovskite structure, which is achieved with the perovskites Ba<small>_0.5</small>Sr<small>_0.5</small>Co<small>_0.8</small>Mn<small>_0.2</small>O<small>_{3−<em>δ</em>}</small> (BSCM) and La<small>_0.5</small>Ba<small>_0.25</small>Sr<small>_0.25</small>Co<small>_0.5</small>Mn<small>_0.5</small>O<small>_{3−<em>δ</em>}</small> (LBSCM). The second combines an active ORR perovskite catalyst (La<small>_0.4</small>Sr<small>_0.6</small>MnO<small>_{3−<em>δ</em>}</small> (LSM)) with an OER active perovskite catalyst (Ba<small>_0.5</small>Sr<small>_0.5</small>Co<small>_0.8</small>Fe<small>_0.2</small>O<small>_{3−<em>δ</em>}</small> (BSCF)) in a physical mixed composite (BSCF/LSM). The success of the two strategies is investigated by measuring the catalysts’ catalytic performance and response to alternating reducing and oxidizing potentials to mimic the dynamic conditions experienced during the operation of URFCs. Additionally, the continuous, potentiodynamic change in Mn, Co, and Fe oxidation states during the ORR and OER is elucidated with <em>operando</em> X-ray absorption spectroscopy (XAS) measurements, revealing key insights into the nature of the active sites. The results reveal important catalyst physiochemical properties and provide a guide for future research and design principles for bifunctional oxygen electrocatalysts.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00084f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141507738","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":"Active and highly durable supported catalysts for proton exchange membrane electrolysers†","authors":"Debora Belami, Matthew Lindley, Umesh S. Jonnalagadda, Annie Mae Goncalves Bullock, Qianwenhao Fan, Wen Liu, Sarah J. Haigh, James Kwan, Yagya N. Regmi and Laurie A. King","doi":"10.1039/D4EY00026A","DOIUrl":"10.1039/D4EY00026A","url":null,"abstract":"<p >The design and development of supported catalysts for the oxygen evolution reaction (OER) is a promising pathway to reducing iridium loading in proton exchange membrane water electrolysers. However, supported catalysts often suffer from poor activity and durability, particularly when deployed in membrane electrode assemblies. In this work, we deploy iridium coated hollow titanium dioxide particles as OER catalysts to achieve higher Ir mass activities than the leading commercial catalysts. Critically, we demonstrate state-of-the-art durabilities for supported iridium catalysts when compared against the previously reported values for analogous device architectures, operating conditions and accelerated stress test profiles. Through extensive materials characterisations alongside rotating disk electrode measurements, we investigate the role of conductivity, morphology, oxidation state and crystallinity on the OER electrochemical performance. Our work highlights a new supported catalyst design that unlocks high-performance OER activity and durability in commercially relevant testing configurations.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00026a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141507739","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}