ACS Materials Au最新文献

Let Us FIGURE It Out: Why Do Scientists Still Make “Bad” Figures? 让我们弄清楚：为什么科学家仍然得出“糟糕”的数字？

IF 5.7

ACS Materials Au Pub Date : 2025-05-14 DOI: 10.1021/acsmaterialsau.5c0003710.1021/acsmaterialsau.5c00037

Aiswarya Rayaroth, Christine Fiedler and Maria Ibáñez*,

引用次数: 0

Let Us FIGURE It Out: Why Do Scientists Still Make "Bad" Figures? 让我们弄清楚：为什么科学家仍然得出“糟糕”的数字？

IF 5.7

ACS Materials Au Pub Date : 2025-05-14 DOI: 10.1021/acsmaterialsau.5c00037

Aiswarya Rayaroth, Christine Fiedler, Maria Ibáñez

引用次数: 0

Interfacial Microenvironment Effects at Laser-Made Gold Nanoparticles Steer Carbon Dioxide Reduction Product Generation. 界面微环境效应在激光制造的金纳米颗粒引导二氧化碳还原产物的产生。

IF 5.7

ACS Materials Au Pub Date : 2025-04-29 eCollection Date: 2025-05-14 DOI: 10.1021/acsmaterialsau.4c00161

Connor P Cox, Qishen Lyu, Madeleine K Wilsey, Likun Cai, Lydia R Schultz, Jason R Maher, Astrid M Müller

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引用次数: 0

Interfacial Microenvironment Effects at Laser-Made Gold Nanoparticles Steer Carbon Dioxide Reduction Product Generation 界面微环境效应在激光制造的金纳米颗粒引导二氧化碳还原产物的产生

IF 5.7

ACS Materials Au Pub Date : 2025-04-29 DOI: 10.1021/acsmaterialsau.4c0016110.1021/acsmaterialsau.4c00161

Connor P. Cox, Qishen Lyu, Madeleine K. Wilsey, Likun Cai, Lydia R. Schultz, Jason R. Maher and Astrid M. Müller*,

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引用次数: 0

Direct Correlation of the Crystalline Phases of La0.9Sr0.1Co1–yFeyO3−δ with the Partial Oxidation of Methane via In Situ Neutron and Synchrotron Diffraction La0.9Sr0.1Co1-yFeyO3−δ晶体相与甲烷部分氧化的直接关联

IF 5.7

ACS Materials Au Pub Date : 2025-04-17 DOI: 10.1021/acsmaterialsau.4c0017710.1021/acsmaterialsau.4c00177

Dennis D. Nguyen, Mara J. Milhander, Elizabeth M. Hitch, Dmitri Leo M. Cordova, Jose L. Gonzalez Jimenez, Juana Mora, Daniel Sandoval, Maxx Q. Arguilla and Allyson M. Fry-Petit*,

{"title":"Direct Correlation of the Crystalline Phases of La0.9Sr0.1Co1–yFeyO3−δ with the Partial Oxidation of Methane via In Situ Neutron and Synchrotron Diffraction","authors":"Dennis D. Nguyen, Mara J. Milhander, Elizabeth M. Hitch, Dmitri Leo M. Cordova, Jose L. Gonzalez Jimenez, Juana Mora, Daniel Sandoval, Maxx Q. Arguilla and Allyson M. Fry-Petit*, ","doi":"10.1021/acsmaterialsau.4c0017710.1021/acsmaterialsau.4c00177","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00177https://doi.org/10.1021/acsmaterialsau.4c00177","url":null,"abstract":"Oxygen transport membranes find broad usage in many technologies, but due to the harsh conditions under which such technologies operate, detailed structural analysis under operational conditions has been limited. This work details the in situ neutron and synchrotron diffraction of the industrially relevant family of compounds, La0.9Sr0.1Co1–yFeyO3−δ (y = 0, 0.25, 0.75, 1), under reductive and oxidative conditions at elevated temperatures ranging from 723 to 1123 K. Quantitative Rietveld refinements determine the molar fraction of all crystalline intermediates and products that form during the reactions of La0.9Sr0.1Co1–yFeyO3−δ (y = 0, 0.25, 0.75, 1) with methane and then air. Coupling in situ diffraction analysis with catalytic product analysis of the partial oxidation of methane allows for the catalytically active phases to be determined. This work shows the strength of in situ diffraction under extreme conditions and the insights it can give about reactions in the solid state that have previously been elusive.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 3","pages":"547–557 547–557"},"PeriodicalIF":5.7,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00177","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940750","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}

