Khalil ur Rehman, Jeyavelan Muthu, Radha Raman, Ian Daniell Santos, Bhartendu Papnai, Ya-Ping Hsieh, Mario Hofmann
{"title":"Magnetic Microactuators Based on Particle Jamming","authors":"Khalil ur Rehman, Jeyavelan Muthu, Radha Raman, Ian Daniell Santos, Bhartendu Papnai, Ya-Ping Hsieh, Mario Hofmann","doi":"10.1021/acsmaterialslett.4c01157","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01157","url":null,"abstract":"Magnetic microactuators and microrobots have the potential to revolutionize remote manipulation and swarm-based collaboration. Unfortunately, conventional approaches to controlling individual magnetic systems cannot be scaled down to the microscale due to fundamental challenges in the generation and modification of magnetic fields. We here demonstrate a novel actuation mechanism that imparts magnetic microactuators with an unprecedented ease of fabrication and dimensional scalability. Through mechanical jamming in binary particle mixtures, magnetic ordering, and pronounced anisotropy could be induced. Combined simulation and experimental investigation confirm the importance of arresting forces from neighboring particles as the origin of this behavior. This sensitivity of magnetic properties to assembly morphology can be exploited to produce novel actuators that utilize minute changes in particle size or pressure. We demonstrate the transduction of particle swelling into magnetic torque locking that enables active magnetic control in microrobots for future remote operating applications.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251696","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}
Lulu Cao, Zhiqiang Cui, Dongxiang Zhang, Yikun Li, Xiaoyan Gao, Rong Shang, Xin-Dong Jiang, Jianjun Du, Xiaohong Sun
{"title":"Novel NIR-II 3,5-Julolidinyl aza-BODIPY for Photothermal Therapy of Gliomas Stem Cells by Brain Stereotactic Injection","authors":"Lulu Cao, Zhiqiang Cui, Dongxiang Zhang, Yikun Li, Xiaoyan Gao, Rong Shang, Xin-Dong Jiang, Jianjun Du, Xiaohong Sun","doi":"10.1021/acsmaterialslett.4c01447","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01447","url":null,"abstract":"Functional dyes with absorption in the second near-infrared window (NIR-II) show great promise in photothermal therapy. Herein, the novel NIR-II 3,5-julolidinyl aza-BODIPY (<b>JLD</b>) was prepared and confirmed by X-ray crystallographic analysis for the first time. The molecular packing structure facilitates the <i>J</i>-aggregation packing mode. Self-assembled <b>JLD</b>-nanoparticles (<b>JLD</b>-NPs) emit fluorescence (λ<sub>em</sub> = 962 nm, Φ<sub>f</sub> = 0.1%), and a peak belt covered a NIR-II range of 900–1300 nm. The photothermal conversion efficiency was high and was calculated to be 79%. <b>JLD</b>-NPs with NIR-II 915 nm laser irradiation had the good tumor-inhibition capability with promoting the apoptosis and inhibiting the stemness of glioblastoma cells by brain stereotactic injection and affect the occurrence of malignant events, such as migration and invasion.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251697","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}
Mahmoud G. Ahmed, Ying Fan Tay, Mengyuan Zhang, Sing Yang Chiam, Lydia H. Wong
{"title":"Tailoring Surface Electronic Structure of Spinel Co3O4 Oxide via Fe and Cu Substitution for Enhanced Oxygen Evolution Reaction","authors":"Mahmoud G. Ahmed, Ying Fan Tay, Mengyuan Zhang, Sing Yang Chiam, Lydia H. Wong","doi":"10.1021/acsmaterialslett.4c00857","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c00857","url":null,"abstract":"Multimetal spinel oxides are promising candidates for the oxygen evolution reaction (OER) due to their ability to offer more accessible active sites and oxygen vacancies (O<sub>vac</sub>). However, the utilization of redox-active species in spinel oxides is limited. Herein, we unveil an efficient multimetal spinel oxide using high-throughput methods. The oxide contains Fe and Cu substituted into Co sites following a stoichiometry of Fe<sub>0.6</sub>Cu<sub>0.6</sub>Co<sub>1.8</sub>O<sub>4</sub>. The dual cation substitution of Fe and Cu manipulates the electronic states and generates O<sub>vac</sub>, thereby generating more accessible active species. This significantly improves the OH<sup>–</sup> adsorption capacity on spinel oxide triggering a more favorable OER reaction with a low overpotential of 265 mV at 10 mA cm<sup>–2</sup> and high durability in an alkaline medium. Our work not only presents the utilization of a high-throughput approach to explore efficient catalysts with optimal composition but also provides useful insights into the modulation of electronic states for enhanced catalytic performance.