ACS Applied Materials & Interfaces最新文献

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Favorable Contact with Low Interfacial Resistance for n-Type TiCoSb-Based Thermoelectric Devices
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c18148
Ajay Kumar Verma, Kishor Kumar Johari, Shamma Jain, Pargam Vashishtha, Billy James Murdoch, Chaitali Dekiwadia, Yoshit Tiwari, Sanjay R. Dhakate, Sumeet Walia, Bhasker Gahtori
{"title":"Favorable Contact with Low Interfacial Resistance for n-Type TiCoSb-Based Thermoelectric Devices","authors":"Ajay Kumar Verma, Kishor Kumar Johari, Shamma Jain, Pargam Vashishtha, Billy James Murdoch, Chaitali Dekiwadia, Yoshit Tiwari, Sanjay R. Dhakate, Sumeet Walia, Bhasker Gahtori","doi":"10.1021/acsami.4c18148","DOIUrl":"https://doi.org/10.1021/acsami.4c18148","url":null,"abstract":"In the past decade, significant efforts have been made to develop efficient half-Heusler (HH) based thermoelectric (TE) materials. However, their practical applications remain limited due to various challenges occurring during the fabrication of TE devices, particularly the development of stable contacts with low interfacial resistance. In this study, we have made an effort to explore a stable contact material with low interfacial resistance for an n-type TiCoSb-based TE material, specifically Ti<sub>0.85</sub>Nb<sub>0.15</sub>CoSb<sub>0.96</sub>Bi<sub>0.04</sub> as a proof of concept, using a straightforward facile synthesis route of spark plasma sintering. We tested many metals with compatible coefficients of thermal expansion to TiCoSb, like Fe and Co. Still, we failed to form proper atomic bonds with the TE material. In contrast, Ti metal bonded correctly but showed very high electrical contact resistance (∼300 mΩ at one side), reducing performance due to Ti diffusion and a high potential barrier at the interface. This issue was addressed by highly doped semiconductor (HDS) contact Ti<sub>0.7</sub>Nb<sub>0.3</sub>CoSb, which matched the TE material in terms of atomic bonding, crystal structure, and stability. The leg with the HDS contact demonstrated superior electronic transport performance and low interface resistance (∼15 mΩ at one side), achieving a maximum output power of 30.7 mW at Δ<i>T</i> = 451 K due to the sharp interface with a low barrier height. These findings suggest that using HDS material as a contact with the same HH TE material would be an effective way to develop a TE device with low interface resistance and high thermal stability.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"68 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981329","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}
引用次数: 0
Synergistic Improvement of Narrow Bandgap PbS Quantum Dot Solar Cells through Surface Ligand Engineering, Near-Infrared Spectral Matching, and Enhanced Electrode Transparency
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c22334
Anjali Sharma, Dipak Dattatray Shinde, Chandan Mahajan, Neha V. Dambhare, Arindam Biswas, Anurag Mitra, Vrushali S. Girade, Arup K. Rath
{"title":"Synergistic Improvement of Narrow Bandgap PbS Quantum Dot Solar Cells through Surface Ligand Engineering, Near-Infrared Spectral Matching, and Enhanced Electrode Transparency","authors":"Anjali Sharma, Dipak Dattatray Shinde, Chandan Mahajan, Neha V. Dambhare, Arindam Biswas, Anurag Mitra, Vrushali S. Girade, Arup K. Rath","doi":"10.1021/acsami.4c22334","DOIUrl":"https://doi.org/10.1021/acsami.4c22334","url":null,"abstract":"The tunability of the energy bandgap in the near-infrared (NIR) range uniquely positions colloidal lead sulfide (PbS) quantum dots (QDs) as a versatile material to enhance the performance of existing perovskite and silicon solar cells in tandem architectures. The desired narrow bandgap (NBG) PbS QDs exhibit polar (111) and nonpolar (100) terminal facets, making effective surface passivation through ligand engineering highly challenging. Despite recent breakthroughs in surface ligand engineering, NBG PbS QDs suffer from uncontrolled agglomeration in solid films, leading to increased energy disorder