A general synthesis approach for supported bimetallic nanoparticles via surface inorganometallic chemistry

Science, Год журнала: 2018, Номер 362(6414), С. 560 - 564

Опубликована: Ноя. 1, 2018

More alloying on silica Controlling the stoichiometry and achieving a high degree of metals at ultrasmall scales for catalysis can be difficult. Double complex salts, formed by cation like Pd(NH 3 ) 4 2+ an anion IrCl 6 2− , should excellent precursors but are poorly soluble difficult to adsorb directly metal oxide surfaces. Ding et al. show that sequentially adsorbing cations anions from organic solvents onto surface, followed heating in hydrogen, creates well-mixed nanoparticles, most less than nanometers diameter, variety alloys. These materials were then tested as catalysts acetylene hydrogenation ethylene. Science this issue p. 560

Язык: Английский

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Optimising surface d charge of AuPd nanoalloy catalysts for enhanced catalytic activity

Nature Communications, Год журнала: 2019, Номер 10(1)

Опубликована: Март 29, 2019

Abstract Understanding the catalytic mechanism of bimetallic nanocatalysts remains challenging. Here, we adopt an adsorbate mediated thermal reduction approach to yield monodispersed AuPd catalysts with continuous change Pd-Au coordination numbers embedded in a mesoporous carbonaceous matrix. The structure nanoalloys is well-defined, allowing for direct determination structure-property relationship. results show that Pd single atom and dimer are active sites base-free oxidation primary alcohols. Remarkably, d -orbital charge on surface serves as descriptor states hence performance. maximum -charge gain occurred composition 33–50 at% corresponds up 9 times enhancement reaction rate compared neat Pd. findings not only open avenue towards rational design but also enable identification key steps involved reactions.

Язык: Английский

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Selective photocatalytic oxidation of methane by quantum-sized bismuth vanadate

Nature Sustainability, Год журнала: 2021, Номер 4(6), С. 509 - 515

Опубликована: Фев. 4, 2021

Язык: Английский

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Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Май 25, 2022

Methane (CH4) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues regarding both conversion selectivity. Herein, visible irradiation (420 nm), synergy of palladium (Pd) atom cocatalyst oxygen vacancies (OVs) on In2O3 nanorods enables superior photocatalytic CH4 activation by O2. The optimized catalyst reaches ca. 100 μmol h-1 C1 oxygenates, with selectivity primary products (CH3OH CH3OOH) up 82.5%. Mechanism investigation elucidates that such induced dedicated function Pd single atoms boosting hole electron transfer, respectively. O2 proven be only source for CH3OH production, while H2O acts as promoter efficient ·OH production facilitates product desorption indicated DFT modeling. This work thus provides new understandings simultaneous regulation activity cocatalysts vacancies.

Язык: Английский

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Water enables mild oxidation of methane to methanol on gold single-atom catalysts

Nature Communications, Год журнала: 2021, Номер 12(1)

Опубликована: Фев. 22, 2021

Abstract As a 100% atom-economy process, direct oxidation of methane into methanol remains as grand challenge due to the dilemma between activation and over-oxidation methanol. Here, we report that water enabled mild with >99% selectivity over Au single atoms on black phosphorus (Au 1 /BP) nanosheets under light irradiation. The mass activity /BP reached 113.5 μmol g catal −1 in pressured 33 bar mixed gas (CH 4 :O 2 = 10:1) at 90 °C irradiation (1.2 W), while energy was 43.4 kJ mol . Mechanistic studies revealed assisted O generate reactive hydroxyl groups •OH radicals Hydroxyl reacted form CH 3 * species, followed by via Considering recycling during whole can also regard catalyst.

Язык: Английский

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