ACS Nanoscience Au最新文献

ACS Nanoscience Au Pub Date : 2024-09-03 DOI: 10.1021/acsnanoscienceau.4c00032

Carolina Guida, Anthony Chappaz, Agnieszka Poulain, Jean-Marc Grenèche, Alexandre Gloter, Nicolas Menguy, Nathaniel Findling, Laurent Charlet

引用次数: 0

Interband and Intraband Hot Carrier-Driven Photocatalysis on Plasmonic Bimetallic Nanoparticles: A Case Study of Au–Cu Alloy Nanoparticles 等离子双金属纳米粒子的带间和带内热载流子驱动光催化：金-铜合金纳米粒子的案例研究

ACS Nanoscience Au Pub Date : 2024-08-30 DOI: 10.1021/acsnanoscienceau.4c00035

Mengqi Sun, Ankai Wang, Min Zhang, Shengli Zou, Hui Wang

{"title":"Interband and Intraband Hot Carrier-Driven Photocatalysis on Plasmonic Bimetallic Nanoparticles: A Case Study of Au–Cu Alloy Nanoparticles","authors":"Mengqi Sun, Ankai Wang, Min Zhang, Shengli Zou, Hui Wang","doi":"10.1021/acsnanoscienceau.4c00035","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00035","url":null,"abstract":"Photoexcited nonthermal electrons and holes in metallic nanoparticles, known as hot carriers, can be judiciously harnessed to drive interesting photocatalytic molecule-transforming processes on nanoparticle surfaces. Interband hot carriers are generated upon direct photoexcitation of electronic transitions between different electronic bands, whereas intraband hot carriers are derived from nonradiative decay of plasmonic electron oscillations. Due to their fundamentally distinct photogeneration mechanisms, these two types of hot carriers differ strikingly from each other in terms of energy distribution profiles, lifetimes, diffusion lengths, and relaxation dynamics, thereby exhibiting remarkably different photocatalytic behaviors. The spectral overlap between plasmon resonances and interband transitions has been identified as a key factor that modulates the interband damping of plasmon resonances, which regulates the relative populations, energy distributions, and photocatalytic efficacies of intraband and interband hot carriers in light-illuminated metallic nanoparticles. As exemplified by the Au–Cu alloy nanoparticles investigated in this work, both the resonant frequencies of plasmons and the energy threshold for the d-to-sp interband transitions can be systematically tuned in bimetallic alloy nanoparticles by varying the compositional stoichiometries and particle sizes. Choosing photocatalytic degradation of Rhodamine B as a model reaction, we elaborate on how the variation of the particle sizes and compositional stoichiometries profoundly influences the photocatalytic efficacies of interband and intraband hot carriers in Au–Cu alloy nanoparticles under different photoexcitation conditions.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142192242","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Orally Administered Silver Nanoparticles Are Absorbed and Migrate to Testes in Mice 口服纳米银粒子可被小鼠吸收并迁移至睾丸

ACS Nanoscience Au Pub Date : 2024-08-29 DOI: 10.1021/acsnanoscienceau.4c00021

Yuma Saeki, Kazuma Higashisaka, Rina Izutani, Jiwon Seo, Kazuki Miyaji, Yuya Haga, Yasuo Tsutsumi

引用次数: 0

Enhancing Electrocatalytic Semihydrogenation of Alkynes via Weakening Alkene Adsorption over Electron-Depleted Cu Nanowires 通过削弱贫电子铜纳米线对烯的吸附来增强炔烃的电催化半加氢反应

ACS Nanoscience Au Pub Date : 2024-08-08 DOI: 10.1021/acsnanoscienceau.4c00030

Dan Luo, Zhiheng Xie, Shuangqun Chen, Tianyi Yang, Yalin Guo, Ying Liu, Zhouhao Zhu, Liyong Gan, Lingmei Liu, Jianfeng Huang

{"title":"Enhancing Electrocatalytic Semihydrogenation of Alkynes via Weakening Alkene Adsorption over Electron-Depleted Cu Nanowires","authors":"Dan Luo, Zhiheng Xie, Shuangqun Chen, Tianyi Yang, Yalin Guo, Ying Liu, Zhouhao Zhu, Liyong Gan, Lingmei Liu, Jianfeng Huang","doi":"10.1021/acsnanoscienceau.4c00030","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00030","url":null,"abstract":"Electrochemical semihydrogenation (ESH) of alkynes to alkenes is an appealing technique for producing pharmaceutical precursors and polymer monomers, while also preventing catalyst poisoning by alkyne impurities. Cu is recognized as a cost-effective and highly selective catalyst for ESH, whereas its activity is somewhat limited. Here, from a mechanistic standpoint, we hypothesize that electron-deficient Cu can enhance ESH activity by promoting the rate-determining step of alkene desorption. We test this hypothesis by utilizing Cu–Ag hybrids as electrocatalysts, developed through a welding process of Ag nanoparticles with Cu nanowires. Our findings reveal that these rationally engineered Cu–Ag hybrids exhibit a notable enhancement (2–4 times greater) in alkyne conversion rates compared to isolated Ag NPs or Cu NWs, while maintaining over 99% selectivity for alkene products. Through a combination of operando and computational studies, we verify that the electron-depleted Cu sites, resulting from electron transfer between Ag nanoparticles and Cu nanowires, effectively weaken the adsorption of alkenes, thereby substantially boosting ESH activity. This work not only provides mechanistic insights into ESH but also stimulates compelling strategies involving hybridizing distinct metals to optimize ESH activity.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141937714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

CO2 Hydrogenation to Methanol over Mesoporous SiO2-Coated Cu-Based Catalysts 在介孔二氧化硅包覆铜基催化剂上将二氧化碳加氢转化为甲醇