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251695","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}
Yixiao Yin, Yinyan Wu, Binghong He, Zekun Xia, Weiguo Zhu, Jun Yeob Lee, Yafei Wang
{"title":"New Concept for HLCT Emitter: Acceptor Molecule in Exciplex System for Highly Efficient and Extremely Low-Efficiency Roll-Off Solution-Processed OLED","authors":"Yixiao Yin, Yinyan Wu, Binghong He, Zekun Xia, Weiguo Zhu, Jun Yeob Lee, Yafei Wang","doi":"10.1021/acsmaterialslett.4c01643","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01643","url":null,"abstract":"The use of hybridized local and charge-transfer (HLCT) emitters as acceptor or donor molecules in exciplex systems is still a novel concept even though HLCT molecules can harvest both singlet and triplet excitons. Herein, two HLCT emitters, 2-<sup><i>t</i></sup>Bu<i>spo</i>Cz-2pTrz and 2-<sup><i>t</i></sup>Bu<i>spo</i>Cz-Me3pTrz, are prepared as acceptors of exciplexes with thermally activated delayed fluorescence (TADF) properties. The exciplex TADF systems constructed by mixing HLCT and TAPC molecules have a minute energy gap between singlet and triplet excited states and unity emission efficiency. Using the exciplex as an emitter, solution-processed devices achieve maximum external quantum efficiency (<i>EQE</i><sub>max</sub>) of 16.6%. Impressively, solution-processed devices with the fabricated exciplexes as hosts exhibit extremely low turn-on voltages and a promising <i>EQE</i><sub>max</sub> of >20%, which is concomitant with an extremely low-efficiency roll-off of 0.5% at 1,000 cd m<sup>–2</sup>. This study explores the potential of HLCT emitters as acceptors of exciplexes and guides the design of efficient exciplex systems.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251698","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}
{"title":"Construction of Sulfur Doped Nickel and Copper Interfaces for Hydrogen Evolution Reaction","authors":"Jiajie Yu, Shiwen Zhang, Yuyang Liu, Yurun Tong, Yijie Zhong, Bin He, Enlai Hu, Jing Zhang, Zhongwei Chen","doi":"10.1021/acsmaterialslett.4c01339","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01339","url":null,"abstract":"Developing efficient and economical electrocatalysts for the hydrogen evolution reaction (HER) is important for high-purity hydrogen generation. Transition metals-based compounds have been considered as promising substitutes for the Pt-based electrocatalysts toward HER. Nevertheless, pure metals display inert HER activity because of their unfavorable adsorption behavior for intermediates. Herein, thiourea engaged electrodeposition was conducted to fabricate sulfur-doped nickel and copper (S–Ni/Cu) nanowires that contain numerous interfaces. Interface and sulfur doping redistributed the electronic states of the electrocatalyst structure, which accelerated the adsorption of hydrogen atoms at active sites and promoted the water dissociation process. Consequently, the HER overpotential of S–Ni/Cu is only 67 mV at 10 mA cm<sup>–2</sup>, with excellent durability.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251700","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}
Zhenye Wang, Di Zhang, Lvpeng Yang, Meichen Xu, Junfeng Liu, Zhi Wang, Yerun Gao, Li-Yuan Zhang, Lianbin Niu, Ming Shao
