Ostwald ripening of supported metal nanoparticles: Role of dimers and other general trends

IF 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Chemical Engineering Science Pub Date : 2025-04-01 Epub Date: 2025-02-17 DOI:10.1016/j.ces.2025.121373
Mikhail Mamatkulov, Vladimir P. Zhdanov
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Abstract

Supported ∼10 nm-sized metal particles are widely employed in applications. Under high temperatures typical for industrial catalysis, such nanoparticles often lose activity due to Ostwald ripening. This process is usually considered to occur via exchange of monomers between nanoparticles. The exchange of dimers is, however, also possible. We present equations allowing estimation of the relative role of these channels of ripening and the ratio of dimer and monomer concentrations on the support. The key factor here is the difference between the sublimation and dimer-formation energies. These energies were calculated for Pt, Pd, Ru, Rh, Ag, Au, and Cu by employing density functional theory with and without spin-orbital coupling. With this input, the conventional channel including monomers is found to dominate. The timescales of ripening and deviation of the power-law-growth exponents from the conventional ones are scrutinized as well.

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负载型金属纳米颗粒的奥斯特瓦尔德成熟:二聚体的作用和其他一般趋势
支持的~ 10nm大小的金属颗粒被广泛应用。在工业催化的典型高温下,这种纳米颗粒往往由于奥斯特瓦尔德成熟而失去活性。这个过程通常被认为是通过纳米颗粒之间的单体交换发生的。然而,二聚体的交换也是可能的。我们提出的方程式允许估计这些成熟通道的相对作用和二聚体和单体浓度在载体上的比例。这里的关键因素是升华和二聚体形成能量之间的差异。利用密度泛函理论计算了Pt、Pd、Ru、Rh、Ag、Au和Cu的能量。有了这个输入,包括单体的传统通道被发现占主导地位。并考察了幂律增长指数的成熟时间尺度和与常规指数的偏差。
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来源期刊
Chemical Engineering Science
Chemical Engineering Science 工程技术-工程:化工
CiteScore
7.50
自引率
8.50%
发文量
1025
审稿时长
50 days
期刊介绍: Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.
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