【AMF论文推荐】深圳大学陈张伟教授团队：高性能交叉型三维锂离子电池电极结构的设计与3D打印|3d打印|交叉型|动力电池|深圳大学|锂离子电池|陈张伟

引用论文

Kun Xu, Ning Zhao, Yide Li, Pei Wang, Zhiyuan Liu, Zhangwei Chen, Jun Shen, Changyong Liu. Design and 3D Printing of Interdigitated Electrode Structures for High-performance Full Lithium-ion Battery. Chinese Journal of Mechanical Engineering: Additive Manufacturing Frontiers, 2022, 1(4): 100053.

https://doi.org/10.1016/j.cjmeam.2022.100053.

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研究背景及目的

锂离子电池具有高能量密度、无记忆效应、环境友好等优点，在实现“双碳”战略目标、构建安全高效的现代能源体系中扮演着重要角色。研制新的材料体系对提升电池比能量至关重要，同时，发展新型的电池结构对发挥材料的性能潜力也具有重要意义。现有涂布电极具有活性材料厚度薄、非活性材料占比高等缺点，能量密度与功率密度的矛盾限制了电极厚度。针对上述问题和挑战，近日深圳大学增材制造研究所陈张伟教授团队刘长勇等人基于3D打印技术，设计并制备了由高电压钴酸锂正极和天然石墨负极构成的交叉型三维锂离子电池，为解决能量密度与功率密度的矛盾探索新的技术途径。研究成果发表在卓越期刊Chinese Journal of Mechanical Engineering: Additive Manufacturing Frontiers上。

论文亮点

通过COMSOL仿真，研究了正负极交叉型三维锂离子电池的锂离子传输机制，并与传统涂布电极对比，证明了交叉型三维锂离子电池克服能量密度和功率密度矛盾的可行性；基于3D打印技术，制备出梳状高电压钴酸锂正极、天然石墨负极，在此基础上，构建出交叉型三维锂离子全电池；评估了3D打印梳状高电压钴酸锂正极半电池以及全电池的电化学性能，实验验证了交叉型三维电池结构克服能量密度和功率密度矛盾的有效性。

图1 三维锂电池的增材制造流程与效果

试验方法

基于COMSOL仿真，对比了涂布薄电极、涂布厚度电极以及交叉型三维电池，研究了电极结构对锂离子传输机制和电池性能的影响。配制适合于3D打印的高电压钴酸锂正极浆料和天然石墨负极浆料，研究了浆料的流变性能，使用直写式3D打印分别制备出梳状的三维正极和负极，表征了电极的微观形貌。最后，组装出高电压钴酸锂正极半电池以及正负极交叉的全电池，进行电化学性能表征。

结果

COMSOL仿真结果表明，通过正负极交叉后，锂离子在正极和负极之间横向扩散，即使在电极厚度达到300 μm时，理论上仍能保持优异的倍率性能；而传统的涂布电极厚度达到300 μm时，比容量随倍率衰减严重；理论上证明了交叉型三维电池结构克服能量密度和功率密度矛盾的可行性。3D打印制备出电极厚度达到289 μm、574 μm以及882 μm的高电压钴酸锂正极/天然石墨负极交叉型三维全电池，结果表明：289 μm厚全电池在0.1 C倍率充放电的首次库伦效率达到81.6%，2.0C倍率的放电比容量可以达到104.9 mAh·g-1， 882 μm厚全电池在2.0 C倍率下放电比容量可以达到43.5 mAh·g-1，面能量密度与功率密度可到达41.4 J·cm-2@ 1.0 C和41.0 mW·cm-2 @ 1.0 C，实验证实了交叉型三维电池结构克服能量密度和功率密度矛盾的有效性。

结论

锂离子的传输机制和速率是决定锂离子性能的关键。通过电池结构的创新，构建更高效的锂离子传输路径，对提升电池的性能具有重要意义。本研究制备的交叉型三维电池结构从仿真和实验上证明了该技术方案的可行性和有效性。然而，制造精度不足、电池装配困难、制造效率低等限制了其潜力的充分挖掘，构建高精度、结构紧凑、空间利用率高的三维锂离子电池仍然面临挑战，有待进一步研究。

