ACS Combinatorial Science最新文献_第2页

Efficient Machine-Learning-Aided Screening of Hydrogen Adsorption on Bimetallic Nanoclusters 高效机器学习辅助筛选双金属纳米团簇对氢的吸附

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-11-04 DOI: 10.1021/acscombsci.0c00102

Marc O. J. Jäger*, Yashasvi S. Ranawat, Filippo Federici Canova, Eiaki V. Morooka, Adam S. Foster

{"title":"Efficient Machine-Learning-Aided Screening of Hydrogen Adsorption on Bimetallic Nanoclusters","authors":"Marc O. J. Jäger*, Yashasvi S. Ranawat, Filippo Federici Canova, Eiaki V. Morooka, Adam S. Foster","doi":"10.1021/acscombsci.0c00102","DOIUrl":"https://doi.org/10.1021/acscombsci.0c00102","url":null,"abstract":"Nanoclusters add an additional dimension in which to look for promising catalyst candidates, since catalytic activity of materials often changes at the nanoscale. However, the large search space of relevant atomic sites exacerbates the challenge for computational screening methods and requires the development of new techniques for efficient exploration. We present an automated workflow that systematically manages simulations from the generation of nanoclusters through the submission of production jobs, to the prediction of adsorption energies. The presented workflow was designed to screen nanoclusters of arbitrary shapes and size, but in this work the search was restricted to bimetallic icosahedral clusters and the adsorption was exemplified on the hydrogen evolution reaction. We demonstrate the efficient exploration of nanocluster configurations and screening of adsorption energies with the aid of machine learning. The results show that the maximum of the d-band Hilbert-transform ?u is correlated strongly with adsorption energies and could be a useful screening property accessible at the nanocluster level.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":null,"pages":null},"PeriodicalIF":3.784,"publicationDate":"2020-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acscombsci.0c00102","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1237219","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}

引用次数: 13

Optical Identification of Materials Transformations in Oxide Thin Films 氧化薄膜中材料转化的光学识别

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-29 DOI: 10.1021/acscombsci.0c00172

Duncan R. Sutherland, Aine Boyer Connolly, Maximilian Amsler, Ming-Chiang Chang, Katie Rose Gann, Vidit Gupta, Sebastian Ament, Dan Guevarra, John M. Gregoire, Carla P. Gomes, R. Bruce van Dover*, Michael O. Thompson*

{"title":"Optical Identification of Materials Transformations in Oxide Thin Films","authors":"Duncan R. Sutherland, Aine Boyer Connolly, Maximilian Amsler, Ming-Chiang Chang, Katie Rose Gann, Vidit Gupta, Sebastian Ament, Dan Guevarra, John M. Gregoire, Carla P. Gomes, R. Bruce van Dover*, Michael O. Thompson*","doi":"10.1021/acscombsci.0c00172","DOIUrl":"https://doi.org/10.1021/acscombsci.0c00172","url":null,"abstract":"Recent advances in high-throughput experimentation for combinatorial studies have accelerated the discovery and analysis of materials across a wide range of compositions and synthesis conditions. However, many of the more powerful characterization methods are limited by speed, cost, availability, and/or resolution. To make efficient use of these methods, there is value in developing approaches for identifying critical compositions and conditions to be used as a priori knowledge for follow-up characterization with high-precision techniques, such as micrometer-scale synchrotron-based X-ray diffraction (XRD). Here, we demonstrate the use of optical microscopy and reflectance spectroscopy to identify likely phase-change boundaries in thin film libraries. These methods are used to delineate possible metastable phase boundaries following lateral-gradient laser spike annealing (lg-LSA) of oxide materials. The set of boundaries are then compared with definitive determinations of structural transformations obtained using high-resolution XRD. We demonstrate that the optical methods detect more than 95% of the structural transformations in a composition-gradient La-Mn-O library and a Ga2O3 sample, both subject to an extensive set of lg-LSA anneals. Our results provide quantitative support for the value of optically detected transformations as a priori data to guide subsequent structural characterization, ultimately accelerating and enhancing the efficient implementation of micrometer-resolution XRD experiments.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":null,"pages":null},"PeriodicalIF":3.784,"publicationDate":"2020-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acscombsci.0c00172","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1348673","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}

引用次数: 4

Bi Alloying into Rare Earth Double Perovskites Enhances Synthesizability and Visible Light Absorption 稀土双钙钛矿的铋合金化提高了合成性能和可见光吸收

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-29 DOI: 10.1021/acscombsci.0c00177

