具有独特模拟生长特性的二维PdS2上原位生成硫酸盐促进硝酸盐的高效电合成。

IF 36.3 1区材料科学 Q1 Engineering

Nano-Micro Letters Pub Date : 2025-06-12 DOI:10.1007/s40820-025-01803-3

Rui Zhang, Hui Mao, Ziyi Wang, Shengke Ma, Shuyao Wu, Qiong Wu, Daliang Liu, Hui Li, Yang Fu, Xiaoning Li, Tianyi Ma

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引用次数: 0

摘要

电催化氮氧化反应（NOR）合成硝酸盐是一种绿色可持续的替代技术，可以取代传统的高能耗奥斯特瓦尔德法。但由于N≡N键的高键能和电解质中析氧反应的竞争，其固氮产率低，选择性差，限制了其应用。另一方面，二维（2D） PdS2作为10族新型过渡金属二硫族化合物（NTMDs）家族的成员，由于其新颖的折叠五边形结构而呈现出有趣的光学和电子性质，但其制备和应用方面的研究很少。本文首次发现了PdS2在不同2D衬底上独特的模拟生长特征，并利用界面工程技术构建了2D/2D异质结构。由于暴露在衬底上的化学基团不同，PdS2随着衬底形态的模仿而生长，呈现出不同的厚度、大小、形状和氧化程度，从而导致所得到的复合催化剂的NOR活性和稳定性存在显著差异。特别是通过在二维衬底上修饰聚（1-乙烯基-3-乙基咪唑溴化）可以得到缺陷较多的薄而小的PdS2纳米板，在制备过程中容易氧化，导致原位生成SO42-，这对降低NOR工艺的活化能起着至关重要的作用，从而提高硝酸盐的生产效率，理论计算证实了这一点。该研究为开发基于NTMDs的新型NOR电催化剂提供了有价值的见解，并突出了界面工程在提高催化性能方面的重要性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

查看原文本刊更多论文

In Situ Generated Sulfate-Facilitated Efficient Nitrate Electrosynthesis on 2D PdS2 with Unique Imitating Growth Feature

Highlights

Unique imitating growth feature for PdS₂ on different 2D substrates has been firstly discovered for constructing 2D/2D heterostructures by interface engineering.
The thin and small PdS₂ nanoplates with active defects can be inducted by poly(1-vinyl-3-ethylimidazolium bromide (PVEIB), resulting in the obtained PdS₂@PVEIB/PPy/GO exhibited the excellent nitrogen oxidation reaction (NOR) electroactivity with the outstanding stability and selectivity.
The in situ generation of SO₄²⁻, caused by the oxidation during the preparation process or exposed in air, as well as at high NOR potential, plays a crucial role in reducing the activation energy of the NOR process, leading to improved efficiency for nitrate production.

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来源期刊

Nano-Micro Letters NANOSCIENCE & NANOTECHNOLOGY-MATERIALS SCIENCE, MULTIDISCIPLINARY

CiteScore

32.60

自引率

4.90%

发文量

981

审稿时长

1.1 months

期刊介绍： Nano-Micro Letters is a peer-reviewed, international, interdisciplinary, and open-access journal published under the SpringerOpen brand. Nano-Micro Letters focuses on the science, experiments, engineering, technologies, and applications of nano- or microscale structures and systems in various fields such as physics, chemistry, biology, material science, and pharmacy.It also explores the expanding interfaces between these fields. Nano-Micro Letters particularly emphasizes the bottom-up approach in the length scale from nano to micro. This approach is crucial for achieving industrial applications in nanotechnology, as it involves the assembly, modification, and control of nanostructures on a microscale.