引用次数: 0

Direct Correlation of the Crystalline Phases of La_0.9Sr_0.1Co_1-y Fe _y O_3-δ with the Partial Oxidation of Methane via In Situ Neutron and Synchrotron Diffraction. La0.9Sr0.1Co1-y Fe y O3-δ晶体相与甲烷部分氧化的直接关联

IF 5.7

ACS Materials Au Pub Date : 2025-04-17 eCollection Date: 2025-05-14 DOI: 10.1021/acsmaterialsau.4c00177

Dennis D Nguyen, Mara J Milhander, Elizabeth M Hitch, Dmitri Leo M Cordova, Jose L Gonzalez Jimenez, Juana Mora, Daniel Sandoval, Maxx Q Arguilla, Allyson M Fry-Petit

{"title":"Direct Correlation of the Crystalline Phases of La0.9Sr0.1Co1-y Fe y O3-δ with the Partial Oxidation of Methane via In Situ Neutron and Synchrotron Diffraction.","authors":"Dennis D Nguyen, Mara J Milhander, Elizabeth M Hitch, Dmitri Leo M Cordova, Jose L Gonzalez Jimenez, Juana Mora, Daniel Sandoval, Maxx Q Arguilla, Allyson M Fry-Petit","doi":"10.1021/acsmaterialsau.4c00177","DOIUrl":"10.1021/acsmaterialsau.4c00177","url":null,"abstract":"Oxygen transport membranes find broad usage in many technologies, but due to the harsh conditions under which such technologies operate, detailed structural analysis under operational conditions has been limited. This work details the in situ neutron and synchrotron diffraction of the industrially relevant family of compounds, La0.9Sr0.1Co1-y Fe y O3-δ (y = 0, 0.25, 0.75, 1), under reductive and oxidative conditions at elevated temperatures ranging from 723 to 1123 K. Quantitative Rietveld refinements determine the molar fraction of all crystalline intermediates and products that form during the reactions of La0.9Sr0.1Co1-y Fe y O3-δ (y = 0, 0.25, 0.75, 1) with methane and then air. Coupling in situ diffraction analysis with catalytic product analysis of the partial oxidation of methane allows for the catalytically active phases to be determined. This work shows the strength of in situ diffraction under extreme conditions and the insights it can give about reactions in the solid state that have previously been elusive.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 3","pages":"547-557"},"PeriodicalIF":5.7,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12082351/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144094879","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}

引用次数: 0

Design Strategies for Coupling CO₂ Reduction Molecular Electrocatalysts to Silicon Photocathodes. 硅光电阴极耦合CO2还原分子电催化剂的设计策略。

IF 5.7

ACS Materials Au Pub Date : 2025-04-14 eCollection Date: 2025-05-14 DOI: 10.1021/acsmaterialsau.5c00010

Simran S Saund, Melissa K Gish, Jeremiah Choate, Trung H Le, Smaranda C Marinescu, Nathan R Neale

{"title":"Design Strategies for Coupling CO2 Reduction Molecular Electrocatalysts to Silicon Photocathodes.","authors":"Simran S Saund, Melissa K Gish, Jeremiah Choate, Trung H Le, Smaranda C Marinescu, Nathan R Neale","doi":"10.1021/acsmaterialsau.5c00010","DOIUrl":"10.1021/acsmaterialsau.5c00010","url":null,"abstract":"We explore strategies for enhancing the electronic interaction between silicon nanocrystals (Si NCs) and surface-tethered molecular Re electrocatalysts ([Re]) as models for CO2-reducing photocathodes. Using density functional theory (DFT) combined with electrochemical, spectroscopic, and photocatalytic measurements, we determine that the intrinsic Si (iSi) NC conduction band energy in iSi-[Re] assemblies is below the [Re] lowest unoccupied molecular orbital (LUMO) and singly occupied molecular orbital energies even for strongly quantum-confined 3.0-3.9 nm diameter hydrogen- and methyl-terminated iSi NCs, respectively. We computationally analyze design strategies to align the semiconductor conduction band edge and electrocatalyst frontier molecular orbitals by varying the iSi NC size, introducing boron as a dopant in the Si NC, and modifying the attachment chemistry to the [Re] complex aryl ligand framework. Our DFT analysis identifies a target hybrid structure featuring B-doped silicon (B:Si) NCs and a direct bond between a surface atom and an sp2-hybridized carbon of the electrocatalyst bipyridine aryl ring ligand (B:Si-CAr[Re]). We synthesize the B:Si-CAr[Re] NC assembly and find evidence of direct hybridization between the B:Si NC and the surface [Re] electrocatalyst LUMO using electrochemical measurements and transient absorption spectroscopy. This work provides a blueprint for the design of new Si photocathode-molecular electrocatalyst hybrids for CO2 reduction and related fuel-forming photocatalytic conversions.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 3","pages":"569-579"},"PeriodicalIF":5.7,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12082352/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144094875","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}