and trap formation. The limited NIR transparency of commonly used indium-doped tin oxide (ITO) electrodes and inadequate NIR radiation from commercially available solar simulators further compromise the true performance of NBG PbS QDs in solar cells. Here, we employ a hybrid ligand strategy based on inorganic cadmium halide and organic thiol molecules, leading to the partial substitution of surface Pb atoms with Cd heteroatoms. This hybrid ligand strategy substantially reduces undesired QD fusion in solid films, improving the photophysical and electronic properties. By modulating the thickness of the ITO layer and managing refraction loss through a ZnO layer coating, we improved NIR transparency to above 80%. We combine an NIR light source with a solar simulator to achieve near-ideal spectral matching for a broader range with standard AM1.5G illumination. Enhancements in surface passivation of QDs, improvements in NIR transparency of electrodes, and a spectral matched light source setup help us achieve solar cell power conversion efficiencies of 12.4%, 4.48%, and 1.37% under AM 1.5G, perovskite filter, and silicon filter illuminations, respectively. A record open-circuit voltage (<i>V</i><sub>oc</sub>) of 0.54 V and short-circuit current density (<i>J</i><sub>sc</sub>) of 38.5 mA/cm<sup>2</sup> are achieved under AM 1.5G illumination. We attribute these advancements in photovoltaic parameters to the reduction in Urbach tail states and intermediate trap density originating from superior surface passivation of QDs.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"92 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981334","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}
引用次数: 0
Porous Silicon Particle-Assisted Mass Spectrometry Technology Unlocks Serum Metabolic Fingerprints in the Progression From Chronic Hepatitis B to Hepatocellular Carcinoma
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c17563
Xinrong Jiang, Liye Tao, Shuo Cao, Zhengao Xu, Shuang Zheng, Huafang Zhang, Xinran Xu, Xuetong Qu, Xingyue Liu, Jiekai Yu, Xiaoming Chen, Jianmin Wu, Xiao Liang
{"title":"Porous Silicon Particle-Assisted Mass Spectrometry Technology Unlocks Serum Metabolic Fingerprints in the Progression From Chronic Hepatitis B to Hepatocellular Carcinoma","authors":"Xinrong Jiang, Liye Tao, Shuo Cao, Zhengao Xu, Shuang Zheng, Huafang Zhang, Xinran Xu, Xuetong Qu, Xingyue Liu, Jiekai Yu, Xiaoming Chen, Jianmin Wu, Xiao Liang","doi":"10.1021/acsami.4c17563","DOIUrl":"https://doi.org/10.1021/acsami.4c17563","url":null,"abstract":"Hepatocellular carcinoma (HCC) is a common malignancy and generally develops from liver cirrhosis (LC), which is primarily caused by the chronic hepatitis B (CHB) virus. Reliable liquid biopsy methods for HCC screening in high-risk populations are urgently needed. Here, we establish a porous silicon-assisted laser desorption ionization mass spectrometry (PSALDI-MS) technology to profile metabolite information hidden in human serum in a high throughput manner. Serum metabolites can be captured in the pore channel of APTES-modified porous silicon (pSi) particles and well-preserved during storage or transportation. Furthermore, serum metabolites captured in the APTES-pSi particles can be directly detected on the LDI-MS without the addition of an organic matrix, thus greatly accelerating the acquisition of metabolic fingerprints of serum samples. The PSALDI-MS displays the capability of high throughput (5 min per 96 samples), high reproducibility (coefficient of variation &lt;15%), high sensitivity (LOD ∼ 1 pmol), and high tolerance to background salt and proteins. In a multicenter cohort study, 1433 subjects including healthy controls (HC), CHB, LC, and HCC volunteers were enrolled and nontargeted serum metabolomic analysis was performed on the PSALDI-MS platform. After the selection of feature metabolites, a stepwise diagnostic model for the classification of different liver disease stages was constructed by the machine learning algorithm. In external testing, the accuracy of 91.2% for HC, 71.4% for CHB, 70.0% for LC, and 95.3% for HCC was achieved by chemometrics. Preliminary studies indicated that the diagnostic model constructed from serum metabolic fingerprint also displays good predictive performance in a prospective observation. We believe that the combination of PSALDI-MS technology and machine learning may serve as an efficient tool in clinical practice.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"45 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981328","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}
