Probing Single-Particle Electrocatalytic Stability: Electrogenerated Chemiluminescence Imaging of Nanoparticle Array DOI

Zhouzhou Zhu,

Xiangfu Hu,

Ying Wei

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: unknown, P. 12228 - 12233

Published: Dec. 5, 2024

Understanding the stability of single nanoparticles is crucial for optimizing their performance in various applications, including catalysis. In this study, we employed electrochemiluminescence (ECL) imaging to investigate temporal individual Au and Pt within precisely engineered arrays. Our results reveal significant differences NPs. While both exhibit initial decay due diffusion limitations, NPs undergo more rapid degradation, attributed surface oxidation detachment. contrast, demonstrate much better with little oxidation. This study provides valuable insights into fundamental behavior single-NP electrocatalysis highlights potential ECL as a powerful tool unraveling complex dynamics nanoscale systems.

Language: Английский

Electrochemiluminescence Microscopy DOI Creative Commons
Sara Knežević, Dongni Han, Baohong Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(29)

Published: May 14, 2024

Electrochemiluminescence (ECL) is rapidly evolving from an analytical method into optical microscopy. The orthogonality of the electrochemical trigger and readout distinguishes it classic microscopy techniques, owing to its near-zero background, remarkable sensitivity, absence photobleaching phototoxicity. In this minireview, we summarize recent advances in ECL imaging technology, emphasizing original configurations which enable biological entities improvement properties by increasing complexity multiplexing bioassays. Additionally, mapping (electro)chemical reactivity space provides valuable information on nanomaterials facilitates deciphering mechanisms for improving their performances diagnostics (electro)catalysis. Finally, highlight achievements at ultimate limits single molecules, photons or chemical reactions, current challenges translate other fields such as material science, catalysis biology.

Language: Английский

Citations

26

Photocatalysis on Hybrid Plasmonic Nanomaterials: From Catalytic Mechanism Study at Single-Particle Level to Materials Design DOI

Fengxia Tong,

Xizhuang Liang,

Xiaolei Bao

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(15), P. 11425 - 11446

Published: July 17, 2024

Plasmonic nanomaterials can convert low-intensity solar energy into chemical due to their surface plasmon resonance (SPR) effect, offering an interesting approach enhancing conversion efficiency. Unraveling the physicochemical mechanisms of hot carrier relaxation and precise design hybrid plasmonic nanostructures are crucial for optimizing potential SPR effect in photocatalysis, especially considering ongoing challenges low quantum efficiency controversial plasmon-enhanced reactions. Characterization analysis methods at single-particle level emerging as powerful tools achieving this objective. It reveal adsorbate–surface interactions, determine reliable structure–activity relationships individual nanoparticles, further analyze catalytic mechanisms. In review, we highlighted progression mechanism studies that include exploration interfacial charge transfer between nanoparticles with adsorber (metal, semiconductors, or molecule), imaging activity, evolution nanostructures, which provided guidance highly efficient nanomaterials. Finally, discuss future prospects field. This review aims offer insights photocatalysis by emphasizing level, goal expediting development high-performing photocatalysts.

Language: Английский

Citations

12

Unveiling the Dynamic Electrocatalytic Activity of Online Synthesized Bimetallic Nanocatalysts via Electrochemiluminescence Microscopy DOI
Jingwei Xue, Conghui Xu, Wei Zhao

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(15), P. 4665 - 4671

Published: April 8, 2024

Effective bimetallic nanoelectrocatalysis demands precise control of composition, structure, and understanding catalytic mechanisms. To address these challenges, we employ a two-in-one approach, integrating online synthesis with real-time imaging Au@Metal core–shell nanoparticles (Au@M NPs) via electrochemiluminescence microscopy (ECLM). Within 120 s, electrodeposition in situ activity screening alternate. ECLM captures transient faradaic processes during potential switches, visualizes electrochemical real-time, tracks dynamics at the single-particle level. Analysis using ECL photon flux density eliminates size effects yields quantitative electrocatalytic results. Notably, nonlinear trend corresponding to shell metal Au surface atomic ratio is discerned, quantifying optimal component Au@M NPs. This approach offers comprehensive behavior deposition process high spatiotemporal resolution, which crucial for tailoring efficient nanocatalysts diverse applications.

