ACS Nano最新文献_第6页

Distorting Local Structures to Modulate Ligand Fields in Vanadium Oxide for High-Performance Aqueous Zinc-Ion Batteries

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-28 DOI: 10.1021/acsnano.4c18250

Heng Liu, Long Yang, Ting Shen, Changyuan Li, Te Kang, Huanhuan Niu, Wei-Hsiang Huang, Chun-Chi Chang, Menghao Yang, Guozhong Cao, Chaofeng Liu

Layered hydrate vanadates are promising cathode materials for aqueous zinc-ion batteries (AZIBs). Various intercalants have been preinserted into the interplanar space of hydrate vanadates with significantly enhanced kinetics and stabilized structures. However, such an enhancement is induced by various intercalants, and the relationship between the property enhancement and the type of intercalant still needs to be revealed. In this work, the distortion of octahedra induced by the preintercalation of benzyltrimethylammonium (BTA⁺) cations into hydrate vanadium pentoxide (V₂O₅·nH₂O, VOH) and the change in ligand field are studied using synchrotron X-ray pair distribution function (PDF) and X-ray absorption fine structure (XAFS). Variations in the local coordination of vanadium alter the ligand field, decreasing the energy of the lowest unoccupied orbitals (e*), which leads to an increased electrochemical potential. Additionally, the introduced BTA⁺ facilitates fast ion diffusion and stabilizes the layer structure. A cathode with a distorted local structure delivers a specific capacity of 408 mAh/g at 0.5 A/g, with a capacity retention of 95% after 3000 cycles at 8 A/g.

{"title":"Distorting Local Structures to Modulate Ligand Fields in Vanadium Oxide for High-Performance Aqueous Zinc-Ion Batteries","authors":"Heng Liu, Long Yang, Ting Shen, Changyuan Li, Te Kang, Huanhuan Niu, Wei-Hsiang Huang, Chun-Chi Chang, Menghao Yang, Guozhong Cao, Chaofeng Liu","doi":"10.1021/acsnano.4c18250","DOIUrl":"https://doi.org/10.1021/acsnano.4c18250","url":null,"abstract":"Layered hydrate vanadates are promising cathode materials for aqueous zinc-ion batteries (AZIBs). Various intercalants have been preinserted into the interplanar space of hydrate vanadates with significantly enhanced kinetics and stabilized structures. However, such an enhancement is induced by various intercalants, and the relationship between the property enhancement and the type of intercalant still needs to be revealed. In this work, the distortion of octahedra induced by the preintercalation of benzyltrimethylammonium (BTA+) cations into hydrate vanadium pentoxide (V2O5·nH2O, VOH) and the change in ligand field are studied using synchrotron X-ray pair distribution function (PDF) and X-ray absorption fine structure (XAFS). Variations in the local coordination of vanadium alter the ligand field, decreasing the energy of the lowest unoccupied orbitals (e*), which leads to an increased electrochemical potential. Additionally, the introduced BTA+ facilitates fast ion diffusion and stabilizes the layer structure. A cathode with a distorted local structure delivers a specific capacity of 408 mAh/g at 0.5 A/g, with a capacity retention of 95% after 3000 cycles at 8 A/g.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"28 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Structured-Defect Engineering of Hexagonal Boron Nitride for Identified Visible Single-Photon Emitters 用于识别可见光单光子发射器的六方氮化硼结构缺陷工程设计

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-28 DOI: 10.1021/acsnano.4c11413

Tsz Wing Tang, Ritika Ritika, Mohsen Tamtaji, Hongwei Liu, Yunxia Hu, Zhenjing Liu, Patrick Ryan Galligan, Mengyang Xu, Jinghan Shen, Jun Wang, Jiawen You, Yuyin Li, GuanHua Chen, Igor Aharonovich, Zhengtang Luo

Visible-range single-photon emitters (SPEs), based on hexagonal boron nitride (hBN), with exceptional optical performance have become an outstanding candidate for quantum optical technology. However, the control of the carbon defect structures to obtain uniform and confined band structure remains elusive, restricting their integration into on-chip quantum devices. Here, we demonstrate tuning of the defect structure of hBN to precisely control the emission in SPEs. The defect structure engineering from CB (carbon substituted at the boron site) to C₂B–CN (carbon doped into two boron sites and one nitrogen site) carbon defect conversion in hBN is realized by regulating the carbon concentration from 0.0005 at % to 0.082 at % in Cu substrates to adjust the carbon diffusion during the CVD process. Meanwhile, the zero-phonon line exhibits a precise shift from the range of 600–610 nm to 630–640 nm; these shifts of the spectral features are further supported by density functional theory results, reflected in changes in the band structure, vibrational degrees of freedom, and electronic transitions. The SPE emission spectrum serves as a valuable tool for identifying the footprint of a carbon point defect structure change. Our project offers evidence of achieving structured defect engineering for tailored emission properties and showcases potential for the integration of advanced 2D material engineering into on-chip quantum devices.

