Jiaxin Li , Hongmei Yu , Jingchen Na , Senyuan Jia , Yutong Zhao , Kaiqiu Lv , Wenzhuo Zhang , Jun Chi , Zhigang Shao
{"title":"Recent advances in selective methanol oxidation electrocatalysts for the co-production of hydrogen and value-added formate†","authors":"Jiaxin Li , Hongmei Yu , Jingchen Na , Senyuan Jia , Yutong Zhao , Kaiqiu Lv , Wenzhuo Zhang , Jun Chi , Zhigang Shao","doi":"10.1039/d4cy00727a","DOIUrl":"10.1039/d4cy00727a","url":null,"abstract":"<div><div>Traditional water splitting is significantly impeded by the sluggish kinetics and large overpotential of the anodic oxygen evolution reaction (OER). Accordingly, replacing the OER with a more thermodynamically favorable organic substance oxidation reaction to combine with the hydrogen evolution reaction (HER) is an innovative strategy to obtain green hydrogen. In this case, the electro-reforming of methanol coupled with the electrochemical HER can realize the energy-saving co-generation of value-added formate and hydrogen. Therefore, controlling the process of methanol oxidation and making it selectively transform to formate have become a worthy topic. Thus far, various catalysts and modification strategies have been developed for the selective methanol oxidation reaction (SMOR). Transition metal-based materials are the most studied catalysts because their moderate catalytic ability can better control the process of methanol oxidation. Electronic structure modulation is the most efficient strategy to improve the SMOR performance of catalysts. However, few systematic reviews on the SMOR have been reported. In light of significant advances achieved recently, herein, we reviewed the recent advances in SMOR electrocatalysts for the co-production of value-added formate and green hydrogen. In particular, the mechanism of the SMOR is initially introduced, including the traditional surface adsorption mechanism and the newly developed lattice oxygen participation mechanism. Subsequently, strategies for catalyst design are analyzed from the aspects of chemical bond activation/inhibition, electronic structure manipulation, dual active site construction, and increasing the number of active sites. Thereafter, performance descriptors involving electrochemical measurements and product detection are discussed to show the basic evaluation criterion, and various catalysts for the SMOR are categorized according to their composition to display the development of catalysts. Finally, conclusions and perspectives are presented. We hope that this comprehensive effort will be helpful in the literature survey of the SMOR and provide inspiration to the SMOR research community, attracting more attention to the electro-upgradation of organic substances coupled with green hydrogen generation.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"14 19","pages":"Pages 5525-5544"},"PeriodicalIF":4.4,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/cy/d4cy00727a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205466","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}
Chuye Quan , Shilei Ji , Ruijia Yao , Ming Du , Chen Chen , Xiaoyang He , Ran Cai , Jianping Yang , Xing'ao Li
{"title":"Layerwise replacement method to achieve high solar-to-hydrogen efficiency for photocatalytic water splitting: a first principles study†","authors":"Chuye Quan , Shilei Ji , Ruijia Yao , Ming Du , Chen Chen , Xiaoyang He , Ran Cai , Jianping Yang , Xing'ao Li","doi":"10.1039/d4cy00688g","DOIUrl":"10.1039/d4cy00688g","url":null,"abstract":"<div><div>Atomically layered stacking (ALS) two-dimensional (2D) materials, owing to their superior electrical properties and flexible tunability in addition to the advantages of traditional 2D materials, have garnered widespread attention in recent years. However, when used as photocatalysts for overall water splitting (OWS), many of them face challenges like low Solar-to-Hydrogen (STH) efficiency and insufficient driving force for photoinduced redox reactions. Here, using Al<sub>2</sub>X<sub>3</sub> (X = S, Se) as samples, we demonstrate the potential of the Layerwise Replacement Method (LRM) in reducing the materials' bandgap, improving their light absorption performance, and boosting the STH efficiency. As anticipated, the Al<sub>2</sub>S<sub>2</sub>Se-t and