Xiaoqing Wu, Tingting Cai, Qian Wu, Jie Meng, Wenqi Wang, Wentao Li, Chuanpeng Hu, Xiaolong Zhang, Daoai Wang
{"title":"Droplet-Based Triboelectric Nanogenerators with Needle Electrodes for Efficient Water Energy Harvesting","authors":"Xiaoqing Wu, Tingting Cai, Qian Wu, Jie Meng, Wenqi Wang, Wentao Li, Chuanpeng Hu, Xiaolong Zhang, Daoai Wang","doi":"10.1021/acsami.4c17442","DOIUrl":"https://doi.org/10.1021/acsami.4c17442","url":null,"abstract":"With the advent of droplet-based triboelectric nanogenerators (D-TENGs), methods for converting raindrop kinetic energy to electrical energy have developed rapidly. However, current D-TENG designs suffer from slow solid–liquid interface separation speeds and susceptibility to liquid residues. These issues compromise the output performance of D-TENGs and limit their applications in high-power electrical appliances. To address this, this study presents a needle electrode droplet-based triboelectric nanogenerator (NED-TENG). The needle electrode functions as the top electrode, optimizing solid–liquid contacts and efficiently harvesting raindrop kinetic energy by leveraging the triboelectric and electrostatic induction mechanisms. This needle electrode is made from one end of a copper wire, with its other end directly connected to the energy harvester. This setup positions all of the wiring on the back of the substrate, accelerating liquid separation, mitigating residue formation, and simplifying device fabrication. Upon assembly of the device, several factors influencing the performance of the fabricated D-TENG and its action mechanisms are explored to improve its output efficiency. Experimental results reveal that the designed D-TENG only requires 6 s to saturate the surface charge of its polytetrafluoroethylene film, achieving a short-circuit current (I<sub>SC</sub>) of up to 4.76 mA and an output voltage (V<sub>0</sub>) of up to 563 V. Overall, this study offers a straightforward and effective approach for harvesting kinetic energy from rainwater.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"89 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462189","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}
Melisa Wei Ning Leoi, Xin Ting Zheng, Yong Yu, Jiajia Gao, Deborah Hui Shan Ong, Clarence Zhi Han Koh, Peng Chen, Le Yang
{"title":"Redefining Metal Organic Frameworks in Biosensors: Where Are We Now?","authors":"Melisa Wei Ning Leoi, Xin Ting Zheng, Yong Yu, Jiajia Gao, Deborah Hui Shan Ong, Clarence Zhi Han Koh, Peng Chen, Le Yang","doi":"10.1021/acsami.4c19307","DOIUrl":"https://doi.org/10.1021/acsami.4c19307","url":null,"abstract":"As a broad class of porous nanomaterials, metal organic frameworks (MOFs) exhibit unique properties, such as broad tunability, high stability, atomically well-defined structure, and ordered uniform porosity. These features facilitate the rational design of MOFs as an outstanding nanomaterial candidate in biosensing, therapeutics delivery, and catalysis applications. Recently, novel modifications of the MOF nanoarchitecture and incorporation of synergistic guest materials have been investigated to achieve well-tailored functional design, gradually bridging the fundamental gap between structure and targeted activity. Specifically, the burgeoning studies of MOF-based high-performance biosensors have aimed to achieve high sensitivity, selectivity, and stability for a large variety of analytes in different sensing matrices. In this review, we elaborate the key roles of MOF nanomaterials in biosensors, including their high stability as a protective framework for biomolecules, their intrinsic sensitivity-enhancing functionalities, and their contribution of catalytic activity as a nanozyme. By examining the main structures of MOFs, we further identify varied structural engineering approaches, such as precursor tuning and guest molecule incorporation, that elucidate the concept of the structure–activity relationship of MOFs. Furthermore, we highlight the unique applications of MOF nanomaterials in electrochemical and optical biosensors for enhanced sensor performances. Finally, the challenges and future perspectives of developing next-generation MOF nanomaterials for biosensor applications are discussed.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"13 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470601","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}
Katarzyna M. Wulfmeier, Juan Pellico, Pedro Machado, M. Alejandra Carbajal, Saskia E. Bakker, Rafael T. M. de Rosales, Kavitha Sunassee, Philip J. Blower, Vincenzo Abbate, Samantha Y. A. Terry
