ACS Applied Materials & Interfaces最新文献

{"title":"Self-Aligned Fluorinated-Organic Ligand for Boosting the Performance of Perovskite Solar Cells","authors":"Yoon Ho Lee, Yuanhao Tang, Raunak Dani, Won-June Lee, Jeong Hui Kim, Gangsan Lee, Jiaonan Sun, Ke Ma, Su Hye Jeong, Wenzhan Xu, Jianguo Mei, Letian Dou","doi":"10.1021/acsami.5c03012","DOIUrl":"https://doi.org/10.1021/acsami.5c03012","url":null,"abstract":"Surface passivation is evident to be one of the most efficient approaches to achieve high efficiency with superior stability of perovskite solar cells (PeSCs). However, most previous approaches to surface passivation involve adding an additional coating process either before or after perovskite film fabrication, thereby introducing an extra processing step and significantly increasing production costs. Here, a simple yet novel one-step interfacial passivation approach was implemented by utilizing the self-aligning properties of fluorinated organic ligands (F4TmI) within a perovskite precursor solution. The inherent propensity of the ligand to spontaneously anchor onto the surface of perovskite guides the crystallization process of perovskites, thus largely enhancing the device performance and humidity stability. The optimized F4TmI-based devices achieved an efficiency of 21.1%, surpassing that of the control (19.8%). Moreover, the device stability significantly improved after the incorporation of F4TmI, maintaining 78.9 and 95.1% of its initial efficiency after aging at 60 °C and 60% relative humidity, respectively, for 330 h.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"3 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875909","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":"Atomic Defect-Directed Epitaxial Growth of Multimetallic Nanorods for High-Efficiency Alcohol Electro-Oxidation","authors":"Yue Liu, Bing Lan, Yiyi Fan, Dongling Wang, Yifei Cao, Fan Zhang, Xiaobin Xie","doi":"10.1021/acsami.5c05024","DOIUrl":"https://doi.org/10.1021/acsami.5c05024","url":null,"abstract":"Site-selective epitaxial growth of metals onto shaped nanoparticles represents a versatile strategy for tailoring nanostructures to optimize the optical and catalytic properties. In this study, we systematically elucidate the critical factors governing the epitaxial growth of silver and platinum atoms onto gold nanorods (Au NRs), revealing that atomic defects on the Au NR surface dictate the deposition sites of Ag and Pt. By precisely modulating epitaxial growth conditions and density of surface atomic defects, we achieve the synthesis of dumbbell-shaped (DS) and thorny-shell (TS) structured Au-AgPt NRs. Notably, the DS-Au-AgPt_0.24 NR catalyst demonstrated exceptional catalytic performance in alcohol fuel cell reactions, driven by their abundant atomic defects and strong strain effects localized at the crown structure. For ethylene glycol electro-oxidation, these DS-Au-AgPt_0.24 NRs achieved a mass activity of 23.5 A mg_Pt^–1 and a specific activity of 156.9 mA cm^–2, which were 4.1 and 11.2 times higher than that of commercial platinum–carbon (Pt/C) catalysts (5.7 A mg_Pt^–1 and 14.0 mA cm^–2), respectively. Our findings not only advance the mechanistic understanding of defect-mediated epitaxial growth in multimetallic systems but also provide a blueprint for designing high-performance catalysts through atomic-scale structural engineering.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"14 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876334","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":"MnCo2O4 as a Photothermal Modifier for BiVO4 Photoanode to Achieve Efficient Photoelectrochemical Water Oxidation","authors":"Haolun Li, Mingxin Lyu, Yanhua Lai, Xingxing Cheng, Zhen Dong","doi":"10.1021/acsami.5c04711","DOIUrl":"https://doi.org/10.1021/acsami.5c04711","url":null,"abstract":"Spinel oxides are widely used to enhance photoanodes’ photoelectrochemical (PEC) water oxidation performance. In this paper, we demonstrate that a p-type photothermal MnCo₂O₄ layer, inserted between BiVO₄ and FeOOH cocatalysts, can significantly enhance PEC performance. On the one hand, the charge recombination is greatly suppressed since p-type MnCo₂O₄ can form a p–n heterojunction with n-type BiVO₄. On the other hand, upon near-infrared (NIR) light irradiation, the deposited MnCo₂O₄ shows excellent photothermal conversion performance that can further facilitate charge transfer and accelerate the water oxidation process by elevating the operating temperature. In addition, the FeOOH cocatalyst is introduced to fully utilize the holes reaching the surface and further enhance the surface oxygen evolution kinetics. Consequently, the carefully constructed BiVO₄/MnCo₂O₄/FeOOH photoanode shows excellent photocurrent (4.71 mA cm^–2) at 1.23 V vs RHE (V_RHE) and superior applied bias photon-to-current efficiency (1.62%) at 0.6 V_RHE. The photocurrent density maintains more than 90% of the initial photocurrent after 4 h of combined solar and NIR light irradiation. Enhancing the PEC catalytic activity of photoelectrodes using photothermal materials is a simple and effective strategy, which can be used to explore PEC activity enhancement in other photoelectrodes.