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引用次数: 0

Decoupling of Photocurrent and Dark Current for Extraordinary Detectivity in Uncooled Middle-Wavelength Infrared Nanohybrid Photodetectors

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-28 DOI: 10.1021/acsnano.4c12802

Maogang Gong, Bo Liu, Andrew Shultz, Russell C. Schmitz, Hugo Barragan Vargas, Saad Alzahrani, Francisco C. Robles Hernandez, Austin Olson, Judy Z. Wu

Nanohybrids of graphene and colloidal semiconductor quantum dots (QDs/Gr) provide a promising quantum sensing scheme for photodetection. Despite exciting progress made in QDs/Gr photodetectors in broadband from ultraviolet to short-wave infrared, the device performance is limited in middle-wave infrared (MWIR) detection. A fundamental question arises as to whether the thermal noise-induced dark current and hence poor signal-to-noise ratio in conventional uncooled MWIR photodetectors persist in QDs/Gr nanohybrids. Herein, we investigated noise, responsivity (R*), and specific detectivity (D*) in HgTe QDs/Gr nanohybrids, revealing that the noise and R* are decoupled in nanohybrids and each can be optimized independently toward its theoretical limit. Specifically, the noise in the QDs/Gr nanohybrids is dominated by that of graphene with a negligible effect from the dark current in HgTe QDs and can be optimized to its intrinsic limit by removing charge doping of adsorbed polar molecules on graphene. Furthermore, the R* is proportional to the photoconductive gain enabled by the strong quantum confinement in QDs and Gr. Achieving high gain in the MWIR spectrum, however, is challenging and requires elimination of charge traps primarily from the surface states of the narrow-bandgap semiconductor HgTe QDs. Using grain-rotation-induced grain-coalescence growth of single-layer and core/shell HgTe QDs, we show the that HgTe QDs surface states caused by Te deficiency can be dramatically suppressed, resulting in high gain up to 4.0 × 10⁷ in the MWIR spectrum. The optimized noise and R* have led to high uncooled MWIR D* up to 2.4 × 10¹¹ Jones, making nanohybrids promising to surpass the fundamental dark-current limit in conventional photodetectors.

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引用次数: 0

Constructing a Graphene-like Layered Carbocatalyst by the Dual Templating Effect for an Efficient Fenton-like Reaction

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-28 DOI: 10.1021/acsnano.4c18558

Tingting Lian, Yang Wang, Jin-Lin Yang, Markus Antonietti

Two-dimensional (2D) carbon materials are receiving increasing attention due to their partly groundbreaking performance in catalysis and electrochemistry based on distinct physiochemical and textural properties. We focus on the challenge to directly achieve a well-developed layered morphology with a high doping level of heteroatoms as the active sites, a standard conflict of interests of high-temperature synthesis. Here, we report a dual-templating strategy to yield graphene-like layered carbon (GLC) by direct carbonization of a texturally prealigned zeolitic imidazolate framework-8 (ZIF-8). The recrystallization of ZIF-8 in an aqueous NaCl solution discloses a 2D packing mode that was retained after freeze-drying with recrystallized NaCl as an exotemplate and a space-confining nanoreactor. Further promoted by the chemical interaction of NaCl in promoting and stabilizing the carbonization process, the final product came with a well-separated layered morphology and high amounts of heteroatoms (16.6 wt % N and 7.5 wt % O). The structurally and catalytically special GLC functioned well in activating peroxymonosulfate-based Fenton-like reactions. It was shown that the reaction proceeded via nonfree-radical-mediated pathways, as reflected in significantly enhanced electron-transfer processes and ultrafast kinetics for pollutant removal. The proposed strategy is expected to afford a broader applicability for the bottom-up design of 2D carbon materials.

