Research progress of medical magnesium alloy properties and its alloying improvement path
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摘要: 医用镁合金耐腐蚀性能和强度相较于传统医用金属材料较差，严重限制了其在医疗器械领域中的应用。研究表明，合金化可以显著改善医用镁合金的性能，但是由于不同合金元素的加入对镁合金力学性能、耐腐蚀性能和生物相容性的影响不同，并且元素对合金的改善效果也存在差异。因此，研究不同元素的添加对医用镁合金性能影响具有重要的意义。本文首先综述了近年来对镁基合金力学性能、腐蚀降解性能及其生物相容性的综合研究，其次分析了镁基合金在添加了不同合金元素下的性能差异，并针对合金化后医用镁基合金材料的局限性，提出了未来发展建议，期望为今后的临床应用提供宝贵经验。Abstract: The corrosion resistance and strength of magnesium alloys are poor compared to traditional medical metal materials, which seriously limits their application in the field of medical devices. Studies have shown that alloying can significantly improve the properties of medical magnesium alloys, but due to the different effects of the addition of different alloying elements on the mechanical properties, corrosion resistance and biocompatibility of magnesium alloys, and there are differences in the improvement effect of the elements on the alloys. Therefore, it is of great significance to study the effects of the addition of different elements on the properties of medical magnesium alloys. This paper firstly reviews the comprehensive studies on the mechanical properties, corrosion degradation properties and their biocompatibility of magnesium-based alloys in recent years, and secondly analyses the differences in the properties of magnesium-based alloys with the addition of different alloying elements, and puts forward suggestions for the future development of medical magnesium-based alloy materials in view of the limitations of alloying and expects to provide valuable experience for future clinical applications.
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图 1 ((a), (b)) 附着在不同表面上的血小板的SEM图像和数量；(c) 不同样品上血小板的环鸟苷单磷酸(cGMP)表达；((d), (e)) 不同样品的溶血率和活化部分凝血活酶时间(APTT)[36]
Significance level *P<0.05 indicates statistical differences compared to Mg; **P<0.05 indicates statistical differences compared to all other groups; PHA—Calcium hydroxyapatite; GOCS—Graphene oxide cholesterol sulfate; Pro—Protein; cGMP—Cyclic guanosine monophosphate; APTT—Activated partial thromboplastin time
Figure 1. ((a), (b)) SEM images and number of platelets attached to different surfaces; (c) cGMP expression of platelets on different samples; ((d), (e)) Haemolysis rate and APTT of different samples[36]
图 2 镁离子通过促进增殖和分化来增强成骨示意图：(a) Mg2+通过Mitogen-Activated Protein Kinase/Extracellular Signal-Regulated Kinase途径(控制干细胞成骨分化的信号通路之一)促进干细胞分化为成骨细胞；(b) Mg2+通过改善成骨分化促进新骨形成；(c) Mg2+通过上调骨髓间充质干细胞中的愈合骨骼中的细胞外基质成分(COL10 A1)和血管内皮生长因子(VEGF)的表达来增强骨再生；(d) Mg2+激活Wingless/Integrated信号通路(在细胞间进行通信和调控的机制)以上调β-连环蛋白及其下游基因(LEF1、DKK1)的表达[37]
MagT1—Magnesium transporter 1; MAPK/ERK—Mitogen-activated protein kinase/extracellular signal-regulated kinase; NFAT—Nuclear factor of activated T-cells; PGC-1α—Peroxisome proliferator-activated receptor gamma coactivator 1-alpha; ERRα—Estrogen-related receptor alpha; VEGF—Vascular endothelial growth factor; hBMSCs—Bone marrow stromal cells; DRG—Dorsal root ganglion; MAGT1—Magnesium transporter 1; TRPM7—Transient receptor potential melastatin 7; CGRP—Calcitonin gene-related peptide; CALCRL-RAMP1—Calcitonin receptor-like receptor-receptor activity-modifying protein 1; PDSC—Periosteum-derived stem cells; cAMP—Cyclic adenosine monophosphate; P—Phosphate; CREM1—cAMP responsive element modulator 1; CTNNB1—Catenin beta 1; LEF1—Lymphoid enhancer-binding factor 1; DKK1—Dickkopf-1; Wnt—Wingless/Integrated
