ACS Earth and Space Chemistry最新文献

{"title":"Spleen-Targeted mRNA Vaccine Doped with Manganese Adjuvant for Robust Anticancer Immunity In Vivo","authors":"Zijin Luo,&nbsp;Yi Lin,&nbsp;Yanan Meng,&nbsp;Mengyao Li,&nbsp;Hongyu Ren,&nbsp;Haoping Shi,&nbsp;Qiang Cheng* and Tuo Wei*,&nbsp;","doi":"10.1021/acsnano.4c0990210.1021/acsnano.4c09902","DOIUrl":"https://doi.org/10.1021/acsnano.4c09902https://doi.org/10.1021/acsnano.4c09902","url":null,"abstract":"<p >The successful application of mRNA vaccines in preventing and treating infectious diseases highlights their potential as therapeutic vaccines for cancer treatment. However, unlike infectious diseases, effective antitumor therapy, particularly for solid tumors, necessitates the activation of more powerful cellular and humoral immunity to achieve clinical efficacy. Here, we report a spleen-targeted mRNA vaccine (Mn@mRNA-LNP) designed to deliver tumor antigen-encoding mRNA and manganese adjuvant (Mn²⁺) simultaneously to dendritic cells (DCs) in the spleen. This delivery system promotes DC maturation and surface antigen presentation and stimulates the production of cytotoxic T cells. Additionally, Mn²⁺ codelivered in the system serves as a safe and effective immune adjuvant, activating the stimulator of interferon genes (STING) signaling pathway and promoting the secretion of type I interferon, further enhancing the antigen-specific T cell responses. Mn@mRNA-LNP effectively inhibits tumor progression in established melanoma and colon tumor models as well as in a model of tumor recurrence after resection. Notably, the combination of Mn@mRNA-LNP with immune checkpoint inhibitors further enhances complete tumor suppression and prolonged the overall survival in mice. Overall, this “All-in-One” mRNA vaccine significantly boosts antitumor immunity responses by improving spleen targeting and immune activation, providing an attractive strategy for the future clinical translation of therapeutic mRNA vaccines.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30701–30715 30701–30715"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577715","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}

{"title":"Flexible Narrow Bandgap Sn–Pb Perovskite Solar Cells with 21% Efficiency Using N,N′-Carbonyldiimidazole Treatments","authors":"Jixi Zeng,&nbsp;Jing Wang,&nbsp;Jinzhao Wang,&nbsp;Jia Li,&nbsp;Jiwen Chen,&nbsp;Feng Wei,&nbsp;Jing Zhang,&nbsp;Weijie Song* and Xi Fan*,&nbsp;","doi":"10.1021/acsnano.4c1103610.1021/acsnano.4c11036","DOIUrl":"https://doi.org/10.1021/acsnano.4c11036https://doi.org/10.1021/acsnano.4c11036","url":null,"abstract":"<p >Flexible tin–lead (Sn–Pb) mixed perovskite solar cells (PSCs) are among the promising flexible photovoltaics, owing to the narrow bandgap (NBG) of Sn–Pb perovskites, flexible and wearable features, and their role as a critical component in all-perovskite tandem photovoltaics. However, the flexible Sn–Pb PSCs suffer from a low power conversion efficiency, no higher than 18.5%, along with limited stability. Herein, we reported an efficient and stable flexible NBG Sn–Pb PSC via an <i>N</i>,<i>N</i>′-carbonyldiimidazole (CDI) passivation strategy. CDI, with strong adsorption energy, preferentially binds to Sn²⁺ compared with oxygen (O₂), thus effectively inhibiting the adsorption of O₂ on perovskite surfaces. The transfer of electron density around Sn²⁺ dramatically decreased, thus suppressing Sn²⁺ oxidation. The CDI treatments endowed the Sn–Pb mixed films with fewer defects, improved crystallinity, better morphology, and matched energy-level alignment. The flexible Sn–Pb devices exhibited a high PCE of 21.02%. Besides, the devices showed enhanced stability and promoted flexibility. This work provides a pathway to visibly increase the efficiency and stability of the flexible Sn–Pb mixed photovoltaic cells.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31390–31400 31390–31400"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609112","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}

