微观浓度场对银生长形貌的调控作用

doi:10.11949/0438-1157.20200090

化工学报 ›› 2020, Vol. 71 ›› Issue (S2): 281-288.DOI: 10.11949/0438-1157.20200090

• 材料化学工程与纳米技术 • 上一篇下一篇

微观浓度场对银生长形貌的调控作用

胥永辉^1,²(),陈道梁³,孙东科³,李金兵⁴,韩永生^1,²()

^1.中国科学院过程工程研究所多相复杂系统国家重点实验室，北京 100190
^2.中国科学院大学化工学院，北京 100049
^3.东南大学机械工程学院，江苏南京 211189
^4.中国石化北京北化院燕山分院，北京 102500

收稿日期:2020-01-20 修回日期:2020-03-05 出版日期:2020-11-06 发布日期:2020-11-06
通讯作者: 韩永生
作者简介:胥永辉（1993—），男，硕士研究生，yhxu@ipe.ac.cn
基金资助:
国家自然科学基金项目(91934302)

Role of micro-concentration field on morphology of silver particles

Yonghui XU^1,²(),Daoliang CHEN³,Dongke SUN³,Jinbing LI⁴,Yongsheng HAN^1,²()

^1.State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
^2.School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
^3.School of Mechanical Engineering, Southeast University, Nanjing 211189, Jiangsu, China
^4.Yanshan Branch of Sinopec Beijing Research Institute of Chemical Industry, Beijing 102500, China

Received:2020-01-20 Revised:2020-03-05 Online:2020-11-06 Published:2020-11-06
Contact: Yongsheng HAN

摘要/Abstract

摘要：

利用原位光学显微镜和计算模拟技术研究了材料生长界面微观浓度场对材料结构演化的影响。在电沉积法制备银颗粒中，通过调控电位在电解液中生成氧化银胶体粒子。在外加电场作用下胶体粒子在溶液中运动，进而带动溶质的定向迁移；通过外加电场控制胶体粒子迁移速度，调控生长界面溶质浓度分布。随胶体粒子迁移速度增加，界面传质增强，颗粒生长前沿扩散层变薄，浓度梯度变大，银颗粒形貌由球状纳米晶变为对称枝晶结构，生长速度由10 μm²/s 增大到60 μm²/s。最后结合格子Boltzmann模拟结果，验证了界面浓度场对银颗粒形貌演化的调控作用。

关键词: 微观浓度场, 银颗粒, 原位研究, 动态生长, 形貌演化, 浓度梯度

Abstract:

To reveal the role of interface micro-concentration distribution on the evolution of materials structure, silver crystallization was investigated by the in-situ optical microscopy and lattice Boltzmann simulations. Silver particles were synthesized by electrodeposition, in which silver oxide colloid particles were generated as the by-products. The migration velocity of colloid particles in the electrolyte was regulated by the electric field. With the increase of migration velocity of colloid particle, mass transfer increased, the diffusion layer in the front of the growth became thinner, and the concentration gradient became sharper. As a result, the morphology of silver particles changed from spherical nanocrystals to symmetrical dendrites, and the growth rate increased from 10 μm²/s to 60 μm²/s simultaneously. Finally, it was proposed that the micro-concentration field in the diffusion layer is the main mechanism dominating the evolution of particle morphology, which was verified by the lattice Boltzmann simulation of convection diffusion and phase transition.

Key words: micro-concentration field, silver particle, in-situ investigation, dynamic growth, morphology evolution, concentration gradient

中图分类号:

TQ 151.5

胥永辉, 陈道梁, 孙东科, 李金兵, 韩永生. 微观浓度场对银生长形貌的调控作用[J]. 化工学报, 2020, 71(S2): 281-288.

Yonghui XU, Daoliang CHEN, Dongke SUN, Jinbing LI, Yongsheng HAN. Role of micro-concentration field on morphology of silver particles[J]. CIESC Journal, 2020, 71(S2): 281-288.

图/表 8

图1 原位观察银颗粒生长的实验装置(a)和胶体粒子的传递方向(b)

Fig.1 Experimental setup for in-situ observation of silver particles growth (a) and direction of colloidal particle transmission (b)

表1 物性参数

Table 1 Physical parameters

参数	符号	数值
初始溶质浓度	c₀	3%
溶质分配系数	k_p	0.17
液相线斜率	m_L	-2.6 K/%(质量)
Gibbs-汤姆逊系数	Γ₀	2.36^-7 mK
液态扩散系数	D_L	3.0^-9 m²/s
固态扩散系数	D_s	3.0^-12
流体运动黏度	ν	5.65657^-7 m²/s
界面动力学各向异性	ε	0.30 m²/s
运动学系数	μ_k,0	2.0^-3 m/(K·s)

图2 胶体粒子调控溶质微观浓度场的示意图(a)，反应过程中阴极前沿的胶体粒子(b)，胶体颗粒的XRD谱图及SEM形貌图(c)

Fig.2 An illustration of solute micro-concentration field regulated by colloidal particles (a)， colloidal particles at the cathode front during reaction (b)， XRD pattern and SEM image of colloidal particles (c)

图3 通过电场强度调控胶体粒子的迁移速度

Fig.3 Migration velocity of colloidal particles regulated by electric field intensity

图4 溶质微观浓度场被调控后所生成的银颗粒形貌和生长速度

Fig.4 Morphology and growth velocity of silver particles after solute micro-concentration field being regulated

图5 不同形貌银颗粒的生长速度

Fig.5 Growth velocity of three morphologies of silver particles

图6 溶质微观浓度场对银颗粒形貌的调控机制

Fig.6 Regulation mechanism of solute micro-concentration field on silver particle morphology

图7 基于lattice Boltzmann模拟下晶粒尖端扩散层和浓度梯度随流速的变化(a),流速u=0.0001(b)、u=0.1(c)扩散层的可视化结果

Fig.7 Variation of diffusion layer and concentration gradient at grain tip with flow velocity obtained by lattice Boltzmann simulation(a), visualization of diffusion layer at u = 0.0001 (b) and u = 0.1 (c)

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微观浓度场对银生长形貌的调控作用

Role of micro-concentration field on morphology of silver particles

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