Size-dependent synthesis and catalytic activities of trimetallic PdAgCu mesoporous nanospheres in ethanol electrooxidation

Lv, Hao; Sun, Lizhi; Zou, Lu; Xu, Dongdong; Yao, Huiqin; Liu, Ben

doi:10.1039/c8sc04696d

Cited by 85 publications

(64 citation statements)

References 53 publications

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“…1e. The mesoporous frameworks appear to be crystallographically continuous which should further facilitate mass/electron transfer during the electrocatalysis and improve electrocatalytic performance accordingly 32,42. The selected area electron diffraction (SAED) micrograph of an individual nanosphere exhibited a series of spots within concentric rings, indicating mesoAu is polycrystalline with a face-centered cubic (fcc) crystalline structure (Fig.…”

Section: Resultsmentioning

confidence: 99%

“…Of the various nanosynthesis methodologies available, soft-templating approaches are the most powerful route to generate spherical mesoporous materials with three-dimensional (3D) interior mesochannels 27–29. In comparison with mesoporous carbon,30,31 oxides28 and even other noble metals,32–34 however, the synthesis of mesoAu nanospheres with precisely tailorable sizes and porosities has never been achieved with soft-templates, because of the challenge of controlling the reduction and crystallization of Au around surfactant templates. In addition, the high mobility of negatively charged AuCl 4 – (Au precursor) enables it to quickly migrate out of the soft templates, resulting in the formation of bulk nanoparticles and/or aggregates.…”

Section: Introductionmentioning

confidence: 99%

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Mesoporous gold nanospheres via thiolate–Au(i) intermediates

Henzie

et al. 2019

Chem. Sci.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Mesoporous gold nanospheres via thiolate–Au(i) intermediates

Henzie

et al. 2019

Chem. Sci.

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“…[20] The crystalline structure and periodic spacing were verified using wide-angle X-ray powder diffraction (Figure 1f) analyses, yielding two distinct sets of diffraction peaks which were indexed to fcc crystal structure of both PdPt (JCPDS: 46-1043 for Pd and JCPDS: 04-0802 for Pt) and Au (JCPDS: 04-0784). [20,23] Notably, the atomic edge and kink sites were observed on the rough surface (inset of Figure 1e), suggesting an unsaturated Au and Pt atomic coordination. Further considering the crystalline nature, we hypothesized that the as-prepared trimetallic alloys exhibited high activity and stability, which are advantageous for the next step LDI enhancement.…”

Section: Resultsmentioning

confidence: 99%

Plasmonic Alloys Reveal a Distinct Metabolic Phenotype of Early Gastric Cancer

et al. 2021

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rate up to 90%, but below 36% in the case of advanced GC patients. [1a] An effective approach of early GC detection requires the combination of initial pre-selection of high-risk individuals and follow-up endoscopy examination, while its largescale application is facing challenges like low cost-efficiency (e.g., inefficient preselection by non-specific risk factors), poor patient compliance, and shortage of experienced endoscopists, etc. [2b] Therefore, it is pressing to develop a rapid and noninvasive method to discover biomarkers and diagnose early GC with an improved prognosis.Liquid biopsy allows the detection of oncotarget biomarkers through non-invasive techniques from biofluids (e.g., blood), holding promise for early screening of GC in clinics. [4] Various genetic (e.g., circulating tumor DNA (ctDNA)) [5] and protein (e.g., carcino embryonic antigen (CEA)) biomarkers in human blood have been discovered for GC diagnosis, but the applicable performance is limited by suboptimal accuracy (e.g., sensitivity of 13% for CEA), [6] high cost (€140 per test), [7] and lack of validation in early GC patients. [1b,8] Besides genes and proteins, metabolites serve as direct signatures of biochemical activity and are associated with gastric carcinogenesis. [9] Mass spectrometry (MS), particularly laser desorption/ionization (LDI) MS, is a powerful analytical tool capable of the simultaneous detection and spatial mapping of various metabolites. [10] However, it is offset in metabolic profiling with Gastric cancer (GC) is a multifactorial process, accompanied by alterations in metabolic pathways. Non-invasive metabolic profiling facilitates GC diagnosis at early stage leading to an improved prognostic outcome. Herein, mesoporous PdPtAu alloys are designed to characterize the metabolic profiles in human blood. The elemental composition is optimized with heterogeneous surface plasmonic resonance, offering preferred charge transfer for photoinduced desorption/ionization and enhanced photothermal conversion for thermally driven desorption. The surface structure of PdPtAu is further tuned with controlled mesopores, accommodating metabolites only, rather than large interfering compounds. Consequently, the optimized PdPtAu alloy yields direct metabolic fingerprints by laser desorption/ionization mass spectrometry in seconds, consuming 500 nL of native plasma. A distinct metabolic phenotype is revealed for early GC by sparse learning, resulting in precise GC diagnosis with an area under the curve of 0.942. It is envisioned that the plasmonic alloy will open up a new era of minimally invasive blood analysis to improve the surveillance of cancer patients in the clinical setting.

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“…Q is the conversion factor, commonly taken as 0.386 mC cm −2 for gold, [ 27 ] 0.420 mC cm −2 for platinum, [ 28 ] and 0.405 mC cm −2 for palladium. [ 29 ] The calculated ECSAs for all noble metal coatings are displayed in Figure 3d. It can be clearly seen that coatings from simply drop‐casted and dried nanoparticle solutions (black) show the smallest accessible, active surface area (10.5–12 m 2 g −1 ), which was expected due to their flat and non‐superstructured nature.…”

Section: Resultsmentioning

confidence: 99%

Cryoaerogels and Cryohydrogels as Efficient Electrocatalysts

Müller

Zámbó

Dorfs

et al. 2021

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Additive‐free cryoaerogel coatings from noble metal nanoparticles are prepared and electrochemically investigated. By using liquid nitrogen or isopentane as cooling medium, two different superstructures are created for each type of noble metal nanoparticle. These materials (made from the same amount of particles) have superior morphological and catalytic properties as compared to simply immobilized, densely packed nanoparticles. The morphology of all materials is investigated with scanning electron microscopy (SEM). Electrochemically active surface areas (ECSAs) are calculated from cyclic voltammetry measurements. The catalytic activity is studied for the ethanol oxidation reaction (EOR). Both are found to be increased for superstructured materials prepared by cryoaerogelation. Furthermore, cryoaerogels with cellular to dendritic structure that arise from freezing with isopentane show the best catalytic performance and highest ECSA. Moreover, as a new class of materials, cryohydrogels are created for the first time by thawing flash‐frozen nanoparticle solutions. Structure and morphology of these materials match with the corresponding types of cryoaerogels and are confirmed via SEM. Even the catalytic activity in EOR is in accordance with the results from cryoaerogel coatings. As a proof of concept, this approach offers a novel platform towards the easier and faster production of cryogelated materials for wet‐chemical applications.

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Size-dependent synthesis and catalytic activities of trimetallic PdAgCu mesoporous nanospheres in ethanol electrooxidation

Abstract: A facile solution-phase synthetic approach is reported to engineer the size effect of sub-100 nm PdAgCu mesoporous nanospheres in ethanol electrooxidation.

Cited by 85 publications

References 53 publications

Mesoporous gold nanospheres via thiolate–Au(i) intermediates

Mesoporous gold nanospheres via thiolate–Au(i) intermediates

Plasmonic Alloys Reveal a Distinct Metabolic Phenotype of Early Gastric Cancer

Cryoaerogels and Cryohydrogels as Efficient Electrocatalysts

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