Pub Date : 2024-10-24DOI: 10.1021/acsmaterialslett.4c0168610.1021/acsmaterialslett.4c01686
Matteo Tollemeto*, Lasse Ho̷jlund Eklund Thamdrup, Zhongyang Zhang, Isidro Badillo-Ramirez, Gavrielle R. Untracht, Peter Eskil Andersen, Line Hagner Nielsen and Anja Boisen,
Microneedle patches have gained significant attention for transdermal drug delivery, particularly those made from hydrophilic polymers for hydrophilic drugs. However, delivering poorly water-soluble lipophilic drugs remains a challenge. Our study introduces a lipid-based microneedle patch capable of effectively delivering lipophilic drugs with mechanically robust needles that penetrate physiological barriers like skin. Using a high-yield melt casting method, we produced needles up to 1200 μm in length with tunable melting points and phase transitions by adjusting lipid compositions. These patches release drugs at body temperature (37 °C). In a proof-of-concept experiment, curcumin, a model lipophilic drug, was fully dissolved and uniformly distributed in the needles, with drug loadings up to 50 wt %. Ex vivo studies demonstrated successful needle penetration and drug release in porcine skin. This lipid-based microneedle platform offers an effective solution for the transdermal, transmucosal, and buccal delivery of lipophilic drugs.
{"title":"Production and Ex Vivo Characterization of Melting Lipid Needle Patches Applied for Transdermal Delivery of Lipophilic Drugs","authors":"Matteo Tollemeto*, Lasse Ho̷jlund Eklund Thamdrup, Zhongyang Zhang, Isidro Badillo-Ramirez, Gavrielle R. Untracht, Peter Eskil Andersen, Line Hagner Nielsen and Anja Boisen, ","doi":"10.1021/acsmaterialslett.4c0168610.1021/acsmaterialslett.4c01686","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01686https://doi.org/10.1021/acsmaterialslett.4c01686","url":null,"abstract":"<p >Microneedle patches have gained significant attention for transdermal drug delivery, particularly those made from hydrophilic polymers for hydrophilic drugs. However, delivering poorly water-soluble lipophilic drugs remains a challenge. Our study introduces a lipid-based microneedle patch capable of effectively delivering lipophilic drugs with mechanically robust needles that penetrate physiological barriers like skin. Using a high-yield melt casting method, we produced needles up to 1200 μm in length with tunable melting points and phase transitions by adjusting lipid compositions. These patches release drugs at body temperature (37 °C). In a proof-of-concept experiment, curcumin, a model lipophilic drug, was fully dissolved and uniformly distributed in the needles, with drug loadings up to 50 wt %. <i>Ex vivo</i> studies demonstrated successful needle penetration and drug release in porcine skin. This lipid-based microneedle platform offers an effective solution for the transdermal, transmucosal, and buccal delivery of lipophilic drugs.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571084","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-24DOI: 10.1021/acsmaterialslett.4c0183310.1021/acsmaterialslett.4c01833
Adélaïde Clavelin, Dat Le Thanh, Ivan Bobrikov, Marcus Fehse, Nicholas E. Drewett, Gabriel A. López, Damien Saurel* and Montserrat Galceran*,
Prussian White (PW) is a strategic cathode material for sodium-ion batteries, offering a high theoretical capacity and voltage. However, the crystalline structure and the electrochemical performance of PW strongly depend on the hydration level, which is difficult to control, leading to discrepancies in the results and interpretations presented in the literature. This work aims to provide a deeper insight into the dehydration process of PW materials and a better understanding of the impact of their fast rehydration, upon exposure to moisture, on their characterization. For this purpose, a Na1.87Mn[Fe(CN)6]0.99·1.99H2O sample was synthesized by a coprecipitation method and subsequently dehydrated to remove water. After thorough characterization, our findings show that drying parameters, such as temperature and pressure, strongly influence the post-drying result. Moreover, the dehydrated samples rehydrate within minutes of exposure to air, which may explain some discrepancies observed in the literature and highlights the necessity to work under fully air-tight conditions.