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"3 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875915","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":"Electrochemical Methane Reforming on La0.5Ce0.5Fe0.5Ni0.5O3−δ Anode in Solid Oxide Electrolysis Cells","authors":"Wenxin Fu, Yige Guo, Jianqiu Zhu, Xiaomin Zhang, Linjuan Zhang, Yuefeng Song, Guoxiong Wang, Xinhe Bao","doi":"10.1021/acsami.5c01874","DOIUrl":"https://doi.org/10.1021/acsami.5c01874","url":null,"abstract":"Coupling the partial oxidation of methane (POM) to the anode of solid oxide electrolysis cells (SOECs) can significantly decrease the open-circuit voltage and electrical energy consumption of the SOECs. However, developing advanced anode for SOEC to selectively convert CH₄ to syngas still remains a great challenge. Herein, we find that Ce substitution at the A-site of La_0.5Ce_0.5Fe_0.5Ni_0.5O_3−δ can effectively alter the chemical state and coordination environment of Ni with the generation of NiO particles, and the air activation could further regulate the oxygen vacancy concentration and decrease the size of NiO particles, which both contribute to the enhanced POM performance with CH₄ conversion of 45.20% and CO selectivity of 92.67% at 650 °C. Moreover, the introduction of POM to the anode could remarkably decrease the electrical energy consumption for CO production from 3.64 kWh m^–3 of conventional SOECs to 0.86 kWh m^–3 of CH₄-assisted SOECs. This study provides an effective strategy for improving the electrochemical performance of CO₂ electrolysis in SOECs while simultaneously converting CH₄ to syngas at the anode.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"53 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876330","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":"Revealing Microstructured Surface Critical Heat Flux Degradation Mechanisms and Synergistic Pool Boiling Enhancement in Fluorinated Fluids","authors":"Leymus Yong Xiang Lum, Pengfei Liu, Hanyang Ye, Jin Yao Ho","doi":"10.1021/acsami.4c22543","DOIUrl":"https://doi.org/10.1021/acsami.4c22543","url":null,"abstract":"Fluorinated dielectric fluids are widely utilized as heat transfer fluids for two-phase cooling of electronics, capitalizing on the fluids’ large latent heat release during boiling for efficient heat flux removal. Recent studies have optimized surface micro/nanostructures on aluminum alloy through chemical etching, achieving more than 2× enhancements in boiling heat transfer coefficients (HTCs) of these fluids compared to plain surfaces. However, these microengineered surfaces suffer from critical heat flux (CHF) reduction of nearly 40%, with the mechanisms driving this CHF reduction remaining unclear. Here, we investigate the mechanism resulting in the poor CHF of microstructured surfaces and develop a guideline to synergistically enhance the HTC and CHF of these surfaces. Immersion boiling tests in fluorinated and nonfluorinated fluids, coupled with wickability and elemental analysis, revealed that surface degeneration─caused by fluorine deposition forming C–F bonds with adventitious carbon─has minimal impact on CHF in fluorinated fluids. To further verify that surface degeneration is not responsible for CHF reduction, pool boiling experiments with cavity sizes from 1 to 5 μm identified the 5 μm cavity surface, AM-H(400)E(5), as achieving the highest HTC in both HFE-7100 and ethanol. However, CHF reductions of 30–50% were consistently observed, regardless of whether the surface transitioned to hydrophobicity or retained superhydrophilicity. Arising from this investigation, it is concluded that the increased nucleation site density on AM-H(400)E(5), which leads to the overcrowding of bubbles, is the primary cause of CHF reduction. To overcome these limitations, we devise a method of hierarchical addition of microstructures on macro-fins to simultaneously enhance HTC and CHF, creating a single-process two-tier hierarchical structure by leveraging on AM to fabricate the macrostructures. The two-tier macro/microstructure design has successfully enhanced HTC and CHF by 99 and 202.2%, respectively, compared to the best single-tier microstructured surface. This approach not only effectively delay undesirable vapor layer formation but also provides a robust guideline for enhancing boiling performance in