Al<sub>2</sub>TeSe<sub>2</sub>-m monolayers demonstrate STH efficiencies exceeding 20%, surpassing the performance of the majority of reported photocatalysts. Additionally, under light excitation, the OER reaction on the Al<sub>2</sub>S<sub>2</sub>Se-t monolayer is exothermic, while on the Al<sub>2</sub>TeSe<sub>2</sub>-m monolayer, the OER energy barrier is reduced to 0.431 eV. Notably, on both materials, the HER energy barriers are approaching 0 eV. The improvement of these properties is primarily ascribed to the modulation of the materials' bandgap <em>via</em> the LRM, and secondarily to the reconstruction of the vertically intrinsic electric field (IEF). Our work not only offers a fresh perspective for the precise manipulation of atomically layered stacked 2D materials but also provides a rational strategy for designing novel and outstanding photocatalysts.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"14 19","pages":"Pages 5644-5652"},"PeriodicalIF":4.4,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205528","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}
Ting-Hao Liu, Shuai Fu, Jin-Tao Gou, Yin-Sheng Zhang, Chang-Wei Hu and Hua-Qing Yang
{"title":"Synergistic promotion of oxygen vacancy and Lewis acidity of Nb2O5 on the preferential hydroxymethyl hydrogenolysis of 5-hydroxymethylfurfural catalyzed by single atom Pt†","authors":"Ting-Hao Liu, Shuai Fu, Jin-Tao Gou, Yin-Sheng Zhang, Chang-Wei Hu and Hua-Qing Yang","doi":"10.1039/D4CY00559G","DOIUrl":"https://doi.org/10.1039/D4CY00559G","url":null,"abstract":"<p >Pt<small><sub>1</sub></small>/Nb<small><sub>2</sub></small>O<small><sub>5</sub></small> exhibits good catalytic performance towards the hydrogenolysis/hydrogenation of HMF. However, the chemical nature that affects its activity and selectivity is not yet clear at the molecular level. For Pt<small><sub>1</sub></small>/Nb<small><sub>2</sub></small>O<small><sub>5</sub></small>, two kinds of Pt-containing active sites are modelled, <em>i.e.</em>, [–(NbO)PtNb(ONb)<small><sub>5</sub></small>–] ([OPtNb]) in the absence of oxygen vacancy, and [–(NbO)PtNb(ONb)<small><sub>4</sub></small>–] ([OPtNb-O<small><sub>v</sub></small>]) in the presence of oxygen vacancy. Over both [OPtNb-O<small><sub>v</sub></small>] and [OPtNb], the catalytic mechanism for hydrogenolysis/hydrogenation of 5-hydroxymethylfurfural (HMF) with H<small><sub>2</sub></small> as an H-source has been theoretically investigated in tetrahydrofuran solution at the GGA-PBE/DNP level. The hydrogenolysis of –CH<small><sub>2</sub></small>OH (hydroxymethyl) groups to –CH<small><sub>3</sub></small> groups is predominated with the cleavage of –CH<small><sub>2</sub></small>–OH bonds as the rate-determining step, whereas the hydrogenation of –CHO (aldehyde) groups to –CH<small><sub>2</sub></small>OH groups is very minor with the addition of –CHO groups as the rate-determining step. Here, 5-methylfurfural (5-MF) is predominant, whereas 2,5-dihydroxymethylfuran (DHMF) is very minor. The strong Lewis acidity of Nb<small><sub>2</sub></small>O<small><sub>5</sub></small> promotes the Pt-site to accept the lone pair electrons of the oxygen atom, in which the oxygen atom of the –CH<small><sub>2</sub></small>OH group is more prone than that of the –CHO group to donate its lone pair electrons to the Pt-site. Thus, Pt<small><sub>1</sub></small>/Nb<small><sub>2</sub></small>O<small><sub>5</sub></small> facilitates the hydrogenolysis of the –CH<small><sub>2</sub></small>OH group and relatively inhibits the hydrogenation of the –CHO group. Compared with [OPtNb], [OPtNb-O<small><sub>v</sub></small>] displays higher catalytic activity. This stems from the promoting effect of oxygen vacancy on the capacity of the Pt-site to receive lone pair electrons of the oxygen atom in the –CH<small><sub>2</sub></small>OH group.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 22","pages":" 6550-6560"},"PeriodicalIF":4.4,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598707","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}
Nien-Chi Chang Liao, R. Sidick Basha, Bo-Hao Shih, Chia-Chun Liu, Miao-Han Wang, Po-Heng Lin and Chin-Fa Lee