{"title":"Dehydration Conditions and Ultrafast Rehydration of Prussian White: Phase Transition Dynamics and Implications for Sodium-Ion Batteries","authors":"Adélaïde Clavelin, Dat Le Thanh, Ivan Bobrikov, Marcus Fehse, Nicholas E. Drewett, Gabriel A. López, Damien Saurel* and Montserrat Galceran*, ","doi":"10.1021/acsmaterialslett.4c0183310.1021/acsmaterialslett.4c01833","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01833https://doi.org/10.1021/acsmaterialslett.4c01833","url":null,"abstract":"<p >Prussian White (PW) is a strategic cathode material for sodium-ion batteries, offering a high theoretical capacity and voltage. However, the crystalline structure and the electrochemical performance of PW strongly depend on the hydration level, which is difficult to control, leading to discrepancies in the results and interpretations presented in the literature. This work aims to provide a deeper insight into the dehydration process of PW materials and a better understanding of the impact of their fast rehydration, upon exposure to moisture, on their characterization. For this purpose, a Na<sub>1.87</sub>Mn[Fe(CN)<sub>6</sub>]<sub>0.99</sub>·1.99H<sub>2</sub>O sample was synthesized by a coprecipitation method and subsequently dehydrated to remove water. After thorough characterization, our findings show that drying parameters, such as temperature and pressure, strongly influence the post-drying result. Moreover, the dehydrated samples rehydrate within minutes of exposure to air, which may explain some discrepancies observed in the literature and highlights the necessity to work under fully air-tight conditions.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialslett.4c01833","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571083","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-23DOI: 10.1021/acsmaterialslett.4c0169910.1021/acsmaterialslett.4c01699
Yekitwork Abebe Temitmie, Muhammad Irfan Haider, Daniele T. Cuzzupè, Lucia V. Mercaldo, Stefan Kraner, Paola Delli Veneri, Amare Benor, Azhar Fakharuddin* and Lukas Schmidt-Mende*,
Narrow-bandgap (NBG) perovskite solar cells based on tin–lead mixed perovskite absorbers suffer from significant open-circuit voltage (VOC) losses due primarily to a high defect density and charge carrier recombination at the device interfaces. In this study, the VOC losses in NBG perovskite single junction cells (Eg = 1.21 eV) are addressed. The optimized NBG subcell is then used to fabricate highly efficient all-perovskite tandem solar cells (TSCs). The improvement in the VOC is achieved via the addition of a thin poly(triarylamine) interlayer between the poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS)-based hole transport layer (HTL) and the NBG perovskite. The optimal bilayer HTL results in a champion power conversion efficiency (PCE) of 20.3%, compared to 17.8% of the PEDOT:PSS-based control device. The VOC improvement of the single-junction NBG cell is also successfully transferred to all-perovskite TSC, resulting in a high VOC of 2.00 V and a PCE of 25.1%.
{"title":"Overcoming the Open-Circuit Voltage Losses in Narrow Bandgap Perovskites for All-Perovskite Tandem Solar Cells","authors":"Yekitwork Abebe Temitmie, Muhammad Irfan Haider, Daniele T. Cuzzupè, Lucia V. Mercaldo, Stefan Kraner, Paola Delli Veneri, Amare Benor, Azhar Fakharuddin* and Lukas Schmidt-Mende*, ","doi":"10.1021/acsmaterialslett.4c0169910.1021/acsmaterialslett.4c01699","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01699https://doi.org/10.1021/acsmaterialslett.4c01699","url":null,"abstract":"<p >Narrow-bandgap (NBG) perovskite solar cells based on tin–lead mixed perovskite absorbers suffer from significant open-circuit voltage (<i>V</i><sub>OC</sub>) losses due primarily to a high defect density and charge carrier recombination at the device interfaces. In this study, the <i>V</i><sub>OC</sub> losses in NBG perovskite single junction cells (<i>E</i><sub>g</sub> = 1.21 eV) are addressed. The optimized NBG subcell is then used to fabricate highly efficient all-perovskite tandem solar cells (TSCs). The improvement in the <i>V</i><sub>OC</sub> is achieved via the addition of a thin poly(triarylamine) interlayer between the poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS)-based hole transport layer (HTL) and the NBG perovskite. The optimal bilayer HTL results in a champion power conversion efficiency (PCE) of 20.3%, compared to 17.8% of the PEDOT:PSS-based control device. The <i>V</i><sub>OC</sub> improvement of the single-junction NBG cell is also successfully transferred to all-perovskite TSC, resulting in a high <i>V</i><sub>OC</sub> of 2.00 V and a PCE of 25.1%.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialslett.4c01699","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142570994","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-18DOI: 10.1021/acsmaterialslett.4c0162010.1021/acsmaterialslett.4c01620
Ryun-Han Koo, Wonjun Shin, Gyuweon Jung, Jangsaeng Kim, Sung-Tae Lee, Jiseong Im, Sung-Ho Park, Jonghyun Ko, Daewoong Kwon* and Jong-Ho Lee*,
We investigate the effects of strain stress on the hafnium zirconium oxide ferroelectric tunnel junctions (FTJs). The impact of strain stress on each layer of the FTJ is investigated depending on the thickness of the metal capping layer and the post-metal-annealing temperature. It is revealed that, for the insulator layer, an increase in strain lead to an increased off-current in the FTJs. In contrast, increased strain stress in the ferroelectric layer directly increases the trap density, leading to an increase in the on-current of the FTJs. Furthermore, we analyze how these strain-induced changes affect the performance and reliability of FTJs in neuromorphic systems. We propose optimization strategies for strain stress in FTJs based on the frequency of neural network updates, highlighting the critical balance between achieving a large dynamic range and ensuring device endurance, aligning device performance with the specific demands and conditions of neural network applications.
