ACS Applied Materials & Interfaces最新文献_第6页

Sensitized Near-Infrared Emission of SiGe Nanocrystals via Heterostructuring with Quasi Two-Dimensional Perovskite

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.5c00173

Yeonjoo Lee, Doyun Kim, Mircea Cotlet, Benjamin Kyle Derby, John Watt, Wanyi Nie, Eric G. Bowes, Sundar Kunwar, Uwe R. Kortshagen, Jinkyoung Yoo

{"title":"Sensitized Near-Infrared Emission of SiGe Nanocrystals via Heterostructuring with Quasi Two-Dimensional Perovskite","authors":"Yeonjoo Lee, Doyun Kim, Mircea Cotlet, Benjamin Kyle Derby, John Watt, Wanyi Nie, Eric G. Bowes, Sundar Kunwar, Uwe R. Kortshagen, Jinkyoung Yoo","doi":"10.1021/acsami.5c00173","DOIUrl":"https://doi.org/10.1021/acsami.5c00173","url":null,"abstract":"The near-infrared (NIR) emission of silicon–germanium alloy nanocrystals (SiGe NCs) was sensitized by heterostructuring with a quasi two-dimensional (Q-2D) perovskite (CsPbBr3 blended with butylammonium bromide (BABr)). Colloidal SiGe NCs were synthesized by using a nonthermal plasma method with chloride precursors. As-synthesized SiGe NCs showed no detectable photoluminescence (PL). Embedding the SiGe NCs within the perovskite matrix via spin coating led to a heterostructure exhibiting dual emissions: green emission at 520 nm from the perovskite and NIR emission at 1035 nm from the SiGe NCs. Time-integrated and resolved PL measurements and transient absorption spectroscopy revealed energy transfer from the perovskite to the SiGe NCs, which sensitized the NIR emission from the SiGe NCs and quenched the green PL for the perovskite. These results demonstrate that Ge alloying can effectively tune the bandgap of Si NCs and highlight the feasibility of heterostructuring perovskites and photoluminescent NCs to enhance or activate their PL. This approach broadens their potential applications in the NIR region.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"48 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866952","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

High-Performance Cr8O21 Cathode Materials with MnO2 as an Activator for High-Energy-Density Lithium Primary Batteries

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.5c01226

Qingfei Meng, Rui Yang, Yuyang Qi, Peng Wang, Shuwei Zhang, Chenglong Jin, Yuliang Cao

{"title":"High-Performance Cr8O21 Cathode Materials with MnO2 as an Activator for High-Energy-Density Lithium Primary Batteries","authors":"Qingfei Meng, Rui Yang, Yuyang Qi, Peng Wang, Shuwei Zhang, Chenglong Jin, Yuliang Cao","doi":"10.1021/acsami.5c01226","DOIUrl":"https://doi.org/10.1021/acsami.5c01226","url":null,"abstract":"Chromium oxides (Cr8O21) have attracted wide application due to their high theoretical capacity and high voltage for lithium primary batteries. However, Cr8O21 is usually prepared by pyrolysis of a CrO3 precursor and suffers from low capacity and poor rate capability due to the fusion of CrO3 during the high-temperature reaction process. Herein, MnO2 was investigated as an activator to study its impact on the electrochemical properties of Cr8O21, which significantly changed with the addition of MnO2 during the calcination process. With the addition of MnO2, the discharge capacity and rate capability of the reaction products (Cr8O21-M) were dramatically improved compared with those of pure Cr8O21. This improvement is attributed to the superior lithium-ion diffusion kinetics caused by the uniform surface structure and porous features, which reduce the charge transfer resistance. As a result, Cr8O21-M10 exhibited an excellent discharge specific capacity of 388 mAh g–1 at 0.1C with discharge voltage plateaus of about 3.0 V (vs Li+/Li), reaching an energy density of 1223 Wh kg–1 based on the cathode material. In addition, Cr8O21-M showed remarkable rate performance, enabling a high-capacity retention of about 70% at 5C. Therefore, it is essential to add an activator agent during the preparation of Cr8O21, which offers a promising avenue for the development of high-energy-density and high-rate-capability Li/Cr8O21 primary batteries.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"138 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866425","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

