Seeded Synthesis of Unconventional 2H-Phase Pd Alloy Nanomaterials for Highly Efficient Oxygen Reduction

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(41), P. 17292 - 17299

Published: Oct. 6, 2021

Crystal phase engineering of noble-metal-based alloy nanomaterials paves a new way to the rational synthesis high-performance catalysts for various applications. However, controlled preparation with unconventional crystal phases still remains great challenge due their thermodynamically unstable nature. Herein, we develop robust and general seeded method synthesize PdCu hexagonal close-packed (hcp, 2H type) also tunable Cu contents. Moreover, galvanic replacement by Pt can be further conducted prepare trimetallic 2H-PdCuPt nanomaterials. Impressively, 2H-Pd67Cu33 nanoparticles possess high mass activity 0.87 A mg-1Pd at 0.9 V (vs reversible hydrogen electrode (RHE)) in electrochemical oxygen reduction reaction (ORR) under alkaline condition, which is 2.5 times that conventional face-centered cubic (fcc) Pd69Cu31 counterpart, revealing important role on determining ORR performance. After incorporation Pt, obtained 2H-Pd71Cu22Pt7 catalyst shows significantly enhanced 1.92 mg-1Pd+Pt RHE), 19.2 8.7 those commercial Pt/C Pd/C, placing it among best reported Pd-based electrocatalysts conditions.

Language: Английский

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Trimetallic AuPtCo Nanopolyhedrons with Peroxidase- and Catalase-Like Catalytic Activity for Glow-Type Chemiluminescence Bioanalysis

Analytical Chemistry, Journal Year: 2021, Volume and Issue: 94(2), P. 847 - 855

Published: Dec. 19, 2021

Chemiluminescence (CL) with stable and glowing light emission is vital for the accurate detection of biomarkers. Moreover, catalyst plays an important role in CL systems. Herein, trimetallic AuPtCo nanopolyhedrons peroxidase- catalase-like catalytic activities are readily synthesized via a one-step reduction method. After reaction substrate ABEI oxidant H2O2, nanozyme can catalyze flash type. Interestingly, it has been found that biofunctionalization surface endow interface slow-diffusion effect, thereby prolonging glow-type CL. On this basis, two biofunctionalized nanocomposites, named as AuPtCo@Cys AuPtCo@Ab, prepared, achieving sensitive selective H2O2 lipoprotein-associated phospholipase A2 (Lp-PLA2), respectively. Further, proposed assays successfully applied determination Lp-PLA2 female vaginal discharge human serum samples, respectively, which exhibit good correlation clinical results. Overall, nanozyme-based analysis demonstrated powerful robust tool biomarker analysis, holds great promise applications.

Language: Английский

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Open-channel metal particle superlattices

Nature, Journal Year: 2022, Volume and Issue: 611(7937), P. 695 - 701

Published: Oct. 26, 2022

Language: Английский

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Near‐Infrared II Plasmonic Au@Au–Ag Dot‐in‐Cubic Nanoframes for In Vivo Surface‐Enhanced Raman Spectroscopic Detection and Photoacoustic Imaging

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(29)

Published: May 13, 2021

Abstract Near‐infrared II (NIR‐II) plasmonic noble‐metallic nanostructures are highly desirable for in vivo photodiagnostics because of their multiple functionalities and deep‐tissue optical imaging capability. Herein, a novel class Au@Au–Ag dot‐in‐cubic nanoframes (DCFs) comprising solid Au core Au–Ag alloy shell with wall hole on each side face is reported, which exhibit remarkable properties spectrally tunable beyond 1400 nm while maintaining small size. The synthesis DCFs principally based the facet‐selective etching Ag atoms co‐deposition edges corners Au@Ag dot‐in‐cubes. geometry (e.g., edge length size) can be controllably tailored by simply varying silver nitrate chloroauric acid concentrations. Superior vitro NIR‐II photoacoustic performances demonstrated. Additionally, surface‐enhanced Raman spectroscopy (SERS) activity evidenced maximum SERS enhancement occurring at plasmon resonance wavelength blue‐shifting from incident laser an excellent effective detection depth. Finally, potential developed highlighted microtumors animals.

Language: Английский

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All-Hot-Spot Bulk Surface-Enhanced Raman Scattering (SERS) Substrates: Attomolar Detection of Adsorbates with Designer Plasmonic Nanoparticles

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(29), P. 13285 - 13293

Published: July 15, 2022

Here we report a synthetic pathway toward Au truncated octahedral dual-rim nanoframes wherein two functional facets are formed including (1) eight hot nanogaps by hexagonal embracing core circular nanorings for near-field focusing and (2) six flat squares that facilitate the formation of well-ordered arrays through self-assembly. The existence intra-nanogaps in single entity enables strong electromagnetic focusing, allowing single-particle surface-enhanced Raman spectroscopy. Then, built "all-hot-spot bulk SERS substrates" with those entities, presence terraces high homogeneity size shape spontaneous self-assembly into highly ordered uniform superlattice, exhibiting limit detection attomolar concentrations 2-naphthalenethiol, which is 6 orders lower than monorim counterparts. observed low originates from combined synergic effect both inter- intraparticle coupling dubbed substrates".

