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Site-Specific Stochastic Rates and Energetics of Ag Nucleation on Highly Ordered Pyrolytic Graphite. 高有序热解石墨上银成核的特定位点随机速率和能量学。
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2024-11-14 DOI: 10.1021/acsnano.4c09981
Iván Elías Mondaca-Medina, Hang Ren
{"title":"Site-Specific Stochastic Rates and Energetics of Ag Nucleation on Highly Ordered Pyrolytic Graphite.","authors":"Iván Elías Mondaca-Medina, Hang Ren","doi":"10.1021/acsnano.4c09981","DOIUrl":"https://doi.org/10.1021/acsnano.4c09981","url":null,"abstract":"<p><p>Nucleation is a fundamentally important step in electrochemical phase transition reactions, e.g., in electrodeposition, which is pertinent for emerging battery technology, nanoparticle synthesis, and many industrial processes. Surface defects have been suggested to enhance nucleation rates. However, directly quantifying the nucleation rates at specific surface sites is challenging due to the ensemble averaging effect in bulk measurements. Herein, we report the measurement of rates and energetics of electronucleation across the model surface of highly oriented pyrolytic graphite (HOPG). Specifically, scanning electrochemical cell microscopy (SECCM) is used to confine the nucleation spatially in the nanoscale cell, allowing one nucleation event to be measured at one time. The scanning capability further allows the mapping of Ag nucleation at the step edge vs basal plane. A stochastic model is developed to extract the nucleation rate and energetics from voltammetric experiments. We observed a ∼57 mV difference in the median nucleation overpotential between the step edge and basal plane, corresponding to a ∼12 kJ mol<sup>-1</sup> difference in the nucleation energy barrier. The voltammetric method to measure the nucleation rate explored here can be extended to understand the heterogeneity of nucleation rates in other electrochemical nucleation systems, e.g., metal anode batteries.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612752","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Increased Formation of Trions and Charged Biexcitons by Above-Gap Excitation in Single-layer WSe2 单层 WSe2 在隙外激发下形成更多的三离子和带电双激子
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2024-11-14 DOI: 10.1021/acsnano.4c13208
Matthew C. Strasbourg, Emanuil S. Yanev, Sheikh Parvez, Sajia Afrin, Cory Johns, Zoe Noble, Thomas P. Darlington, Erik M. Grumstrup, James C. Hone, P. James Schuck, Nicholas J. Borys
{"title":"Increased Formation of Trions and Charged Biexcitons by Above-Gap Excitation in Single-layer WSe2","authors":"Matthew C. Strasbourg, Emanuil S. Yanev, Sheikh Parvez, Sajia Afrin, Cory Johns, Zoe Noble, Thomas P. Darlington, Erik M. Grumstrup, James C. Hone, P. James Schuck, Nicholas J. Borys","doi":"10.1021/acsnano.4c13208","DOIUrl":"https://doi.org/10.1021/acsnano.4c13208","url":null,"abstract":"Two-dimensional semiconductors exhibit pronounced many-body effects and intense optical responses due to strong Coulombic interactions. Consequently, subtle differences in photoexcitation conditions can strongly influence how the material dissipates energy during thermalization. Here, using multiple excitation spectroscopies, we show that a distinct thermalization pathway emerges at elevated excitation energies, enhancing the formation of trions and charged biexcitons in single-layer WSe<sub>2</sub> by up to 2× and 5× , respectively. Power- and temperature-dependent measurements lend insights into the origin of the enhancement. These observations underscore the complexity of excited state relaxation in monolayer semiconductors, provide insights for the continued development of carrier thermalization models, and highlight the potential to precisely control excitonic yields and probe nonequilibrium dynamics in 2D semiconductors.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"43 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610584","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanical Writing of Polar Skyrmionic Topological States via Extrinsic Dzyaloshinskii-Moriya-like Flexoelectricity in Ferroelectric Thin Films. 通过铁电薄膜中的外在 Dzyaloshinskii-Moriya 类柔电性实现极性 Skyrmionic 拓扑状态的机械写入。
