Xiuyue Sun, Zihao Wo, Haowen Sun, Ni Yang, Xiwen Zhang
{"title":"Gelatin–Cellulose Nanofibril Aerogels Featuring Porous Sidewalls for Durable Solar Desalination","authors":"Xiuyue Sun, Zihao Wo, Haowen Sun, Ni Yang, Xiwen Zhang","doi":"10.1021/acsami.5c16351","DOIUrl":"https://doi.org/10.1021/acsami.5c16351","url":null,"abstract":"Solar-driven interfacial evaporation represents a promising strategy for sustainable freshwater production. However, its practical application is hindered by poor salt resistance and mechanical instability. Herein, an aerogel evaporator with vertically aligned channels was fabricated through directional freeze-drying, using gelatin/cellulose nanofibrils (CNF) as the porous matrix and carbon nanotubes (CNTs) as the photothermal component. Remarkably, by tuning gelatin/CNF ratios, pore size, distribution and sidewall pores were successfully controlled. These sidewall pores function as interchannel ion exchange units, thus promoting salt ion diffusion. Contrary to conventional understanding, the results demonstrate that larger pore size alone does not guarantee better salt resistance. Instead, an optimal balance between pore size and sidewall pore distribution leads to significantly improved salt resistance and higher evaporation rates. The optimized aerogel exhibits outstanding salt resistance, superior mechanical performance and long-term stability in solar desalination, exhibiting high evaporation rates of 2.25 kg·m<sup>–2</sup>·h<sup>–1</sup> (pure water) and 2.20 kg·m<sup>–2</sup>·h<sup>–1</sup> (3.5 wt % brine) under 1 sun. Furthermore, the aerogel demonstrates remarkable water purification capabilities for both acidic/alkaline wastewater and dye-contaminated solutions. This study reveals the critical role of sidewall pores in vertically aligned aerogel channels, providing special insights for balancing high salt resistance and rapid evaporation in aerogel evaporator design.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"8 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209803","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":"Heterogeneous Doping of Nanodiamond Grains with Exfoliated 2D NbSe2 Nanostructures for Highly Sensitive Ammonia Gas Sensors at Room Temperature","authors":"Adhimoorthy Saravanan, Bohr-Ran Huang, Deepa Kathiravan, Hsieh-Chih Tsai","doi":"10.1021/acsami.5c16578","DOIUrl":"https://doi.org/10.1021/acsami.5c16578","url":null,"abstract":"Herein, a first-time report details the development of a heterogeneous nanodiamond (ND) grain-niobium diselenide (NbSe<sub>2</sub>) hybrid for room-temperature ammonia (NH<sub>3</sub>) gas sensing. Exfoliated NbSe<sub>2</sub> nanorods, potentially formed via sonochemical exfoliation, exhibit semiconducting behavior with a band gap of 2.29 eV. The ND–NbSe<sub>2</sub> hybrid demonstrates higher NH<sub>3</sub> selectivity compared to pristine NbSe<sub>2</sub> and ND. This hybrid achieves a significantly higher response of 11.3% with faster response and recovery times (81.2 and 70.6 s) than those of ND (5.9%) and NbSe<sub>2</sub> (4.5%) at a lower concentration of 100 ppm. Also, the stability of the as-fabricated ND toward NH<sub>3</sub> gas is exceptional when compared to that of NbSe<sub>2</sub>. This explains the level of influence of ND on the present ND–NbSe<sub>2</sub> hybrid heterostructure. Moreover, the heterojunction formation with a change in the resistivity of the sample is involved in the sensing mechanism. This can be ascribed to the correlation of energy gaps between the ND grains (4.43 eV) and NbSe<sub>2</sub> nanorods (2.29 eV), which promotes electron transportation from the conduction band of NbSe<sub>2</sub> to ND at the applied voltage. In addition, the NbSe<sub>2</sub>–ND hybrids offer excellent stability for long-term gas detection. Furthermore, it is expected that this study will inspire the development of 2D-NbSe<sub>2</sub>–nanodiamond hybrid materials for advanced gas-sensing applications.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"25 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209804","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}
Greta Zvirzdine, Sarunas Zukauskas, Alma Rucinskiene, Enayat Mohsenzadeh, Raimonda Boguzaite, Almira Ramanaviciene, Maksym Pogorielov, Vilma Ratautaite, Arunas Ramanavicius