{"title":"Copper cluster complex-catalyzed C–S bond formation†","authors":"Nien-Chi Chang Liao, R. Sidick Basha, Bo-Hao Shih, Chia-Chun Liu, Miao-Han Wang, Po-Heng Lin and Chin-Fa Lee","doi":"10.1039/D4CY00968A","DOIUrl":"https://doi.org/10.1039/D4CY00968A","url":null,"abstract":"<p >Three distinct copper cluster complexes (<strong>A–C</strong>) containing Cu–O ligated Schiff-base ligands were synthesized and their bonding was investigated by single-crystal X-ray crystallographic studies. These complexes effectively catalyze the C–S cross coupling reaction of less reactive aliphatic thiols to synthesize thioether derivatives. This coupling reaction also tolerates well and is compatible with aryl thiols. The peculiar C(sp<small><sup>2</sup></small>)–SC(sp<small><sup>3</sup></small>) bond formation distinctly took place with high efficiency using low loading of copper cluster complex catalysts. The present report describes an alternative protocol to construct active copper cluster complexes from readily accessible, cheap and efficient ligands. These complexes are air stable, practical, easy to handle and catalyze C–S coupling reactions with good yields.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 22","pages":" 6609-6620"},"PeriodicalIF":4.4,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598659","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}
Jingjing Jiang , Yuyao Chen , Shijian Zhou , Haoran Xie , Changlai Li , Zheng Wei , Yan Kong
{"title":"Dual defect sites at g-C3N4 synergistically induce the electron localization effect for boosting photocatalytic H2O2 production†","authors":"Jingjing Jiang , Yuyao Chen , Shijian Zhou , Haoran Xie , Changlai Li , Zheng Wei , Yan Kong","doi":"10.1039/d4cy01101e","DOIUrl":"10.1039/d4cy01101e","url":null,"abstract":"<div><div>Defect engineering (such as doping of non-metallic elements or vacancies) is a universally effective modification to improve the electronic structure and physical properties of g-C<sub>3</sub>N<sub>4</sub>, which has been widely applied in various photocatalytic systems. However, the key mechanism between the defect sites is not clear. In this work, elemental sulfur and N vacancies are sequentially introduced into g-C<sub>3</sub>N<sub>4</sub> by two consecutive thermal calcination for photocatalytic green synthesis of H<sub>2</sub>O<sub>2</sub>. The experimental and characterization results reveal the important roles of the dual defect sites in the photocatalytic H<sub>2</sub>O<sub>2</sub> reaction mechanism: sulfur doping can effectively broaden the visible-light response range of g-C<sub>3</sub>N<sub>4</sub>, and nitrogen vacancies can significantly enhance the adsorption of O<sub>2</sub> molecules. More importantly, dual defect sites induce the change of the charge distribution at g-C<sub>3</sub>N<sub>3</sub>, which results to the electron localization effect, enhancing the ability of the carriers to separate and transfer. After one hour of visible light irradiation, the H<sub>2</sub>O<sub>2</sub> generation rate of the dual defect modified photocatalysts is as high as 1593.34 μmol g<sup>−1</sup>, which is 14.31-fold higher compared to that of pristine g-C<sub>3</sub>N<sub>4</sub>. This work provides a viable strategy for understanding and rationalizing the design of photocatalysts with desirable defect structures.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"14 22","pages":"Pages 6701-6709"},"PeriodicalIF":4.4,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598746","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":"Switching of selectivity from benzaldehyde to benzoic acid using MIL-100(V) as a heterogeneous catalyst in aerobic oxidation of benzyl alcohol†","authors":"Duygu Hacıefendioğlu , Ali Tuncel","doi":"10.1039/d4cy00832d","DOIUrl":"10.1039/d4cy00832d","url":null,"abstract":"<div><div>A vanadium-centered metal organic framework [MIL-100(V)] was synthesized as a heterogeneous catalyst allowing the selectivity to be switched from almost quantitative formation of benzaldehyde (Bz-CHO) to quantitative formation of benzoic acid (Bz-COOH) by changing only the temperature in the aerobic oxidation of benzyl alcohol (Bz-OH). The aerobic oxidation of Bz-OH was performed using molecular oxygen or air in the temperature range of 60–120 °C. A Bz-CHO formation yield of 98.1% was obtained with quantitative Bz-OH conversion at 80 °C. When the oxidation