other fluorinated fluids, including refrigerants R134a and R1234ze(E).","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"14 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875862","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":"Cascade DNA Structural Transitions Enable Stimuli-Responsive Hydrogels","authors":"Michael Shao Min Ho, Alycia Zi Ting Lim, Yujie Ke, Wei Wei Loh, Xin Ting Zheng, Le Yang, Zhaogang Dong, Fuke Wang, Jason Y. C. Lim, Yuwei Hu","doi":"10.1021/acsami.5c01581","DOIUrl":"https://doi.org/10.1021/acsami.5c01581","url":null,"abstract":"Cascade interactions are fundamental to enzyme catalysis and cellular activities, enabling dynamic and adaptive responses to environmental stimuli. DNA-based cascade systems have been widely employed to mimic biological processes, such as immune responses and DNAzyme catalysis, achieved mainly through the hybridization interaction. Herein, we present a cascade DNA system involving single-stranded sequences, noncanonical cofactor-bridged duplexes, and canonical duplexes to construct and dissociate hydrogel matrices. In this work, thymine-rich oligonucleotides (T-strands) exist as single-stranded random coils in a buffer at pH 7.2. Upon the introduction of a low-molecular-weight cofactor, melamine (MA), a supramolecular noncanonical configuration, termed the T-MA-T duplex, is formed. Subsequent addition of adenine-rich oligonucleotides (A-strands) to the system leads to the replacement of MA cofactors and the formation of more energetically favorable canonical A-T duplex structures. These consecutive structural transitions are further utilized as dynamic bridging elements in stimuli-responsive DNA hydrogels, facilitating liquid–hydrogel–liquid phase transitions. Moreover, we demonstrate precisely controlled release profiles of doxorubicin from the DNA hydrogel. This approach, leveraging both noncanonical and canonical DNA configurations in triggered cascade structural transitions, opens avenues for developing molecular switches, electronic nanodevices, adaptive materials, and other advanced applications.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"15 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875906","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":"Frontiers in Bioinspired Polymer-Based Helical Nanofibers from Electrospinning","authors":"Pengpeng Li, Jiahao Zhang, Xinlong Liu, Zifan Xu, Xin Zhang, Jinsong Ma, Guohua Sun, Lianlong Hou","doi":"10.1021/acsami.5c04110","DOIUrl":"https://doi.org/10.1021/acsami.5c04110","url":null,"abstract":"Helices are among the most significant structures in nature, representing an emerging group of materials distinguished by their unique helical geometry. Recently, helical nanofibers have attracted considerable attention due to their exceptional structural characteristics and versatile applications in various fields, including tissue engineering, biomedicine, nanotechnology, and chiral materials. Therefore, developing methods to fabricate biomimetic helical fibers on demand, which can exhibit a diverse range of physical properties and forms, is of great interest across multiple disciplines. Despite the significant interest in helical fibrous materials, the fabrication of such complex structures at the micro- or nanoscale level remains a major challenge. Electrospinning offers a simple and versatile technique for producing micro- and nanofibers in various helical shapes. This review systematically summarizes and classifies the state-of-the-art advancements in electrospun helical nanofibers into four categories based on their forming mechanisms: viscoelastic asymmetric contraction, bending instability motion, jet-induced buckling response, and rotary winding molding. Additionally, the recent applications of these helical nanofibrous materials in areas such as environmental remediation, interactive textiles, and biomedical engineering are also summarized. Furthermore, the current challenges and future perspectives in the field are put forward. We anticipate that the insights provided will contribute to the rational design of advanced artificial helical materials, thereby enhancing their practical applications in the future.