{"title":"Electrochemical Salicylic Acid Sensor Based on Molecularly Imprinted Polypyrrole","authors":"Greta Zvirzdine, Sarunas Zukauskas, Alma Rucinskiene, Enayat Mohsenzadeh, Raimonda Boguzaite, Almira Ramanaviciene, Maksym Pogorielov, Vilma Ratautaite, Arunas Ramanavicius","doi":"10.1021/acsami.5c11951","DOIUrl":"https://doi.org/10.1021/acsami.5c11951","url":null,"abstract":"This study aims to provide new insights into the development of an electrochemical salicylic acid (SA) sensor based on a molecularly imprinted polymer (MIP). Polypyrrole (Ppy) based MIP and nonimprinted polymer (NIP) layers were deposited on the platinum electrode and evaluated in a three-electrode electrochemical cell. The study used amperometry for monomer polymerization, cyclic voltammetry (CV) for the overoxidation of the polymer layer, and differential pulse voltammetry (DPV) for analyte detection. Selectivity was evaluated by comparing the electrochemical signals of SA with those of 3-hydroxybenzoic acid and melamine. Results confirm the selectivity of the electrochemical sensor. Density functional theory (DFT) calculations were performed to analyze the rebinding and recognition mechanism. The results of DFT calculations support the experimental findings. In conclusion, the polypyrrole-based MIP sensor exhibits higher selectivity and sensitivity toward salicylic acid detection compared to melamine and even to its isomer, 3-hydroxybenzoic acid (3-HBA).","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"114 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203923","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":"Surficial Pore Structure on Polyetheretherketone Implants Regulates Mechanical Properties to Promote Macrophage M2 Polarization","authors":"Yixuan Chen, Sida Liu, Gandong Zhou, Changning Sun, Minghai Ma, Rou Huang, Xing Li, Xiao Liang, Changquan Shi, Zhaowei Gao, Weiwei Wu, Xiaolong Yan, Lei Wang, Jing Han","doi":"10.1021/acsami.5c14803","DOIUrl":"https://doi.org/10.1021/acsami.5c14803","url":null,"abstract":"The surficial micro–nanostructure on polyetheretherketone (PEEK) can increase the biocompatibility of biomaterials and promote macrophage M2 polarization to induce soft tissue integration. However, because it is difficult to obtain a uniform and controllable surficial micro–nanostructure on PEEK, the regulation rules and underlying mechanisms for macrophage M2 polarization remain poorly understood. In this study, we used a hot pressing technique to fabricate uniform submicrometer porous structures with sizes of 200, 500, and 800 nm on PEEK material. These structures can significantly increase the hydrophilicity of the interface and decrease the stiffness of the materials. Furthermore, a cellular experiment was performed to investigate the optimal size of the submicrometer structure for macrophage M2 polarization, and 200 nm pores on PEEK can significantly promote macrophage polarization toward the reparative M2 phenotype, accompanied by increased secretion of cytokines such as TGF-β1 and Arg1. Indirect coculture assays further confirmed that these polarized macrophages enhanced the proliferation and migration of vascular endothelial cells and fibroblasts. Transcriptomic analysis and molecular biology experiments revealed that the 200 nm porous interface can lead to downregulation of Piezo1, Yap1, and NF-κB and upregulation of STAT6 and TGF-β1 in the process of macrophage M2 polarization. Moreover, the C57 mouse experiment showed the improved soft tissue integration surrounding the PEEK implants with 200 nm pores, accompanied by better vascularization and fibrosis. This study highlights that 200 nm porous PEEK implants can modulate macrophage M2 polarization to promote soft tissue integration, and this process relies on the activation of the Piezo1/TGF-β1 signaling pathway.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"37 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209801","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}
Jinkui Wang, Mujie Li, Zhaoxia Zhang, Tao Mi, Junyi Luo, Dawei He