{"title":"In Vitro and In Vivo Radiotoxicity and Biodistribution of Thallium-201 Delivered to Cancer Cells by Prussian Blue Nanoparticles","authors":"Katarzyna M. Wulfmeier, Juan Pellico, Pedro Machado, M. Alejandra Carbajal, Saskia E. Bakker, Rafael T. M. de Rosales, Kavitha Sunassee, Philip J. Blower, Vincenzo Abbate, Samantha Y. A. Terry","doi":"10.1021/acsami.4c21700","DOIUrl":"https://doi.org/10.1021/acsami.4c21700","url":null,"abstract":"Thallium-201 (<i>t</i><sub>1/2</sub> = 73 h) emits around 37 Auger and other secondary electrons per decay and is highly radiotoxic when internalized into cancer cells. However, the lack of effective chelators hinders its application in molecular radiotherapy. This study evaluates Prussian blue nanoparticles, coated with citric acid (<sup>201</sup>Tl-caPBNPs) or chitosan (<sup>201</sup>Tl-chPBNPs), as a <sup>201</sup>Tl delivery vehicle compared with unbound <sup>201</sup>Tl<sup>+</sup>. Cellular uptake and efflux kinetics and radiotoxicity using clonogenic and γH2AX DNA damage assays were evaluated in vitro for both nanoparticle types. Subcellular localization was also assessed using electron microscopy with energy-dispersive X-ray spectroscopy. Biodistribution of <sup>201</sup>Tl-chPBNPs was evaluated in vivo in mice bearing subcutaneous A549 tumor xenografts, using single photon computed tomography imaging and ex vivo tissue counting. Compared with unbound <sup>201</sup>Tl<sup>+</sup>, <sup>201</sup>Tl-chPBNPs showed higher cellular uptake, while <sup>201</sup>Tl-caPBNP uptake was reduced. Both showed delayed efflux of <sup>201</sup>Tl from cancer cells. PBNPs prelocalized within cells enhanced the capture and retention of <sup>201</sup>Tl<sup>+</sup> ions. Both types of PBNPs accumulated in cytoplasmic vesicular compartments and were not visible in the nuclei. Furthermore, <sup>201</sup>Tl-radiolabeled chPBNPs but not <sup>201</sup>Tl-caPBNPs showed significantly greater radiotoxicity than unbound <sup>201</sup>Tl<sup>+</sup> per Becquerel of radiotoxicity provided in media, resulting from their higher uptake and delayed efflux. However, when corrected for the greater activity accumulated in cells and delayed efflux, the radiotoxicity of <sup>201</sup>Tl-chPBNPs was lower than that of unbound <sup>201</sup>Tl<sup>+</sup>, possibly due to differences in subcellular localization. These findings highlight the potential of chPBNPs for enhancing the uptake and retention of <sup>201</sup>Tl in cancer cells and development of targeted radionuclide therapy.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"20 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462073","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}
{"title":"Design of an Advanced Composite Surface for Low Ice Adhesion: Integrating Active and Passive Anti-/Deicing Strategies to Disrupt Icing Interfaces","authors":"Yuanhui Ni, Xianxian Cui, Zehui Zhao, Jingru Quan, Guangwei Liu, Xiaolin Liu, Huawei Chen","doi":"10.1021/acsami.4c21344","DOIUrl":"https://doi.org/10.1021/acsami.4c21344","url":null,"abstract":"Icing presents substantial economic challenges and endangers equipment safety. Contemporary anti-icing research emphasizes the integration of active and passive technologies, with a particular focus on mitigating ice adhesion for more efficient anti-icing and deicing solutions. In this study, a multilayer composite antideicing surface is developed, integrating energy storage, photo-/electro-thermal functionalities, and superslippery properties. The top quasi-solid slippery layer, composed of epoxy resin embedded with oil-stored graphene nanoparticles, provides stable hydrophobic performance for various water-based liquids, reducing ice adhesion to approximately 25 kPa. Furthermore, the energy storage layer at the base introduces heterogeneity in the icing timeline across regions, leveraging volumetric expansion during the water phase transition to disturb the ice interface, achieving adhesion reductions to around 12 kPa. The intermediate layer features photo-/electro-thermal capabilities, enabling surface temperature elevation upon application of electrical or optical energy, melting interfacial ice, and forming a liquid film. This process disrupts the frozen interface, further lowering the ice adhesion force to below 1 kPa. The synergistic interaction between photo-/electro-thermal effects and the superslippery surface significantly enhances the anti-icing and deicing efficiency of the composite structure. These findings offer promising advancements for engineering applications requiring high-efficiency active and passive anti-icing/deicing strategies.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"82 2 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470595","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}