temperature was set to 100 °C, a Bz-COOH formation yield of 100% was achieved with quantitative Bz-OH conversion. The suitability of a serial reaction mechanism including Bz-CHO formation from Bz-OH and Bz-COOH formation from Bz-CHO as the first and second stage reactions, respectively was investigated for the aerobic oxidation process. The apparent first-order rate constants determined for first and second stage reactions demonstrated that the first-stage reaction was faster with respect to the second one. The proposed kinetic model allowed the calculation of apparent activation energies for Bz-CHO formation from Bz-OH and Bz-COOH formation from Bz-CHO as 77.3 and 149.2 kJ mol<sup>−1</sup>, respectively. The presence of hydroxyl (·OH) and superoxide anion (O<sub>2</sub>˙<sup>−</sup>) radicals in the aerobic oxidation was demonstrated by radical scavenging runs. A mechanism was proposed based on the crystalline structure of MIL-100(V) and the radical types identified by the scavenging runs. This study opens a new path for tuning of selectivity towards Bz-CHO or Bz-COOH, for the first time, using a transition metal based catalyst synthesized by a one-pot hydrothermal reaction.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"14 22","pages":"Pages 6524-6536"},"PeriodicalIF":4.4,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/cy/d4cy00832d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598705","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}
Yu-Hui Luo , Sheng Tao , Fei Chen , Zhi-Hong Du , Hao Zhang , Min Li , Ning Liu
{"title":"Boron–pyridine nitrogen cooperative catalytic conversion of carbon dioxide and epoxides to cyclic carbonates†","authors":"Yu-Hui Luo , Sheng Tao , Fei Chen , Zhi-Hong Du , Hao Zhang , Min Li , Ning Liu","doi":"10.1039/d4cy01052c","DOIUrl":"10.1039/d4cy01052c","url":null,"abstract":"<div><div>A type of N-heterocyclic carbene (NHC)-diboron adduct was used as a catalyst for the coupling of CO<sub>2</sub> with epoxides. A multifunctional organocatalyst, which contains both boron as a Lewis acidic site and pyridine nitrogen as a Lewis basic site, offers an efficient alternative to traditional organoboron catalysts for the conversion of CO<sub>2</sub> and epoxides into cyclic carbonates. The NHC-diboron adduct, in combination with tetrabutylammonium iodide (TBAI) as a nucleophile, catalyzes the coupling of CO<sub>2</sub> and epoxides to obtain the cyclic carbonates in high yields under relatively mild conditions (50 °C and 1 MPa of CO<sub>2</sub>). The cooperative activation of NHC-diboron adducts was elaborated by <em>in situ</em> infrared spectroscopy and electrospray ionization-high-resolution mass spectrometry (ESI-HRMS). These results suggested that the Lewis acid boron center in NHC-diboron adduct activates the epoxide by coordination with its oxygen atom to promote ring opening and that the pyridine nitrogen acts as a Lewis basic site to activate CO<sub>2</sub>.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"14 22","pages":"Pages 6692-6700"},"PeriodicalIF":4.4,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598745","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}
D. J. Ward , D. J. Saccomando , F. Vilela , G. Walker , S. M. Mansell
{"title":"Flow chemistry enhances catalytic alcohol-to-alkene dehydration†","authors":"D. J. Ward , D. J. Saccomando , F. Vilela , G. Walker , S. M. Mansell","doi":"10.1039/d4cy00913d","DOIUrl":"10.1039/d4cy00913d","url":null,"abstract":"<div><div>Hf(OTf)<sub>4</sub> was identified as an excellent catalyst for the low temperature (180 °C) dehydration of 1-hexanol to hexenes and 2-methyl-1-butanol to 2-methylbutenes. Batch conditions limited yields of alkene to 50% despite >90% conversions of 1-hexanol, 16% yield and 55% conversion for 2-methyl-1-butanol, but dramatically better yields were achieved using flow chemistry. For 2-methyl-1-butanol, steady-state conditions were achieved at 180 °C at flow rates of 0.1–0.2 mL min<sup>−1</sup> that gave excellent mass balance and allowing selectivities and activities to be meaningfully compared. Hf(OTf)<sub>4</sub> was the most active (51 h<sup>−1</sup>) with a selectivity of 50% at 50% conversion. Optimising for the production of purer alkene was achieved by raising the pressure producing 2.1 g h<sup>−1</sup> of 2-methylbutenes (up to 98% pure by mass).</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"14 22","pages":"Pages 6641-6650"},"PeriodicalIF":4.4,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/cy/d4cy00913d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598661","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}