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引用次数: 0

Monolayer WSe2 Field-Effect Transistor Performance Enhancement by Atomic Defect Engineering and Passivation

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-27 DOI: 10.1021/acsnano.4c16831

Yuanqiu Tan, Shao-Heng Yang, Chih-Pin Lin, Fernando J. Vega, Jun Cai, Hao-Yu Lan, Rahul Tripathi, Sahej Sharma, Zhongxia Shang, Tuo-Hung Hou, Thomas E. Beechem, Joerg Appenzeller, Zhihong Chen

Monolayer two-dimensional (2D) transition metal dichalcogenides (TMDs) have emerged as leading candidates for next-generation electronic devices beyond silicon, owing to their atomically thin structure and superior electrostatic control. However, their integration into industrial applications remains limited due to high densities of lattice defects and challenges in achieving stable and effective doping. In this work, we present a passivation and doping technique that significantly recovers and enhances the electrical properties of monolayer tungsten diselenide (WSe₂). Our defect-facilitated (NH₄)₂S surface passivation approach has achieved robust enhancements in both the on-state and off-state performance of monolayer WSe₂ p-type field-effect transistors (p-FETs), enhancing channel mobility 3-fold, reaching a subthreshold slope (SS_min) value of 70 mV/dec, on-currents of 110 μA/μm, and I_max/I_min > 10⁹, while maintaining stability across a range of conditions. Furthermore, we establish a strong correlation between device off-state performance and the full width at half-maximum (fwhm) of the Raman characterization peak. The defect engineering approach, combined with (NH₄)₂S treatment at room temperature, offers a viable pathway for passivation and substitutional doping, advancing the potential for improved charge transport in future 2D TMD-based electronic devices.

单层二维（2D）过渡金属二掺杂物（TMDs）因其原子级薄结构和卓越的静电控制能力，已成为硅以外下一代电子设备的主要候选材料。然而，由于晶格缺陷的高密度以及实现稳定有效掺杂的挑战，它们在工业应用中的集成度仍然有限。在这项工作中，我们提出了一种钝化和掺杂技术，可显著恢复和增强单层二硒化钨（WSe2）的电学特性。我们的缺陷促进（NH4）2S 表面钝化方法实现了单层 WSe2 p 型场效应晶体管（p-FET）通态和非通态性能的强劲提升，将沟道迁移率提高了 3 倍，阈下斜率（SSmin）值达到 70 mV/dec，导通电流达到 110 μA/μm，Imax/Imin > 109，同时在一系列条件下保持了稳定性。此外，我们还在器件的离态性能和拉曼特性峰的半最大全宽（fwhm）之间建立了紧密的相关性。缺陷工程方法与室温下的（NH4）2S 处理相结合，为钝化和替代掺杂提供了一条可行的途径，从而提高了未来基于二维 TMD 的电子器件的电荷传输潜力。

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引用次数: 0

Ozonated Monolayer Graphene for Extended Performance and Durability in Hydrogen Fuel Cell Electric Vehicles

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-27 DOI: 10.1021/acsnano.5c02055

Shanmukh Kutagulla, Patrick Carmichael, Matthew Coupin, Devi Mutyala, Nicholas Ignacio, Nam Hoang Le, Isabel Terry Caldino Bohn, Ji-Won Kim, Keldy Stephen Mason, Jamie Warner, Narayana Aluru, Brian A. Korgel, Zachariah A. Page, Deji Akinwande

In the landscape of proton exchange membrane fuel cells (PEMFCs), there is a strong need for durable, low hydrogen crossover membranes that retain high current output and proton conductivity during operation. This study presents the use of UV-Ozone induced defects in graphene to eliminate the proton conductivity penalty commonly associated with traditional crossover mitigation strategies. We report a defect engineered graphene material that demonstrates an increase in hydrogen/proton selectivity of 27%, a decrease in H₂ crossover of 24%, with limited to no impact on current output. Furthermore, we demonstrate a membrane that is 39% more durable than state of the art GORE Select membranes and shows no loss in performance after a 100 h accelerated stress test (AST). This study illustrates the viability of 2D material membranes to sieve between H₂ and H₃O⁺ in industrial testing conditions and serve as highly scalable and durable fuel cell membranes that represent a significant upgrade over current state of the art membranes for hydrogen fuel cell vehicles and clean energy generation.