{"title":"Realization of Evaporated Electrode-Based Intrinsically Stretchable Ternary Organic Solar Cells through Encapsulation Strategy","authors":"Zhenye Wang, Di Zhang, Lvpeng Yang, Meichen Xu, Junfeng Liu, Zhi Wang, Yerun Gao, Li-Yuan Zhang, Lianbin Niu, Ming Shao","doi":"10.1021/acsmaterialslett.4c01548","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01548","url":null,"abstract":"The mechanical properties of organic solar cells are of great importance to ensure their application in wearable or stretchable electronics. Here, we introduce polymer acceptor (N2200) into the active layer blend, and realize intrinsically stretchable organic solar cells (<i>is</i>-OSCs) with evaporated electrode via encapsulation strategy. The incorporation of N2200 simultaneously enhances the mechanical stretchability and PCE of <i>is</i>-OSCs, attributed to the enhanced polymer chain entanglement, and N2200 can act as tie molecules to provide electric connection among small molecule domains. More importantly, encapsulating the evaporated electrode-based <i>is</i>-OSCs leads to significant improvement in its mechanical stretchability, with 80% PCE retention under a large strain of 20%, compared to <2.5% strain for the unencapsulated ones. Additionally, encapsulated <i>is</i>-OSCs retained 67% PCE after 1000 test cycles at a stretch strain of 15%, whereas unencapsulated devices can only retain 33% PCE after 200 test cycles under a small strain of 5%.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251732","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}
Shao-Chen Wang, Xiang Ji, Rui Hou, Longlong Qi, Peng Jing, Xuan Xu, Baocang Liu, Jun Zhang
{"title":"Fabrication of Cu–CeO2 Catalyst with Abundant Interfacial Cu+–O–Ce3+–OV (Oxygen Vacancy) Sites for Boosting CO2 Electroreduction to Methane","authors":"Shao-Chen Wang, Xiang Ji, Rui Hou, Longlong Qi, Peng Jing, Xuan Xu, Baocang Liu, Jun Zhang","doi":"10.1021/acsmaterialslett.4c01683","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01683","url":null,"abstract":"Accelerating the conversion of *CO to *CHO and promoting the adsorption and hydrogenation of *CHO are the keys to achieving a highly selective electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to CH<sub>4</sub> over Cu-based catalysts. Herein, a novel electrocatalyst comprising highly dispersed Cu nanoclusters (Cu<sub>NCs</sub>) supported on oxygen vacancy (O<sub>V</sub>)-rich CeO<sub>2</sub> on carbon paper (Cu<sub>NCs</sub>–CeO<sub>2</sub>/CP) with plentiful interfacial Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> sites is constructed via a facile electrodeposition method. Various <i>in situ</i>/<i>ex situ</i> characterizations and theoretical calculations unveil that the Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> sites can effectively regulate the pathway of the CO<sub>2</sub>RR, accelerate the *CO → *CHO process, stabilize the *CHO and *OCH<sub>3</sub> intermediates, and promote their hydrogenation to produce CH<sub>4</sub>. Furthermore, the critical role of Ce<sup>3+</sup> and the O<sub>V</sub> species in forming Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> to maintain the electrocatalytic CO<sub>2</sub>RR activity is revealed. The optimized Cu<sub>NCs</sub>–CeO<sub>2</sub>/CP electrocatalyst exhibits a CH<sub>4</sub> Faradaic efficiency of 68.3% at 500 mA cm<sup>–2</sup>, with a high partial current density of 340 mA cm<sup>–2</sup>.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251733","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}
{"title":"Enhancing Nanomaterial-Based Optical Spectroscopic Detection of Cancer through Machine Learning","authors":"Célia Sahli, Kenry","doi":"10.1021/acsmaterialslett.4c01267","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01267","url":null,"abstract":"Optical spectroscopic techniques relying on light–matter interactions, such as Raman scattering, fluorescence, and infrared absorbance spectroscopy, offer numerous advantages to complement existing cancer detection methods. By combining these spectroscopic techniques with rationally engineered nanomaterials, cancer cells and tissues can be more specifically targeted, and the readout signals can be substantially enhanced. Further integration of machine learning with its potential to identify subtle malignancy indicators may significantly improve the capability of nanomaterial-enabled optical spectroscopy to delineate cancer more precisely. As such, the synergistic integration of optical spectroscopy, nanomaterials, and machine learning may provide unique opportunities for the development of more selective, sensitive, and accurate cancer diagnostic technologies, which can be leveraged to optimize therapeutic strategies and minimize unnecessary interventions to ultimately enhance patient survival outcomes. This Perspective describes numerous strategies incorporating optical spectroscopy, nanomaterials, and machine learning to improve cancer detection and summarizes our outlook on the current landscape and potential future directions of this emerging field.