In Situ Synthesis of Plasticized Bacterial Cellulose Films for Daily Packaging Using Biobased Plasticizers

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.5c03851

Yihai Yan, Guoqiang Chen, Yibing Zhang, Wenxue Dai, Shuaijun Deng, Shagufta Afreen, Lei Wang, Haibo Zhang

{"title":"In Situ Synthesis of Plasticized Bacterial Cellulose Films for Daily Packaging Using Biobased Plasticizers","authors":"Yihai Yan, Guoqiang Chen, Yibing Zhang, Wenxue Dai, Shuaijun Deng, Shagufta Afreen, Lei Wang, Haibo Zhang","doi":"10.1021/acsami.5c03851","DOIUrl":"https://doi.org/10.1021/acsami.5c03851","url":null,"abstract":"Bacterial cellulose (BC) naturally decomposes in the environment without releasing toxins or microplastics, making it a promising alternative to conventional plastics. However, its inherent brittleness after drying limits its broader application. This study investigates four biobased plasticizers─epoxy soybean oil, castor oil, tributyl citrate (TBC), and tributyl trans-aconitate (TBA)─to enhance the flexibility of BC through in situ modification. By combining a gel-assisted biosynthesis with an in situ spray plasticization method, biobased plasticizers are uniformly incorporated into the nanofiber network of BC, resulting in films with significantly improved flexibility and transparency. Among the biobased plasticizers, TBC and TBA showed the most effective plasticization, increasing the E% to 9.63 and 11.90%, respectively, corresponding to 6.3-fold and 7.5-fold enhancements compared to the control. This approach not only improves the mechanical properties of BC but also streamlines production by enabling a simplified processing method. The findings underscore the potential of plasticized BC biomaterials in replacing fossil-based plastics and advancing the development of sustainable materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"108 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Greatly Enhanced Radiative Recombination at High Exciton Density in Acid-Treated 2D Alloy

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.4c18618

Matej Sebek, Gang Wu, Zeng Wang, Michael Sullivan, Debbie Hwee Leng Seng, Xiao Di Su, Nguyen Thi Kim Thanh, Jinghua Teng

{"title":"Greatly Enhanced Radiative Recombination at High Exciton Density in Acid-Treated 2D Alloy","authors":"Matej Sebek, Gang Wu, Zeng Wang, Michael Sullivan, Debbie Hwee Leng Seng, Xiao Di Su, Nguyen Thi Kim Thanh, Jinghua Teng","doi":"10.1021/acsami.4c18618","DOIUrl":"https://doi.org/10.1021/acsami.4c18618","url":null,"abstract":"Enhanced photoluminescence (PL) in transition metal dichalcogenides (TMDs) is critical for their application in optoelectronics. In this study, we report a 99 × PL enhancement in a superacid bis(trifluoromethane) sulfonimide (TFSI)-treated MoS2(1–x)Se2x alloy. The alloy’s optical bandgap is tunable by changing its stoichiometry, allowing for PL enhancement at tailored positions. The PL enhancement is robust even at high excitation power, overcoming the limitation of exciton–exciton annihilation observed in MoS2. Through molecular dynamics simulations and spectroscopic analysis, we demonstrate that the MoS2(1–x)Se2x monolayer inherently exhibits moderate strain, which shifts the van Hove singularity in the S-rich domain. Furthermore, density functional theory calculations reveal the absence of a pronounced van Hove feature in the alloy configuration. Our findings extend the range of materials amenable to superacid treatment and open new avenues for optoelectronic applications, particularly those requiring high excitation powers.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"9 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862395","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Ferroelectric α-In2Se3 Semi-floating Gate Transistors for Multilevel Memory and Optoelectronic Logic Gate 用于多级存储器和光电逻辑门的铁电 α-In2Se3 半浮栅晶体管

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.5c01586

Yanze Song, Zhidong Pan, Chengming Luo, Yue Wang, Tao Zheng, Yuan Pan, Nabuqi Bu, Ruiyang Xu, Nengjie Huo