{"title":"Transdermal Minimally Invasive Optical Multiplex Detection of Protein Biomarkers by Nanopillars Array-Embedded Microneedles","authors":"Adva Raz,&nbsp;Hila Gubi,&nbsp;Adam Cohen and Fernando Patolsky*,&nbsp;","doi":"10.1021/acsnano.4c1161210.1021/acsnano.4c11612","DOIUrl":"https://doi.org/10.1021/acsnano.4c11612https://doi.org/10.1021/acsnano.4c11612","url":null,"abstract":"<p >Biomarkers detection has become essential in medical diagnostics and early detection of life-threatening diseases. Modern-day medicine relies heavily on painful and invasive tests, with the extraction of large volumes of venous blood being the most common tool of biomarker detection. These tests are time-consuming, complex, expensive and require multiple sample manipulations and trained staff. The application of “intradermal” biosensors utilizing microneedles as minimally invasive sensing elements for capillary blood biomarkers detection has gained extensive interest in the past few years as a central point-of-care (POC) detection platform. Herein, we present a diagnosis paradigm based on vertically aligned nanopillar array-embedded microneedles sampling-and-detection elements for the direct optical detection and quantification of biomarkers in capillary blood. We present here a demonstration of the simple fabrication route for the creation of a multidetection-zone silicon nanopillar array, embedded in microneedle elements, followed by their area-selective chemical modification, toward the multiplex intradermal biomarkers detection. The utilization of the rapid and specific antibody–antigen binding, combined with the intrinsically large sensing area created by the nanopillar array, enables the simultaneous efficient ultrafast and highly sensitive intradermal capillary blood sampling and detection of protein biomarkers of clinical relevance, without requiring the extraction of blood samples for the <i>ex vivo</i> biomarkers analysis. Through preliminary <i>in vitro</i> and <i>in vivo</i> experiments, the direct intradermal in-skin blood extraction-free platform has demonstrated excellent sensitivity (low pM) and specificity for the accurate multiplex detection of protein biomarkers in capillary blood.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30848–30862 30848–30862"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnano.4c11612","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577736","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}

{"title":"Coordinatively Unsaturated Co Single-Atom Catalysts Enhance the Performance of Lithium–Sulfur Batteries by Triggering Strong d–p Orbital Hybridization","authors":"Lei Chen,&nbsp;Jing Xia,&nbsp;Zhuangzhuang Lai,&nbsp;Dandan Wu,&nbsp;Ji Zhou,&nbsp;Shang Chen,&nbsp;Xiaodong Meng,&nbsp;Zhongli Wang,&nbsp;Haifeng Wang,&nbsp;Lirong Zheng*,&nbsp;Linli Xu,&nbsp;Xian-Wei Lv*,&nbsp;Christopher W. Bielawski and Jianxin Geng*,&nbsp;","doi":"10.1021/acsnano.4c0872810.1021/acsnano.4c08728","DOIUrl":"https://doi.org/10.1021/acsnano.4c08728https://doi.org/10.1021/acsnano.4c08728","url":null,"abstract":"<p >The catalytic activities displayed by single-atom catalysts (SACs) depend on the coordination structure. SACs supported on carbon materials often adopt saturated coordination structures with uneven distributions because they require high-temperature conditions during synthesis. Herein, bisnitrogen-chelated Co SACs that are coordinatively unsaturated are prepared by integrating a Co complex into a conjugated microporous polymer (CMP-CoN₂). Compared with saturated analogues, i.e., tetranitrogen-chelated Co SACs (denoted as CMP-CoN₄), CMP-CoN₂ exhibits higher electrocatalytic activity in polysulfide conversions due to an enhanced hybridization between the 3d orbitals of the Co atoms and the 3p orbitals of the S atoms in the polysulfide. As a result, sulfur cathodes prepared with CoN₂ deliver outstanding performance metrics, including a high specific capacity (1393 mA h g^–1 at 0.1 C), a superior rate capacity (673.2 mA h g^–1 at 6 C), and a low capacity decay rate (of only 0.045% per cycle at 2 C over 1000 cycles). They also outperform sulfur cathodes that contain CMP-CoN₄ or CMPs that are devoid of Co SACs. This work reveals how the catalytic activity displayed by SACs is affected by their coordination structures, and the rules that underpin the structure–activity relationship may be extended to designing electrocatalysts for use in other applications.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31123–31134 31123–31134"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609247","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}