{"title":"Strain–Stress Impact on Ferroelectric Devices: A Multilayer Analysis and Optimization Strategy for Neural Networks","authors":"Ryun-Han Koo, Wonjun Shin, Gyuweon Jung, Jangsaeng Kim, Sung-Tae Lee, Jiseong Im, Sung-Ho Park, Jonghyun Ko, Daewoong Kwon* and Jong-Ho Lee*, ","doi":"10.1021/acsmaterialslett.4c0162010.1021/acsmaterialslett.4c01620","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01620https://doi.org/10.1021/acsmaterialslett.4c01620","url":null,"abstract":"<p >We investigate the effects of strain stress on the hafnium zirconium oxide ferroelectric tunnel junctions (FTJs). The impact of strain stress on each layer of the FTJ is investigated depending on the thickness of the metal capping layer and the post-metal-annealing temperature. It is revealed that, for the insulator layer, an increase in strain lead to an increased off-current in the FTJs. In contrast, increased strain stress in the ferroelectric layer directly increases the trap density, leading to an increase in the on-current of the FTJs. Furthermore, we analyze how these strain-induced changes affect the performance and reliability of FTJs in neuromorphic systems. We propose optimization strategies for strain stress in FTJs based on the frequency of neural network updates, highlighting the critical balance between achieving a large dynamic range and ensuring device endurance, aligning device performance with the specific demands and conditions of neural network applications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571167","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-18DOI: 10.1021/acsmaterialslett.4c0156410.1021/acsmaterialslett.4c01564
Wei Gu, Yuan Zhang, Wan Chen, Jieli Zhu, Yuyang Zhang, Baoliang Cheng, Qing Li* and Qingqing Miao*,
Type I photodynamic therapy (PDT), which utilizes type I photoreactions and is less O2-dependent, is expected to exert ideal synergistic therapy performance when combined with targeted radionuclide therapy (TRT). However, this combination has been less explored. To achieve it, this study presents a sequentially dual-targeted molecular theranostic probe for combining TRT and antihypoxic activatable PDT against prostate cancer. The probe achieves prostate-specific membrane antigen (PSMA)-mediated lock-and-key targeting ability and monoamine oxidase A (MAO-A) hydrolysis with activated fluoro-photoacoustic signals and O2•– generation. The PSMA motif not only enhances the targeting specificity but also increases the intracellular accumulation capacity of probe and promotes more MAO-A activation. In this regard, an enhanced inhibition of tumor growth is obtained for combined activatable antihypoxic PDT and TRT in comparison to any single regimen, including the commercial 177Lu-PSMA-617, thereby demonstrating the effective antitumor effect. This study provides a potential solution for a combination of TRT and PDT for effective tumor therapy.