引用次数: 0
Correction to “Screening of Short-Chain Antimicrobial Peptide LKARI with Broad-Spectrum Bactericidal Properties and Its Application in Promoting Wound Healing”
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c23115
Han Wu, Yumei Wang, Zekai Ren, Xin Liu, Mingtao Yu, Yang Cao, Hailin Cong, Bing Yu, Youqing Shen
{"title":"Correction to “Screening of Short-Chain Antimicrobial Peptide LKARI with Broad-Spectrum Bactericidal Properties and Its Application in Promoting Wound Healing”","authors":"Han Wu, Yumei Wang, Zekai Ren, Xin Liu, Mingtao Yu, Yang Cao, Hailin Cong, Bing Yu, Youqing Shen","doi":"10.1021/acsami.4c23115","DOIUrl":"https://doi.org/10.1021/acsami.4c23115","url":null,"abstract":"In our original article, three errors appear, all of which were caused by incorrect placement of images during the layout process in Figures 3, 4 and 9. At the same time, we noticed that the wound healing at Day 11 and Day 14 in Figure 8 is not significantly different, so we have removed the wound healing image from Day 11 in Figure 8. These corrections do not affect the results and conclusions of the original publication. All authors agree with these corrections and sincerely apologize for the errors. Figure 3. Antibacterial peptide chain and biocompatibility of the antibacterial hydrogel. Figure 4. Antimicrobial peptide LKARI and penicillin–streptomycin resistance. Figure 8. Treatment of <i>Escherichia coli</i> and <i>Candida albicans</i> infection models. Figure 9. Pathological analysis of healing wound. Specifically, the SEM image of blood cells in Figure 3A for LKARI-gel was incorrectly formatted. In Figure 4B, the image for the 8th generation plate was mistakenly duplicated as the 6th generation plate. In Figure 9A, the liver H&amp;E stained tissue image for the LKARI-gel + S. aureus group was incorrectly labeled due to a naming error. This article has not yet been cited by other publications.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"52 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981415","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}
引用次数: 0
Halogen-Free Wide Band Gap Polymer Donors Based on Dicyanobithiophene for Efficient Organic Solar Cells
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c17974
Xiyue Yuan, Bo Zhang, Youle Li, Feixiang Zhao, Wenkui Wei, Yue Zhang, Junyu Li, Yuchuan Tian, Zaifei Ma, Zheng Tang, Zhitian Liu, Fei Huang, Yong Cao, Chunhui Duan
{"title":"Halogen-Free Wide Band Gap Polymer Donors Based on Dicyanobithiophene for Efficient Organic Solar Cells","authors":"Xiyue Yuan, Bo Zhang, Youle Li, Feixiang Zhao, Wenkui Wei, Yue Zhang, Junyu Li, Yuchuan Tian, Zaifei Ma, Zheng Tang, Zhitian Liu, Fei Huang, Yong Cao, Chunhui Duan","doi":"10.1021/acsami.4c17974","DOIUrl":"https://doi.org/10.1021/acsami.4c17974","url":null,"abstract":"Conjugated polymer donors have always been one of the important components of organic solar cells (OSCs), particularly those featuring simple synthetic routes, proper energy levels, and appropriate aggregation behavior. In this work, we employed a nonfused electron-deficient building block, dicyanobithiophene (2CT), for constructing high-performance donors. Combining this with side-chain engineering, two novel halogen-free polymer donors, PB2CT-BO and PB2CT-HD, were reported. PB2CT-BO with shorter alkyl chains on the thiophene π bridges exhibited enhanced packing ordering and improved polymer crystallinity. When paired with BTP-CN-HD as the electron acceptor, the PB2CT-BO-based OSC attained an impressive power conversion efficiency (PCE) of 14.2% within a bulk-heterojunction (BHJ) configuration. Additionally, the active layers were refined through a layer-by-layer (LbL) approach, leading to a more organized molecular packing and an improved fibrillar network. Consequently, the OSC employing PB2CT-BO processed with the LbL approach achieved a notable PCE of 15.3%. This enhancement is credited to a reduced energy loss (<i>E</i><sub>loss</sub>) of 0.514 eV and the formation of a favorable morphology. This study highlights the considerable promise of the 2CT unit in the progression of high-efficiency polymer donors with a reduced <i>E</i><sub>loss</sub>.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"52 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981325","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}
引用次数: 0
Modification of the Se/MoOx Rear Interface for Efficient Wide-Band-Gap Trigonal Selenium Solar Cells
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c15892
Feixiong Bao, Lianglan Liu, Xinlong Wang, Binquan Xiao, Huanyong Li, Huidong Yang, Kai Shen, Yaohua Mai
{"title":"Modification of the Se/MoOx Rear Interface for Efficient Wide-Band-Gap Trigonal Selenium Solar Cells","authors":"Feixiong Bao, Lianglan Liu, Xinlong Wang, Binquan Xiao, Huanyong Li, Huidong Yang, Kai Shen, Yaohua Mai","doi":"10.1021/acsami.4c15892","DOIUrl":"https://doi.org/10.1021/acsami.4c15892","url":null,"abstract":"Trigonal selenium (t-Se) is a promising wide-band-gap photovoltaic material with a high absorption coefficient, abundant resources, simple composition, nontoxicity, and a low melting point, making it suitable for absorbers in advanced indoor and tandem photovoltaic applications. However, severe electrical losses at the rear interface of the t-Se absorber, caused by work function and lattice mismatches, limit the voltage output and overall performance. In this study, a strategy to enhance carrier transport and collection by modifying interfacial chemical interactions is proposed. By applying a controlled heat process during the deposition of the MoO<sub><i>x</i></sub> hole transport layer, a chemical interaction at the t-Se/MoO<sub><i>x</i></sub> interface can be facilitated. This results in the formation of an interfacial MoSe<sub><i>x</i></sub> layer, leading to improved valence band alignment and reduced barrier and recombination losses. As a result, the performance of t-Se thin-film solar cells is improved compared to those without the heating process.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"16 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981324","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}
引用次数: 0
Self-Healing Superhydrophobic Coatings with Multiphase Repellence Property
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c19317
Zhongshan Wang, Yuanyuan Hou, Ashish Yadav, Tangjian Chen, Yongling Wu, Changyou Yan, Mingming Liu
{"title":"Self-Healing Superhydrophobic Coatings with Multiphase Repellence Property","authors":"Zhongshan Wang, Yuanyuan Hou, Ashish Yadav, Tangjian Chen, Yongling Wu, Changyou Yan, Mingming Liu","doi":"10.1021/acsami.4c19317","DOIUrl":"https://doi.org/10.1021/acsami.4c19317","url":null,"abstract":"Developing versatile, scalable, and durable coatings that repel various matters in different service environments is of great importance for engineered materials applications but remains highly challenging. Here, the mesoporous silica microspheres (HMS) fabricated by the hard template method were utilized as micro-nanocontainers to encapsulate the hydrophobic agent of perfluorooctyltriethoxysilane (F13) and the corrosion inhibitor of benzotriazole (BTA), forming the functional microsphere of F-HMS(BTA). Moreover, the synthesized organosilane-modified silica sol adhesive (SMP) and F-HMS(BTA) were further employed as the binder and functional filler to construct a superhydrophobic self-healing coating of SMP@F-HMS(BTA) on various engineering metals through scalable spraying. The prepared coating exhibits good mechanical durability and strong resistance to accretion of multiphase substances including