Jelle W. Bos, Job G. A. Vloedgraven, Sophie C. C. Wiedemann, Leo van Dongen, Roel C. J. Moonen, Bas Wels, Peter H. Berben, Bennie H. Reesink, Peter de Peinder, Eelco T. C. Vogt and Bert M. Weckhuysen
{"title":"γ-Stearolactone ring-opening by zeolites for the production of branched saturated fatty acids†","authors":"Jelle W. Bos, Job G. A. Vloedgraven, Sophie C. C. Wiedemann, Leo van Dongen, Roel C. J. Moonen, Bas Wels, Peter H. Berben, Bennie H. Reesink, Peter de Peinder, Eelco T. C. Vogt and Bert M. Weckhuysen","doi":"10.1039/D4CY00782D","DOIUrl":"10.1039/D4CY00782D","url":null,"abstract":"<p >C<small><sub>18</sub></small> branched saturated fatty acids (BSFA) are used as ingredients in cosmetics and lubricants and are produced <em>via</em> the hydrogenation of C<small><sub>18</sub></small> branched unsaturated fatty acids (BUFA). Industrial-grade C<small><sub>18</sub></small> BUFA contain the odorous by-product γ-stearolactone (GSL), which must be removed by acid-catalysed ring-opening of GSL into oleic acid. Zeolites such as Y and beta can facilitate the ring-opening, but due to the dimensions of GSL the activity is expected to be limited by diffusion into the micropores. Hence, zeolites Y and beta were modified <em>via</em> hydrothermal treatment and acid leaching and used in the GSL ring-opening reaction. While modification of zeolite beta led to a reduction in acidity of more than 50%, the material displayed much-enhanced activity compared to the parent material. In a batch reactor steamed beta zeolites were able to convert all GSL within 2 h, compared to 5 h for the parent zeolite. Infrared spectroscopy studies of adsorbed pyridine reveal that likely a beneficial change in Brønsted/Lewis acid site ratio is responsible for the increased activity. Lewis acid sites in zeolites are known to catalyse double bond isomerisation, which could greatly enhance GSL conversion by reducing the reverse formation of GSL from oleic acid. We believe that these insights can be used to further improve GSL ring-opening activity and inspire research on the ring-opening of other biomass derived lactones.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 24","pages":" 7037-7047"},"PeriodicalIF":4.4,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11589803/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142749412","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}
Jonathan Y. C. Ting , George Opletal , Amanda S. Barnard
{"title":"Unsupervised pattern recognition on the surface of simulated metal nanoparticles for catalytic applications†","authors":"Jonathan Y. C. Ting , George Opletal , Amanda S. Barnard","doi":"10.1039/d4cy01000k","DOIUrl":"10.1039/d4cy01000k","url":null,"abstract":"<div><div>The application of supervised machine learning to the study of catalytic metal nanoparticles has been shown to deliver excellent performance for a range of predictive tasks. However, this success assumes that the particles have been thoroughly characterised and that the property labels are known. Even in exclusively computational studies, the labelling of metal nanoparticles remains the bottleneck for most machine learning studies due to either high computational costs or low relevance to the experimental properties of interest. To facilitate more widespread use of machine learning in catalysis, a computationally affordable strategy to describe metal nanoparticles by a label that is relevant to their catalytic activities is needed. In this study we propose an entirely data-driven approach that can be automated to characterise the patterns and catalytic activities of the surface atoms of simulated metal nanoparticles, and evaluate its utility for catalytic applications.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"14 22","pages":"Pages 6651-6661"},"PeriodicalIF":4.4,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598662","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}