I 型光动力疗法(PDT)利用 I 型光反应,对氧气的依赖性较低,与放射性核素靶向疗法(TRT)联合使用有望发挥理想的协同治疗效果。然而,对这种组合的探索还较少。为了实现这一目标,本研究提出了一种顺序双靶向分子治疗探针,用于结合 TRT 和抗缺氧活化光导疗法治疗前列腺癌。该探针具有前列腺特异性膜抗原(PSMA)介导的锁钥靶向能力和单胺氧化酶A(MAO-A)水解能力,并能产生活化的荧光声信号和氧气。PSMA 基序不仅增强了靶向特异性,还提高了探针在细胞内的蓄积能力,并促进更多的 MAO-A 激活。因此,与任何单一方案(包括商用 177Lu-PSMA-617 方案)相比,可激活的抗缺氧 PDT 和 TRT 联合疗法可增强对肿瘤生长的抑制,从而显示出有效的抗肿瘤效果。这项研究为结合 TRT 和 PDT 有效治疗肿瘤提供了一种潜在的解决方案。
{"title":"Sequentially Dual-Targeted Molecular Theranostic Probe for Radionuclide and Anti-Hypoxic Activatable Photodynamic Therapy of Cancer","authors":"Wei Gu, Yuan Zhang, Wan Chen, Jieli Zhu, Yuyang Zhang, Baoliang Cheng, Qing Li* and Qingqing Miao*, ","doi":"10.1021/acsmaterialslett.4c0156410.1021/acsmaterialslett.4c01564","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01564https://doi.org/10.1021/acsmaterialslett.4c01564","url":null,"abstract":"<p >Type I photodynamic therapy (PDT), which utilizes type I photoreactions and is less O<sub>2</sub>-dependent, is expected to exert ideal synergistic therapy performance when combined with targeted radionuclide therapy (TRT). However, this combination has been less explored. To achieve it, this study presents a sequentially dual-targeted molecular theranostic probe for combining TRT and antihypoxic activatable PDT against prostate cancer. The probe achieves prostate-specific membrane antigen (PSMA)-mediated lock-and-key targeting ability and monoamine oxidase A (MAO-A) hydrolysis with activated fluoro-photoacoustic signals and O<sub>2</sub><sup>•–</sup> generation. The PSMA motif not only enhances the targeting specificity but also increases the intracellular accumulation capacity of probe and promotes more MAO-A activation. In this regard, an enhanced inhibition of tumor growth is obtained for combined activatable antihypoxic PDT and TRT in comparison to any single regimen, including the commercial <sup>177</sup>Lu-PSMA-617, thereby demonstrating the effective antitumor effect. This study provides a potential solution for a combination of TRT and PDT for effective tumor therapy.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571161","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-17DOI: 10.1021/acsmaterialslett.4c0160510.1021/acsmaterialslett.4c01605
Francisco Bevilacqua, Robin Girod, Victor F. Martín, Manuel Obelleiro-Liz, Gail A. Vinnacombe-Willson, Kyle Van Gordon, Johan Hofkens, Jose Manuel Taboada, Sara Bals and Luis M. Liz-Marzán*,
The production of colloidal metal nanostructures with complex geometries usually involves shape-directing additives, such as metal ions or thiols, which stabilize high-index facets. These additives may however affect the nanoparticles’ surface chemistry, hindering applications, e.g., in biology or catalysis. We report herein the preparation of gold bipyramids with no need for additives and shape yields up to 99%, using pentatwinned Au nanorods as seeds and cetyltrimethylammonium chloride as surfactant. For high-growth solution:seed ratios, the bipyramids exhibit an unusual “belted” structure. Three-dimensional electron microscopy revealed the presence of high-index {117}, {115}, and {113} side facets, with {113} and {112} facets at the belt. Belted bipyramids exhibit strong near-field enhancement and high extinction in the near-infrared, in agreement with electromagnetic simulations. These Ag-free bipyramids were used to seed chiral overgrowth using 1,1′-binaphthyl-2,2′-diamine as a chiral inducer, with g-factor up to 0.02, likely the highest reported for bipyramid seeds so far.