{"title":"Ozonated Monolayer Graphene for Extended Performance and Durability in Hydrogen Fuel Cell Electric Vehicles","authors":"Shanmukh Kutagulla, Patrick Carmichael, Matthew Coupin, Devi Mutyala, Nicholas Ignacio, Nam Hoang Le, Isabel Terry Caldino Bohn, Ji-Won Kim, Keldy Stephen Mason, Jamie Warner, Narayana Aluru, Brian A. Korgel, Zachariah A. Page, Deji Akinwande","doi":"10.1021/acsnano.5c02055","DOIUrl":"https://doi.org/10.1021/acsnano.5c02055","url":null,"abstract":"In the landscape of proton exchange membrane fuel cells (PEMFCs), there is a strong need for durable, low hydrogen crossover membranes that retain high current output and proton conductivity during operation. This study presents the use of UV-Ozone induced defects in graphene to eliminate the proton conductivity penalty commonly associated with traditional crossover mitigation strategies. We report a defect engineered graphene material that demonstrates an increase in hydrogen/proton selectivity of 27%, a decrease in H2 crossover of 24%, with limited to no impact on current output. Furthermore, we demonstrate a membrane that is 39% more durable than state of the art GORE Select membranes and shows no loss in performance after a 100 h accelerated stress test (AST). This study illustrates the viability of 2D material membranes to sieve between H2 and H3O+ in industrial testing conditions and serve as highly scalable and durable fuel cell membranes that represent a significant upgrade over current state of the art membranes for hydrogen fuel cell vehicles and clean energy generation.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"16 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143506830","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Operando Photoemission Imaging of the Energy Landscape from a 2D Material-Based Field-Effect Transistor.

IF 15.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-27 DOI: 10.1021/acsnano.5c00256

Dario Mastrippolito, Mariarosa Cavallo, Davy Borowski, Erwan Bossavit, Clement Gureghian, Albin Colle, Tommaso Gemo, Adrien Khalili, Huichen Zhang, Ankita Ram, Erwan Dandeu, Sandrine Ithurria, Johan Biscaras, Pavel Dudin, Jean-Francois Dayen, José Avila, Emmanuel Lhuillier, Debora Pierucci

As the integration of transition metal dichalcogenides (TMDC) becomes more advanced for optoelectronics, it is increasingly relevant to develop tools that can correlate the structural properties of the materials with their electrical output. To do so, the determination of the electronic structure must go beyond the hypothesis that the properties of the pristine material remain unaffected after the device integration, which generates changes in the dielectric environment, including electric fields that are likely to renormalize the electronic spectrum. Here, we demonstrate that nanobeam photoemission spectroscopy is a well-suited tool to unveil the device energy landscape under operando conditions. Both the gate vertical field and the drain in-plane vectorial electric field can be determined with a sub-μm resolution. We provide a correlative description of a field-effect transistor to connect its bias-modified energy landscape with the transistor electrical output. The method appears highly suited to unveil how the actual geometry of the flake (thickness, edge effect, presence of structural defects, etc.) is driving the current flow within the device. Lastly, the method appears fully compatible with traditional device fabrication, therefore making it relevant for systematic rational optimization of TMDC-based electronic devices.

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引用次数: 0

Realizing the Synergy of Interface and Dual-Defect Engineering for Molybdenum Disulfide Enables Efficient Sodium-Ion Storage

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-27 DOI: 10.1021/acsnano.4c17967

Heng Zhang, Youcun Bai, Wei Sun, Xiaogang Yang, Ruguang Ma, Liming Dai, Chang Ming Li

Engineering-rich electrocatalyst defects play a critical role in greatly promoting the charge storage/transfer capability of an energy storage/conversion system. Here, an ingenious and effective two-step strategy was used to synthesize a bimetallic sulfide/oxide composite with a coaxial carbon coating, starting from mixing well-dispersed MoO₃ nanobelts and Co-PAA compound, followed by a selective etching process. The simultaneous formation of dual defects of interlayer defect and sulfur-rich vacancies as well as MoO₂/MoS_2-x/CoS heterojunctions noticeably enhances both electron transfer and ion diffusion kinetics. The ultrathin carbon protective layer on the surface of the composite ensures its high conductivity and excellent structural stability. The composite electrode shows a high reversible capacity (158.3 mAh g^–1 at 10 A g^–1 after 4000 cycles) and outstanding long-cycle stability (0.04% per cycle over 2100 cycles at 20 A g^–1). A full cell based on MoO₂/MoS_2–x/CoS@N, S–C anode, and Na₃V₂(PO₄)₃ cathode can maintain a reversible capacity of 128.1 mAh g^–1 after 600 cycles at 1 A g^–1, surpassing that based on MoO₂/MoS₂ and is very comparable in performance with the state-of-the-art Na-ion full cells. Moreover, density functional theory (DFT) calculations, electrochemical kinetics analysis, and in situ Raman and ex-situ X-ray diffraction characterization were carried out to elucidate the involved scientific mechanisms of sodium storage.