{"title":"Proximity-Induced Exchange Interaction and Prolonged Valley Lifetime in MoSe2/CrSBr Van-Der-Waals Heterostructure with Orthogonal Spin Textures","authors":"Andreas Beer,&nbsp;Klaus Zollner,&nbsp;Caique Serati de Brito,&nbsp;Paulo E. Faria Junior,&nbsp;Philipp Parzefall,&nbsp;Talieh S. Ghiasi,&nbsp;Josep Ingla-Aynés,&nbsp;Samuel Mañas-Valero,&nbsp;Carla Boix-Constant,&nbsp;Kenji Watanabe,&nbsp;Takashi Taniguchi,&nbsp;Jaroslav Fabian,&nbsp;Herre S. J. van der Zant,&nbsp;Yara Galvão Gobato and Christian Schüller*,&nbsp;","doi":"10.1021/acsnano.4c0733610.1021/acsnano.4c07336","DOIUrl":"https://doi.org/10.1021/acsnano.4c07336https://doi.org/10.1021/acsnano.4c07336","url":null,"abstract":"<p >Heterostructures, composed of semiconducting transition-metal dichalcogenides (TMDC) and magnetic van-der-Waals materials, offer exciting prospects for the manipulation of the TMDC valley properties via proximity interaction with the magnetic material. We show that the atomic proximity of monolayer MoSe₂ and the antiferromagnetic van-der-Waals crystal CrSBr leads to an unexpected breaking of time-reversal symmetry, with originally perpendicular spin directions in both materials. The observed effect can be traced back to a proximity-induced exchange interaction via first-principles calculations. The resulting spin splitting in MoSe₂ is determined experimentally and theoretically to be on the order of a few meV. Moreover, we find a more than 2 orders of magnitude longer valley lifetime of spin-polarized charge carriers in the heterostructure, as compared to monolayer MoSe₂/SiO₂, driven by a Mott transition in the type-III band-aligned heterostructure.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31044–31054 31044–31054"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnano.4c07336","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609248","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}

{"title":"Super High-k Unit-Cell-Thick α-CaCr2O4 Crystals","authors":"Hui Li,&nbsp;Chuan Xu,&nbsp;Zhibo Liu,&nbsp;Tianya Zhou,&nbsp;Jinmeng Tong,&nbsp;Qiang Wang,&nbsp;Xuanya Liu,&nbsp;Qianqian Jin,&nbsp;Hui-Ming Cheng and Wencai Ren*,&nbsp;","doi":"10.1021/acsnano.4c0703210.1021/acsnano.4c07032","DOIUrl":"https://doi.org/10.1021/acsnano.4c07032https://doi.org/10.1021/acsnano.4c07032","url":null,"abstract":"<p >High-dielectric-constant (high-<i>k</i>) insulators are indispensable components to integrate semiconductors into metal-oxide-semiconductor field-effect transistors with sub-10 nm channel length, where the equivalent oxide thickness (EOT) of high-<i>k</i> insulator needs to be decreased to subnanometer scale. The traditional insulators, including Al₂O₃, SiO₂, and HfO₂, fit well with the existing silicon industry but suffer from serious degeneration of insulating properties, such as large leakage currents caused by high-density borders and interface traps, when their thicknesses are reduced to a few nanometers. Here, we synthesize a high-quality nonlayered ultrathin α-CaCr₂O₄ crystal down to unit-cell thickness (∼1.2 nm) by an elements slow-supply chemical vapor deposition (CVD) method. The unit-cell-thick α-CaCr₂O₄ crystals show a super high dielectric constant of 87.34, which is over 20 times higher than that of well-known layered insulator <i>h</i>-BN and corresponds to an EOT below 1 nm. Furthermore, it has a high breaking strength (39 GPa) and excellent stability. This strategy can also be used to fabricate other ultrathin ternary oxides, such as high-<i>k</i> ultrathin FeNb₂O₆ crystals, demonstrating the universality of the CVD method.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31014–31020 31014–31020"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609168","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}

