Faraday Discussions最新文献

{"title":"An interpretable machine learning framework for prediction of adsorption energies and generative design of active sites on arbitrary catalysts.","authors":"Matthew S Johnson, Richard H West, Judit Zádor","doi":"10.1039/d5fd00143a","DOIUrl":"10.1039/d5fd00143a","url":null,"abstract":"<p><p>We present a highly interpretable and efficient machine learning framework for predictive and generative modeling of adsorption energies on surfaces using subgraph isomorphic decision trees (SIDTs). Extracting graph representations of 344 756 relaxed geometries and their associated adsorption energies from the OC20 database, we used them to train a 24 777-node SIDT that achieves 0.36 eV MDAE, 0.54 eV MAE, and 0.82 eV RMSE. We then developed and implemented novel techniques to use SIDTs as generative models enabling efficient catalyst optimization for arbitrary objective functions and constraints as a function of the adsorption energies and prediction uncertainties of multiple adsorbates and the catalyst structure itself. In particular, our SIDT provides substructure representations of the subdistributions of adsorption energy, rather than mere samples from the subdistributions, as is commonly done in traditional generative modeling. We show how this can be exploited for efficient and interpretable catalyst active site design in two examples. For the ammonia decomposition reaction sequence, we show that we are able to use our generative techniques to minimize the overall barrier height of the sequence generating catalyst substructures predicted to decrease the overall barrier from 2.7 eV on Pt(111) to 0.4 eV. We also discuss how we can exploit the accurate SIDT uncertainties and the interpretability of the SIDT to identify regions of chemical space that are in need of improved coverage and might be improved using active-learning schemes.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"386-404"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808841","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}

{"title":"New experimental methods for observing catalysts in action: general discussion.","authors":"Maximilian Albers, Líney Árnadóttir, Simon R Bare, Jingguang G Chen, Beatriz Roldan Cuenya, Audrey Dannar, Abhaya K Datye, Chiara Demingo, David A Duncan, Jan Fingerhut, David W Flaherty, Philipp Alexander Fredersdorff, Artur Góra, Elad Gross, Philipp Grosse, Justin Hargreaves, Georg Held, Stig Helveg, Patrick Hubert, Igor Kowalec, Florian Kraushofer, Santosh Kumar, Barbara A J Lechner, Mathieu Lizée, Edvin Lundgren, Iwao Matsuda, Hernan Mazzei, Andy Mount, Van Canh Nguyen, Pinkie Ntola, Gareth S Parkinson, Patricia Poths, Christian Reece, Swetlana Schauermann, Tibor Szilvási, Steven L Tait, Vandana Amarnath Tiwari, Matthijs A van Spronsen, Timon Wagner, Alec M Wodtke, Jingyi Yang","doi":"10.1039/d6fd90024k","DOIUrl":"10.1039/d6fd90024k","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"539-566"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148816886","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}

{"title":"Impact of artificial intelligence on heterogeneous catalysis: general discussion.","authors":"Anastassia N Alexandrova, Líney Árnadóttir, Simon K Beaumont, Audrey Dannar, Chiara Demingo, Jan Fingerhut, David W Flaherty, Lucas Foppa, Alessandro Fortunelli, Artur Góra, Elad Gross, Matthew S Johnson, Alexander Kandratsenka, Igor Kowalec, Florian Kraushofer, Bjarne Kreitz, Mathieu Lizée, Andrew J Logsdail, Iwao Matsuda, Hernan Mazzei, Yu Murano, Akhil S Nair, Pinkie Ntola, Patricia Poths, Christian Reece, Swetlana Schauermann, Christopher Sheldon, Mzamo Shozi, Tibor Szilvási, Steven L Tait, Vandana Amarnath Tiwari, Mohammad Ussama, Veronique Van Speybroeck, Richard H West, Judit Zádor, Shuoqi Zhang","doi":"10.1039/d6fd90023b","DOIUrl":"10.1039/d6fd90023b","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"405-444"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148811655","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}

{"title":"Rational design of dynamic and self-repairing active sites: general discussion.","authors":"Anastassia N Alexandrova, Nail E H Barama, Simon R Bare, Jingguang G Chen, Audrey Dannar, Abhaya K Datye, Chiara Demingo, Zdenek Dohnalek, Jody Druce, Ubong Etim, David W Flaherty, Alessandro Fortunelli, Elad Gross, Justin Hargreaves, Georg Held, Stig Helveg, Florian Kraushofer, Bjarne Kreitz, Santosh Kumar, Barbara A J Lechner, Andrew J Logsdail, Gareth S Parkinson, Patricia Poths, Christian Reece, Beatriz Roldan Cuenya, Steven L Tait, Gamze Tanriver, Matthijs A van Spronsen, Jenny G Vitillo, Alec M Wodtke, Jingyi Yang","doi":"10.1039/d6fd90021f","DOIUrl":"10.1039/d6fd90021f","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"636-657"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148811648","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}