在生产具有复杂几何形状的胶体金属纳米结构时,通常需要使用金属离子或硫醇等形状定向添加剂来稳定高指数刻面。然而,这些添加剂可能会影响纳米粒子的表面化学性质,从而阻碍其在生物或催化等领域的应用。我们在本文中报告了无需添加剂的金双锥体制备方法,以五孪晶金纳米棒为种子,十六烷基三甲基氯化铵为表面活性剂,制备出的金双锥体形状良率高达 99%。在高生长溶液与种子比的情况下,双锥体呈现出一种不寻常的 "带状 "结构。三维电子显微镜显示存在高指数的{117}、{115}和{113}侧刻面,带状刻面为{113}和{112}。带状双锥体表现出很强的近场增强能力和很高的近红外消光能力,这与电磁模拟结果一致。这些无银双锥体被用于以 1,1′-联萘-2,2′-二胺为手性诱导剂的手性过度生长种子,其 g 因子高达 0.02,可能是迄今为止报道的双锥体种子中最高的。
{"title":"Additive-Free Synthesis of (Chiral) Gold Bipyramids from Pentatwinned Nanorods","authors":"Francisco Bevilacqua, Robin Girod, Victor F. Martín, Manuel Obelleiro-Liz, Gail A. Vinnacombe-Willson, Kyle Van Gordon, Johan Hofkens, Jose Manuel Taboada, Sara Bals and Luis M. Liz-Marzán*, ","doi":"10.1021/acsmaterialslett.4c0160510.1021/acsmaterialslett.4c01605","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01605https://doi.org/10.1021/acsmaterialslett.4c01605","url":null,"abstract":"<p >The production of colloidal metal nanostructures with complex geometries usually involves shape-directing additives, such as metal ions or thiols, which stabilize high-index facets. These additives may however affect the nanoparticles’ surface chemistry, hindering applications, e.g., in biology or catalysis. We report herein the preparation of gold bipyramids with no need for additives and shape yields up to 99%, using pentatwinned Au nanorods as seeds and cetyltrimethylammonium chloride as surfactant. For high-growth solution:seed ratios, the bipyramids exhibit an unusual “belted” structure. Three-dimensional electron microscopy revealed the presence of high-index {117}, {115}, and {113} side facets, with {113} and {112} facets at the belt. Belted bipyramids exhibit strong near-field enhancement and high extinction in the near-infrared, in agreement with electromagnetic simulations. These Ag-free bipyramids were used to seed chiral overgrowth using 1,1′-binaphthyl-2,2′-diamine as a chiral inducer, with <i>g</i>-factor up to 0.02, likely the highest reported for bipyramid seeds so far.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialslett.4c01605","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1021/acsmaterialslett.4c0090210.1021/acsmaterialslett.4c00902
Xiaohui Yao, Dongxu Cui, Changyan Zhu, Jingting He, Fanfei Meng, Shuai Yang, Man Dong, Guogang Shan*, Min Zhang, Chunyi Sun*, Xinlong Wang and Zhongmin Su,
Two-dimensional metal–organic frameworks (2D MOF) have attracted great attention in the electrocatalytic reduction of CO2 owing to their well-defined structure and high surface area. Nevertheless, how to combine accessible metal active sites with high electron transfer still poses challenges in structural assembly. Herein, two-dimensional AgCe-MOFs with intralayer π–π stacking interactions were assembled by linking one-dimensional Ce–O chains to Ag(I). Its nanosheet can be facilely prepared via self-exfoliation upon the loss of uncoordinated interlayer acetonitrile. The 2D AgCe-MOF nanosheets’ merits of more exposed active sites and efficient electron transfer channels have displayed outstanding electrochemical performance and 99.5% selectivity in electrocatalytic CO2 reduction to CO. The establishment of efficient electrical transport channels and high exposure of catalytic sites in a framework through designed supramolecular interactions is expected to be a potential strategy for the construction of efficient electrocatalysts.
二维金属有机框架(2D MOF)因其明确的结构和高比表面积而在二氧化碳的电催化还原中备受关注。然而,如何将易接近的金属活性位点与高电子传递结合起来,仍然是结构组装中的难题。本文通过将一维 Ce-O 链与 Ag(I) 连接,组装出具有层内 π-π 堆垛相互作用的二维 AgCe-MOF。在失去非配位层间乙腈后,通过自剥离可以方便地制备其纳米片。二维 AgCe-MOF 纳米片具有更多暴露的活性位点和高效电子传递通道的优点,在电催化 CO2 还原成 CO 的过程中表现出卓越的电化学性能和 99.5% 的选择性。通过设计超分子相互作用在框架中建立高效电子传输通道和高暴露催化位点有望成为构建高效电催化剂的一种潜在策略。
{"title":"Self-exfoliating Bimetallic Metal–Organic Framework Layer with Intralayer π–π Interactions for Efficient Electrical Transport and CO2 Electroreduction","authors":"Xiaohui Yao, Dongxu Cui, Changyan Zhu, Jingting He, Fanfei Meng, Shuai Yang, Man Dong, Guogang Shan*, Min Zhang, Chunyi Sun*, Xinlong Wang and Zhongmin Su, ","doi":"10.1021/acsmaterialslett.4c0090210.1021/acsmaterialslett.4c00902","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c00902https://doi.org/10.1021/acsmaterialslett.4c00902","url":null,"abstract":"<p >Two-dimensional metal–organic frameworks (2D MOF) have attracted great attention in the electrocatalytic reduction of CO<sub>2</sub> owing to their well-defined structure and high surface area. Nevertheless, how to combine accessible metal active sites with high electron