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251699","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}
Edwin B. Clatworthy, Rémy Guillet-Nicolas, Philippe Boullay, Michael Badawi, Yann Foucaud, Eddy Dib, Nicolas Barrier, Arnold A. Paecklar, Maxime Debost, Sajjad Ghojavand, Jean-Pierre Gilson, Izabel Medeiros-Costa, Svetlana Mintova
{"title":"Ultrathin BPH Nanosheets with Exceptional Water Adsorption Properties","authors":"Edwin B. Clatworthy, Rémy Guillet-Nicolas, Philippe Boullay, Michael Badawi, Yann Foucaud, Eddy Dib, Nicolas Barrier, Arnold A. Paecklar, Maxime Debost, Sajjad Ghojavand, Jean-Pierre Gilson, Izabel Medeiros-Costa, Svetlana Mintova","doi":"10.1021/acsmaterialslett.4c01625","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01625","url":null,"abstract":"The synthesis of ultrathin BPH zeolite nanosheets from an aluminosilicate colloidal suspension using exclusively inorganic structure directing agents under mild conditions is reported. The improved synthesis yields nanosheets of 4–7 nm and a Si/Al ratio of 1.5; combined 3D electron diffraction and DFT calculations reveal the spatial distribution of extra-framework cations throughout the microporous structure. The ultrathin BPH nanosheets exhibit high and regular intersheet mesoporosity, and substantially improved thermal stability. The notable mesoporosity bestows exceptional water adsorption behavior typically unseen for zeolites; the as-prepared material consists of up to 49% adsorbed H<sub>2</sub>O by weight and adsorbs up to 32 wt % H<sub>2</sub>O at 90% relative humidity. <sup>2</sup>H MAS NMR spectroscopy identifies different types of O<sup>2</sup>H environments ascribed to silanol species exhibiting two motion behaviors. H<sub>2</sub>O sorption analysis demonstrates reproducible behavior over multiple cycles and low temperature regeneration, making the ultrathin BPH nanosheets attractive candidates for gas drying and membrane applications.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251766","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}
{"title":"Sodium into γ-Graphyne Multilayers: An Intercalation Compound for Anodes in Metal-Ion Batteries","authors":"Massimiliano Bartolomei, Giacomo Giorgi","doi":"10.1021/acsmaterialslett.4c01119","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01119","url":null,"abstract":"The bulk synthesis of γ-graphyne has been recently achieved and evidenced a multilayered structure, which suggests its potential exploitation as a substitute of graphite-based anode materials for metals heavier than lithium (Li). In fact, each of its regular pores of sub-nanometric size features an optimal environment for hosting a single sodium (Na) ion, as reported here by means of accurate electronic structure calculations. We show that the graphyne<i>/</i>Na ion coupling mimics that found on the graphene<i>/</i>Li ion in terms of metal-single layer interaction and equilibrium distance. More importantly, in contrast to what is found for graphite, we demonstrate that graphyne intercalation compounds with Na are thermodynamically stable and feature an optimal storage capacity of 372 mAh·g<sup>–1</sup>. These findings, together with a limited crystal structure expansion upon Na intercalation, a low metal diffusion barrier as well as high electrical conductivity, pave the way to the development of novel graphyne-based anodes for efficient Na-ion batteries.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251736","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}