Figure 2. Schematic diagram of magnesium ions enhancing osteogenesis by promoting proliferation and differentiation: (a) Mg2+ promotes differentiation of stem cells into osteoblasts via Mitogen-Activated Protein Kinase/Extracellular Signal-Regulated Kinase pathway (one of the signaling pathways controlling osteogenic differentiation of stem cells); (b) Mg2+ promotes new bone formation by improving osteogenic differentiation; (c) Mg2+ enhances bone regeneration by upregulating extracellular matrix components in healing bone (COL10 A1) and vascular endothelial growth factor (VEGF) expression in bone marrow mesenchymal stem cells; (d) Mg2+ activates Wingless/Integrated signaling pathway (mechanisms for communication and regulation between cells) upregulates the expression of β-linked protein and its down-stream genes (LEF1, DKK1)[37]
图 4 Mg-4Zn-0.5Ca-xMn合金在Hank'溶液中30天的腐蚀速率及其飞行时间二次离子质谱法(ToF-SIMS)对氯离子、MnO和MnO2薄膜进行2D成像分析：(a) Mg-4Zn-0.5Ca；(b) Mg-4Zn-0.5Ca-0.4Mn；(c) 4 h后Hank'溶液中的Mg-0Zn-5.0Ca-8.2Mn合金[69]
Figure 4. Depicts the corrosion rate of Mg-4Zn-0.5Ca-xMn alloy in the Hank's solution for 30 days, along with the 2D imaging analysis of chloride ions, MnO, and MnO2 thin films using time-of-flight secondary ion mass spectrometry (ToF-SIMS): (a) Mg-4Zn-0.5Ca; (b) Mg-4Zn-0.5Ca-0.4Mn;(c) Mg-0Zn-5.0Ca-8.2Mn alloy after 4 h in Hank's solution[69]
图 5 植入前后肝肾功能的主要血清生化指标水平：(a) 丙氨酸氨基转移酶；(b) 天冬氨酸氨基转移酶；(c) 肌酐；(d) 血尿素氮；(e)血清镁[75]
Figure 5. Levels of the main serum biochemical indicators of liver and kidney function before and after implantation: (a) Alanine aminotransferase; (b) Aspartate aminotransferase; (c) Creatinine; (d) Blood urea nitrogen; (e) Serum magnesium[75]
ALT—Alanine aminotransferase
图 6 镁铟合金腐蚀过程中电化学置换反应的横截面机制示意图：(a)铟离子在镁表面的吸附和置换反应等腐蚀过程；(b) 短时间(25天)浸泡后形成的腐蚀层；(c)长期(200天)浸泡后形成的腐蚀层[79]
Figure 6. Cross-sectional mechanism of electrochemical replacement reactions during corrosion of magnesium-indium alloys: (a) Corrosion processes such as adsorption of indium ions on the magnesium surface and replacement reactions; (b) Corrosion layer formed after a short period of time (25 days) of immersion; (c) Corrosion layer formed after a long period of time (200 days) of immersion[79]
表 1 不同医用植入材料的力学性能对比[20]
Table 1. Comparison of mechanical properties of different medical implant materials[20]
Performance indicators Density/(g·cm−3) Elasticity modulus/GPa Yield strength/MPa Fracture toughness/MPa Natural bone 1.8-2.1 3-20 130-180 3-6 Mg 1.74-2.0 41-45 65-100 15-40 Ti alloy 4.4-4.5 110-117 758-1117 55-115 Co-Cr alloy 8.3-9.2 230 450-1000 N/A Stainless steel 7.9-8.1 189-205 170-310 50-200 Hydroxyapatite 3.1 73-117 600 0.7 D, L-polylactic acid 1.26 1.9-2.4 Not available Not available β-calcium phosphate 3.07 33-90 140-154 Not available Note: N/A—Not available. 
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表 2 医用镁合金器材植入标准
Table 2. Criteria for implantation of medical magnesium alloy devices
Medical use Yield strength/MPa Tensile strength/MPa Compression strength/MPa Modulus of elasticity/GPa Corrosion rate/ (mm·year−1) Biodegradation rate/month Ref. Vascular stents 100-300 200-500 200-500 5-20 Less than 0.5 Based on specific clinical needs [42-44] Splint 150-300 200-400 250-500 45-60 Less than 0.2 4-12 [45-46] Bone screw 50-200 100-300 150-300 40-60 Less than 0.2 Based on specific clinical needs [47-49]