transfer still poses challenges in structural assembly. Herein, two-dimensional AgCe-MOFs with intralayer π–π stacking interactions were assembled by linking one-dimensional Ce–O chains to Ag(I). Its nanosheet can be facilely prepared via self-exfoliation upon the loss of uncoordinated interlayer acetonitrile. The 2D AgCe-MOF nanosheets’ merits of more exposed active sites and efficient electron transfer channels have displayed outstanding electrochemical performance and 99.5% selectivity in electrocatalytic CO<sub>2</sub> reduction to CO. The establishment of efficient electrical transport channels and high exposure of catalytic sites in a framework through designed supramolecular interactions is expected to be a potential strategy for the construction of efficient electrocatalysts.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571125","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1021/acsmaterialslett.4c0136710.1021/acsmaterialslett.4c01367
Jungmok Oh, Junho Lee, Jisu Park, Namgi Jeon, Gyoung S. Na, Hyunju Chang, Joonsuk Huh, Hyun Woo Kim* and Yongju Yun*,
Recent advances in data-driven approaches using the machine learning (ML) method have enabled the discovery of high-performance materials. This paper presents a hybrid framework that combines ML models with a metaheuristic optimization algorithm, to explore improved heterogeneous catalysts for propane dehydrogenation (PDH). The framework proposes multiple PDH catalysts, utilizing our laboratory-scale database. A unique five-component catalyst, 2.4Ga 2.2Pt 1.7B 1.3Zr/Al2O3, exhibits superior performance, achieving a propylene yield of 58% at 600 °C. This work highlights the excellent predictive capability of the framework and offers a new data-driven approach for developing high-performance materials for heterogeneous catalysis.
最近,使用机器学习(ML)方法的数据驱动方法取得了进展,从而能够发现高性能材料。本文介绍了一种混合框架,它将 ML 模型与元启发式优化算法相结合,用于探索丙烷脱氢 (PDH) 的改进型异相催化剂。该框架利用我们的实验室规模数据库,提出了多种 PDH 催化剂。一种独特的五组分催化剂 2.4Ga 2.2Pt 1.7B 1.3Zr/Al2O3 表现出卓越的性能,在 600 °C 时丙烯产率达到 58%。这项工作凸显了该框架卓越的预测能力,并为开发高性能的异相催化材料提供了一种新的数据驱动方法。
{"title":"Data-Driven Development of Heterogeneous Catalysts for Propane Dehydrogenation with Machine Learning and Metaheuristic Optimization","authors":"Jungmok Oh, Junho Lee, Jisu Park, Namgi Jeon, Gyoung S. Na, Hyunju Chang, Joonsuk Huh, Hyun Woo Kim* and Yongju Yun*, ","doi":"10.1021/acsmaterialslett.4c0136710.1021/acsmaterialslett.4c01367","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01367https://doi.org/10.1021/acsmaterialslett.4c01367","url":null,"abstract":"<p >Recent advances in data-driven approaches using the machine learning (ML) method have enabled the discovery of high-performance materials. This paper presents a hybrid framework that combines ML models with a metaheuristic optimization algorithm, to explore improved heterogeneous catalysts for propane dehydrogenation (PDH). The framework proposes multiple PDH catalysts, utilizing our laboratory-scale database. A unique five-component catalyst, 2.4Ga 2.2Pt 1.7B 1.3Zr/Al<sub>2</sub>O<sub>3</sub>, exhibits superior performance, achieving a propylene yield of 58% at 600 °C. This work highlights the excellent predictive capability of the framework and offers a new data-driven approach for developing high-performance materials for heterogeneous catalysis.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571121","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Herein, to tackle the current issue of ignoring cell interactions and spatial heterogeneity in in vitro glomerulus models, a core–shell composite gel microsphere with interzonal intercommunication was developed. By adjusting the diameter ratio of the Dex-Alg/PEG-Alg droplet to the GelMA droplet, the size, shape, and compartment ratio of the droplet can be controlled. This setup keeps compartments separate yet interconnected, closely resembling the spatial arrangement of cells in glomeruli and their physiological state. Noteworthily, glomerular endothelial cells, which are supported by mesangial cells, form blood vessels, whereas podocytes form an epithelial barrier. Key functional proteins were increased, and electron imaging revealed the creation of the basement membrane. Moreover, Doxorubicin-treated models demonstrated enhanced cell death, podocyte loss, and kidney damage, which were reduced by dexrazoxane. Thus, we believe that in vitro 3D glomerular models with zone structures have significant potential for glomerular research.