前景与应用

本研究制备的高电压钴酸锂正极/天然石墨负极交叉型三维全电池，有望通过结构优化，克服能量密度和功率密度的矛盾，用于构建高比能、高活性材料负载量的厚电极，进一步减少电池中非活性材料如集流体和隔膜的使用量和占比，提升锂离子电池性能。

团队带头人介绍

陈张伟，深圳大学长聘教授、博士生导师、优秀学者、增材制造研究所所长，增材制造学科带头人，广东省特支计划高层次人才，广东省高校优秀青年创新人才，连续两年入选斯坦福大学全球前2%顶尖科学家“年度影响力”榜单 (2020-2021),。西安交通大学和法国里昂中央理工大学双硕士、英国伦敦帝国理工学院博士。至今从事陶瓷等高性能材料3D打印研究15年。在Prog Mater Sci、Nano Energy (2篇)、Acta Mater (3篇)、Addit Manuf (9篇)、J Adv Ceram (5篇)、Virtual Phys Prototyp (5篇)、J Euro Ceram Soc (10篇)、Ceram Int (12篇) 等知名期刊发表论文110余篇，单篇最高被引超1000次，20余篇影响因子大于10，入选ESI全球高被引3篇，热点论文2篇。研究成果获《科技日报》、《新华网》、《人民网》、3D Printing Industry、3DPrint.com 等多家国内外媒体的长篇报道。任第一届中国陶瓷增材制造前沿科学家论坛创始主席、组织举办ICC8、CICC12/13等权威国际会议中的陶瓷增材论坛并做特邀报告20余次。任SCI/EI期刊Journal of Advanced Ceramics、《无机材料学报》和《材料工程》等9家期刊编委/青年编委。主持国家、省、市级项目20余项。目前是中国机械工程学会增材制造分会委员、中国硅酸盐学会测试分会理事，以及中国、欧盟、加拿大、新加坡、瑞士、新西兰等国家基金项目函评专家。

作者介绍

刘长勇（本文通讯作者），深圳大学机电与控制工程学院长聘副教授，主要从事新能源器件增材制造、金属增材制造等领域的研究。近年来主持国家自然科学基金、广东省、深圳市等各类科研项目多项，发表学术论文60余篇，获授权专利20余项。

团队研究方向

陶瓷和金属增材制造工艺方面的研究，包括：(a)光固化技术；(b)低温直写技术；(c)喷墨打印技术；(d)激光选区熔化技术；(e)激光熔覆技术。

近年团队发表文章

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[2] M Idrees, S Batool, M Din, M Javed, S Ahmed, Z Chen*, Material-structure-property integrated additive manufacturing of batteries, Nano Energy, 2023, 109: 108247

[3] M Idrees, S Batool, J Cao, M Javed, S Xiong, C Liu, Z Chen*, 3D Printed PC/SiOC@ Zn Hybrid Composite as Dendrite-Free Anode for Zn-Ion Battery, Nano Energy, 2022, 100: 107505

[4] J Huang, ZD Chen, C Wen, T Ling, Z Chen*, Thermally assisted 3D printing of bio-polymer with high solute loading with improved mechanical properties, Additive Manufacturing, 2022, 59A: 103088

[5] J Cao, K Miao, S Xiong, F Su, D Gao, X Lin, Z Liu, P Wang, C Liu, Z Chen*, 3D printing and in situ transformation of SiCnw/SiC structures, Additive Manufacturing, 2022, 58: 103053

[6] F Su, Z Su, Y Liu, X Lin, J Cao, Z Liu, P Wang, C Liu, Z Chen*, Generative shaping and material-forming (GSM) enables structure engineering of complex-shaped Li4SiO4 ceramics based on 3D printing of ceramic/polymer precursors, Additive Manufacturing, 2022, 57: 102963