{"title":"Realizing the Synergy of Interface and Dual-Defect Engineering for Molybdenum Disulfide Enables Efficient Sodium-Ion Storage","authors":"Heng Zhang, Youcun Bai, Wei Sun, Xiaogang Yang, Ruguang Ma, Liming Dai, Chang Ming Li","doi":"10.1021/acsnano.4c17967","DOIUrl":"https://doi.org/10.1021/acsnano.4c17967","url":null,"abstract":"Engineering-rich electrocatalyst defects play a critical role in greatly promoting the charge storage/transfer capability of an energy storage/conversion system. Here, an ingenious and effective two-step strategy was used to synthesize a bimetallic sulfide/oxide composite with a coaxial carbon coating, starting from mixing well-dispersed MoO3 nanobelts and Co-PAA compound, followed by a selective etching process. The simultaneous formation of dual defects of interlayer defect and sulfur-rich vacancies as well as MoO2/MoS2-x/CoS heterojunctions noticeably enhances both electron transfer and ion diffusion kinetics. The ultrathin carbon protective layer on the surface of the composite ensures its high conductivity and excellent structural stability. The composite electrode shows a high reversible capacity (158.3 mAh g–1 at 10 A g–1 after 4000 cycles) and outstanding long-cycle stability (0.04% per cycle over 2100 cycles at 20 A g–1). A full cell based on MoO2/MoS2–x/CoS@N, S–C anode, and Na3V2(PO4)3 cathode can maintain a reversible capacity of 128.1 mAh g–1 after 600 cycles at 1 A g–1, surpassing that based on MoO2/MoS2 and is very comparable in performance with the state-of-the-art Na-ion full cells. Moreover, density functional theory (DFT) calculations, electrochemical kinetics analysis, and in situ Raman and ex-situ X-ray diffraction characterization were carried out to elucidate the involved scientific mechanisms of sodium storage.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"4 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Surface Enhanced Raman Scattering for Biomolecular Sensing in Human Healthcare Monitoring

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-27 DOI: 10.1021/acsnano.4c15877

Stacey Laing, Sian Sloan-Dennison, Karen Faulds, Duncan Graham

Since the 1980s, surface enhanced Raman scattering (SERS) has been used for the rapid and sensitive detection of biomolecules. Whether a label-free or labeled assay is adopted, SERS has demonstrated low limits of detection in a variety of biological matrices. However, SERS analysis has been confined to the laboratory due to several reasons such as reproducibility and scalability, both of which have been discussed at length in the literature. Another possible issue with the lack of widespread adoption of SERS is that its application in point of use (POU) testing is only now being fully explored due to the advent of portable Raman spectrometers. Researchers are now investigating how SERS can be used as the output on several POU platforms such as lateral flow assays, wearable sensors, and in volatile organic compound (VOC) detection for human healthcare monitoring, with favorable results that rival the gold standard approaches. Another obstacle that SERS faces is the interpretation of the wealth of information obtained from the platform. To combat this, machine learning is being explored and has been shown to provide quick and accurate analysis of the generated data, leading to sensitive detection and discrimination of many clinically relevant biomolecules. This review will discuss the advancements of SERS combined with POU testing and the strength that machine learning can bring to the analysis to produce a powerful combined platform for human healthcare monitoring.

{"title":"Surface Enhanced Raman Scattering for Biomolecular Sensing in Human Healthcare Monitoring","authors":"Stacey Laing, Sian Sloan-Dennison, Karen Faulds, Duncan Graham","doi":"10.1021/acsnano.4c15877","DOIUrl":"https://doi.org/10.1021/acsnano.4c15877","url":null,"abstract":"Since the 1980s, surface enhanced Raman scattering (SERS) has been used for the rapid and sensitive detection of biomolecules. Whether a label-free or labeled assay is adopted, SERS has demonstrated low limits of detection in a variety of biological matrices. However, SERS analysis has been confined to the laboratory due to several reasons such as reproducibility and scalability, both of which have been discussed at length in the literature. Another possible issue with the lack of widespread adoption of SERS is that its application in point of use (POU) testing is only now being fully explored due to the advent of portable Raman spectrometers. Researchers are now investigating how SERS can be used as the output on several POU platforms such as lateral flow assays, wearable sensors, and in volatile organic compound (VOC) detection for human healthcare monitoring, with favorable results that rival the gold standard approaches. Another obstacle that SERS faces is the interpretation of the wealth of information obtained from the platform. To combat this, machine learning is being explored and has been shown to provide quick and accurate analysis of the generated data, leading to sensitive detection and discrimination of many clinically relevant biomolecules. This review will discuss the advancements of SERS combined with POU testing and the strength that machine learning can bring to the analysis to produce a powerful combined platform for human healthcare monitoring.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"210 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Hierarchical Tandem Catalysis Promotes CO Spillover and Trapping for Efficient CO2 Reduction to C2+ Products