{"title":"Ferroelectric α-In2Se3 Semi-floating Gate Transistors for Multilevel Memory and Optoelectronic Logic Gate","authors":"Yanze Song, Zhidong Pan, Chengming Luo, Yue Wang, Tao Zheng, Yuan Pan, Nabuqi Bu, Ruiyang Xu, Nengjie Huo","doi":"10.1021/acsami.5c01586","DOIUrl":"https://doi.org/10.1021/acsami.5c01586","url":null,"abstract":"Progress in artificial intelligence (AI) demands efficient data storage and high-speed processing. Traditional von Neumann architecture, with space separation of memory and computing units, struggles with increased data transmission, causing power inefficiency and date latency. To address this challenge, we designed a semi-floating gate transistor (SFGT) that integrates data storage and logical operation into a single device by employing a ferroelectric semiconductor α-In2Se3 as a semi-floating gate layer. Leveraging the ferroelectric polarization of α-In2Se3, the device exhibits improved non-volatile memory performance with a high program/erase ratio of 1 × 106 and reliable durability over 1000 cycles. Through the dual-gate modulation, the SFGT achieves multilevel storage function with at least seven controllable programming states and performs three types of digital logic gate operations (“AND”, “NOR”, and “OR”) at an ultralow bias of 10 mV. Compared to traditional FGT architectures, the α-In2Se3-based semi-floating gate structure achieves multifunctional integration of data storage and logic computing, effectively addressing energy consumption and time delay issues in data transmission, making it highly significant for applications in data-intensive and low-power integrated circuits.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"6 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866791","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Synergistic Cu2O@Ni(OH)2 Core–Shell Electrocatalyst for High-Efficiency Nitrate Reduction to Ammonia

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.4c22282

Zunjie Zhang, Bingcheng Ge, Mengran Liu, Tianfang Yang, Shuaitong Wang, Yang Liu, Yingjie Yang, Shuyan Gao

{"title":"Synergistic Cu2O@Ni(OH)2 Core–Shell Electrocatalyst for High-Efficiency Nitrate Reduction to Ammonia","authors":"Zunjie Zhang, Bingcheng Ge, Mengran Liu, Tianfang Yang, Shuaitong Wang, Yang Liu, Yingjie Yang, Shuyan Gao","doi":"10.1021/acsami.4c22282","DOIUrl":"https://doi.org/10.1021/acsami.4c22282","url":null,"abstract":"The electrocatalytic reduction reaction of nitrate (NO3RR) is anticipated to convert nitrogen-containing pollutants into valuable ammonia products. Copper-based catalysts have received great attention because of their good performance in the NO3RR due to the strong binding energy with *NO3 intermediates. However, the poor H2O dissociation ability of Cu is unable to provide H• in time for the hydrogenation reaction of NOx, thus hindering the electroreduction of the NO3–. Herein, we designed a shell–core nanocube electrocatalyst Cu2O@Ni(OH)2-x (x represents the molar ratio of Ni/Cu) using the liquid phase reduction combined with the etching and precipitation method for electrocatalytic NO3RR. Due to the synergistic effect between the strong nitrate activation ability of Cu and the excellent H2O dissociation ability of Ni(OH)2, Cu2O@Ni(OH)2-3.3% shows an impressive ammonia yield rate (557.9 μmol h–1 cm–2) and Faradaic efficiency (97.4%) at −0.35 V vs. RHE. Operando Raman and Auger electron spectroscopy observe the reduction of Cu2O to Cu during the NO3RR process. Density functional theory calculations combined with electron paramagnetic resonance analysis reveals that Ni(OH)2 can lower the activation energy barrier of H2O dissociation, thereby promoting the generation of H• and accelerating the hydrogenation of *NO during the NO3RR. This research provides an efficient Cu-based catalyst for reducing NO3– and may motivate the development of effective ammonia electrocatalysts for further experimentation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"52 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866423","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Advances in the Development and Application of δ-Bi2O3-Based Ionic Conductors for Ceramic Electrochemical Cells

