Enhancing Green Ammonia Electrosynthesis through Bi–Mo Bimetallic Oxides on Two-Dimensional Ti3C2Tx MXene under Ambient Conditions

IF 9.6 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2025-03-27 DOI:10.1021/acsmaterialslett.4c0267910.1021/acsmaterialslett.4c02679

Rui Zhang, Shanna An, Jiali Ren, Min Ma, Qingzhong Xue and Jian Tian*,

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Abstract

In this paper, Bi–Mo bimetallic oxides (Bi₂Mo₃O₁₂) were successfully grown on two-dimensional (2D) Ti₃C₂T_x MXene nanosheets by a hydrothermal reaction to form Bi₂Mo₃O₁₂@Ti₃C₂T_x composites and used for an electrocatalytic nitrogen reduction reaction. The experimental results show that in a 0.1 M Na₂SO₄ electrolyte the NH₃ yield rate of Bi₂Mo₃O₁₂@Ti₃C₂T_x reaches 78.52 μg^–1 mg^–1_cat. at −0.7 V vs RHE. This result is much higher than those of Bi₂Mo₃O₁₂ (23.45 μg h^–1 mg^–1_cat.) and Ti₃C₂T_x MXene (16.34 μg h^–1 mg^–1_cat.) alone. And the Faraday efficiency (FE) of Bi₂Mo₃O₁₂@Ti₃C₂T_x reaches the highest value of 49.38% at −0.55 V vs RHE (Bi₂Mo₃O₁₂, 12.16%; Ti₃C₂T_x MXene, 9.3%). Meanwhile, the ¹H NMR spectrum of ¹⁵N proves that the N of NH₃ in the experiment comes from the N₂ atmosphere passed during the experiment. Density functional theory (DFT) calculations indicate that the reduction pathway of N₂ on Bi₂Mo₃O₁₂@Ti₃C₂T_x is dominated by the distal pathway.

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环境条件下二维Ti3C2Tx MXene双金属氧化物增强绿色氨电合成

本文通过水热反应在二维（2D） Ti3C2Tx MXene纳米片上成功生长了Bi-Mo双金属氧化物（Bi2Mo3O12），形成Bi2Mo3O12@Ti3C2Tx复合材料，并用于电催化氮还原反应。实验结果表明，在0.1 M Na2SO4电解液中，Bi2Mo3O12@Ti3C2Tx的NH3产率达到78.52 μg-1 mg-1cat。在−0.7 V vs RHE下。该结果远高于Bi2Mo3O12 （23.45 μg h-1 mg-1cat .）和Ti3C2Tx MXene （16.34 μg h-1 mg-1cat .）单独使用。Bi2Mo3O12@Ti3C2Tx的法拉第效率（FE）在−0.55 V时达到最大值49.38%，而RHE (Bi2Mo3O12, 12.16%；Ti3C2Tx MXene, 9.3%)。同时，15N的1H NMR谱也证明了实验中NH3的N来自于实验过程中通过的N2大气。密度泛函理论（DFT）计算表明，N2在Bi2Mo3O12@Ti3C2Tx上的还原途径以远端途径为主。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.