Paul F. Newhouse, Lan Zhou, Mitsutaro Umehara, David A. Boyd, Edwin Soedarmadji, Joel A. Haber, John M. Gregoire*

{"title":"Bi Alloying into Rare Earth Double Perovskites Enhances Synthesizability and Visible Light Absorption","authors":"Paul F. Newhouse, Lan Zhou, Mitsutaro Umehara, David A. Boyd, Edwin Soedarmadji, Joel A. Haber, John M. Gregoire*","doi":"10.1021/acscombsci.0c00177","DOIUrl":"https://doi.org/10.1021/acscombsci.0c00177","url":null,"abstract":"A high throughput combinatorial synthesis utilizing inkjet printing of precursor inks was used to rapidly evaluate Bi-alloying into double perovskite oxides for enhanced visible light absorption. The fast visual screening of photo image scans of the library plates identifies 4-metal oxide compositions displaying an increase in light absorption, which subsequent UV–vis spectroscopy indicates is due to bandgap reduction. Structural characterization by X-ray diffraction (XRD) and Raman spectroscopy demonstrates that the visually darker composition range contains Bi-alloyed Sm2MnNiO6 (double perovskite structure), of the form (Bi,Sm)2MnNiO6. Bi alloying not only increases the visible absorption but also facilitates crystallization of this structure at the relatively low annealing temperature of 615 °C. Investigation of additional seven combinations of a rare earth (RE) and a transition metal (TM) with Bi and Mn indicates that Bi-alloying on the RE site occurs with similar effect in the family of rare earth oxide double perovskites.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":null,"pages":null},"PeriodicalIF":3.784,"publicationDate":"2020-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acscombsci.0c00177","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1323876","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}

引用次数: 4

Profiling SARS-CoV-2 Main Protease (MPRO) Binding to Repurposed Drugs Using Molecular Dynamics Simulations in Classical and Neural Network-Trained Force Fields 基于经典力场和神经网络训练力场的分子动力学模拟分析SARS-CoV-2主蛋白酶(MPRO)与改用药物的结合

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-29 DOI: 10.1021/acscombsci.0c00140

Aayush Gupta, Huan-Xiang Zhou*

{"title":"Profiling SARS-CoV-2 Main Protease (MPRO) Binding to Repurposed Drugs Using Molecular Dynamics Simulations in Classical and Neural Network-Trained Force Fields","authors":"Aayush Gupta, Huan-Xiang Zhou*","doi":"10.1021/acscombsci.0c00140","DOIUrl":"https://doi.org/10.1021/acscombsci.0c00140","url":null,"abstract":"The current COVID-19 pandemic caused by a novel coronavirus SARS-CoV-2 urgently calls for a working therapeutic. Here, we report a computation-based workflow for efficiently selecting a subset of FDA-approved drugs that can potentially bind to the SARS-CoV-2 main protease MPRO. The workflow started with docking (using Autodock Vina) each of 1615 FDA-approved drugs to the MPRO active site. This step selected 62 candidates with docking energies lower than ?8.5 kcal/mol. Then, the 62 docked protein–drug complexes were subjected to 100 ns of molecular dynamics (MD) simulations in a molecular mechanics (MM) force field (CHARMM36). This step reduced the candidate pool to 26, based on the root-mean-square-deviations (RMSDs) of the drug molecules in the trajectories. Finally, we modeled the 26 drug molecules by a pseudoquantum mechanical (ANI) force field and ran 5 ns hybrid ANI/MM MD simulations of the 26 protein–drug complexes. ANI was trained by neural network models on quantum mechanical density functional theory (wB97X/6-31G(d)) data points. An RMSD cutoff winnowed down the pool to 12, and free energy analysis (MM/PBSA) produced the final selection of 9 drugs: dihydroergotamine, midostaurin, ziprasidone, etoposide, apixaban, fluorescein, tadalafil, rolapitant, and palbociclib. Of these, three are found to be active in literature reports of experimental studies. To provide physical insight into their mechanism of action, the interactions of the drug molecules with the protein are presented as 2D-interaction maps. These findings and mappings of drug–protein interactions may be potentially used to guide rational drug discovery against COVID-19.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":null,"pages":null},"PeriodicalIF":3.784,"publicationDate":"2020-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acscombsci.0c00140","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1347676","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}

引用次数: 24

High-Throughput Exploration of Metal Vanadate Thin-Film Systems (M–V–O, M = Cu, Ag, W, Cr, Co, Fe) for Solar Water Splitting: Composition, Structure, Stability, and Photoelectrochemical Properties 高通量探索金属钒酸盐薄膜系统(M - v - o, M = Cu, Ag, W, Cr, Co, Fe)用于太阳能水分解:组成，结构，稳定性和光电化学性质