Language: Английский

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The green chemistry paradigm in modern organic synthesis

Russian Chemical Reviews, Journal Year: 2023, Volume and Issue: 92(12), P. RCR5104 - RCR5104

Published: Dec. 1, 2023

After the appearance of green chemistry concept, which was introduced in vocabulary early 1990s, its main statements have been continuously developed and modified. Currently, there are 10–12 cornerstones that should form basis for an ideal chemical process. This review analyzes accumulated experience achievements towards design products processes reduce or eliminate use generation hazardous substances. The presents views leading Russian scientists specializing various fields this subject, including homogeneous heterogeneous catalysis, fine basic organic synthesis, electrochemistry, polymer chemistry, based on bio-renewable feedstocks energetic compounds materials. A new approach to quantitative evaluation environmental friendliness by authors is described. <br> bibliography includes 1761.

Language: Английский

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Recent advances on CO2 reduction reactions using single-atom catalysts

Renewable and Sustainable Energy Reviews, Journal Year: 2023, Volume and Issue: 190, P. 114086 - 114086

Published: Nov. 18, 2023

Language: Английский

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Seeded Synthesis of Hollow PdSn Intermetallic Nanomaterials for Highly Efficient Electrocatalytic Glycerol Oxidation

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(35)

Published: June 1, 2023

Intermetallic nanomaterials have shown promising potential as high-performance catalysts in various catalytic reactions due to their unconventional crystal phases with ordered atomic arrangements. However, controlled synthesis of intermetallic tunable and unique hollow morphologies remains a challenge. Here, seeded method is developed synthesize PdSn nanoparticles (NPs) two different phases, that is, orthorhombic Pd2 Sn monoclinic Pd3 Sn2 . Benefiting from the rational regulation phase morphology, obtained NPs deliver excellent electrocatalytic performance toward glycerol oxidation reaction (GOR), outperforming solid NPs, commercial Pd/C, which places it among best reported Pd-based GOR electrocatalysts. The mechanism using catalyst investigated by operando infrared reflection absorption spectroscopy, reveals cleaves CC bond more easily compared Pd/C. This work can pave an appealing route diverse novel morphology for applications.

Language: Английский

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Multiple Stepwise Synthetic Pathways toward Complex Plasmonic 2D and 3D Nanoframes for Generation of Electromagnetic Hot Zones in a Single Entity

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(3), P. 270 - 283

Published: Jan. 24, 2023

ConspectusRational design of nanocrystals with high controllability via wet chemistry is critical importance in all areas nanoscience and nanotechnology research. Specifically, morphologically complex plasmonic nanoparticles have received considerable attention because light-matter interactions are strongly associated the size shape nanoparticles. Among many types nanostructures, nanoframes (NFs) controllable structural intricacy could be excellent candidates as strong light-entrappers inner voids well surface area, leading to highly effective interaction light analytes compared their solid counterparts. However, so far studies on single-rim-based NFs suffered from insufficient near-field focusing capability due simplicity (e.g., a single rim or NF molded simple platonic solids), which necessitates conceptually new architecture. If one considers stereoscopic nanostructure dual, triple, multiple resonant intra-nanogaps each crystallographic facet nanocrystals, unprecedented physicochemical properties expected. Realizing such intraparticle plasmon coupling localized resonance very challenging lack synthetic strategic principles systematic control, require deep understanding chemistry. Moreover, realizing those architectures homogeneity bottom-up method where diverse particle involved more challenging. Although there been several reports used for catalysis, techniques production structurally uniformity an correlation between complexity entity electromagnetic remained elusive.In this Account, we will summarize highlight rational pathways two-dimensional (2D) three-dimensional (3D) unique structures characterize optical properties. This strategy based publications our group during last 10 years. First, introduce chemical step transformation triangular Au nanoplates circular hexagonal plates, sacrificial layers formation NFs. Then, describe methods how synthesize monorim-based using Pt scaffolds different shapes correlate near-field. stepwise 2D wherein starting evolved produce circular, triangular, hexagonal, crescent, Y-shaped hot zones. discuss can rims diameters concentrically connected, by exploiting toolkits eccentric concentric growth Au, borrowing concept total synthesis that frequently adopted organic We then dual-rim-faceted frame-in-frame 3D matryoshka geometries well-faceted control intra-nanogaps. Finally, importantly, provide examples advanced hierarchical produced controlling geometrical nanoparticles, number rims, components, expansion library.

Language: Английский

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Oriented Assembled Prussian Blue Analogue Framework for Confined Catalytic Decomposition of Ammonium Perchlorate

Small, Journal Year: 2023, Volume and Issue: 19(20)

Published: Jan. 15, 2023

The design of highly dispersed active sites hollow materials and unique contact behavior with the components to be catalyzed provide infinite possibilities for exploring limits catalyst capacity. In this study, synthesis strategy open 3-dimensional frame structure Prussian blue analogues (CoFe-PBA) was explored through self-transformation, which jointly guided by template mediated epitaxial growth, restricted assembly directional assembly. Additionally, good application prospect CoFe-PBA as combustion discussed. results show that unexpected thermal decomposition can achieved limiting AP(ammonium perchlorate) framework CoFe-PBA. high temperature stage AP advanced 283.6 °C weight loss rate reach 390.03% min-1 . In-situ monitoring shows accelerate formation NO NO2 calculation reaction kinetics proved catalytic process realized increasing nucleation factor. On basis, mechanism on discussed, possible interaction between during heating proposed. At same time, another interesting functional prevent from caking

Language: Английский

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