Language: Английский

Citations

10

Enhanced Electrochemiluminescence at the Gas/Liquid Interface of Bubbles Propelled into Solution DOI
Sara Knežević, Joseba Totoricaguena-Gorriño, Rajendra Kumar Reddy Gajjala

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(32), P. 22724 - 22735

Published: Aug. 2, 2024

Electrochemiluminescence (ECL) is typically confined to a micrometric region from the electrode surface. This study demonstrates that ECL emission can extend up several millimeters away employing electrogenerated chlorine bubbles. The mechanism behind this bubble-enhanced was investigated using an Au microelectrode in chloride-containing and chloride-free electrolyte solutions. We discovered at gas/solution interface driven by two parallel effects. First, bubble corona effect facilitates generation of hydroxyl radicals capable oxidizing luminol while attached Second, hypochlorite generated sustains for over 200 s extends range 5 mm into solution, following detachment. new approach increase intensity luminol-based assays 5-fold compared conventional method. demonstrated through glucose bioassay, midrange mobile phone camera detection. These findings significantly expand potential applications extending its effective time space.

Language: Английский

Citations

10

Ultrasensitive Electrochemiluminescence Biosensor with ZIF‐67@MXene as an Efficient Co‐Reaction Accelerator and Plasmonic Nanozyme as a Smart Signal Amplification Probe DOI
Jing Wang, Ran Seon Hong, Zhen Yang

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 18, 2024

Abstract Exploring novel electrochemiluminescence (ECL) co‐reaction accelerators to construct ultrasensitive sensing systems is a prominent focus for developing advanced ECL sensors. However, challenges still remain in finding highly efficient and understanding their promoting mechanisms. In this paper, ZIF‐67@MXene nanosheet composites, with conductive in‐plane structure confined‐stable pore/channel, are designed act as high‐efficient achieve significant enhancement the luminol‐H 2 O based system. Mechanism investigation suggests that hydroxyl radicals (·OH) singlet oxygen ( 1 ) can be selectively preferentially generated on due stable absorption of ·OH , leading remarkable efficiency luminol (830%). Finally, by designing plasmonic NH ‐MIL‐88@Pd nanozyme, an “on‐off” switch immunosensor constructed detection prostate‐specific antigen (PSA). Based multiple signal amplification effect, linear range PSA expanded three orders magnitude. The limit also improved from 1.44 × 10 −11 9.1 −13 g mL −1 . This work proposes effective method preparation provides new strategy sensitive cancer markers.

Language: Английский

Citations

8

Light Conversion by Electrochemiluminescence at Semiconductor Surfaces DOI
Yuting Zhao,

Jean-Gérard Descamps,

Yoan Léger

et al.

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: 57(15), P. 2144 - 2153

Published: July 17, 2024

ConspectusElectrochemiluminescence (ECL) is the electrochemical generation of light. It involves an interfacial charge transfer that produces excited state a luminophore at electrode surface. ECL powerful readout method widely employed for immunoassays and clinical diagnostics progressively evolving into microscopy technique. On other hand, photoelectrochemistry illuminated semiconductors field research deals with photogenerated carriers solid-liquid interface. This concept offers several advantages such as considerable lowering onset potential required triggering reaction well light addressable chemistry, via spatial confinement redox reactions locally semiconductor electrodes. The combination termed photoinduced (PECL). through minority solid/liquid PECL results in conversion incident photons (λ

Language: Английский

Citations

6

Infrared photoinduced electrochemiluminescence microscopy of single cells DOI Creative Commons
Julie Descamps, Yiran Zhao, Bertrand Goudeau

et al.