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.4c21320

Incheol Jeong, Hyeongmin Yu, Donghun Lee, Ki-Min Roh, Eric D. Wachsman, Kang Taek Lee

{"title":"Advances in the Development and Application of δ-Bi2O3-Based Ionic Conductors for Ceramic Electrochemical Cells","authors":"Incheol Jeong, Hyeongmin Yu, Donghun Lee, Ki-Min Roh, Eric D. Wachsman, Kang Taek Lee","doi":"10.1021/acsami.4c21320","DOIUrl":"https://doi.org/10.1021/acsami.4c21320","url":null,"abstract":"The increasing demand for sustainable energy solutions has driven interest in ceramic electrochemical cells, which are also known as solid oxide electrochemical cells, for high-efficiency power generation and hydrogen production. Ceramic electrochemical cells offer fuel flexibility and reduced CO2 emissions. However, high operating temperatures (>700 °C) result in higher costs and performance degradation. Efforts to lower the operating temperatures have led to advancements in materials, particularly Bi2O3-based ionic conductors, which are known for their superior oxygen ion conductivity. Despite their potential, Bi2O3-based materials suffer from instability at the expense of facile ionic transport. This review examines recent research addressing these challenges, focusing on intrinsic properties, chemical compositions, cell designs, and fabrication methods to improve the stability and performance. Additionally, the potential of incorporating Bi3+ into other oxides is explored. The discussion and summary in this review aim to guide the rational design of ceramic electrochemical cells operating at low temperatures with Bi2O3-based ionic conductors.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"7 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Metal Oxide–Metal Organic Framework Layers for Discrimination of Multiple Gases Employing Machine Learning Algorithms

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.5c02081

Alishba T. John, Jing Qian, Qi Wang, Fabian S. Garay-Rairan, Y. M. Nuwan D. Y. Bandara, Artem Lensky, Krishnan Murugappan, Hanna Suominen, Antonio Tricoli

{"title":"Metal Oxide–Metal Organic Framework Layers for Discrimination of Multiple Gases Employing Machine Learning Algorithms","authors":"Alishba T. John, Jing Qian, Qi Wang, Fabian S. Garay-Rairan, Y. M. Nuwan D. Y. Bandara, Artem Lensky, Krishnan Murugappan, Hanna Suominen, Antonio Tricoli","doi":"10.1021/acsami.5c02081","DOIUrl":"https://doi.org/10.1021/acsami.5c02081","url":null,"abstract":"The increasing demand for gas molecule detection emphasizes the need for portable sensor devices possessing selectivity, a low limit of detection (LOD), and a large dynamic range. Despite substantial progress in developing nanostructured sensor materials with heightened sensitivity, achieving sufficient selectivity remains a challenge. Here, we introduce a strategy to enhance the performance of chemiresistive gas sensors by combining an advanced sensor design with machine learning (ML). Our sensor architecture consists of a tungsten oxide (WO3) nanoparticle network, as the primary sensing layer, with an integrated zeolitic imidazolate framework (ZIF-8) membrane layer, used to induce a gas-specific delay to the diffusion of analytes, sharing conceptual similarities to gas chromatography. However, the miniaturized design and chemical activity of the ZIF-8 results in a nontrivial impact of the ZIF-8 membrane on the target analyte diffusivity and sensor response. An ML method was developed to evaluate the response dynamics with a panel of relevant analytes including acetone, ethanol, propane, and ethylbenzene. Our advanced sensor design and ML algorithm led to an excellent capability to determine the gas molecule type and its concentration, achieving accuracies of 97.22 and 86.11%, respectively, using a virtual array of 4 sensors. The proposed ML method can also reduce the necessary sensing time to only 5 s while maintaining an accuracy of 70.83%. When compared with other ML methods in the literature, our approach also gave superior performance in terms of sensitivity, specificity, precision, and F1-score. These findings show a promising approach to overcome a longstanding challenge of the highly miniaturized but poorly selective semiconductor sensor technology, with impact ranging from environmental monitoring to explosive detection and health care.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"19 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866429","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Complexity at a Humid Interface: Throwing Fresh Light on Atmospheric Corrosion

