激光熔覆(CrFeNiAl)100-xMox高熵合金涂层的组织及耐磨耐蚀性能

赵小凤; 崔洪芝; 姜迪; 宋晓杰

激光熔覆(CrFeNiAl)_100-xMo_x高熵合金涂层的组织及耐磨耐蚀性能

赵小凤¹,
崔洪芝^{1, 2, ,},
姜迪¹,
宋晓杰¹

1.
山东科技大学　材料科学与工程学院, 青岛 266950
2.
中国海洋大学　材料科学与工程学院, 青岛 266100

基金项目: 国家自然科学基金 (51971121)；山东省重大科技创新工程项目(2019JZZY010303；2019JZZY010360)

详细信息

通讯作者:
崔洪芝，博士，教授，博士生导师，研究方向为高能束表面强化、增材制造、耐磨蚀抗热震材料等　E-mail: cuihongzhi@ouc.edu.cn

中图分类号: TG174.4
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- 被引次数: 0
出版历程
- 收稿日期: 2022-12-05
- 修回日期: 2023-01-13
- 录用日期: 2023-02-08
- 网络出版日期: 2023-03-02

Microstructure, wear and corrosion resistance of (CrFeNiAl)_100-xMo_xhigh-entropy alloy coatings by laser cladding

1.
School of Materials Science and Engineering, Shandong University of Science and Technology, Qingdao 266590, China
2.
School of Materials Science and Engineering, Ocean University of China, Qingdao 266100, China

Funds: National Natural Science Foundation of China(51971121); Major-Special Science and Technology Projects in Shandong Province (2019JZZY010303; 2019JZZY010360)

摘要

摘要: 海洋资源的开发利用对海洋工程装备提出了更高的要求。风力发电设备、石油钻杆和海上平台等装备的支撑和运作部件在服役过程中不可避免的遭受腐蚀和磨损失效，开发耐磨耐蚀材料对零部件表面进行防护是延长设备服役寿命的有效措施。高熵合金由于其独特的四大效应(高熵效应、晶格畸变效应、缓慢扩散效应和鸡尾酒效应)，可以获得比其他合金更优异的性能。Cr、Al、Ti、Mo等元素常用来提高高熵合金的耐蚀性。但是由于Mo会在σ相等析出物的周围造成元素的偏析，降低耐蚀性，如何实现耐磨和耐蚀的同步提高还需要进一步研究。本文采用激光熔覆技术在304不锈钢上制备不同Mo含量的(CrFeNiAl)_100-xMo_x (x=6，8，11，14 at%) 高熵合金涂层，研究不同Mo含量对涂层的微观结构、硬度、耐磨和耐蚀性能的影响。涂层并没有生成σ相等物相，而是生成了BCC+B2双相，并且在枝晶内部析出纳米级别的B2相。由于固溶强化和第二相强化作用，涂层的硬度逐渐提高，硬度最高达到636.6 HV_0.2，耐磨性也逐渐提高。在3.5 wt.% NaCl溶液中，腐蚀电流密度随着Mo含量的增加，先减小后增大，(CrFeNiAl)₉₂Mo₈的腐蚀电流密度和钝化电流密度均小于304不锈钢，耐蚀性最好，同时具有较好的耐磨性。1(CrFeNiAl)_100-xMo_x涂层的(a)硬度，(b)磨损体积，(c)Tafel曲线
- 激光熔覆 /
- 高熵合金涂层 /
- 硬度 /
- 耐磨性 /
- 耐蚀性
Abstract: For the corrosion and wear failure of materials used in the marine environment, the (CrFeNiAl)_100-xMo_x high-entropy alloy coatings were prepared on 304 stainless steel (304ss) by laser cladding. The phase composition, microstructure, hardness, wear resistance and corrosion resistance of the coatings were analyzed. The results show that the coatings are composed of BCC+B2 phases. With the increase of Mo, the content of B2 phase gradually increases, and nano scale B2 phase precipitates in the dendrite. The hardness of the coating increases with the increase of Mo content, the highest hardness reaches 636.6 HV_0.2, and the wear resistance increases gradually. The corrosion current density firstly decreases and then increases with the increase of Mo, indicating that the corrosion resistance of the coating firstly increases and then decreases in 3.5 wt% NaCl solution. The results of immersion corrosion show that the coatings are selectively dissolved in the interdendritic region. The corrosion current density and passivation current density of (CrFeNiAl)₉₂Mo₈ coating are lower than 304 ss, and the corrosion resistance is the best with good wear resistance. Adding appropriate Mo element can improve the wear resistance and corrosion resistance of (CrFeNiAl)_100-xMo_x coatings.
- laser cladding /
- high-entropy alloy coatings /
- hardness /
- wear resistance /
- corrosion resistance