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2024-11-14 DOI: 10.1021/acsnano.4c06137
Kohta Kasai, Takashi Nojima, Yu Wang, Tao Xu, Hiroyuki Hirakata, Takahiro Shimada
{"title":"Mechanical Writing of Polar Skyrmionic Topological States via Extrinsic Dzyaloshinskii-Moriya-like Flexoelectricity in Ferroelectric Thin Films.","authors":"Kohta Kasai, Takashi Nojima, Yu Wang, Tao Xu, Hiroyuki Hirakata, Takahiro Shimada","doi":"10.1021/acsnano.4c06137","DOIUrl":"10.1021/acsnano.4c06137","url":null,"abstract":"<p><p>Exploring complex topological structures in condensed matter has shown promising applications in nanotechnology. Although polar topologies such as chiral vortices and skyrmions have been observed in ferroelectric heterostructures, their existence in simple systems has posed challenges due to the absence of intrinsic noncollinear interaction (like Dzyaloshinskii-Moriya interaction in ferromagnetics). Here, we demonstrate that a nanoindentation mechanically switches local polarizations to stable polar topologies, including skyrmions, within a room-temperature PbTiO<sub>3</sub> thin film via the flexoelectric effect as a noncollinear (Dzyaloshinskii-Moriya-like) driving force using phase-field simulations. In addition, by moving the indenter, the continuous polarization switching leads to the \"writing\" of arbitrary polar patterns (such as donut-like skyrmionium). Furthermore, the written topologies can be \"erased\" by applying a voltage with the same conducted indenter. Therefore, this study shows the writing and erasing process of room-temperature polar topologies in a ferroelectric thin film, which significantly advances their potential applications.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612750","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Supramolecular Self-Assembled Nanoprodrug for Enhanced Ferroptosis Therapy. 用于增强铁中毒疗法的超分子自组装纳米药物
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2024-11-14 DOI: 10.1021/acsnano.4c09254
Zhengwei Yu, Xin Xie, Qing Li, Yong Huang, Siqin Chen, Wentao Song, Jianwu Tian, Zhiyao Li, Chongzhi Wu, Bowen Li
{"title":"A Supramolecular Self-Assembled Nanoprodrug for Enhanced Ferroptosis Therapy.","authors":"Zhengwei Yu, Xin Xie, Qing Li, Yong Huang, Siqin Chen, Wentao Song, Jianwu Tian, Zhiyao Li, Chongzhi Wu, Bowen Li","doi":"10.1021/acsnano.4c09254","DOIUrl":"https://doi.org/10.1021/acsnano.4c09254","url":null,"abstract":"<p><p>Ferroptosis can induce cell death that leverages Fe<sup>2+</sup>-triggered Fenton reactions within living organisms, leading to an excessive accumulation of lipid peroxides (LPOs) and inducing cell death. Ferroptosis can effectively circumvent the inevitable drug resistance encountered with traditional apoptotic therapies. However, several issues remain in the clinical application of ferroptosis anticancer therapy, primarily due to the poor efficiency of intracellular Fenton reaction. To address this issue, we developed a supramolecular self-assembled codelivery nanoprodrug (DOX@C18Fc-Q[7] NPs) composed of ferrocene (Fc)-based supramolecular amphiphiles (C18Fc-Q[7]) and a nicotinamide adenine dinucleotide phosphate oxidase 4 (NOX4) activator (doxorubicin, DOX). The C18Fc-Q[7] is based on Fc linked to a hydrophobic long-chain alkane via a disulfide linkage, which interacts with hydrophilic Q[7] to form self-assembled amphiphiles. Importantly, the host-guest interaction between Q[7] and Fc effectively enhances the solubility of Fc while maintaining the stability of the Fe<sup>2+</sup> source. Moreover, C18Fc-Q[7] also acts as a good carrier for loading DOX due to its good self-assembly. In cancer cells, elevated glutathione (GSH) triggers the disassembly of nanoprodrug, leading to the release of DOX, which upregulates NOX4 expression and increases H<sub>2</sub>O<sub>2</sub> level, thereby promoting an efficient Fenton reaction for Fc-induced ferroptosis. Moreover, DOX induces cell death through apoptosis, providing a synergistic effect to further enhance the ferroptosis therapy. <i>In vivo</i> studies have demonstrated that this enhanced ferroptosis therapy effectively inhibits tumor growth and metastasis while maintaining good biosafety.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612746","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Turn Hood into Good: Recycling Silicon from Mesoporous Silica Nanoparticles through Magnesium Modification to Lower Toxicity and Promote Tissue Regeneration. 化腐朽为神奇:通过镁改性从介孔二氧化硅纳米颗粒中回收硅,以降低毒性并促进组织再生。