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-26 DOI: 10.1021/acscombsci.0c00150

Swati Kumari, João R. C. Junqueira, Wolfgang Schuhmann, Alfred Ludwig*

{"title":"High-Throughput Exploration of Metal Vanadate Thin-Film Systems (M–V–O, M = Cu, Ag, W, Cr, Co, Fe) for Solar Water Splitting: Composition, Structure, Stability, and Photoelectrochemical Properties","authors":"Swati Kumari, João R. C. Junqueira, Wolfgang Schuhmann, Alfred Ludwig*","doi":"10.1021/acscombsci.0c00150","DOIUrl":"https://doi.org/10.1021/acscombsci.0c00150","url":null,"abstract":"Combinatorial synthesis and high-throughput characterization of thin-film materials libraries enable to efficiently identify both photoelectrochemically active and inactive, as well as stable and instable systems for solar water splitting. This is shown on six ternary metal vanadate (M–V–O, M = Cu, Ag, W, Cr, Co, Fe) thin-film materials libraries, fabricated using combinatorial reactive magnetron cosputtering with subsequent annealing in air. By means of high-throughput characterization of these libraries correlations between composition, crystal structure, photocurrent density, and stability of the M–V–O systems in different electrolytes such as acidic, neutral and alkaline media were identified. The systems Cu–V–O and Ag–V–O are stable in alkaline electrolyte and exhibited photocurrents of 170 and 554 μA/cm2, respectively, whereas the systems W–V–O, Cr–V–O, and Co–V–O are not stable in alkaline electrolyte. However, the Cr–V–O and Co–V–O systems showed an enlarged photoactive region in acidic electrolyte, albeit with very low photocurrents (<10 μA/cm2). Complete data sets obtained from these different screening sets, including information on nonpromising systems, lays groundwork for their use to predict new systems for solar water splitting, for example, by machine learning.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":null,"pages":null},"PeriodicalIF":3.784,"publicationDate":"2020-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acscombsci.0c00150","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"825702","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}

引用次数: 8

Development of Measurement Tools for High-Throughput Experiments of Synchrotron Radiation XRD and XAFS on Powder Libraries 粉末库同步辐射XRD和XAFS高通量实验测量工具的研制

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-23 DOI: 10.1021/acscombsci.0c00174

Kenjiro Fujimoto*, Akihisa Aimi, Shingo Maruyama

引用次数: 2

Progress in Natural Compounds/siRNA Co-delivery Employing Nanovehicles for Cancer Therapy 基于纳米载体的天然化合物/siRNA共递送在癌症治疗中的进展

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-23 DOI: 10.1021/acscombsci.0c00099

Milad Ashrafizadeh, Ali Zarrabi, Kiavash Hushmandi, Farid Hashemi, Ebrahim Rahmani Moghadam, Mehdi Raei, Mahshad Kalantari, Shima Tavakol, Reza Mohammadinejad, Masoud Najafi*, Franklin R. Tay, Pooyan Makvandi*

{"title":"Progress in Natural Compounds/siRNA Co-delivery Employing Nanovehicles for Cancer Therapy","authors":"Milad Ashrafizadeh, Ali Zarrabi, Kiavash Hushmandi, Farid Hashemi, Ebrahim Rahmani Moghadam, Mehdi Raei, Mahshad Kalantari, Shima Tavakol, Reza Mohammadinejad, Masoud Najafi*, Franklin R. Tay, Pooyan Makvandi*","doi":"10.1021/acscombsci.0c00099","DOIUrl":"https://doi.org/10.1021/acscombsci.0c00099","url":null,"abstract":"Chemotherapy using natural compounds, such as resveratrol, curcumin, paclitaxel, docetaxel, etoposide, doxorubicin, and camptothecin, is of importance in cancer therapy because of the outstanding therapeutic activity and multitargeting capability of these compounds. However, poor solubility and bioavailability of natural compounds have limited their efficacy in cancer therapy. To circumvent this hurdle, nanocarriers have been designed to improve the antitumor activity of the aforementioned compounds. Nevertheless, cancer treatment is still a challenge, demanding novel strategies. It is well-known that a combination of natural products and gene therapy is advantageous over monotherapy. Delivery of multiple therapeutic agents/small interfering RNA (siRNA) as a potent gene-editing tool in cancer therapy can maximize the synergistic effects against tumor cells. In the present review, co-delivery of natural compounds/siRNA using nanovehicles are highlighted to provide a backdrop for future research.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":null,"pages":null},"PeriodicalIF":3.784,"publicationDate":"2020-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acscombsci.0c00099","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1332100","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}

