Microfluidic Tailoring of a Ru Nanodots/Carbon Heterocatalyst for Electrocatalytic Nitrogen Fixation

Liu, Hengyuan; Wu, Xingjiang; Xu, Jianhong

doi:10.1021/acsanm.3c01966

Cited by 5 publications

(2 citation statements)

References 38 publications

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“…Various functionalized materials have been successfully synthesized through the microfluidic platforms, such as monodisperse nanoparticles, 47 carbon dots, 48 perovskite nanocrystals, 49 and heterostructured carbon materials. 50 However, to our knowledge, microfluidic fabrication for two-dimensional heterocatalysts with ultrasmall active sites has never been reported.…”

Section: ■ Introductionmentioning

confidence: 99%

Two-Dimensional N-Doped Carbon with Embedded Microfluidic-Architected Fe, Mo Nanodots toward Efficient Electrocatalytic Nitrogen Reduction

Liu,

Zeng

et al. 2024

ACS Sustainable Chem. Eng.

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Electrocatalytic nitrogen reduction reaction (ENRR) is emerging as a promising routine for the sustainable production of ammonia. Hindered by the strong triple bond in N 2 and unfavorable hydrogen evolution reaction, it is critical to develop efficient catalysts with excellent activity and selectivity. Herein, we propose a novel microfluidic platform that achieves the continuous synthesis and morphology regulation of a twodimensional heterocatalyst FeMo/g-C 3 N 4 through a precipitation process in a confined space. Owing to the rapid mixing and microfluidic manipulation, FeMo/g-C 3 N 4 maintains an overwhelmingly favorable structure compared to the batch methods. Benefiting from the ultrasmall active sites (0.86 nm), homogeneous nanodot distribution, and abundant 2D surface, the promoted N 2 chemisorption and competitive ENRR performance can be simultaneously ensured, as confirmed by the experimental studies. By varying the applied working potential, the optimal ammonia yield can be determined as 33.25 μg h −1 mg cat.−1 at −1.2 V. This work innovatively opens a pathway for morphological fine structural tuning of two-dimensional heterocatalysts, further promoting the ENRR field's development.

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Section: ■ Introductionmentioning

confidence: 99%

Two-Dimensional N-Doped Carbon with Embedded Microfluidic-Architected Fe, Mo Nanodots toward Efficient Electrocatalytic Nitrogen Reduction

Liu,

Zeng

et al. 2024

ACS Sustainable Chem. Eng.

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“…Ammonia (NH 3 ) is one of the most important chemicals in chemical production and is extensively used in many fields such as chemical industry, agriculture, and medicine. − Currently, most NH 3 is synthesized using the conventional Haber–Bosch process, but it requires high temperature and pressure and causes large amounts of CO 2 emissions. − Therefore, developing a sustainable NH 3 synthesis under mild conditions is an urgent direction. − In recent years, the electrocatalytic nitrogen reduction reaction (NRR) has attracted much attention because of its mild reaction conditions and the fact that it is driven by a renewable power source. − Nevertheless, the difficulty of breaking the NN bond and the competitive hydrogen evolution reaction (HER) result in low selectivity and Faraday efficiency (FE). − Therefore, it is crucial to develop electrocatalysts with high activity for the NRR.…”

Section: Introductionmentioning

confidence: 99%

Boron-Doped PdRh Mesoporous Nanotubes for Electrocatalytic Nitrogen Reduction to Ammonia

Yang,

Zhang,

et al. 2024

ACS Appl. Nano Mater.

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It is important to achieve sustainable ammonia production under mild conditions, and the electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy. However, the precise construction of highly active NRR electrocatalysts for ammonia synthesis remains challenging. Here, we construct Bdoped PdRh mesoporous nanotubes (B-PdRh MNTs) as efficient NRR electrocatalysts. The mesoporous nanotubular structure provides abundant active sites, and B doping enhances the adsorption energy of N 2 . As such, the NH 3 yield and Faraday efficiency of B-PdRh MNTs reach 12.03 μg h −1 mg cat −1 and 16.28% under 0.1 M Na 2 SO 4 , respectively. This work provides strategies for B-doped catalysts for efficient electrocatalytic NRR applications.

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A Novel Bubble‐based Microreactor for Enhanced Mass Transfer Dynamics toward Efficient Electrocatalytic Nitrogen Reduction

Liu,

et al. 2023

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Electrocatalytic nitrogen reduction reaction (eNRR) is a promising method for sustainable ammonia production. Although the majority of studies on the eNRR are devoted to developing efficient electrocatalysts, it is critical to study the influence of mass transfer because of the poor N2 transfer efficiency. Herein, a novel bubble‐based microreactor (BBMR) is proposed that efficiently promotes the mass transfer behavior during the eNRR using microfluidic strategies. The BBMR possesses abundant triphasic interfaces and provides spatial confinement and accurate potential control, ensuring rapid mass transfer dynamics and improved eNRR performance, as confirmed by experimental and simulation studies. The ammonia yield of the reaction over Ag nanoparticles can be enhanced to 31.35 µg h−1 mgcat.−1, which is twice that of the H‐cell. Excellent improvements are also achieved using Ru/C and Fe/g‐CN catalysts, with 5.0 and 8.5 times increase in ammonia yield, respectively. This work further demonstrates the significant effect of mass transfer on the eNRR performance and provides an effective strategy for process enhancement through electrode design.

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Microfluidic Tailoring of a Ru Nanodots/Carbon Heterocatalyst for Electrocatalytic Nitrogen Fixation

Cited by 5 publications

References 38 publications

Two-Dimensional N-Doped Carbon with Embedded Microfluidic-Architected Fe, Mo Nanodots toward Efficient Electrocatalytic Nitrogen Reduction

Two-Dimensional N-Doped Carbon with Embedded Microfluidic-Architected Fe, Mo Nanodots toward Efficient Electrocatalytic Nitrogen Reduction

Boron-Doped PdRh Mesoporous Nanotubes for Electrocatalytic Nitrogen Reduction to Ammonia

A Novel Bubble‐based Microreactor for Enhanced Mass Transfer Dynamics toward Efficient Electrocatalytic Nitrogen Reduction

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