ACS Nanoscience Au Pub Date : 2024-07-18 DOI: 10.1021/acsnanoscienceau.4c00016

Luiz H. Vieira, Marco A. Rossi, Letícia F. Rasteiro, José M. Assaf, Elisabete M. Assaf

引用次数: 0

CO2 Hydrogenation to Methanol over Mesoporous SiO2-Coated Cu-Based Catalysts 在介孔二氧化硅包覆铜基催化剂上将二氧化碳加氢转化为甲醇

IF 4.8

ACS Nanoscience Au Pub Date : 2024-07-18 DOI: 10.1021/acsnanoscienceau.4c0001610.1021/acsnanoscienceau.4c00016

Luiz H. Vieira*, Marco A. Rossi, Letícia F. Rasteiro, José M. Assaf and Elisabete M. Assaf*,

引用次数: 0

Metabolomics Analysis for Unveiling the Toxicological Mechanism of Silver Nanoparticles Using an In Vitro Gastrointestinal Digestion Model 利用体外胃肠道消化模型进行代谢组学分析以揭示银纳米粒子的毒理机制

ACS Nanoscience Au Pub Date : 2024-06-25 DOI: 10.1021/acsnanoscienceau.4c00012

Yongjiu Chen, Ruixia Wang, Ming Xu

{"title":"Metabolomics Analysis for Unveiling the Toxicological Mechanism of Silver Nanoparticles Using an In Vitro Gastrointestinal Digestion Model","authors":"Yongjiu Chen, Ruixia Wang, Ming Xu","doi":"10.1021/acsnanoscienceau.4c00012","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00012","url":null,"abstract":"The increasing use of silver nanoparticles (AgNPs) in consumer products has led to concerns about potential health risks after oral exposure as a result of the transformation and absorption in the gastrointestinal tract (GIT). However, the intricate condition of the GIT poses challenges in understanding the fate and toxicity of AgNPs as they traverse from the mouth to the rectum. For an in-depth understanding of the nanobio interactions, we employed a simulated digestion model to investigate alterations in the physicochemical properties of AgNPs in vitro. Meanwhile, we investigated the underlying toxicological mechanisms of digested AgNPs in enterocytes through metabolomics analysis. In contrast to route means that primarily apply salt solutions to mimic dietary digestion, this in vitro model is a semidynamic sequential digestion system that includes artificial oral, gastric, and intestinal fluids, which are similar to those under physiological conditions including electrolytes, enzymes, bile, pH, and time of digestion. Our results suggest that the formation of Ag–Cl and Ag–S species within the simulated digestion model can lead to an increase in the size of digested AgNPs and that the acidic condition promotes the release of Ag+ from particles. More critically, the presence of digestive enzymes and high concentrations of salt enhances the uptake of Ag by human colon enterocytes, ultimately promoting ROS generation and exacerbating cytotoxicity. Metabolomics analysis further reveals that the sequentially digested AgNPs may disorder lipid metabolism, including the biosynthesis of unsaturated fatty acids and arachidonic acid metabolism, thus increasing the possibility of ferroptosis activation in enterocytes. These findings offer significant insights into the fate and potential adverse effects of AgNPs in the GIT, providing important implications for assessing the health risks of AgNPs via oral exposure.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141510132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tuning Chemical DNA Ligation within DNA Crystals and Protein–DNA Cocrystals 调谐 DNA 晶体和蛋白质-DNA 共晶体内的化学 DNA 连接

ACS Nanoscience Au Pub Date : 2024-06-25 DOI: 10.1021/acsnanoscienceau.4c00013

Abigail R. Orun, Caroline K. Slaughter, Ethan T. Shields, Ananya Vajapayajula, Sara Jones, Rojina Shrestha, Christopher D. Snow

{"title":"Tuning Chemical DNA Ligation within DNA Crystals and Protein–DNA Cocrystals","authors":"Abigail R. Orun, Caroline K. Slaughter, Ethan T. Shields, Ananya Vajapayajula, Sara Jones, Rojina Shrestha, Christopher D. Snow","doi":"10.1021/acsnanoscienceau.4c00013","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00013","url":null,"abstract":"Biomolecular crystals can serve as materials for a plethora of applications including precise guest entrapment. However, as grown, biomolecular crystals are fragile in solutions other than their growth conditions. For crystals to achieve their full potential as hosts for other molecules, crystals can be made stronger with bioconjugation. Building on our previous work using carbodiimide 1-ethyl-3-(3-(dimethylamino)propyl)carbodiimide (EDC) for chemical ligation, here, we investigate DNA junction architecture through sticky base overhang lengths and the role of scaffold proteins in cross-linking within two classes of biomolecular crystals: cocrystals of DNA-binding proteins and pure DNA crystals. Both crystal classes contain DNA junctions where DNA strands stack up end-to-end. Ligation yields were studied as a function of sticky base overhang length and terminal phosphorylation status. The best ligation performance for both crystal classes was achieved with longer sticky overhangs and terminal 3′phosphates. Notably, EDC chemical ligation was achieved in crystals with pore sizes too small for intracrystal transport of ligase enzyme. Postassembly cross-linking produced dramatic stability improvements for both DNA crystals and cocrystals in water and blood serum. The results presented may help crystals containing DNA achieve broader application utility, including as structural biology scaffolds.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141530001","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Noble Metal Plasmon–Molecular Catalyst Hybrids for Renewable Energy Relevant Small Molecule Activation 用于可再生能源相关小分子活化的贵金属质子-分子催化剂混合体

ACS Nanoscience Au Pub Date : 2024-06-10 DOI: 10.1021/acsnanoscienceau.4c00009

Tannu Kaushik, Suchismita Ghosh, Thinles Dolkar, Rathindranath Biswas, Arnab Dutta

引用次数: 0