引用次数: 0

Design Strategies for Coupling CO2 Reduction Molecular Electrocatalysts to Silicon Photocathodes 硅光电阴极耦合CO2还原分子电催化剂的设计策略

IF 5.7

ACS Materials Au Pub Date : 2025-04-14 DOI: 10.1021/acsmaterialsau.5c0001010.1021/acsmaterialsau.5c00010

Simran S. Saund, Melissa K. Gish, Jeremiah Choate, Trung H. Le, Smaranda C. Marinescu and Nathan R. Neale*,

{"title":"Design Strategies for Coupling CO2 Reduction Molecular Electrocatalysts to Silicon Photocathodes","authors":"Simran S. Saund, Melissa K. Gish, Jeremiah Choate, Trung H. Le, Smaranda C. Marinescu and Nathan R. Neale*, ","doi":"10.1021/acsmaterialsau.5c0001010.1021/acsmaterialsau.5c00010","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.5c00010https://doi.org/10.1021/acsmaterialsau.5c00010","url":null,"abstract":"We explore strategies for enhancing the electronic interaction between silicon nanocrystals (Si NCs) and surface-tethered molecular Re electrocatalysts ([Re]) as models for CO2-reducing photocathodes. Using density functional theory (DFT) combined with electrochemical, spectroscopic, and photocatalytic measurements, we determine that the intrinsic Si (iSi) NC conduction band energy in iSi–[Re] assemblies is below the [Re] lowest unoccupied molecular orbital (LUMO) and singly occupied molecular orbital energies even for strongly quantum-confined 3.0–3.9 nm diameter hydrogen- and methyl-terminated iSi NCs, respectively. We computationally analyze design strategies to align the semiconductor conduction band edge and electrocatalyst frontier molecular orbitals by varying the iSi NC size, introducing boron as a dopant in the Si NC, and modifying the attachment chemistry to the [Re] complex aryl ligand framework. Our DFT analysis identifies a target hybrid structure featuring B-doped silicon (B:Si) NCs and a direct bond between a surface atom and an sp2-hybridized carbon of the electrocatalyst bipyridine aryl ring ligand (B:Si–CAr[Re]). We synthesize the B:Si–CAr[Re] NC assembly and find evidence of direct hybridization between the B:Si NC and the surface [Re] electrocatalyst LUMO using electrochemical measurements and transient absorption spectroscopy. This work provides a blueprint for the design of new Si photocathode-molecular electrocatalyst hybrids for CO2 reduction and related fuel-forming photocatalytic conversions.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 3","pages":"569–579 569–579"},"PeriodicalIF":5.7,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.5c00010","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940746","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}

引用次数: 0

Tailoring Cu-Based Catalysts Supported on ZrO₂-Al₂O₃ for Efficient and Selective Ethanol Conversion to Ethyl Acetate. ZrO2-Al2O3负载cu基催化剂用于乙醇高效选择性转化为乙酸乙酯。

IF 5.7

ACS Materials Au Pub Date : 2025-04-10 eCollection Date: 2025-05-14 DOI: 10.1021/acsmaterialsau.5c00017

Isabel C Freitas, Davi D Petrolini, Jean Marcel R Gallo, Paula C P Caldas, Daniela C de Oliveira, João B O Santos, Clelia Mara de Paula Marques, José Maria Correa Bueno