{"title":"Preparation of 3D Zonal and Interactional Glomerular Models Based on Composite Core–Shell Hydrogel Microspheres","authors":"Menghan Yang, Meiying Hong, Guanxiong Wang, Siping Wang, Rui Shen, Jianxiu Guo*, Chongyang Shen* and Yaolei Wang*, ","doi":"10.1021/acsmaterialslett.4c0165810.1021/acsmaterialslett.4c01658","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01658https://doi.org/10.1021/acsmaterialslett.4c01658","url":null,"abstract":"<p >Herein, to tackle the current issue of ignoring cell interactions and spatial heterogeneity in in vitro glomerulus models, a core–shell composite gel microsphere with interzonal intercommunication was developed. By adjusting the diameter ratio of the Dex-Alg/PEG-Alg droplet to the GelMA droplet, the size, shape, and compartment ratio of the droplet can be controlled. This setup keeps compartments separate yet interconnected, closely resembling the spatial arrangement of cells in glomeruli and their physiological state. Noteworthily, glomerular endothelial cells, which are supported by mesangial cells, form blood vessels, whereas podocytes form an epithelial barrier. Key functional proteins were increased, and electron imaging revealed the creation of the basement membrane. Moreover, Doxorubicin-treated models demonstrated enhanced cell death, podocyte loss, and kidney damage, which were reduced by dexrazoxane. Thus, we believe that <i>in vitro</i> 3D glomerular models with zone structures have significant potential for glomerular research.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571124","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1021/acsmaterialslett.4c0171210.1021/acsmaterialslett.4c01712
Zhidong Wei*, Yuchen Zhang, Jiawei Yan, Jiasheng Chi, Huoshuai Huang, Qianxiang Su, Junying Liu and Wenfeng Shangguan*,
In this work, the grinding angle hexahedron SrTiO3 was prepared and modified by Al doping methods, which could improve its photocatalytic overall water splitting performance. The Raman spectrum results indicated that the TiO6 polarizability could be modified with γ-Al2O3 doping. More importantly, the 27Al NMR spectroscopy analysis indicated that the AlO4, which originated from the nano γ-Al2O3 as the Al-doping sources, tends to be transformed into AlO6 to form α-Al2O3 to influence the TiO6 polarizability and further accelerates the separation of the photocarriers via AlO6 served as the trap of the photogenerated holes, which could be proved by the dynamic analysis of transient absorption spectroscopy (TAS).
{"title":"Revealing the Photocatalytic Dynamic Mechanism of TiO6 Polarization Regulation in Al-Doped SrTiO3: γ-Al2O3 Phase Transformation for Trapping the Photogenerated Holes","authors":"Zhidong Wei*, Yuchen Zhang, Jiawei Yan, Jiasheng Chi, Huoshuai Huang, Qianxiang Su, Junying Liu and Wenfeng Shangguan*, ","doi":"10.1021/acsmaterialslett.4c0171210.1021/acsmaterialslett.4c01712","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01712https://doi.org/10.1021/acsmaterialslett.4c01712","url":null,"abstract":"<p >In this work, the grinding angle hexahedron SrTiO<sub>3</sub> was prepared and modified by Al doping methods, which could improve its photocatalytic overall water splitting performance. The Raman spectrum results indicated that the TiO<sub>6</sub> polarizability could be modified with γ-Al<sub>2</sub>O<sub>3</sub> doping. More importantly, the <sup>27</sup>Al NMR spectroscopy analysis indicated that the AlO<sub>4</sub>, which originated from the nano γ-Al<sub>2</sub>O<sub>3</sub> as the Al-doping sources, tends to be transformed into AlO<sub>6</sub> to form α-Al<sub>2</sub>O<sub>3</sub> to influence the TiO<sub>6</sub> polarizability and further accelerates the separation of the photocarriers via AlO<sub>6</sub> served as the trap of the photogenerated holes, which could be proved by the dynamic analysis of transient absorption spectroscopy (TAS).</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571123","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}