{"title":"Synergistic Surface–Interface Catalysis in Potassium-Loaded Cu/CoOx Catalysts to Boost Ethanol Production from CO2 Hydrogenation","authors":"Yunpeng Zhang, Guoli Fan, Lirong Zheng, Feng Li","doi":"10.1021/acsami.4c18112","DOIUrl":"https://doi.org/10.1021/acsami.4c18112","url":null,"abstract":"Nowadays, ethanol production from CO<sub>2</sub> hydrogenation has emerged as a viable pathway for CO<sub>2</sub> capture and efficient utilization. However, catalysts based on nonprecious metals still face significant challenges in achieving high catalytic efficiency for ethanol production. In this study, we constructed K-incorporated CuCo-based catalysts, which were obtained from Cu–Co–Al layered double hydroxide precursors, for efficient CO<sub>2</sub> hydrogenation to produce ethanol. It was shown that the incorporation of K into catalysts could finely tune the electronic structures of copper and cobalt species, thereby promoting the formation of substantial surface Co<sup>2+</sup>–O<sub>v</sub>–Co<sup>2+</sup> (O<sub>v</sub>: oxygen vacancy), Co–O–K, and Cu<sup>+</sup>–O–K structures. Notably, as-constructed Cu/CoO<sub><i>x</i></sub> catalyst bearing a K loading of 3 wt % achieved an impressively high ethanol selectivity of 38.8% at 200 °C as well as a remarkably high ethanol production rate of 2.76 mmol<sub>EtOH</sub>·g<sub>cat</sub><sup>–1</sup>·h<sup>–1</sup> at 260 °C. Based on multiple structural characterizations, spectroscopic analysis, and density functional theory calculations, it was uncovered that defective CoO<sub><i>x</i></sub> and Cu<sup>+</sup>–O–K structures promoted the generation of formate intermediates during CO<sub>2</sub> hydrogenation, and meanwhile, the effective coadsorption of K<sup>+</sup> and Cu<sup>+</sup> stabilized formate intermediates. Accordingly, active K<sup>+</sup>, Cu<sup>+</sup> and CoO<sub><i>x</i></sub> species over CuCo-based catalysts exhibited synergistic catalysis, which significantly improved the CH<sub><i>x</i></sub>-HCOO coupling process at K-loaded Cu/CoO<sub><i>x</i></sub> interfaces to boost ethanol production. This study presents a novel surface–interface engineering approach for designing non-noble-metal-based catalysts for efficient ethanol production from CO<sub>2</sub> hydrogenation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"38 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470596","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}
{"title":"Effect of Fluorine Contamination from Multilayer Dielectric Grating Fabrication on Picosecond-Laser-Induced Damage Resistance","authors":"Kun Shuai, Keqiang Qiu, Xiaofeng Liu, Yuanan Zhao, Guang Xu, Dawei Li, Miaomiao Zhang, Yan Zhou, Jian Sun, Yun Cui, Yilin Hong, Yaping Dai, Jianda Shao","doi":"10.1021/acsami.4c21677","DOIUrl":"https://doi.org/10.1021/acsami.4c21677","url":null,"abstract":"Contamination introduced by multilayer dielectric grating (MLDG) fabrication increases the risk of laser-induced damage when exposed to intense laser fields, consequently reducing the laser-induced damage resistance of MLDGs in picosecond–petawatt laser systems. While considerable efforts have focused on cleaning methods to minimize contamination, studies on optimizing the etching process remain limited. In this study, two different beam-current etching protocols were employed in fabricating MLDGs and thin films to comprehensively evaluate the adverse effects of subsurface defects introduced by the etching process. The results revealed that the etching process introduced penetration of fluorine contamination defects, and the degree of fluorine contamination increased in the high-beam etching (HBE) protocol. Furthermore, the quantity of typical shallow damage pits exhibited a significant increase in the HBE films under 7.6 ps laser irradiation, and the 0% laser-induced damage thresholds of gratings and thin films fabricated through the low-beam etching (LBE) protocol achieved significant improvements of 33% and 26%, respectively, compared to those obtained with the HBE protocol. The LBE protocol will be employed in meter-scale grating fabrication to improve picosecond laser damage resistance.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"3 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470603","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}
Kohei Okubo, Haruka Yoshino, Hitoshi Miyasaka, Hitoshi Kasai, Kouki Oka
{"title":"Iodine-Based Chemical Polymerization Enables the Development of Neat Amorphous Porous Organic Polymers","authors":"Kohei Okubo, Haruka Yoshino, Hitoshi Miyasaka, Hitoshi Kasai, Kouki Oka","doi":"10.1021/acsami.4c22197","DOIUrl":"https://doi.org/10.1021/acsami.4c22197","url":null,"abstract":"Amorphous porous organic polymers (POPs), with high porosity and high chemical and thermal stability, have been investigated for various applications. Most amorphous POPs are synthesized by electropolymerization or chemical polymerization. However, nonhomogeneous film formation in electropolymerization and residual metal-derived impurities in chemical polymerization are challenges. This study developed a novel chemical polymerization method for amorphous POPs using iodine as an oxidant. Specifically, we synthesized a representative amorphous POP, polytriphenylamine (pTPA). The pTPA was obtained as a powder through solution polymerization and as a thin film via vapor-assisted polymerization. Postreaction, ethanol was used to remove iodine completely. Notably, even though pTPA was constructed from rigid structures, the nitrogen-induced gate-opening phenomenon was exhibited for the first time as amorphous POPs. These results demonstrate that impurity-free amorphous POPs exhibit inherent flexibility against their rigid chemical structure. The novel iodine-based chemical polymerization enables us to synthesize neat amorphous POPs and to explore their pure functions.