{"title":"Neutrophil-Mimetic Upconversion Photosynthetic Nanosystem Derived from Microalgae for Targeted Treatment of Thromboembolic Stroke","authors":"Xingping Quan,&nbsp;Chang Liu,&nbsp;Jinfen Chen,&nbsp;Yiyang Li,&nbsp;Zhen Yuan,&nbsp;Ying Zheng,&nbsp;Greta S. P. Mok,&nbsp;Ruibing Wang* and Yonghua Zhao*,&nbsp;","doi":"10.1021/acsnano.4c0624710.1021/acsnano.4c06247","DOIUrl":"https://doi.org/10.1021/acsnano.4c06247https://doi.org/10.1021/acsnano.4c06247","url":null,"abstract":"<p >Thromboembolic stroke constitutes the majority of brain strokes, resulting in elevated mortality and morbidity rates, as well as significant societal and economic burdens. Although intravenous thrombolysis serves as the standard clinical treatment, its narrow therapeutic window and the inflammatory response induced by tissue plasminogen activator (tPA) administration limit its efficacy. In the initial stages of stroke, the abrupt cessation of blood flow leads to an energy metabolism disorder, marked by a substantial decrease in adenosine triphosphate (ATP) and nicotinamide adenine dinucleotide phosphate (NADPH) levels, causing irreversible damage to neural cells. In this study, we introduce a neutrophil-mimetic, microalgae-derived upconversion photosynthetic nanosystem designed for targeted treatment of thromboembolic stroke. This system features upconversion nanoparticles coated with a thylakoid membrane and wrapped in an activated neutrophil membrane, further decorated with ROS-responsive thrombolytic tPA on its surface. The neutrophil-mimetic design facilitates high targeting specificity and accumulation at the thrombus site after intravenous administration. Upon exposure to elevated levels of reactive oxygen species (ROS) at the thrombus location, the nanosystem promptly demonstrated potent thrombolytic efficacy through the surface-modified tPA. Furthermore, near-infrared II (NIR-II) laser irradiation activated the generation of ATP and NADPH, which inhibited inflammatory cell infiltration, platelet activation, oxidative stress, and neuronal injury. This constructed nanoplatform not only showcases exceptional targeting efficiency at the stroke site and controllable release of the thrombolytic agent but also facilitates ATP/NADPH-mediated thrombolytic, anti-inflammatory, antioxidative stress, and neuroprotective effects. Additionally, it offers valuable insights into the potential therapeutic applications of microalgae-based derivatives in managing thromboembolic stroke.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30307–30320 30307–30320"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577716","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}

{"title":"Emerging Chirality and Moiré Dynamics in Twisted Layered Material Heterostructures","authors":"Andrea Silva,&nbsp;Xiang Gao,&nbsp;Melisa M. Gianetti,&nbsp;Roberto Guerra,&nbsp;Nicola Manini,&nbsp;Andrea Vanossi*,&nbsp;Michael Urbakh* and Oded Hod,&nbsp;","doi":"10.1021/acsnano.4c0502210.1021/acsnano.4c05022","DOIUrl":"https://doi.org/10.1021/acsnano.4c05022https://doi.org/10.1021/acsnano.4c05022","url":null,"abstract":"<p >Moiré superstructures arising at twisted 2D interfaces have recently attracted the attention of the scientific community due to exotic quantum states and unique mechanical and tribological behaviors that they exhibit. Here, we predict the emergence of chiral distortions in twisted layered interfaces of finite dimensions. This phenomenon originates in intricate interplay between interfacial interactions and contact boundary constraints. A metric termed the fractional chiral area is introduced to quantify the overall chirality of the moiré superstructure and to characterize its spatial distribution. Despite the equilibrium nature of the discovered energetic and structural chirality effects, they are shown to be manifested in the twisting dynamics of layered interfaces, which demonstrates a continuous transition from stick–slip to smooth rotation with no external trigger.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"30957–30965 30957–30965"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609169","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}