Chemical Science, Journal Year: 2023, Volume and Issue: 15(6), P. 2055 - 2061

Published: Dec. 8, 2023

Electrochemiluminescence (ECL) is evolving rapidly from a purely analytical technique into powerful microscopy. Herein, we report the imaging of single cells by photoinduced ECL (PECL; λem = 620 nm) stimulated an incident near-infrared light (λexc 1050 nm). The were grown on metal-insulator-semiconductor (MIS) n-Si/SiOx/Ir photoanode that exhibited stable and bright PECL emission. large anti-Stokes shift allowed for recording well-resolved images with high sensitivity. microscopy demonstrated at remarkably low onset potential 0.8 V; this contrasts classic ECL, which blind potential. Two modes are reported: (i) positive (PECL+), showing cell membranes labeled [Ru(bpy)3]2+ complex; (ii) shadow label-free (PECL-) morphology, luminophore in solution. Finally, adding new dimension stimulus, should find promising applications to image study photoactive nanoparticles biological entities.

Language: Английский

Citations

10

Photoinduced Electrochemiluminescence Immunoassays DOI
Dongni Han, Jasmina Vidić, Dechen Jiang

et al.

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(45), P. 18262 - 18268

Published: Nov. 1, 2024

Optimization of electrochemiluminescence (ECL) immunoassays is highly beneficial for enhancing clinical diagnostics. A major challenge the improvement operation conditions required bead-based using typical [Ru(bpy)3]2+/tri-n-propylamine (TPrA) system. In this study, we report a heterogeneous immunoassay based on near-infrared photoinduced ECL, which facilitates imaging and quantitative analysis [Ru(bpy)3]2+-modified immunobeads at low anodic potential. The photovoltage generated by photoanode under light promotes oxidation processes electrode/electrolyte interface, thus considerably lowering onset potential both TPrA ECL emission. anti-Stokes shift between excitation (invisible to human eyes) visible emitted results in clear stable signal from immunobeads. addition, it offers possibility site-selective photoexcitation process. This approach not only meets performance traditional accuracy but also additional benefits lower requirements enhanced stability, providing new perspective optimization commercial immunoassays.

Language: Английский

Citations

4

Near-IR Photoinduced Electrochemiluminescence Imaging with Structured Silicon Photoanodes DOI
Yiran Zhao, Borja Sepúlveda, Julie Descamps

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(9), P. 11722 - 11729

Published: Feb. 23, 2024

Infrared (IR) imaging devices that convert IR irradiation (invisible to the human eye) a visible signal are based on solid-state components. Here, we introduce an alternative concept light-addressable electrochemistry (i.e., spatially confined under action of light stimulus) involves use liquid electrolyte. In this method, projection near-IR image (λexc = 850 or 840 nm) onto photoactive Si-based photoanode, immersed into phase, triggers locally photoinduced electrochemiluminescence (PECL) efficient [Ru(bpy)3]2+-TPrA system. This leads local conversion (λPECL 632 light. We demonstrate compared planar Si photoanodes, micropillar array large enhancement generation and considerably improves resolution PECL by preventing photogenerated minority carriers from diffusing laterally. These results important for design original can lead applications in photothermal analytical chemistry.

Language: Английский

Citations

3

Ternary Heterojunction ZnS‐ZnIn2S4‐In2S3 Efficiently Catalyzes Triethylamine to Enhance Electrochemiluminescence Imaging Signals DOI Open Access
Jingui Chen, Yue Jia, Huaiqing Zhao

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 20, 2024

Abstract The visualization of electrode reactions is significant for ultra sensitive detection. Traditional electrochemiluminescence (ECL) detection method can hardly visualize reactions. Combining ECL imaging technology and traditional methods overcome the lack visual feedback key information in sensor construction. In contrast to cyclic voltammetry testing, applying a constant voltage surface results more stable signal. this study, methionine‐stabilized gold nanoclusters (Met‐AuNCs) are used as efficient near‐infrared luminescent clusters, triethylamine (TEA) coreactants construct an acetamiprid (ACT). ternary heterojunction ZnS‐ZnIn 2 S 4 ‐In 3 (Z‐Z‐I) forms stepwise electron transfer mode, facilitating rapid generation free radicals TEA. Furthermore, Z‐Z‐I serves substrate, providing large loading area DNA chain, which lays foundation wide range. Such has linear range (100 f m 1 µ ) achieves low limit (42 fM) ACT This study not only provides accurate detecting agricultural products but also foretells promising application electrochemiluminescent sensors.

Language: Английский

Citations

3