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"35 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462075","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}
{"title":"MoS2-Coated MOF-Derived Hollow Heterostructures for Electromagnetic Wave Absorption","authors":"Yue Sun, Yanxiang Wang, Dongming Liu, Haotian Jiang, Bohan Ding, Jinghe Guo, Shichao Dai","doi":"10.1021/acsami.4c23019","DOIUrl":"https://doi.org/10.1021/acsami.4c23019","url":null,"abstract":"Structural design constitutes one of the crucial approaches for augmenting the wave-absorbing capacity of electromagnetic wave (EMW) absorbers, and the incorporation of cavity structures represents a typical methodology therein. In this work, the MoS<sub>2</sub>-coated metal–organic framework (MOF)-derived Hollow-MoS<sub>2</sub>@CNS@CoS<sub>2</sub> composite materials (HCNSs) were prepared by combining tannic acid-protected etching, carbonization, and hydrothermal methods. Especially, HCNS700, which possessed both a hollow structure and a layered heterogeneous structure, demonstrated excellent EMW absorption properties. It attained an optimal reflection loss of −63.63 dB at 16.4 GHz and −58.97 dB at 10.4 GHz, along with an extremely low thickness. In addition, the radar cross section simulation demonstrated that HCNS700 possessed excellent electromagnetic stealth capabilities. Its excellent performance is put down to the multiple loss mechanisms brought by the special structure, including multiple scattering of EMW caused by the hollow structure, interface polarization caused by the heterogeneous interfaces of MoS<sub>2</sub>, CoS<sub>2</sub>, and the carbon matrix, dipole polarization caused by element doping and defects, and optimization of impedance matching by MoS<sub>2</sub>. This research offers a novel concept for the design of EMW-absorbing materials with hollow heterogeneous layered structures.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"15 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462077","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}
Connor J. MacRobbie, Navid Assi, Jack Ehling, Anqi Wang, John Z. Wen
{"title":"Superhydrophobic Nanoenergetic Combustion for Underwater Cavity Generation","authors":"Connor J. MacRobbie, Navid Assi, Jack Ehling, Anqi Wang, John Z. Wen","doi":"10.1021/acsami.4c21880","DOIUrl":"https://doi.org/10.1021/acsami.4c21880","url":null,"abstract":"Generation of underwater cavities requires rapid expansion of a gaseous volume, which may be achieved via the exothermic reactions of nanoenergetics. This work reports first the formation of combustion-induced vaporous cavitation and its dynamics. A superhydrophobic, stearic acid (SA)-coated, core–shell nanocomposite was developed to address the challenges associated with the high hydrophilicity of metallic nanoparticles and the subsequent deactivation of aluminum by water, which hinders ignition and flame propagation. With 1% SA, Al@CuO@SA combusted violently, achieving a maximum cavity volume above 25 mL and a cavity growth rate of up to 13 L/s using only 20 mg of material. 5% SA allowed Al@CuO@SA to stay submerged for 2 weeks and retain excellent reactivity. The combustion performance was tuned by adjusting the sample composition to control the reactivity and the material properties of the nanoenergetics. The rates of cavity growth and decay were investigated using high-speed imaging and analyzed in a nondimensional analysis to demonstrate the key characteristics of combustion-induced cavitation. It was observed that the cavity generation process occurs across several stages including SA decomposition around 300 °C, creating a small bubble surrounding the sample, which reduces heat loss to water and promotes the thermite reaction, and the exothermic reaction at 600 °C, resulting in the formation and rapid growth of the major cavity. Thermal analyses during controlled heating and during combustion provided insights into the reaction mechanisms.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"50 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470628","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}