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"136 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875912","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":"Breaking the Activity-and-Selectivity Seesaw while Enhancing Heat Management via the Lattice Effect of a Single-Atom Alloy","authors":"Fengyu Zhang, Yanping Yang, Qian Wang, Xiaomeng Chen, Lulu Xie, Xintao Li, Dianqing Li, Junting Feng, Xue Duan","doi":"10.1021/acsami.5c02716","DOIUrl":"https://doi.org/10.1021/acsami.5c02716","url":null,"abstract":"When single-atom catalysts are oriented toward practical applications, in addition to balancing the seesaw between activity and selectivity, the capability of thermal management also merits attention. Herein, we proposed a facility approach that, based on active Pd in the state of a single atom, tunes the guest Cu size to simultaneously enhance the effect of d-electron domination and the heat transfer behavior in microregions. Along with the Cu size in an order of magnitude increase, more delocalized electrons were generated and transferred to isolated Pd sites, with the d band center shifting from 1.438 to 1.052 eV, closer to the Fermi level. Simultaneously, more long-range ordered lattices are much favorable for transferring in situ generated thermally phonons with the diffusivity surging from 12.36 to 103.49 mm²/s. The optimized Pd₁Cu-SAA catalyst exhibited state-of-the-art performance in acetylene hydrogenation, achieving full conversion at 140 °C, with 95.3% selectivity and good stability in the test period.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"14 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876331","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":"Understanding Nanoconfinement Effects on Electrochemical Redox Reactions with Reduced Graphite Oxide as a Model Electrode","authors":"Kaiya Nakasone, Akira Sakima, Taku Iiyama, Ryusuke Futamura, Daisuke Takimoto","doi":"10.1021/acsami.5c00939","DOIUrl":"https://doi.org/10.1021/acsami.5c00939","url":null,"abstract":"Micropores smaller than 1 nm in carbon materials have garnered significant attention for their ability to induce confinement effects. Anomalous improvements in the specific capacitance and reversibility of electrochemical redox reactions have been reported. However, due to limitations in synthetic methods, carbon materials with identical physical properties but varying pore sizes have not yet been successfully prepared. In this study, we investigate the relationship between the pore size of carbon materials and the reversibility of the redox reaction of quinone-based molecules using reduced graphite oxide (rGO) as a model electrode material. Cross-linked graphite oxide (GO) and rGO exhibit minimal changes in surface properties while allowing precise tuning of the interlayer distance at the ångström level. The Δ<i>E</i>_p values of the redox reaction of quinone-based molecules on cross-linked rGO decrease with decreasing interlayer distance. These findings strongly indicate that the reversibility of the redox reaction can be enhanced by reducing the pore sizes of carbon materials. This study clearly demonstrates the origin of the relationship between the pore size and reversibility of the redox reactions of quinone-based molecules.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"33 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875863","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":"Benzophenone-Based Polymers and Covalent Organic Framework for Photocatalytic Molecular Oxygen Activation","authors":"Jian Zeng, Wei Yu, Haomin Xu, Xiangyu Zhang, Qinghua Xu, Jiong Lu, Kian Ping Loh, Jishan Wu","doi":"10.1021/acsami.5c03943","DOIUrl":"https://doi.org/10.1021/acsami.5c03943","url":null,"abstract":"Photosensitization by photoactive materials requires well-designed molecular engineering to enable continuous photochemical processes. However, developing a heavy-atom-free (HAF) strategy to enhance the photoactivity of photosensitizers remains a significant challenge. In this study, we introduce a novel strategy to enhance photosensitization by incorporating benzophenone-rich components into 3D polymers (<b>BQP1</b> and <b>BQP2</b>) and the 2D covalent organic framework (<b>BQ-TMT COF</b>). This incorporation accelerates both charge carrier separation and intersystem crossing, thereby significantly improving photo-to-chemical energy conversion and electron transfer reactions. Notably, the crystalline <b>BQ-TMT COF</b> enables efficient photocatalytic molecular O₂ activation, producing both ¹O₂ and O₂^<b>·</b>– with high efficiency and recyclability. It demonstrates selective photocatalytic oxidation in ¹O₂-mediated sulfide transformations. Moreover, the material performs well in O₂^<b>·</b>–-mediated oxidation, including the hydroxylation of boronic acids and oxidation of amines to imines. The <b>BQ-TMT COF</b>-based photoelectrode generates a photocurrent of approximately 20.7 μA·cm^–2 at 0.4 V vs RHE and achieves a high photocatalytic hydrogen production rate. Our study demonstrates a HAF heterogeneous photosensitizer with efficient photoactive small molecule activation through molecular engineering.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"2 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875911","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}