{"title":"Genetically Engineered Glycosylphosphatidylinositol-Anchored Anti-GD2 Nanobody-Exosome Mimetics for Targeted Osteosarcoma Therapy In Vitro and In Vivo","authors":"Jinkui Wang, Mujie Li, Zhaoxia Zhang, Tao Mi, Junyi Luo, Dawei He","doi":"10.1021/acsami.5c12922","DOIUrl":"https://doi.org/10.1021/acsami.5c12922","url":null,"abstract":"This study focuses on the engineering of exosome mimetics (EMs) that are decorated with an antidisialoganglioside (GD2) nanobody for targeting osteosarcoma. We engineer the anti-GD2 nanobody coding vector into HEK-293T (293T) cells and fuse it with the decay-accelerating factor (DAF)-derived glycosylphosphatidylinositol (GPI) anchor signal peptide. The sequential extrusion method was used to produce the targeted EMs. These engineered GD2-targeted EMs (GD2-EMs) possess the same exosome markers as regular exosomes, are produced in large quantities, have a nanoscale size, and feature a surface anti-GD2 nanobody. Furthermore, they demonstrate increased internalization in osteosarcoma cells compared to unmodified EMs. In animal experiments using nude mice, the GD2-EMs exhibited superior tumor targeting, confirming their efficacy in vivo. In conclusion, the study successfully engineered anti-GD2 EMs, which showed promising results as a drug delivery system for osteosarcoma, indicating that engineering anti-GD2 EMs may be a viable approach for combating this disease.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"2 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203924","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}
Md Farhan Hossain, Ljalem Hadush Abrha, Amir Abdul Razzaq, Regan Ogilvie, William Charles Dirks, Haiden Studer, Christopher Poches, Bhubnesh Lama, Himal Oli, Santosh R. P. Bandlamudi, Xuguang Li, Krzysztof Pupek, Zhenzhen Yang, Tula R. Paudel, Weibing Xing
{"title":"Mechanistic Study of Functional Electrolyte Solvents for High-Voltage Lithium Batteries","authors":"Md Farhan Hossain, Ljalem Hadush Abrha, Amir Abdul Razzaq, Regan Ogilvie, William Charles Dirks, Haiden Studer, Christopher Poches, Bhubnesh Lama, Himal Oli, Santosh R. P. Bandlamudi, Xuguang Li, Krzysztof Pupek, Zhenzhen Yang, Tula R. Paudel, Weibing Xing","doi":"10.1021/acsami.5c16368","DOIUrl":"https://doi.org/10.1021/acsami.5c16368","url":null,"abstract":"The pervasive use of Ni-rich cathode active materials, e.g., LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811), for high-energy-density Li-ion batteries (LIBs) has been hindered by rapid battery capacity decay when cycled with high charge cutoff voltages due to electrolyte decomposition in the conventional carbonate solvent-based electrolytes, oxidative parasitic side reactions at the electrolyte/cathode interface, and irreversible phase changes in the cathode active materials leading to dissolution of transition metals into the electrolytes. Various functional electrolyte solvents have been studied to tackle the above technical challenges, yet the roles of individual solvents in the performance of LIBs remain poorly understood. In this study, we systematically investigate electrochemical performance mechanisms of fluorinated and organosilicon single solvents and cosolvents, for the first time, in high-voltage Li/NMC811 batteries, using electrochemical and analytical characterizations and density functional theory modeling. We observe that some unique combinations of the functional solvents can lead to exceptionally stable high-voltage cycle performance in the Ni-rich cathode-based LIBs. Our mechanistic study reveals that the synergistic effect of solvents plays a vital role in enabling electrochemical stability at both the Ni-rich cathode and the Li metal anode. Understanding the electrochemical performance mechanisms of functional solvents can greatly help in designing and formulating advanced electrolytes that enable the development of high-voltage, high-energy-density, long-cycle-life lithium batteries.