{"title":"Chemical mechanisms and system analysis in heterogeneous catalysis: general discussion.","authors":"Anastassia N Alexandrova, Nail El Hocine Barama, Simon R Bare, Mark E Bernard, Jingguang G Chen, Abhaya K Datye, Chiara Demingo, Rasika E A Dissanayake, Zdenek Dohnalek, David A Duncan, Jan Fingerhut, David W Flaherty, Abolfazl Ghaderian, Artur Góra, Elad Gross, Justin Hargreaves, Georg Held, Patrick Hubert, Alexander Kandratsenka, Marc T M Koper, Florian Kraushofer, Bjarne Kreitz, Santosh Kumar, Barbara A J Lechner, Mathieu Lizée, Andrew J Logsdail, Edvin Lundgren, Iwao Matsuda, Hernan Mazzei, Xiangchao Meng, Yu Murano, Akhil S Nair, Florian Nitz, Jens K Nørskov, Gianfranco Pacchioni, Gareth S Parkinson, Jiří Pavelec, Patricia Poths, Christian Reece, Beatriz Roldan Cuenya, Swetlana Schauermann, Christopher Sheldon, Mzamo Shozi, Tibor Szilvási, Steven L Tait, Vandana Amarnath Tiwari, Mohammad Ussama, Matthijs A van Spronsen, Jenny G Vitillo, Alec M Wodtke, Judit Zádor, Shuoqi Zhang","doi":"10.1039/d6fd90022d","DOIUrl":"10.1039/d6fd90022d","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"196-256"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148811605","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}

{"title":"Thermophysical properties of adsorbates with beyond-DFT accuracy from DFT data through error cancellation.","authors":"Seth G Porter, Bjarne Kreitz","doi":"10.1039/d5fd00144g","DOIUrl":"10.1039/d5fd00144g","url":null,"abstract":"<p><p>Predictive multiscale modeling of heterogeneously catalyzed reactions requires accurate enthalpies of adsorbates. These properties are typically calculated from density functional theory (DFT) using exchange-correlation functionals with the generalized-gradient approximation (GGA) since more accurate electronic structure methods are not feasible. Therefore, the derived enthalpies are subject to large inaccuracies. We address this challenge through an error-cancellation approach that builds on the connectivity-based hierarchy (CBH) to derive enthalpies of formation of adsorbates with beyond-DFT accuracy without increasing computational cost. This method constructs reactions that conserve the electronic configuration between the target and the reference species, leading to error cancellation. The method is applied to adsorbates on Pt(111), Ni(111), and MgO(100). With the CBH method, it is possible to determine enthalpies of formation that are in excellent agreement with experimental measurements for a range of adsorbates and across many GGA exchange-correlation functionals, clearly outperforming conventional referencing approaches. Additionally, the method combines available experimental surface science data with gas-phase thermochemistry data and DFT data in a global thermochemical network. More accurate enthalpies of formation have a tremendous impact on the predictive performance of multiscale models and enable more conclusive insights into reaction mechanisms of catalytic reactions.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"118-137"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808570","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}

{"title":"Concluding remarks: Faraday discussion on surface science and heterogeneous catalysis, a view from the bridge.","authors":"Simon K Beaumont","doi":"10.1039/d6fd00103c","DOIUrl":"10.1039/d6fd00103c","url":null,"abstract":"<p><p>The fields of surface science and heterogeneous catalysis are often inherently scientific investigations of the same fundamental phenomena from different (but potentially complementary) perspectives. It is little wonder therefore that this juncture has for many years been a point of note for scientists in either area. Although their long-standing interaction has often helped to refine and shape thinking, it has also fostered a degree of mutual cynicism, encapsulated in the oft-heard choruses that \"catalysis is too empirical to offer fundamental insight\" and that \"surface science is too idealized to mean anything in the real world.\" These concluding remarks attempt summarize aspects of the <i>Faraday Discussion</i> meeting entitled \"Bridging the gap from surface science to heterogeneous catalysis\" held at Burlington House, London, UK in April 2026. In particular, drawing on discussions with other attendees, I have tried to summarise some of the key themes: both progress overcoming gaps at the interface of these two fields and perhaps new gaps that emerge as a result of improved insight as the fields advance their own understanding and meet new challenges.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"658-666"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148589625","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}