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表 3 Mg-Zn合金的力学性能与腐蚀速率
Table 3. Mechanical properties and corrosion rate of Mg-Zn alloy
Alloy/wt% Fabrication method Yield strength/MPa Ultimate tensile strength/MPa Elongation/% Corrosion rate/ (mm·year−1) Immersion test solution Ref. Mg-1Zn As-Cast 110 211 [82] Mg-1Zn-0.5Sn 115 239 Mg-4Zn As-extruded 118 223 15.4 1.87 Phosphate buffered saline (PBS) [83] Mg-4Zn-1Sn 133 234 18 0.62 Mg-4Zn-1.5Sn 142 238 20.9 0.45 Mg-4Zn-2Sn 147 250 19.8 0.77 Mg-4Zn-0.5Ni As-cast 17 0.32 3.5wt%KCl solution [84] Mg-4Zn-1Ni 22.1 1.72 Mg-4Zn-2Ni 20.3 62.08 Mg-4Zn-4Ni 20.1 76.27 Mg-0.5Zn-0.2Ca As-extruded 119 224 25 0.22 0.5wt%NaCl solution [85] Mg-0.5Zn-0.2Ge 171 249 10 0.21 Mg-6Zn-0.5Ce As-extruded 183 286 18.16 [86] Mg-3Zn-0.2Ca As-extruded 298.17 15.75 [87] Mg-0.5Zn-0.5Nd As-cast 126 213 32.2 [88] Mg-2Zn-0.5Ca As-extruded 326 25.1 15.02 Simulated body fluid (72 h) [74] Mg-8Li-2Al As-extruded 115 12.8 19.43 [89]
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表 4 Mg-RE合金的力学性能与腐蚀速率
Table 4. Mechanical properties and corrosion rate of Mg-RE alloy
Alloy/wt% Fabrication method Yield strength/MPa Ultimate tensile strength/MPa Elongation/% Corrosion rate/ (mm·year−1) Immersion test solution Ref. Mg-7Y-0.5Nd As-Cast 151 257 14 36.75 3.5wt% NaCl solution (72 h) [90] Mg-7Y-1Nd 157 269 13 25.51 Mg-7Y-1.5Nd 165 285 10 19.69 Mg-1Y As-extruded 72 174 48 2.153 3.5wt% NaCl solution (168 h) [91] Mg-1Y-0.3Gd 84 188 59 1.985 Mg-1Y-0.6Gd 86 188 52 0.575 Mg-2Gd As-extruded 115 189 49 — — [92] Mg-2Gd-0.5Mn 84 172 51 — — Mg-2Gd-1.3Mn 132 206 45 — — Mg-2Gd-1.5Mn 154 219 42 — — Mg-2Gd-2Mn 189 243 33 — — Mg-0.3Sc As-extruded 50 162 16 — — [93] Mg-0.3Sc-1Zn 111 228 19 — — Mg-0.3Sc-3Zn 113 250 21 — — Mg-0.3Sc-6Zn 117 260 25 — — Mg-2Gd As-extruded 111 191 23.1 — — [94] Mg-2Gd-0.1Ni 142 212 20.8 — — Mg-2Gd-0.2Ni 168 239 19.1 — — Mg-2Gd-0.3Ni 234 287 18.1 — —
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表 5 镁基四元合金的力学性能与腐蚀速率
Table 5. Mechanical properties and corrosion rate of magnesium-based tetrameric alloys
Alloy/wt% Fabrication method Yield strength/MPa Ultimate tensile strength/MPa Elongation/% Corrosion rate/(mm·year−1) Immersion test solution Ref. Mg-6Zn-0.5Ce-1Mn As-extruded 232 304 14.7 — — [86] Mg-3Zn-0.2Ca-0.1Ag As-extruded — 300.45 15.72 — — [87] Mg-3Zn-0.2Ca-0.3Ag — 305.33 16.47 — — Mg-3Zn-0.2Ca-0.5Ag — 282.64 14.93 — — Mg-3Zn-0.2Ca-0.7Ag — 293.25 16.06 — — Mg-0.5Zn-0.5Nd-3Sc As-Cast 82 174 17.1 — — [88] Mg-0.5Zn-0.5Nd-6Sc 101 180 14.4 — — Mg-0.5Zn-0.5Nd-3Sc As-extruded 110 207 29.8 — — Mg-0.5Zn-0.5Nd-6Sc 153 223 21.7 — — Mg-2Zn-0.5Ca-0.5Sr As-extruded — 340 19 14.26 — [74] Mg-2Zn-0.5Ca-1.0Sr — 334 20.4 17.9 — Mg-8Li-2Al-1.5Sn As-extruded — 136 10.4 10.49 — [89] Mg-8Li-2Al-1.5Nd — 129 10 41 — Mg-8Li-2Al-1.5Ca — 125 8 14.88 — Mg-0.6Zr-0.5Sr-0.5Sc As-Cast 63 73 — 32.9 Hank's balanced salt solution
(2 h)[95] Mg-0.6Zr-0.5Sr-1Sc 54 72 — 22.4 Mg-0.6Zr-0.5Sr-2Sc 77 81 — 18.1 Mg-0.6Zr-0.5Sr-3Sc 74 95 — 14.5 Mg-8.5Gd-5Y-0.2Al As-extruded 263 376 12.82 3.8 3.5wt% NaCl solution [96] Mg-8.5Gd-5Y-0.5Al 264 363 7.71 8.11 Mg-8.5Gd-5Y-0.8Al 276 377 5.29 18.61 Mg-8.5Gd-5Y-1.1Al 289 390 3.05 33.84
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