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.4c21013

Michael Dowhyj, Kiran Kousar, Francis P. Lydiatt, Dimitri Chekulaev, Monika S. Walczak, Robert Temperton, James N.O’Shea, W. Stephen Walters, Andrew G. Thomas, Robert Lindsay

{"title":"Complexity at a Humid Interface: Throwing Fresh Light on Atmospheric Corrosion","authors":"Michael Dowhyj, Kiran Kousar, Francis P. Lydiatt, Dimitri Chekulaev, Monika S. Walczak, Robert Temperton, James N.O’Shea, W. Stephen Walters, Andrew G. Thomas, Robert Lindsay","doi":"10.1021/acsami.4c21013","DOIUrl":"https://doi.org/10.1021/acsami.4c21013","url":null,"abstract":"Atmospheric corrosion of metals arising from exposure to water vapor is a pervasive problem across a wide range of practical scenarios, including nuclear material storage and historical artifact conservation. Frequently, it is hypothesized that this phenomenon becomes an issue once the number of monolayers of water growing atop a substrate is sufficient to facilitate corrosion chemistry, but supporting evidence remains scarce. We apply both near ambient pressure X-ray photoelectron spectroscopy and vibrational sum frequency spectroscopy to further elucidate the interaction of water vapor with zinc, a common engineering substrate for corrosion protection applications. Data acquired as a function of relative humidity indicate that water sorption is much more complex than expected, involving micropore filling and capillary condensation in the adventitious carbon layer covering the zinc surface. These results suggest that current mechanistic models for atmospheric corrosion, as well as other interfacial phenomena occurring in humid environments, require extensive revision and should embrace explicit consideration of the role of surface carbon contamination.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"26 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862639","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Design and Biodistribution of PEGylated Core–Shell X-ray Fluorescent Nanoparticle Contrast Agents

IF 9.5 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-04-23 DOI: 10.1021/acsami.5c01902

Giovanni M. Saladino, Bertha Brodin, Mihai Ciobanu, Nuzhet I. Kilic, Muhammet S. Toprak, Hans M. Hertz

{"title":"Design and Biodistribution of PEGylated Core–Shell X-ray Fluorescent Nanoparticle Contrast Agents","authors":"Giovanni M. Saladino, Bertha Brodin, Mihai Ciobanu, Nuzhet I. Kilic, Muhammet S. Toprak, Hans M. Hertz","doi":"10.1021/acsami.5c01902","DOIUrl":"https://doi.org/10.1021/acsami.5c01902","url":null,"abstract":"Nanoparticle (NP) uptake by macrophages and their accumulation in undesired organs such as the liver and spleen constitute a major barrier to the effective delivery of NPs to targeted tissues for bioimaging and therapeutics. Surface functionalization with polyethylene glycol (PEG) has been demonstrated to be a promising strategy to limit NP sequestration, although its longitudinal stability under physiological conditions and impact on the NP biodistribution have not been investigated with an in vivo quantitative approach. X-ray fluorescence (XRF) imaging has been employed to noninvasively map the in vivo biodistribution of purposely designed molybdenum-based contrast agents, leading to submillimeter resolution, elemental specificity, and high penetration depth. In the present work, we design a stepwise layering approach for NP synthesis to investigate the role of chemisorbed and physisorbed PEG on silica-coated molybdenum-based contrast agents in affecting their in vivo biodistribution, using whole-body XRF imaging. Comparative quantitative in vivo studies indicated that physisorbed PEG (1.5 kDa) did not substantially affect the biodistribution, while the chemisorption route with mPEG-Si (6–9 PEG units) led to significant macroscopic variations in the biodistribution, leading to a reduction in NP uptake by the liver. Furthermore, the results highlighted the major role of the spleen in compensating for the limited sequestration by the liver, microscopically validated with a multiscale imaging approach with fluorophore doping of the silica shell. These findings demonstrated the promising role of XRF imaging for the rapid assessment of surface-functionalized contrast agents with whole-body in vivo quantitative pharmacokinetic studies, establishing the groundwork for developing strategies to identify and bypass undesired NP uptake.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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