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图 1 原始粉末的形貌

Figure 1. Morphologies of raw powders

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图 2 (CrFeNiAl)_100-xMo_x涂层的XRD图谱：(a) XRD 图谱；(b) 局部放大图

Figure 2. XRD patterns of (CrFeNiAl)_100-xMo_x coatings: (a) XRD patterns; (b) Local magnification patterns

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图 3 (CrFeNiAl)_100-xMo_x涂层的截面宏观形貌：(a) Mo6；(b) Mo8；(c) Mo11；(d) Mo14

Figure 3. Macro morphologies of cross section of (CrFeNiAl)_100-xMo_x coatings: (a) Mo6; (b) Mo8; (c) Mo11; (d) Mo14

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图 4 (CrFeNiAl)_100-xMo_x 涂层中部的微观组织形貌：(a) Mo6；(b) Mo8；(c) Mo11；(d) Mo14

Figure 4. Topography of microstructure in the middle of (CrFeNiAl)_100-xMo_x coatings: (a) Mo6; (b) Mo8; (c) Mo11; (d) Mo14

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图 5 Mo14的TEM图像：(a) Bright-field TEM 图像； (b)~(c) 晶粒内部的局部放大图；(d) 两个物相的HRTEM 和SEAD图；(e) 相界面的IFFT图

Figure 5. TEM characterization of Mo14: (a) Bright-field TEM image; (b)~(c) Local magnified image of grain interior; (d) HRTEM image and SEAD-pattern of two phases; (e) IFFT image of the interface of the phases

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图 6 Mo14枝晶内部的TEM-HAADF和TEM-EDS图谱

Figure 6. TEM-HAADF image and TEM-EDS mappings in dendrite of Mo14

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图 7 (CrFeNiAl)_100-xMo_x涂层的显微硬度

Figure 7. Microhardness of (CrFeNiAl)_100-xMo_x coatings

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图 8 (CrFeNiAl)_100-xMo_x涂层的摩擦系数

Figure 8. Coefficient of (CrFeNiAl)_100-xMo_x coatings

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图 9 (CrFeNiAl)_100-xMo_x涂层的磨痕截面轮廓(a)和磨损体积(b)

Figure 9. Wear sectional profiles (a) and wear volume losses (b) of (CrFeNiAl)_100-xMo_x coatings

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图 10 (CrFeNiAl)_100-xMo_x涂层磨损表面的SEM形貌和三维形貌：(a1)~(a3) Mo6; (b1)~(b3) Mo8; (c1)~(c3) Mo11; (d1)~(d3) Mo14

Figure 10. SEM morphologies and three-dimensional morphologies of the worn surfaces of (CrFeNiAl)_100-xMo_x coatings：(a1)~(a3) Mo6; (b1)~(b3) Mo8; (c1)~(c3) Mo11; (d1)~(d3) Mo14

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图 11 (CrFeNiAl)_100-xMo_x涂层和304 ss的动电位极化曲线

Figure 11. Potentiodynamic polarization curve of (CrFeNiAl)_100-xMo_x coatings and 304 ss

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图 12 (CrFeNiAl)_100-xMo_x涂层和304 ss的Nyquist (a)和 Bode图(b)

Figure 12. Nyquist plots (a) and Bode plots (b) of (CrFeNiAl)_100-xMo_x coatings and 304 ss

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图 13 (CrFeNiAl)_100-xMo_x涂层和304 ss的等效电路图