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2025-02-27 DOI: 10.1021/acsnano.5c00696

Lei Bian, Yu Bai, Jia-Yi Chen, Hong-Kai Guo, Shize Liu, Hao Tian, Nana Tian, Zhong-Li Wang

The electrochemical CO₂ reduction reaction (CO₂RR) to produce multicarbon (C₂₊) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel or valuable chemicals; however, producing C₂₊ at high current densities is still a challenge. Herein, we design a hierarchically structured tandem catalysis electrode for greatly improved catalytic activity and selectivity for C₂₊ products. The tandem catalysis electrode is constructed of a sputtered Ag nanoparticle layer on a hydrophobic polytetrafluoroethylene (PTFE) membrane and a layer of nitrogen-doped carbon (NC)-modified Cu nanowire arrays. The Cu nanowire arrays are in situ grown on PTFE by electrochemical oxidation of sputtered CuAl alloy, in which the chemical etching of metal Al induces the formation of a Cu nanowire array structure. Within hierarchical configuration, CO can be efficiently generated on an active Ag layer and then spillover and transfer to NC-modified Cu nanowire array layer, in which Cu/NC interfaces can enhance *CO trapping and adsorption. During the CO₂RR, the optimized tandem catalysis electrode achieves superior Faradaic efficiencies of 53.5% and 87.5% for ethylene (C₂H₄) and C₂₊ products at the current density of 519.0 mA cm^–2, respectively, with a high C₂₊/C₁ ratio of 10.42 and long-term stability up to 50 h. In situ Raman and attenuated total reflection-surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) confirm that the Ag–Cu–NC tandem catalysis system significantly enhances the linear adsorption of *CO intermediates and the dissociation of H₂O, improves the C–C coupling capability, and stabilizes the key intermediate *OCCOH to produce C₂₊ products.

{"title":"Hierarchical Tandem Catalysis Promotes CO Spillover and Trapping for Efficient CO2 Reduction to C2+ Products","authors":"Lei Bian, Yu Bai, Jia-Yi Chen, Hong-Kai Guo, Shize Liu, Hao Tian, Nana Tian, Zhong-Li Wang","doi":"10.1021/acsnano.5c00696","DOIUrl":"https://doi.org/10.1021/acsnano.5c00696","url":null,"abstract":"The electrochemical CO2 reduction reaction (CO2RR) to produce multicarbon (C2+) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel or valuable chemicals; however, producing C2+ at high current densities is still a challenge. Herein, we design a hierarchically structured tandem catalysis electrode for greatly improved catalytic activity and selectivity for C2+ products. The tandem catalysis electrode is constructed of a sputtered Ag nanoparticle layer on a hydrophobic polytetrafluoroethylene (PTFE) membrane and a layer of nitrogen-doped carbon (NC)-modified Cu nanowire arrays. The Cu nanowire arrays are in situ grown on PTFE by electrochemical oxidation of sputtered CuAl alloy, in which the chemical etching of metal Al induces the formation of a Cu nanowire array structure. Within hierarchical configuration, CO can be efficiently generated on an active Ag layer and then spillover and transfer to NC-modified Cu nanowire array layer, in which Cu/NC interfaces can enhance *CO trapping and adsorption. During the CO2RR, the optimized tandem catalysis electrode achieves superior Faradaic efficiencies of 53.5% and 87.5% for ethylene (C2H4) and C2+ products at the current density of 519.0 mA cm–2, respectively, with a high C2+/C1 ratio of 10.42 and long-term stability up to 50 h. In situ Raman and attenuated total reflection-surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) confirm that the Ag–Cu–NC tandem catalysis system significantly enhances the linear adsorption of *CO intermediates and the dissociation of H2O, improves the C–C coupling capability, and stabilizes the key intermediate *OCCOH to produce C2+ products.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"33 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518478","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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