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"74 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209805","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":"Enhanced Stability of Vanadium-Based Electrode Materials Using Multi-Component Hybrids for High-Performance Zinc-Ion Batteries","authors":"Zhiqiang Dai, Xueqing Zhang, Kittima Lolupiman, Chengwu Yang, Pattaraporn Woottapanit, Wanwisa Limphirat, Suttipong Wannapaiboon, Xinyu Zhang, Jiaqian Qin","doi":"10.1021/acsami.5c13283","DOIUrl":"https://doi.org/10.1021/acsami.5c13283","url":null,"abstract":"The limited availability of cathode materials for rechargeable aqueous zinc-ion batteries (ZIBs), which have great potential for grid-scale energy storage applications, remains a significant obstacle to development. In this study, we proposed a Li<sub>3</sub>VO<sub>4</sub>–LiV<sub>2</sub>O<sub>5</sub>-based (LiVO-w) nanocomposite structure obtained by simple high-temperature calcination and water washing as a high-performance cathode. The LiVO-w cathode demonstrates a high specific capacity (310.43 mAh g<sup>–1</sup> at 1 A g<sup>–1</sup> and 130.52 mAh g<sup>–1</sup> at 20 A g<sup>–1</sup>) and excellent cycling stability (100% capacity retention after 4000 cycles at 10 A g<sup>–1</sup> and 85.13% capacity retention after 10,000 cycles). In addition, ex situ X-ray diffraction (XRD) shows the structural transformation of LiVO-w during the self-assembly process. During the first charge process, the multivalent and multistructured LiVO-w undergoes an increase in the valence of V, accompanied by the generation of Zn<sub>3</sub>(OH)<sub>2</sub>V<sub>2</sub>O<sub>7</sub>·H<sub>2</sub>O on the surface of the matrix. The charge and discharge process after self-assembly mainly corresponds to the generation and decomposition of Zn<sub>3</sub>(OH)<sub>2</sub>V<sub>2</sub>O<sub>7</sub>·H<sub>2</sub>O. This excellent self-assembled matrix realizes the realization of LiVO-w cathodes with high capacity and high-capacity retention, representing a major advancement in the commercial development of ZIBs for the development of LiVO-w positive electrode materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"7 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203939","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":"Composition Regulation Enables Stable CsPbBr3/Cs4PbBr6 Glass Nanocomposites for Color-Rich Backlight Displays","authors":"Enrou Mei, Yanling Lin, Xiaojuan Liang, Weidong Xiang","doi":"10.1021/acsami.5c15674","DOIUrl":"https://doi.org/10.1021/acsami.5c15674","url":null,"abstract":"In this work, CsPbBr<sub>3</sub>/Cs<sub>4</sub>PbBr<sub>6</sub>@glass composites were synthesized by incorporating lead carbonate (PbCO<sub>3</sub>) into a lithium–aluminum–silicate–boron (Li–Al–Si–B) glass matrix. PbCO<sub>3</sub> decomposes to PbO, which reacts in situ with melt Br to form PbBr<sub>2</sub>, triggering CsPbBr<sub>3</sub>/Cs<sub>4</sub>PbBr<sub>6</sub> nucleation in Br-rich microdomains; CO<sub>2</sub> release concurrently creates stress-relieving micropores, outperforming direct PbBr<sub>2</sub> addition. This composite exhibited remarkable photoluminescence properties, with a photoluminescence quantum yield (PLQY) reaching as high as 86.71%. In an accelerated aging experiment conducted over 120 h, the fluorescence intensity was maintained at 95% of its original value. Even after 60 days of immersion in water, the luminescence intensity remained at 94% of the initial intensity, demonstrating its outstanding resistance to environmental degradation. To further explore its potential for display applications, we prepared a CsPbBr<sub>3</sub>/Cs<sub>4</sub>PbBr<sub>6</sub>/CsPbBrI<sub>2</sub>@glass@polystyrene (PS) film. This film exhibited an impressive color gamut, covering 123% of the National Television System Committee (NTSC) 1953 standard and 91.3% of the ITU-R Recommendation BT.2020 (Rec.2020) standard. The high PLQY and excellent stability of CsPbBr<sub>3</sub>/Cs<sub>4</sub>PbBr<sub>6</sub>@glass make it highly suitable for LCD applications and offer broad prospects for industrial-scale production.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"121 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209802","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}
Christine Ilona Seidl, Bonan Zhao, Xinye Gao, Rüdiger Berger, Lin Jian, Kaloian Koynov, Meike Gangluff, Rivka Fontijn, Lu Su, Jeroen Bussmann, Heyang Zhang, Matthias Barz