{"title":"Nanocarriers Targeting Circular RNA ADARB1 Boost Radiosensitivity of Nasopharyngeal Carcinoma through Synergically Promoting Ferroptosis","authors":"Dan Wang,&nbsp;Le Tang,&nbsp;Mingjian Chen,&nbsp;Zhaojian Gong,&nbsp;Chunmei Fan,&nbsp;Hongke Qu,&nbsp;Yixuan Liu,&nbsp;Lei Shi,&nbsp;Yongzhen Mo,&nbsp;Yumin Wang,&nbsp;Qijia Yan,&nbsp;Pan Chen,&nbsp;Bo Xiang,&nbsp;Qianjin Liao,&nbsp;Zhaoyang Zeng,&nbsp;Guiyuan Li,&nbsp;Weihong Jiang*,&nbsp;Steven X. Wu* and Wei Xiong*,&nbsp;","doi":"10.1021/acsnano.4c0767610.1021/acsnano.4c07676","DOIUrl":"https://doi.org/10.1021/acsnano.4c07676https://doi.org/10.1021/acsnano.4c07676","url":null,"abstract":"<p >Nasopharyngeal carcinoma (NPC) is a common malignant tumor of the head and neck, prevalent in regions such as Southern China and Southeast Asia. Radiotherapy serves as the primary clinical treatment for this carcinoma. However, resistance to radiotherapy is a fundamental cause of treatment failure and patient mortality, with the underlying mechanisms yet to be fully elucidated. We identified a recently characterized circular RNA, circADARB1, which is markedly upregulated in NPC tissues and closely associated with poor prognosis and radiotherapy resistance. Both in vitro and in vivo experiments demonstrated that circADARB1 inhibited ferroptosis, thereby inducing radiotherapy resistance in NPC cells. Building on these findings, we synthesized a biomimetic nanomaterial consisting of semiconducting polymer nanoparticles wrapped in cell membranes, designed to deliver both siRNA targeting circADARB1 and iron ions. The application of this nanomaterial not only efficiently suppressed the expression of circADARB1 and boosted intracellular iron concentrations, but also enhanced ferroptosis induced by radiotherapy, improving the radiosensitivity of NPC cells. Furthermore, our study revealed that circADARB1 upregulated the expression of heat shock protein HSP90B1, which repaired misfolded SLC7A11 and GPX4 proteins triggered by radiotherapy, thereby preserving their stability and biological functions. Mechanistically, SLC7A11 facilitated cysteine transportation into cells and glutathione synthesis, while GPX4 employed glutathione to mitigate intracellular lipid peroxidation induced by radiotherapy, shielding cells from oxidative damage and inhibiting ferroptosis, and ultimately leading to radiotherapy resistance in NPC cells. Our investigation elucidates molecular mechanisms with substantial clinical relevance, highlights the promising application prospects of nanotechnology in precision cancer therapy.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31055–31075 31055–31075"},"PeriodicalIF":15.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609246","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}

{"title":"A Machine Learning-Optimized System for Pulsatile, Photo- and Chemotherapeutic Treatment Using Near-Infrared Responsive MoS2-Based Microparticles in a Breast Cancer Model","authors":"Maria Kanelli,&nbsp;Neelkanth M. Bardhan,&nbsp;Morteza Sarmadi,&nbsp;Behnaz Eshaghi,&nbsp;Shahad K. Alsaiari,&nbsp;William T. Rothwell,&nbsp;Apurva Pardeshi,&nbsp;Dhruv Varshney,&nbsp;Dominique C. De Fiesta,&nbsp;Howard Mak,&nbsp;Virginia Spanoudaki,&nbsp;Nicole Henning,&nbsp;Ashutosh Kumar,&nbsp;Jooli Han,&nbsp;Angela M. Belcher*,&nbsp;Robert Langer* and Ana Jaklenec*,&nbsp;","doi":"10.1021/acsnano.4c0784310.1021/acsnano.4c07843","DOIUrl":"https://doi.org/10.1021/acsnano.4c07843https://doi.org/10.1021/acsnano.4c07843","url":null,"abstract":"<p >Multimodal cancer therapies are often required for progressive cancers due to the high persistence and mortality of the disease and the negative systemic side effects of traditional therapeutic methods. Thus, the development of less invasive modalities for recurring treatment cycles is of clinical significance. Herein, a light-activatable microparticle system was developed for localized, pulsatile delivery of anticancer drugs with simultaneous thermal ablation by applying controlled ON–OFF thermal cycles using near-infrared laser irradiation. The system is composed of poly(caprolactone) microparticles of 200 μm size containing molybdenum disulfide (MoS₂) nanosheets as the photothermal agent and hydrophilic doxorubicin or hydrophobic violacein, as model drugs. Upon irradiation, the nanosheets heat up to ≥50 °C leading to polymer softening and release of the drug. MoS₂ nanosheets exhibit high photothermal conversion efficiency and require low-power laser irradiation. A machine learning algorithm was applied to acquire the optimal laser operation conditions. In a mouse subcutaneous model of 4T1 triple-negative breast cancer, 25 microparticles were intratumorally administered, and after 3-cycle laser treatment, the system conferred synergistic phototherapeutic and chemotherapeutic effects. Our on-demand, pulsatile synergistic treatment resulted in increased median survival up to 39 days post start of treatment compared to untreated mice, with complete eradication of the tumors at the primary site. Such a system is therapeutically relevant for patients in need of recurring cycles of treatment on small tumors, since it provides precise localization and low invasiveness and is not cross-resistant with other treatments.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30433–30447 30433–30447"},"PeriodicalIF":15.8,"publicationDate":"2024-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577628","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}