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2024-11-14 DOI: 10.1021/acsnano.4c12519
Guanqi Liu, Ruidi Xia, Mixiao Gui, Linjun Zhang, Xuan Zhou, Junlong Xue, Yihua Cai, Yang Cao, Yin Xiao, Zetao Chen
{"title":"Turn Hood into Good: Recycling Silicon from Mesoporous Silica Nanoparticles through Magnesium Modification to Lower Toxicity and Promote Tissue Regeneration.","authors":"Guanqi Liu, Ruidi Xia, Mixiao Gui, Linjun Zhang, Xuan Zhou, Junlong Xue, Yihua Cai, Yang Cao, Yin Xiao, Zetao Chen","doi":"10.1021/acsnano.4c12519","DOIUrl":"https://doi.org/10.1021/acsnano.4c12519","url":null,"abstract":"<p><p>Mesoporous silica nanoparticles (MSNs) have gained wide application as excellent carrier materials; however, their limited degradation in the biological system and potential chronic toxicity pose challenges to their clinical applications. Previous studies have focused on optimizing the elimination performance of MSNs; interestingly, silicon has been well-documented as an essential body component. Therefore, converting MSNs into a form readily utilizable by the organism is a way to turn waste into a valuable resource. However, the recycling and utilization of MSNs are associated with significant hurdles. This study proposes an approach to impede the formation of siloxane, the crucial core in MSNs, by introducing a gradient concentration of Mg<sup>2+</sup>. The invasion of Mg<sup>2+</sup> significantly reduces the stability of Si-O-Si bonds by substituting silicon ions while preserving the functional three-dimensional structure. Recycling the increased release of Mg and Si ions enhances cellular antioxidant capacity, reduces oxidative stress reactions, improves mitochondrial function, and regulates macrophage inflammatory states. The proposed approach to converting MSN materials shows significant advantages for tissue regeneration in the periodontal defect model. This study opens an insight for applying MSNs in clinical applications in regenerative medicine.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612754","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interfacial Charge Transfer in One-Dimensional AgBr Encapsulated inside Single-Walled Carbon Nanotube Heterostructures 单壁碳纳米管异质结构中封装的一维 AgBr 的界面电荷转移
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2024-11-13 DOI: 10.1021/acsnano.4c09474
Tian Che, Shuai Liu, Yatong Wang, Pin Zhao, Chengpeng Yang, Xiaohang Pan, Hongze Ji, Lin Geng, Qiong Sun, Ziyi Hu, Alei Li, Chengxu Zhou, Li-Chun Xu, Yunlei Zhong, Dan Tian, Yong Yang, Lixing Kang
{"title":"Interfacial Charge Transfer in One-Dimensional AgBr Encapsulated inside Single-Walled Carbon Nanotube Heterostructures","authors":"Tian Che, Shuai Liu, Yatong Wang, Pin Zhao, Chengpeng Yang, Xiaohang Pan, Hongze Ji, Lin Geng, Qiong Sun, Ziyi Hu, Alei Li, Chengxu Zhou, Li-Chun Xu, Yunlei Zhong, Dan Tian, Yong Yang, Lixing Kang","doi":"10.1021/acsnano.4c09474","DOIUrl":"https://doi.org/10.1021/acsnano.4c09474","url":null,"abstract":"The advent of one-dimensional van der Waals heterostructure (1D vdWH) nanomaterials has provided valuable opportunities for the advancement of electronic or optical devices, as well as for exploring various condensed matter phenomena. Electron transfer is a fundamental process in host–guest interactions, significantly influencing nanoscale physicochemical processes. Elucidating the mechanism by which the host influences the electronic structure of the guest is essential for elucidating these interactions. This study reports the successful synthesis of a material system consisting of precisely resolved AgBr nanowires encapsulated within single-walled carbon nanotubes (SWCNTs) that has been successfully synthesized and utilized to investigate the intrinsic electron transfer across 1D vdWHs. Cyclic voltammetry (CV) was employed to investigate the 1D vdWH interaction between AgBr and SWCNTs, which provided a more intuitive and accurate characterization of the charge transfer from SWCNTs to AgBr. Furthermore, Kelvin probe force microscopy showed a 149 mV reduction in the average surface potential of carbon nanotubes after AgBr filling, supporting the efficacy of CV in probing electron dynamics in 1D vdWHs. Finally, theoretical calculations indicated a charge transfer of 0.11 e<sup>–</sup> per simulation cell, reinforcing the effectiveness of CV in assessing the interactions within 1D vdWHs.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"72 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhanced Control of Single-Molecule Emission Frequency and Spectral Diffusion 增强对单分子发射频率和光谱扩散的控制