引用次数: 61

Simultaneous Measurements of Photoabsorption and Photoelectrochemical Performance for Thickness Optimization of a Semiconductor Photoelectrode 半导体光电极厚度优化的光吸收和光电化学性能的同时测量

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-22 DOI: 10.1021/acscombsci.0c00113

Naoya Murakami*, Ryo Watanabe

引用次数: 3

Use of Target-Displaying Magnetized Yeast in Screening mRNA-Display Peptide Libraries to Identify Ligands 利用目标显示磁化酵母筛选mrna显示肽库以鉴定配体

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-22 DOI: 10.1021/acscombsci.0c00171

Kaitlyn Bacon, John Bowen, Hannah Reese, Balaji M. Rao*, Stefano Menegatti*

{"title":"Use of Target-Displaying Magnetized Yeast in Screening mRNA-Display Peptide Libraries to Identify Ligands","authors":"Kaitlyn Bacon, John Bowen, Hannah Reese, Balaji M. Rao*, Stefano Menegatti*","doi":"10.1021/acscombsci.0c00171","DOIUrl":"https://doi.org/10.1021/acscombsci.0c00171","url":null,"abstract":"This work presents the first use of yeast-displayed protein targets for screening mRNA-display libraries of cyclic and linear peptides. The WW domains of Yes-Associated Protein 1 (WW-YAP) and mitochondrial import receptor subunit TOM22 were adopted as protein targets. Yeast cells displaying WW-YAP or TOM22 were magnetized with iron oxide nanoparticles to enable the isolation of target-binding mRNA-peptide fusions. Equilibrium adsorption studies were conducted to estimate the binding affinity (KD) of select WW-YAP-binding peptides: KD values of 37 and 4 μM were obtained for cyclo[M-AFRLC-K] and its linear cognate, and 40 and 3 μM for cyclo[M-LDFVNHRSRG-K] and its linear cognate, respectively. TOM22-binding peptide cyclo[M-PELNRAI-K] was conjugated to magnetic beads and incubated with yeast cells expressing TOM22 and luciferase. A luciferase-based assay showed a 4.5-fold higher binding of TOM22+ yeast compared to control cells. This work demonstrates that integrating mRNA- and yeast-display accelerates the discovery of peptide ligands.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":null,"pages":null},"PeriodicalIF":3.784,"publicationDate":"2020-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acscombsci.0c00171","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1327417","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}

引用次数: 2

Optimization of Criteria for an Efficient Screening of New Thermoelectric Compounds: The TiNiSi Structure-Type as a Case-Study 新型热电化合物高效筛选标准的优化:以TiNiSi结构型为例

IF 3.784 3区化学

ACS Combinatorial Science Pub Date : 2020-10-20 DOI: 10.1021/acscombsci.0c00133

Celine Barreteau*, Jean-Claude Crivello, Jean-Marc Joubert, Eric Alleno

{"title":"Optimization of Criteria for an Efficient Screening of New Thermoelectric Compounds: The TiNiSi Structure-Type as a Case-Study","authors":"Celine Barreteau*, Jean-Claude Crivello, Jean-Marc Joubert, Eric Alleno","doi":"10.1021/acscombsci.0c00133","DOIUrl":"https://doi.org/10.1021/acscombsci.0c00133","url":null,"abstract":"High-throughput calculations can be applied to a large number of compounds, in order to discover new useful materials. In the present work, ternary intermetallic compounds are investigated, to find new potentially interesting materials for thermoelectric applications. The screening of stable nonmetallic compounds required for such applications is performed by calculating their electronic structure, using DFT methods. In the first section, the study of the density of states at the Fermi level, of pure elements, binary and ternary compounds, leads to empirically chose the selection criterion to distinguish metals from nonmetals. In the second section, the TiNiSi structure-type is used as a case-study application, through the investigation of 570 possible compositions. The screening leads to the selection of 12 possible semiconductors. The Seebeck coefficient and the lattice thermal conductivity of the selected compounds are calculated in order to identify the most promising ones. Among them, TiNiSi, TaNiP, or HfCoP are shown to be worth a detailed experimental investigation.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":null,"pages":null},"PeriodicalIF":3.784,"publicationDate":"2020-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acscombsci.0c00133","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1321427","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}

引用次数: 4