{"title":"Polypept(o)ide Based Biodegradable Cylindrical Polymer Brushes: Controlling Size, Shape, Surface Functionality, and Stability.","authors":"Christine Ilona Seidl, Bonan Zhao, Xinye Gao, Rüdiger Berger, Lin Jian, Kaloian Koynov, Meike Gangluff, Rivka Fontijn, Lu Su, Jeroen Bussmann, Heyang Zhang, Matthias Barz","doi":"10.1021/acsami.5c15018","DOIUrl":"https://doi.org/10.1021/acsami.5c15018","url":null,"abstract":"<p><p>Cylindrical polymer brushes (CPBs) enable remarkable control over nanoparticle properties solely through sequential polymerization. The spatial dimensions and functionality of the resulting polymeric nanoparticles can be adjusted by the ratio of backbone to side chain length and the chemical nature of both parts. In this work, we present a convenient and straightforward synthetic pathway to polypept(o)ide-based CPBs using a \"grafting-from\" strategy utilizing poly-l-lysine (pLys) as the macroinitiator backbone and polysarcosine (pSar) as the side chain. End-capping of pSar chains with azido-butyric acid pentafluorophenyl ester enables facile surface functionalization by click chemistry (e.g., dye labeling). This strategy allows for straightforward control over nanoparticle size (<i>R</i><sub>h</sub> from 12 to 41 nm), shape (aspect ratio from 1.7 to 8.3), and molecular weights (from 350 to 2980 kg mol<sup>-1</sup>). Despite the high grafting density of pSar side chains from the pLys backbone (>85%), enzymatic degradation is feasible by the natural protease B from<i>Streptomyces griseus</i>and enables the analysis of pSar side chains upon cleavage (<i>Đ</i> = 1.03-1.04). Interestingly, these CPBs exhibit thermal stability in phosphate-buffered saline at elevated temperatures (60 °C for 24 h) and display notable circulation in zebrafish embryos (up to 3 days). Therefore, CPBs based on polypept(o)ides not only allow for precise tuning of size, shape, and surface functionality but also display high biocompatibility and extended circulation time in zebrafish, leveraging the stealth-like properties of pSar.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204956","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}
Jake Heinlein, Yulian He, Yuqi Song, Tianshuo Zhao, Yingjie Feng, Rito Yanagi, Yamuna Paudel, Matthew Y. Sfeir, Conrad Kocoj, Peijun Guo, Shu Hu, Lisa Pfefferle
{"title":"Engineering Direct S-Scheme Heterojunctions with Ultrafast Interfacial Charge Transfer: A Case Study on 2-Dimensional α-Fe2O3/Cu2O Interfaces","authors":"Jake Heinlein, Yulian He, Yuqi Song, Tianshuo Zhao, Yingjie Feng, Rito Yanagi, Yamuna Paudel, Matthew Y. Sfeir, Conrad Kocoj, Peijun Guo, Shu Hu, Lisa Pfefferle","doi":"10.1021/acsami.5c12210","DOIUrl":"https://doi.org/10.1021/acsami.5c12210","url":null,"abstract":"Longer wavelengths of light contain less energy but comprise more of the solar spectrum, making them important to incorporate into any process aiming for high efficiency. Here, we developed a novel redox-mediated synthetic mechanism to construct a heterojunction with strongly coupled interfaces. Specifically, an α-Fe<sub>2</sub>O<sub>3</sub>/Cu<sub>2</sub>O/CuO nanosheet composite was synthesized, forming an S-scheme α-Fe<sub>2</sub>O<sub>3</sub>/Cu<sub>2</sub>O electronic interface, a burgeoning class of materials designed to upconvert longer wavelengths of light and utilize solar energy more effectively. Through a series of experiments including X-ray photoelectron spectroscopy (XPS), ultraviolet–visible (UV–Vis) diffuse reflectance spectroscopy (UV–Vis-DRS), electrochemical impedance spectroscopy (EIS), and photocatalytic measurements, we were able to fully confirm the electronic structure of the α-Fe<sub>2</sub>O<sub>3</sub>/Cu<sub>2</sub>O interfacial heterojunction. These characterizations demonstrate the S-scheme flow of electrons, which is further supported by COMSOL numerical simulations. The successful formation of the S-scheme heterojunction is made possible through the direct Fe–O–Cu covalent bonding at the interface. These bonds provide ultrafast interfacial charge transfer pathways on picosecond time scales followed by long-lived charge-separated states, as quantified by our transient optical experiments. The proposed redox-mediated synthetic strategy provides a valuable guideline for constructing effective solid heterojunctions with strongly coupled interfaces, which are desirable for various applications in catalysis, energy storage, electronics, photovoltaics, and beyond.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"11 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209799","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}