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Operando Spectroscopy of Catalysts Exploiting Multi-technique and Modulated Excitation Approaches. 利用多技术和调制激发方法对催化剂进行操作光谱分析。
IF 1.2 4区 化学
Chimia Pub Date : 2024-05-29 DOI: 10.2533/chimia.2024.313
Filippo Buttignol, Luca Maggiulli, Ilia Kochetygov, Ivo Alxneit, Davide Ferri
{"title":"Operando Spectroscopy of Catalysts Exploiting Multi-technique and Modulated Excitation Approaches.","authors":"Filippo Buttignol, Luca Maggiulli, Ilia Kochetygov, Ivo Alxneit, Davide Ferri","doi":"10.2533/chimia.2024.313","DOIUrl":"https://doi.org/10.2533/chimia.2024.313","url":null,"abstract":"<p><p>Operando spectroscopy combines the in situ determination of material structure by spectroscopy/diffraction techniques with the measurement of material performance, which is conversion/selectivity in the field of heterogeneous catalysis. A central question in operando spectroscopy is whether the signatures visible by the characterization methods are responsible for catalyst performance. Individual analytical methods can provide useful information, but their combination (multi-technique approach) is essential to obtain a complete perspective on molecular reaction mechanisms. This approach must be coupled to experimental protocols and mathematical algorithms enabling the ability to disentangle the contribution of the active structure from the unresponsive one. Here, we report an account with examples from our own research activities in catalysis science.</p>","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141185770","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Operando X-ray Absorption Spectroscopy as a Powerful Tool for Uncovering Property-Activity Relationships for Oxygen Evolution Transition Metal Oxide Catalysts. 运算X射线吸收光谱是揭示氧进化过渡金属氧化物催化剂性质-活性关系的有力工具。
IF 1.2 4区 化学
Chimia Pub Date : 2024-05-29 DOI: 10.2533/chimia.2024.320
Emiliana Fabbri, Thomas J Schmidt
{"title":"Operando X-ray Absorption Spectroscopy as a Powerful Tool for Uncovering Property-Activity Relationships for Oxygen Evolution Transition Metal Oxide Catalysts.","authors":"Emiliana Fabbri, Thomas J Schmidt","doi":"10.2533/chimia.2024.320","DOIUrl":"https://doi.org/10.2533/chimia.2024.320","url":null,"abstract":"<p><p>The development of a sustainable and environmentally friendly energy economy encompasses efficient hydrogen production from renewable energy via electrolysis. In this context, great efforts have recently been dedicated to the development of more efficient and cost-effective electrocatalysts. Understanding the mechanism of the oxygen evolution reaction (OER) on transition metal oxide catalysts is of great interest, but the reaction and system complexity render the characterization of active sites and the understanding of reaction mechanisms challenging. Time resolved Quick X-ray Absorption Spectroscopy (XAS) can provide dynamic snapshots of the electronic and local structure of nanocatalysts, revealing the 'real active phase' of the catalyst, which can substantially differ from the as-prepared catalyst powder or the catalyst in form of an electrode under non-operating conditions. In this contribution, several examples will be presented showing how operando XAS can reveal catalyst-support interactions, changes in the reaction mechanism, and dynamic reversible/irreversible changes in the electronic and local structure of OER catalysts.</p>","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141185775","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
X-ray Spectroscopy at the SuperXAS and Debye Beamlines: from in situ to Operando. SuperXAS 和 Debye 光束线的 X 射线光谱学：从原位到 Operando。
IF 1.2 4区 化学
Chimia Pub Date : 2024-05-29 DOI: 10.2533/chimia.2024.304
Aram Bugaev, Adam H Clark, Nina S Genz, Olga V Safonova, Grigory Smolentsev, Maarten Nachtegaal
{"title":"X-ray Spectroscopy at the SuperXAS and Debye Beamlines: from in situ to Operando.","authors":"Aram Bugaev, Adam H Clark, Nina S Genz, Olga V Safonova, Grigory Smolentsev, Maarten Nachtegaal","doi":"10.2533/chimia.2024.304","DOIUrl":"https://doi.org/10.2533/chimia.2024.304","url":null,"abstract":"<p><p>Understanding structure-performance relationships are essential for the rational design of new functional materials or in the further optimization of (catalytic) processes. Due to the high penetration depth of the radiation used, synchrotron-based hard X-ray techniques (with energy > 4.5 keV) allow the study of materials under realistic conditions (in situ and operando) and thus play an important role in uncovering structure-performance relationships. X-ray absorption and emission spectroscopies (XAS and XES) give insight into the electronic structure (oxidation state, spin state) and local geometric structure (type and number of nearest neighbor atoms, bond distances, disorder) up to ~5 Å around the element of interest. In this mini review, we will give an overview of the in situ and operando capabilities of the SuperXAS beamline, a facility for hard X-ray spectroscopy, through recent examples from studies of heterogeneous catalysts, electrochemical systems, and photoinduced processes. The possibilities for time-resolved experiments in the time range from ns to seconds and longer are illustrated. The extension of X-ray spectroscopy at the new Debye beamline combined with operando X-ray scattering and diffraction and further developments of time-resolved XES at SuperXAS will open new possibilities after the Swiss Light Source upgrade mid 2025.