large molecule compounds, liquids, and ice crystals, demonstrating good antifouling and anti-icing properties. Moreover, the coatings possess hydrophobic and anticorrosion self-healing properties owing to the self-migration release of the functional additives in the micro-nanocontainers, showing the “active–passive” synergistic properties mechanism. At a frequency of 0.01 Hz, the charge transfer resistance <i>R</i><sub>ct</sub> and the constant phase element <i>C</i><sub>cpe</sub> were measured to be 2.62 × 10<sup>9</sup> Ω cm<sup>2</sup> and 9.63 × 10<sup>–10</sup> F cm<sup>2</sup>, respectively. In addition, the corrosion current density was reduced by 3–5 orders of magnitude, indicating superior corrosion resistance. This work provides a feasible strategy to prepare functional protective coatings for a wide range of applications in addressing adhesion and corrosion issues.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"20 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981331","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}
引用次数: 0
Lateral Carrier Diffusion in Ion-Implanted Ultra-Small Blue III-Nitride MicroLEDs
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c14784
Julia Slawinska, Grzegorz Muziol, Anna Kafar, Czeslaw Skierbiszewski
{"title":"Lateral Carrier Diffusion in Ion-Implanted Ultra-Small Blue III-Nitride MicroLEDs","authors":"Julia Slawinska, Grzegorz Muziol, Anna Kafar, Czeslaw Skierbiszewski","doi":"10.1021/acsami.4c14784","DOIUrl":"https://doi.org/10.1021/acsami.4c14784","url":null,"abstract":"Ultrasmall micro-light-emitting diodes (μLEDs), sized below 10 μm, are indispensable to create the next-generation augmented and virtual reality (AR/VR) devices. Their high brightness and low power consumption could not only enhance the user experience by providing vivid and lifelike visuals but also extend device longevity. However, a notable challenge emerges: a decrease in efficiency with a reduced size. This study casts light on this critical issue by investigating the lateral carrier diffusion in ion-implanted μLEDs. The implanted area restricts the carrier injection and defines the μLED size to diameters of 10, 5, and 2 μm without introduction of nonradiative recombination centers in the quantum well area. We observed a drop of efficiency for smaller devices, similar to the case of conventional μLEDs with etched sidewalls. Electroluminescence of μLEDs was studied using a Gaussian beam telescope to analyze light intensity profiles and hence the spatial carrier distribution within the active region of μLEDs. Lateral diffusion length was determined to be 11.2 μm at <i>j</i> = 1 A/cm<sup>2</sup> and decreased down to 2.4 μm for <i>j</i> = 1000 A/cm<sup>2</sup>. We explain the underlying mechanism behind the size-dependent efficiency observed in μLEDs, attributed to lateral carrier diffusion.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"74 6 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981323","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}
引用次数: 0
Conventional versus Unconventional Oxygen Reduction Reaction Intermediates on Single Atom Catalysts
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c23082
Tahereh Jangjooye Shaldehi, Soosan Rowshanzamir, Kai S. Exner, Francesc Viñes, Francesc Illas
{"title":"Conventional versus Unconventional Oxygen Reduction Reaction Intermediates on Single Atom Catalysts","authors":"Tahereh Jangjooye Shaldehi, Soosan Rowshanzamir, Kai S. Exner, Francesc Viñes, Francesc Illas","doi":"10.1021/acsami.4c23082","DOIUrl":"https://doi.org/10.1021/acsami.4c23082","url":null,"abstract":"The oxygen reduction reaction (ORR) stands as a pivotal process in electrochemistry, finding applications in various energy conversion technologies such as fuel cells, metal-air batteries, and chlor-alkali electrolyzers. Hereby, a comprehensive density functional theory (DFT) investigation is presented into the proposed conventional and unconventional ORR mechanisms using single-atom catalysts (SACs) supported on nitrogen-doped graphene (NG) as model systems. Several