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2024-11-13 DOI: 10.1021/acsnano.4c08382
Rocco Duquennoy, Simon Landrieux, Daniele De Bernardis, Juergen Mony, Maja Colautti, Lin Jin, Wolfram H.P. Pernice, Costanza Toninelli
{"title":"Enhanced Control of Single-Molecule Emission Frequency and Spectral Diffusion","authors":"Rocco Duquennoy, Simon Landrieux, Daniele De Bernardis, Juergen Mony, Maja Colautti, Lin Jin, Wolfram H.P. Pernice, Costanza Toninelli","doi":"10.1021/acsnano.4c08382","DOIUrl":"https://doi.org/10.1021/acsnano.4c08382","url":null,"abstract":"The Stark effect provides a powerful method to shift the spectra of molecules, atoms, and electronic transitions in general, becoming one of the simplest and most straightforward ways to tune the frequency of quantum emitters by means of a static electric field. At the same time, in order to reduce the emitter sensitivity to charge noise, inversion symmetric systems are typically designed, providing a stable emission frequency with a quadratic-only dependence on the applied field. However, such nonlinear behavior might be reflected in correlations between the tuning ability and unwanted spectral fluctuations. Here, we provide experimental evidence of this trend using molecular quantum emitters in the solid state cooled down to liquid helium temperatures. We finally combine the electric field generated by electrodes, which is parallel to the molecule’s induced dipole, with optically excite long-lived charge states acting in the perpendicular direction. Based on the anisotropy of the molecule’s polarizability, our two-dimensional control of the local electric field allows us not only to tune the emitter’s frequency but also to sensibly suppress the spectral instabilities associated with field fluctuations.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"11 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609856","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Correction to “Antibiotic-Like Activity of Atomic Layer Boron Nitride for Combating Resistant Bacteria” 对 "原子层氮化硼的抗生素类活性可用于抗击耐药细菌 "的更正
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2024-11-13 DOI: 10.1021/acsnano.4c14729
Yanxia Pan, Huizhen Zheng, Guanna Li, Yanan Li, Jie Jiang, Jie Chen, Qianqian Xie, Di Wu, Ronglin Ma, Xi Liu, Shujuan Xu, Jun Jiang, Xiaoming Cai, Meng Gao, Weili Wang, Han Zuilhof, Mingliang Ye, Ruibin Li
{"title":"Correction to “Antibiotic-Like Activity of Atomic Layer Boron Nitride for Combating Resistant Bacteria”","authors":"Yanxia Pan, Huizhen Zheng, Guanna Li, Yanan Li, Jie Jiang, Jie Chen, Qianqian Xie, Di Wu, Ronglin Ma, Xi Liu, Shujuan Xu, Jun Jiang, Xiaoming Cai, Meng Gao, Weili Wang, Han Zuilhof, Mingliang Ye, Ruibin Li","doi":"10.1021/acsnano.4c14729","DOIUrl":"https://doi.org/10.1021/acsnano.4c14729","url":null,"abstract":"We identified an error in our recent publication. Specifically, two H&amp;E images were erroneously uploaded in the lung tissue panel (ctrl group) of Figure 3D and heart tissue panel (Ag NP group by oropharyngeal instillation) of Figure S5. The corrected images are provided below. This error does not alter any of the reported results, interpretations, or conclusions of the study. This article has not yet been cited by other publications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"5 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609859","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Correction to“Simultaneous Mapping of the Nanoscale Organization and Redox State of Extracellular Space in Living Brain Tissue” 对 "同时绘制活体脑组织细胞外空间的纳米级组织和氧化还原状态图 "的更正
