Interfacial adsorption-diffusion behavior and titanium-induced catalytic mechanism in Cu-Sn-Ti brazed diamond: First-principles and experimental study

IF 4.3 3区材料科学 Q2 MATERIALS SCIENCE, COATINGS & FILMS

Diamond and Related Materials Pub Date : 2025-05-08 DOI:10.1016/j.diamond.2025.112430

Bing Cui , Tao Jiang , Quanbin Du , Lei Wang , Ang Li , Zhanjiang Fang

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Abstract

To investigate the adsorption and diffusion behaviors of interfacial elements and the formation mechanism of the interfacial structure in Cu-Sn-Ti brazed diamond, first-principles calculations were employed to systematically evaluate the adsorption and migration properties of Cu, Sn, and Ti atoms on the diamond (111) surface. A comparative analysis of binding energies and electronic structures was conducted among the Cu-Sn-Ti filler alloy, pure Cu, and the diamond (111) surface. Furthermore, Raman spectroscopy was utilized to quantify the graphitization degree of post-brazed diamond. The results revealed that Ti plays a critical role in enhancing the interfacial bonding strength and structural stability between the Cu-based filler alloy and diamond. The adsorption energies of Cu, Sn and Ti at their optimal adsorption sites on the diamond (111) surface were calculated as follows: E_absTi (9.86 eV) > E_absSn (6.94 eV) > E_absCu (4.11 eV), and the change rate of layer spacing between first and second layer of diamond was 19.62 % after the adsorption of Ti atoms. The diffusion energy barrier values of Cu, Sn and Ti on the diamond (111) crystal surface are Ti (0.53 eV)

>

Sn (0.314 eV)

>

Cu (0.218 eV), respectively. This means that: the diffusion difficulty of Cu or Sn atoms on the diamond crystal surface is low and the adsorption performance is poor, and Ti atoms can seize the adsorption sites of Cu or Sn atoms on the diamond crystal surface. Under conditions of co-adsorption by identical atoms, such as (Cu-Cu@diamond) or (Ti-Ti@diamond), the adsorption performance of individual atoms on the diamond surface is enhanced, whereas co-adsorption by (Sn-Sn@diamond) tends to weaken the adsorption performance of individual atoms on the diamond surface. Co-adsorption by different types of atoms generally reduces the adsorption performance of each atom on the diamond surface. Raman experimental results show that there is a clear graphitization peak in diamond after the addition of Ti, and that Ti plays a crucial role in improving the bonding strength between the Cu-based filler alloy and the diamond crystal surface.

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Cu-Sn-Ti钎焊金刚石界面吸附扩散行为及钛诱导催化机理：第一性原理与实验研究

为了研究Cu-Sn-Ti钎焊金刚石中界面元素的吸附和扩散行为以及界面结构的形成机制，采用第一性原理计算方法系统地评价了Cu、Sn和Ti原子在金刚石（111）表面的吸附和迁移性能。对比分析了Cu- sn - ti填充合金、纯Cu和金刚石（111）表面的结合能和电子结构。利用拉曼光谱对钎焊后金刚石的石墨化程度进行了量化。结果表明，Ti对提高cu基钎料合金与金刚石的界面结合强度和结构稳定性起着至关重要的作用。Cu、Sn和Ti在金刚石（111）表面最佳吸附位点的吸附能计算如下：EabsTi (9.86 eV) >；EabsSn (6.94 eV) >；eabcu (4.11 eV)，吸附Ti原子后，第一层和第二层金刚石层间距变化率为19.62%。Cu、Sn和Ti在金刚石（111）晶体表面的扩散能垒值分别为Ti (0.53 eV)>；Sn (0.314 eV) >；Cu （0.218 eV）。这意味着：Cu或Sn原子在金刚石晶体表面的扩散难度较低，吸附性能较差，而Ti原子可以抢占Cu或Sn原子在金刚石晶体表面的吸附位点。在相同原子的共吸附条件下，如（Cu-Cu@diamond）或（Ti-Ti@diamond），单个原子在金刚石表面的吸附性能增强，而（Sn-Sn@diamond）的共吸附往往会削弱单个原子在金刚石表面的吸附性能。不同类型原子的共吸附一般会降低每个原子在金刚石表面的吸附性能。拉曼实验结果表明，加入Ti后，金刚石中存在明显的石墨化峰，表明Ti对提高cu基填充合金与金刚石晶体表面的结合强度起着至关重要的作用。

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来源期刊

Diamond and Related Materials 工程技术-材料科学：综合

CiteScore

6.00

自引率

14.60%

发文量

702

审稿时长

2.1 months

期刊介绍： DRM is a leading international journal that publishes new fundamental and applied research on all forms of diamond, the integration of diamond with other advanced materials and development of technologies exploiting diamond. The synthesis, characterization and processing of single crystal diamond, polycrystalline films, nanodiamond powders and heterostructures with other advanced materials are encouraged topics for technical and review articles. In addition to diamond, the journal publishes manuscripts on the synthesis, characterization and application of other related materials including diamond-like carbons, carbon nanotubes, graphene, and boron and carbon nitrides. Articles are sought on the chemical functionalization of diamond and related materials as well as their use in electrochemistry, energy storage and conversion, chemical and biological sensing, imaging, thermal management, photonic and quantum applications, electron emission and electronic devices. The International Conference on Diamond and Carbon Materials has evolved into the largest and most well attended forum in the field of diamond, providing a forum to showcase the latest results in the science and technology of diamond and other carbon materials such as carbon nanotubes, graphene, and diamond-like carbon. Run annually in association with Diamond and Related Materials the conference provides junior and established researchers the opportunity to exchange the latest results ranging from fundamental physical and chemical concepts to applied research focusing on the next generation carbon-based devices.