Figure 13. Equivalent circuits of (CrFeNiAl)_100-xMo_x coatings and 304 ss

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图 14 (CrFeNiAl)_100-xMo_x涂层在1 M HCl 溶液浸泡120 h的腐蚀形貌的SEM图像和三维形貌：(a1)~(a2) Mo6；(b1)~(b2) Mo8；(c1)~(c2) Mo11；(d1)~(d2) Mo14

Figure 14. SEM and three-dimensional morphologies of (CrFeNiAl)_100-xMo_x coatings after immersion in 1 M HCl for 120 h: (a1)~(a2) Mo6; (b1)~(b2) Mo8; (c1)~(c2) Mo11; (d1)~(d2) Mo14

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表 1 (CrFeNiAl)_100-xMo_x 涂层的化学成分(at%)

Table 1. Chemical composition of (CrFeNiAl)_100-xMo_x coatings (at%)

Sample	Cr	Fe	Ni	Al	Mo
Mo6	23.50	23.50	23.50	23.50	6.00
Mo8	23.00	23.00	23.00	23.00	8.00
Mo11	22.25	22.25	22.25	22.25	11.00
Mo14	21.50	21.50	21.50	21.50	14.00

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表 2 元素之间的混合焓$ \Delta {H}_{AB}^{\mathrm{m}\mathrm{i}\mathrm{x}} $ (kJ·mol⁻¹)^[30]

Table 2. Mixing enthalpy $ \Delta {H}_{AB}^{\mathrm{m}\mathrm{i}\mathrm{x}} $ of the elements (kJ·mol⁻¹)^[30]

Element	Cr	Fe	Ni	Mo	Al
Cr		−1	−7	0	−10
Fe			−2	−2	−11
Ni				−7	−22
Mo					−5
Notes: $ \Delta {H}_{AB}^{\mathrm{m}\mathrm{i}\mathrm{x}} $−Mixing enthalpy, which is approximately equal to the value heat of mixing between A and B^[30]. The more negative $ \Delta {H}_{AB}^{\mathrm{m}\mathrm{i}\mathrm{x}} $ is, the easier for A and B to form compounds^[28].

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表 3 (CrFeNiAl)_100-xMo_x涂层和304 ss的腐蚀电位、腐蚀电流密度和钝化电流密度

Table 3. Corrosion potential, corrosion current density and passivation current density of (CrFeNiAl)_100-xMo_x coatings and 304 ss

Sample	E_corr/mV	I_corr/(μA·cm^-2)	I_p/(μA·cm^-2)
304 ss	-326.90	0.53	2.32
Mo6	-221.60	0 .65	1.18
Mo8	-184.40	0.40	0.91
Mo11	-179.20	0.42	1.31
Mo14	-200.90	0.65	0.95
Notes: E_corr-Corrosion potential; I_corr-Corrosion current density; I_p-Passivation current density.

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表 4 (CrFeNiAl)_100-xMo_x涂层和304 ss的等效电路的拟合参数

Table 4. Fitting parameters of the equivalent circuit model of (CrFeNiAl)_100-xMo_x coatings and 304 ss

Sample	R_s /(Ω·cm²)	R_f /(10³Ω·cm²)	R_ct /(10³Ω·cm²)	Y₁ /(μF·cm⁻²⁾	n₁	Y₂ /(μF·cm⁻²)	n₂	χ²
304 ss	7.4	6.4	82.6	100.5	0.87	199.7	0.94	2.0×10⁻³
Mo6	3.6	2.6	127.5	57.6	0.75	551.4	0.91	7.6×10⁻⁴
Mo8	2.0	2.6	366.3	53.6	0.64	678.9	0.86	6.2×10⁻⁴
Mo11	1.8	2.2	360.1	64.3	0.84	106.5	0.85	4.8×10⁻⁴
Mo14	1.6	7.4	268.5	21.3	0.59	67.3	0.86	8.0×10⁻⁴
Notes: R_s-Solution resistance; R_f-Outer layer resistance; R_ct-Inner layer resistance; Y₁-Capacitance of the outer layer; Y₂-Capacitance of inner layer; n₁-CPE_f index; n₂-CPE_ct index; χ² -Good fitting quality.

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