</p>","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141185790","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Design and Application of a Gas Diffusion Electrode (GDE) Cell for Operando and In Situ Studies. 用于操作和现场研究的气体扩散电极 (GDE) 单元的设计与应用。
IF 1.2 4区 化学
Chimia Pub Date : 2024-05-29 DOI: 10.2533/chimia.2024.344
Gustav K H Wiberg, Rebecca K Pittkowski, Stefanie Punke, Olivia Aalling-Frederiksen, Kirsten M Ø Jensen, Matthias Arenz
{"title":"Design and Application of a Gas Diffusion Electrode (GDE) Cell for Operando and In Situ Studies.","authors":"Gustav K H Wiberg, Rebecca K Pittkowski, Stefanie Punke, Olivia Aalling-Frederiksen, Kirsten M Ø Jensen, Matthias Arenz","doi":"10.2533/chimia.2024.344","DOIUrl":"https://doi.org/10.2533/chimia.2024.344","url":null,"abstract":"<p><p>Presented here is an electrochemical three-electrode Gas Diffusion Electrode (GDE) cell tailored for operandoand in situ investigations of electrocatalytic processes, with a particular focus on X-ray scattering studies. The optimized cell is engineered to accommodate the minimal sample-detector distances requisite for comprehensive X-ray total scattering investigations. An in-depth understanding of catalytic processes requires their study under 'working' conditions. Configured as a flow-cell, the setup therefore enables the examination of electrocatalysts under high current densities and associated gas evolution phenomena, particularly pertinent for reactions like the oxygen evolution reaction (OER). Notably, its transparency simplifies cell alignment, troubleshooting, and facilitates scans through the catalyst layer, crucial for background corrections. Demonstrating its versatility, we showcase its utility through Small Angle X-ray Scattering (SAXS), X-ray Diffraction (XRD), and X-ray Pair Distribution Function (PDF) analyses of total scattering data.</p>","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141185742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Operando Spectroscopy to Understand Dynamic Structural Changes of Solid Catalysts. 用 Operando 光谱法了解固体催化剂的动态结构变化。
IF 1.2 4区 化学
Chimia Pub Date : 2024-05-29 DOI: 10.2533/chimia.2024.288
Bidyut Bikash Sarma, Jan-Dierk Grunwaldt
{"title":"Operando Spectroscopy to Understand Dynamic Structural Changes of Solid Catalysts.","authors":"Bidyut Bikash Sarma, Jan-Dierk Grunwaldt","doi":"10.2533/chimia.2024.288","DOIUrl":"https://doi.org/10.2533/chimia.2024.288","url":null,"abstract":"<p><p>Solid materials like heterogeneous catalysts are highly dynamic and continuously tend to change when exposed to the reaction environment. To understand the catalyst system under true reaction conditions,operando spectroscopy is the key to unravel small changes, which can ultimately lead to a significant difference in catalytic activity and selectivity. This was also the topic of the 7th International Congress on Operando Spectroscopy in Switzerland in 2023. In this article, we discuss various examples to introduce and demonstrate the importance of this area, including examples from emission control for clean air (e.g. CO oxidation), oxidation catalysis in the chemical industry (e.g. oxidation of isobutene), future power-to-X processes (electrocatalysis, CO2 hydrogenation to methanol), and non-oxidative conversion of methane. All of these processes are equally relevant to the chemical industry. Complementary operando techniques such as X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and Raman spectroscopy were utilized to derive the ultimate structure of the catalyst. The variety of conditions requires distinctly different operando cells that can reach a temperature range of 400-1000 °C and pressures up to 40 bar. The best compromise for both the spectroscopy and the catalytic reaction is needed. As an outlook, we highlight emerging methods such as modulation-excitation spectroscopy (MES) or quick-extended X-ray absorption fine structure (QEXAFS) and X-ray photon in/out techniques, which can provide better sensitivity or extend X-ray based operando studies.</p>","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141185773","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Editorial. 社论
IF 1.2 4区 化学
Chimia Pub Date : 2024-05-29
Davide Ferri, Maarten Nachtegaal
{"title":"Editorial.","authors":"Davide Ferri, Maarten Nachtegaal","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141185745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Quasi-operando Transmission Electron Microscopy Diagnostics for Electrocatalytic Processes in Liquids. 液体中电催化过程的准操作透射电子显微镜诊断。