{"title":"Tailoring Cu-Based Catalysts Supported on ZrO2-Al2O3 for Efficient and Selective Ethanol Conversion to Ethyl Acetate.","authors":"Isabel C Freitas, Davi D Petrolini, Jean Marcel R Gallo, Paula C P Caldas, Daniela C de Oliveira, João B O Santos, Clelia Mara de Paula Marques, José Maria Correa Bueno","doi":"10.1021/acsmaterialsau.5c00017","DOIUrl":"10.1021/acsmaterialsau.5c00017","url":null,"abstract":"Selective conversion of ethanol to ethyl acetate is of significant industrial and environmental relevance, providing a sustainable route for adding value to ethanol. This study investigated Cu-based catalysts supported on ZrO2-Al2O3, focusing on the relationships among copper loading, metal-oxide interactions, and catalytic performance. Systematic variation of the copper content revealed that the Cu+/Cu0 ratio and the particle size distribution are crucial determinants of product selectivity. Lower copper loadings favored acetaldehyde production due to a higher Cu+/Cu0 ratio, while higher loadings favored Cu0 species and enhanced ethyl acetate selectivity by facilitating the formation of acyl species at the metal-oxide interface. The incorporation of ZrO2 was important for the creation of active sites necessary for condensation reactions. Advanced characterization techniques ((diffuse reflectance infrared Fourier transform spectroscopy DRIFTS)-CO, X-ray photoelectron spectroscopy (XPS), and extended X-ray absorption fine structure (EXAFS)) elucidated key electronic and structural properties, showing the need to tailor the copper loading and the composition of the support to ensure efficient and sustainable ethanol conversion.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 3","pages":"593-608"},"PeriodicalIF":5.7,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12082363/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144095059","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}

引用次数: 0

Tailoring Cu-Based Catalysts Supported on ZrO2–Al2O3 for Efficient and Selective Ethanol Conversion to Ethyl Acetate ZrO2-Al2O3负载cu基催化剂用于乙醇高效选择性转化为乙酸乙酯

IF 5.7

ACS Materials Au Pub Date : 2025-04-09 DOI: 10.1021/acsmaterialsau.5c0001710.1021/acsmaterialsau.5c00017

Isabel C. Freitas, Davi D. Petrolini, Jean Marcel R. Gallo, Paula C. P. Caldas, Daniela C. de Oliveira, João B. O. Santos, Clelia Mara de Paula Marques and José Maria CorreaBueno*,

{"title":"Tailoring Cu-Based Catalysts Supported on ZrO2–Al2O3 for Efficient and Selective Ethanol Conversion to Ethyl Acetate","authors":"Isabel C. Freitas, Davi D. Petrolini, Jean Marcel R. Gallo, Paula C. P. Caldas, Daniela C. de Oliveira, João B. O. Santos, Clelia Mara de Paula Marques and José Maria CorreaBueno*, ","doi":"10.1021/acsmaterialsau.5c0001710.1021/acsmaterialsau.5c00017","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.5c00017https://doi.org/10.1021/acsmaterialsau.5c00017","url":null,"abstract":"Selective conversion of ethanol to ethyl acetate is of significant industrial and environmental relevance, providing a sustainable route for adding value to ethanol. This study investigated Cu-based catalysts supported on ZrO2–Al2O3, focusing on the relationships among copper loading, metal–oxide interactions, and catalytic performance. Systematic variation of the copper content revealed that the Cu+/Cu0 ratio and the particle size distribution are crucial determinants of product selectivity. Lower copper loadings favored acetaldehyde production due to a higher Cu+/Cu0 ratio, while higher loadings favored Cu0 species and enhanced ethyl acetate selectivity by facilitating the formation of acyl species at the metal–oxide interface. The incorporation of ZrO2 was important for the creation of active sites necessary for condensation reactions. Advanced characterization techniques ((diffuse reflectance infrared Fourier transform spectroscopy DRIFTS)-CO, X-ray photoelectron spectroscopy (XPS), and extended X-ray absorption fine structure (EXAFS)) elucidated key electronic and structural properties, showing the need to tailor the copper loading and the composition of the support to ensure efficient and sustainable ethanol conversion.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 3","pages":"593–608 593–608"},"PeriodicalIF":5.7,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.5c00017","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940706","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}

引用次数: 0