{"title":"Compensation effects between the apparent activation energy and pre-exponential factor in simple models of electrocatalytic hydrogen evolution.","authors":"Jan Fingerhut, Rifael Z Snitkoff-Sol, Maximilian Albers, Rafaël E Vos, Onno van der Heijden, Marc T M Koper","doi":"10.1039/d5fd00163c","DOIUrl":"10.1039/d5fd00163c","url":null,"abstract":"<p><p>Understanding how activation energies and entropies vary with electrode potential is central to interpreting electrocatalytic kinetics, yet temperature-dependent analyses often yield apparent \"compensation effects\" whose physical origin remains debated. Here, we model the hydrogen evolution reaction (HER) through both Volmer-Heyrovsky and Volmer-Tafel mechanisms to determine under which conditions compensation effects emerge-even when the entropic contribution to the activation barriers of the individual reaction steps is, by assumption, potential-independent. By simulating steady state currents across realistic potential and temperature ranges and extracting apparent Arrhenius parameters, we identify two general origins of compensation-like behavior: (i) shifts in the effective rate law arising from changes in coverage or in the rate-determining step, and (ii) the presence of multiple active sites with different equilibrium potentials of reaction steps. Both phenomena generate non-constant Tafel slopes and curvature in Arrhenius plots, producing Constable-plot (log₁₀ <i>A</i>_app<i>vs. E</i>_app) relations that mimic intrinsic entropy-enthalpy compensation. Our results demonstrate that compensation effects in electrocatalysis can arise purely from kinetic coupling and site heterogeneity rather than from fundamental thermodynamic scaling, underscoring the need for caution when interpreting temperature-dependent kinetic data. We propose that meaningful mechanistic insight requires measurements on well-defined single-crystal electrodes within potential regions where Tafel slopes remain constant.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"100-117"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13127248/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808844","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}

{"title":"CO on a Rh/Fe₃O₄ single-atom catalyst: high-resolution infrared spectroscopy and near-ambient-pressure scanning tunnelling microscopy.","authors":"Nail El Hocine Barama, Chunlei Wang, Panukorn Sombut, David Rath, Adam Lagin, Martin Ormoš, Lena Puntscher, Faith J Lewis, Zdeněk Jakub, Florian Kraushofer, Moritz Eder, Matthias Meier, Michael Schmid, Ulrike Diebold, Cesare Franchini, Peter Matvija, Jiří Pavelec, Gareth S Parkinson","doi":"10.1039/d5fd00158g","DOIUrl":"10.1039/d5fd00158g","url":null,"abstract":"<p><p>Infrared reflection absorption spectroscopy (IRAS) offers a powerful route to bridging the materials and pressure gaps between surface science and powder catalysis. Using a newly developed IRAS setup optimised for dielectric single crystals, we investigate CO adsorption on the model single-atom catalyst Rh/Fe₃O₄(001). IRAS resolves three species: monocarbonyls at isolated, twofold-coordinated Rh adatoms, monocarbonyls at fivefold-coordinated Rh atoms embedded in the surface, and <i>gem</i>-dicarbonyls at isolated, twofold-coordinated Rh adatoms. Under ultra-high vacuum (UHV) conditions, RhCO monocarbonyl species at adatom sites dominate. Rh(CO)₂<i>gem</i>-dicarbonyl formation is kinetically hindered and occurs predominantly through CO-induced dissociation of Rh dimers rather than sequential adsorption of two CO molecules at an isolated, twofold Rh adatom. The sequential-adsorption pathway to Rh(CO)₂ becomes accessible at millibar CO pressures as evidenced by near-ambient-pressure scanning tunnelling microscopy (NAP-STM). These findings link the UHV behaviour to that expected under realistic reaction conditions. Assignments of the vibrational frequencies to individual species rely on isotopic labelling, thermal treatments, and a review of previous SPM, XPS, and TPD data, supported by density functional theory (DFT)-based calculations. While theory provides qualitative insight, such as the instability of dicarbonyls on fivefold-coordinated Rh atoms, it does not yet reproduce experimental frequencies quantitatively and is sensitive to the computational parameters, highlighting the need for robust experimental benchmarks. The spectroscopic fingerprints established here provide a reliable foundation for identifying Rh coordination environments in oxide-supported single-atom catalysts.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"172-195"},"PeriodicalIF":3.1,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13196844/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148004150","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}

{"title":"Spiers Memorial Lecture: Emerging semiconductors viewed through the lens of a scanning electron microscope.","authors":"Robert W Martin","doi":"10.1039/d6fd00115g","DOIUrl":"10.1039/d6fd00115g","url":null,"abstract":"<p><p>As new materials are developed, or as their applications develop, it is important to have a range of characterisation techniques to understand their properties with a view to improving their performance. This paper considers a suite of characterisation techniques based on scanning electron microscopy to study emerging semiconductors or semiconductors with emerging applications, with an emphasis on combining multiple different techniques ideally measured simultaneously. Cathodoluminescence (CL) hyperspectral imaging is used to assess the optical properties and wavelength dispersive X-ray (WDX) provides compositional information, with an electron probe microanalyser facilitating their combined use. Electron channeling contrast imaging (ECCI) and electron backscatter diffraction (EBSD) furnish structural information, and electron beam induced current (EBIC) gives electrical information. The techniques are introduced using examples from the III-nitride semiconductors, followed by examples of scanning electron beam investigations of perovskite solar absorber layers, UV-emitting aluminium gallium nitride structures and 2D materials.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2026-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13576039/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148965795","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}