IF 1.2 4区 化学
Chimia Pub Date : 2024-05-29 DOI: 10.2533/chimia.2024.339
Vasiliki Tileli
{"title":"Quasi-operando Transmission Electron Microscopy Diagnostics for Electrocatalytic Processes in Liquids.","authors":"Vasiliki Tileli","doi":"10.2533/chimia.2024.339","DOIUrl":"https://doi.org/10.2533/chimia.2024.339","url":null,"abstract":"<p><p>The need to relate the mechano-physico-chemical phenomena in liquid-based electrocatalysts to the stages of start-up, operation, and shut-down phases is one of the major challenges that the energy community is facing. Understanding these phenomena will pave the way for the tailor-made design of efficient, commercially viable electrocatalytic systems. Transmission electron microscopy plays an important role in the investigation of local electrocatalytic effects, complementing other operando characterization techniques. Herein, after attempting to define the meaning of operando methodologies in relation to electron microscopy studies, the progress in the field is reviewed in terms of the knowledge gained about the catalysts, the solid-liquid interfaces, and the solid-liquid-gas interfacial phenomena for several electrocatalytic reactions. Finally, the parameters that require consideration in operando ec-LPTEM studies of electrocatalytic systems are discussed.</p>","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141185777","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
An Innovative Approach for Analyzing Phytotoxins as Micropollutants in the Environment 分析环境中作为微污染物的植物毒素的创新方法
IF 1.2 4区 化学
Chimia Pub Date : 2024-04-24 DOI: 10.2533/chimia.2024.263
Xiaomeng Liang, Thomas D. Bucheli, Jan H. Christensen, Nikoline Juul Nielsen
{"title":"An Innovative Approach for Analyzing Phytotoxins as Micropollutants in the Environment","authors":"Xiaomeng Liang, Thomas D. Bucheli, Jan H. Christensen, Nikoline Juul Nielsen","doi":"10.2533/chimia.2024.263","DOIUrl":"https://doi.org/10.2533/chimia.2024.263","url":null,"abstract":"","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140661732","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Time-resolved Spectroelectrochemical Investigation of Organic Mixed Conductors 有机混合导体的时间分辨光谱电化学研究
IF 1.2 4区 化学
Chimia Pub Date : 2024-04-24 DOI: 10.2533/chimia.2024.192
P. Cavassin, Natalie Banerji
{"title":"Time-resolved Spectroelectrochemical Investigation of Organic Mixed Conductors","authors":"P. Cavassin, Natalie Banerji","doi":"10.2533/chimia.2024.192","DOIUrl":"https://doi.org/10.2533/chimia.2024.192","url":null,"abstract":"Organic mixed ionic and electronic conductors (OMIECs) are an emerging class of materials that have been applied for a wide range of electrochemical applications. Due to the complexity inherent to the ionic-electroniccoupling, understanding the underlying mechanisms involved in the OMIEC operation is an exciting and very lively research field. In this work, we highlight the use of time-resolved Vis-NIR spectroelectrochemistry tocharacterize these materials. We discuss an example, where we show that by combining this tool with spectraldecomposition, we are able to understand fundamental aspects of the doping in an OMIEC film. The methodswe present here can be generalized and used to characterize any electrochromic material.","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140665444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Electrocatalytic Conversion of Small Molecules Utilizing Concerted Proton-electron Transfer Mediators 利用协同质子-电子转移介质实现小分子的电催化转化
IF 1.2 4区 化学
Chimia Pub Date : 2024-04-24 DOI: 10.2533/chimia.2024.251
Alessandro Walker, Victor Mougel
{"title":"Electrocatalytic Conversion of Small Molecules Utilizing Concerted Proton-electron Transfer Mediators","authors":"Alessandro Walker, Victor Mougel","doi":"10.2533/chimia.2024.251","DOIUrl":"https://doi.org/10.2533/chimia.2024.251","url":null,"abstract":"Activation of small molecules such as CO2, N2 or organic substrates and their subsequent transformation into complex value-added chemicals by electrocatalysis, utilizing renewable energy sources under ambientconditions, has gained considerable interest in the last few years. However, activation of these chemically inertmolecules is hindered by their intrinsically high activation energy barrier presupposing the development of tailored catalytic systems, often precluding selective transformation to the desired target products. Recent studies have shown that the utilization of concerted proton-electron transfer (CPET) mediators (med-H) may facilitate these challenging electrocatalytic reactions.","PeriodicalId":9957,"journal":{"name":"Chimia","volume":null,"pages":null},"PeriodicalIF":1.2,"publicationDate":"2024-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140664324","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
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