reaction intermediates have been identified that appear to be more stable than the ones postulated in the conventional mechanism, which follows the *OOH, *O, and *OH intermediates. This finding particularly holds for adsorbed *O<sub>2</sub>, which can have different adsorption geometries, ranging from η<sup>1</sup>Ο<sub>2</sub> or η<sup>2</sup>Ο<sub>2</sub> superoxo complexes as well as sin and anti complexes, with the two O-related ligands binding on the same or opposite sides, respectively. In the case of M@NG (M = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, and Pt), the ORR follows these unconventional *O<sub>2</sub> intermediates, whereas for Cr@NG and Cu@NG classical and unconventional *O<sub>2</sub> intermediates compete. We approximate the electrocatalytic activity using the concept of the thermodynamic overpotential and demonstrate that the conventional mechanism gives rise to a smaller overpotential compared to mechanisms following unconventional intermediates during the four proton-coupled electron transfer steps. Our trend study indicates that transition metals with fewer <i>d</i> electrons reveal smaller electrocatalytic activity due to a larger thermodynamic overpotential. Among the investigated SAC systems, Co emerges as a promising candidate, with thermodynamic overpotential and limiting potential values of 0.38 and 0.85 V vs the standard hydrogen electrode, respectively, with the conventional mechanism being favored, and with Cu appearing as the second-best candidate.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"15 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981414","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}
引用次数: 0
Modular Engineering of Lysostaphin with Significantly Improved Stability and Bioavailability for Treating MRSA Infections
IF 9.5 2区 材料科学
ACS Applied Materials & Interfaces Pub Date : 2025-01-15 DOI: 10.1021/acsami.4c18004
Jingwei Liu, Yumei Li, Shuang Wang, Bo Jia, Jiaxin Li, Jiangchao Qian, Jingjing Li, Chao Ma, Hongjie Zhang, Kai Liu, Fan Wang
{"title":"Modular Engineering of Lysostaphin with Significantly Improved Stability and Bioavailability for Treating MRSA Infections","authors":"Jingwei Liu, Yumei Li, Shuang Wang, Bo Jia, Jiaxin Li, Jiangchao Qian, Jingjing Li, Chao Ma, Hongjie Zhang, Kai Liu, Fan Wang","doi":"10.1021/acsami.4c18004","DOIUrl":"https://doi.org/10.1021/acsami.4c18004","url":null,"abstract":"Methicillin-resistant <i>Staphylococcus aureus</i> (MRSA) is a refractory pneumonia-causing pathogen due to the antibiotic resistance and the characteristics of persisting inside its host cell. Lysostaphin is a typical bacteriolytic enzyme for degrading bacterial cell walls via hydrolysis of pentaglycine cross-links, showing potential to combat multidrug-resistant bacteria. However, there are still grand challenges for native lysostaphin because of its poor shelf stability and limited bioavailability. To tackle these limitations, a modular assembly strategy is proposed to actively engineer the native lysostaphin, involving nanoassembly preparation via fusing with lysine-rich polypeptide. The engineered lysine component significantly improves the membrane-penetration capability of lysostaphin, greatly increasing its intracellular antibacterial activity by 12-fold compared to wild-type lysostaphin. Notably, the half-life of the nanoassembled lysostaphin is approximately 13 times longer than that of its native counterpart, greatly outperforming other studies. Most importantly, the shelf stability of our engineered lysostaphin is significantly improved, retaining over 99.9% of antibacterial activity after 12 weeks at room temperature. This modular assembly strategy successfully enhances the overall performance of lysostaphin, offering great promise for a platform technique to refine enzymatic material for widespread clinical demands.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"8 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981326","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}
引用次数: 0
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