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2024-11-13 DOI: 10.1021/acsnano.4c15022
Hua-Jie Chen, Liang Zhao, Lei Wang, Zhi-Gang Wang, Dai-Wen Pang, Shu-Lin Liu
{"title":"Correction to“Simultaneous Mapping of the Nanoscale Organization and Redox State of Extracellular Space in Living Brain Tissue”","authors":"Hua-Jie Chen, Liang Zhao, Lei Wang, Zhi-Gang Wang, Dai-Wen Pang, Shu-Lin Liu","doi":"10.1021/acsnano.4c15022","DOIUrl":"https://doi.org/10.1021/acsnano.4c15022","url":null,"abstract":"Page 22254. The corresponding and first authors’ affiliations are corrected as follows and in the Author Information of this Correction: Engineering Research Center of Nano-Geomaterials of Ministry of Education, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, P. R, China; State Key Laboratory of Medicinal Chemical Biology, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Research Center for Analytical Sciences, College of Chemistry, and School of Medicine, Nankai University, Tianjin 300071, P. R. China. The conclusions of this work have not been affected. This article has not yet been cited by other publications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"34 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Oxide-Perovskites for Automotive Catalysts Biotransform and Induce Multicomponent Clearance and Hazard 用于汽车催化剂的氧化物-超微晶石 生物转化和诱导多组分清除与危害
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2024-11-13 DOI: 10.1021/acsnano.4c10135
Veronica Di Battista, Pernille Høgh Danielsen, Agnieszka Gajewicz-Skretna, Andrzej Kedziorski, Svenja B. Seiffert, Lan Ma-Hock, Trine Berthing, Alicja Mortensen, Andreas Sundermann, Lars Michael Skjolding, Ulla Vogel, Anders Baun, Wendel Wohlleben
{"title":"Oxide-Perovskites for Automotive Catalysts Biotransform and Induce Multicomponent Clearance and Hazard","authors":"Veronica Di Battista, Pernille Høgh Danielsen, Agnieszka Gajewicz-Skretna, Andrzej Kedziorski, Svenja B. Seiffert, Lan Ma-Hock, Trine Berthing, Alicja Mortensen, Andreas Sundermann, Lars Michael Skjolding, Ulla Vogel, Anders Baun, Wendel Wohlleben","doi":"10.1021/acsnano.4c10135","DOIUrl":"https://doi.org/10.1021/acsnano.4c10135","url":null,"abstract":"Oxide-perovskites designed for automotive catalysts contain multiple metal elements whose presence is crucial to achieving the targeted performance. They are highly stable in exhaust operating conditions; however, little is known about their stability under physiological conditions. As some of the metallic components are hazardous to humans and the environment, perovskite benefits in cleaner air must be balanced with risks in a Safe and Sustainable Design (SSbD) approach. New approach methodologies (NAMs), including in chemico and in silico methods, were used for testing hazards and benefits, including catalytic activity and tolerance for temporary excess of oxygen under dynamic driving conditions. The composition and surface properties of six different lanthanum-based oxide-perovskites compromised their stability under lung physiological conditions, influencing the oxidative damage of the particles and the bioacessibility of leaching metals. We found consistent biotransformation of the oxide-perovskite materials at pH 4.5. The leached lanthanum ions, but not other metals, respeciated into lanthanum phosphate nanoparticles, which increased the overall oxidative damage in additive synergy. The NAM results in the presented SSbD approach were challenged by in vivo studies in rats and mice, which confirmed multicomponent clearance from lungs into urine and supported the comparative ranking of effects against well-characterized spinel materials. Among the perovskites, the version with reduced nickel content and doped with palladium offered the best SSbD balance, despite not improving the conventional benchmark catalytic performance and related sustainability benefits. Redesign by industry may be necessary to better fulfill all SSbD dimensions.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"16 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609860","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","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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