[7] S Xiong, J Liu, J Cao, Z Li, M Idrees, X Lin, Z Long, Z Liu, P Wang, C Liu, Z Chen*, 3D printing of crack-free dense polymer-derived ceramic monoliths and lattice skeletons with improved thickness and mechanical performance, Additive Manufacturing, 2022, 57: 102964

[8] F Su, Y Liu, C Zhang, Z Luo, J Cao, Z Liu, P Wang, C Liu, Z Chen*, Photopolymerization and reaction sintering enabled generative shaping and material-forming of complex ceramic structures with high performance, Additive Manufacturing, 2022, 51: 102651

[9] J Cao, M Idrees, G Tian, J Liu, S Xiong, J Yuan, P Wang, Z Liu, C Liu, Z Chen*, Complex SiC-based structures with high specific strength fabricated by vat photopolymerization and one-step pyrolysis, Additive Manufacturing, 2021, 48B: 102430

[10] P Qu, D Xiong, Z Zhu, Z Gong, Y Li, Y Li, L Fan, Z Liu, P Wang, C Liu, Z Chen*, Inkjet printing additively manufactured multilayer SOFCs using high quality ceramic inks for performance enhancement, Additive Manufacturing, 2021, 48A: 102394

[11] C Liu, D Yan, J Tan, Z Mai, Z Cai, Y Dai, M Jiang, P Wang, Z Liu, C Li, C Lao*, Z Chen*, Development and experimental validation of a hybrid selective laser melting and CNC milling system, Additive Manufacturing, 2020, 36: 101550

[12] Y Liu, Z Chen*, J Li, B Gong, L Wang, C Lao, P Wang, C Liu, Y Feng, X Wang, 3D printing of ceramic cellular structures for potential nuclear fusion applications, Additive Manufacturing, 2020, 35: 101348

[13] Z Li, Z Chen*, J Liu, Y Fu, C Liu, P Wang, M Jiang, C Lao, Additive manufacturing of lightweight and high-strength polymer-derived SiOC ceramics, Virtual and Physical Prototyping, 2020, 15(2): 163-177

[14] SJ Yu, P Wang*, HC Li, R Setchi, MW Wu, ZY Liu, ZW Chen, S Waqar, Heterogeneous microstructure and mechanical behaviour of Al-8.3 Fe-1.3 V-1.8 Si alloy produced by laser powder bed fusion, Virtual and Physical Prototyping 2023, 18 (1): e2155197

[15] Y Wu, X Zhao, Q Chen, C Yang, M Jiang, C Liu, Z Jia, Z Chen, T Yang, Z Liu*, Strengthening and fracture mechanisms of a precipitation hardening high-entropy alloy fabricated by selective laser melting, Virtual and Physical Prototyping 2022, 17 (3), 451-467

[16] D Zhao, Q Yang, D Wang, M Yan, P Wang, M Jiang, C Liu, D Diao, C Lao, Z Chen, Z Liu*, Y Wu, Z Lu*, Ordered nitrogen complexes overcoming strength-ductility trade-off in an additively manufactured high entropy alloy, Virtual and Physical Prototyping, 2020, 15 (1): 532-542

[17] X Wei, M Jin, H Yang, X Wang, Y Long, Z Chen*, Advances in 3D printing of magnetic materials: fabrication, properties and their applications, Journal of Advanced Ceramics, 2022, 11(5): 665-701

[18] C Liu, Y Qiu, Y Liu, K Xu, N Zhao, C Lao, J Shen, Z Chen*, Novel 3D grid porous Li4Ti5O12 thick electrodes fabricated by 3D printing for high performance lithium-ion batteries, Journal of Advanced Ceramics, 2022, 11(2): 295-307

[19] Z Zhu, Z Gong, P Qu, Z Li, S Rasaki, Z Liu, P Wang, C Liu, C Lao, Z Chen*, Additive manufacturing of thin electrolyte layers via inkjet printing of highly-stable ceramic inks, Journal of Advanced Ceramics, 2021, 10(2): 279-290

[20] S Rasaki, D Xiong, S Xiong, F Su, Z Chen*, Photopolymerization-based additive manufacturing of ceramics: A systematic review, Journal of Advanced Ceramics, 2021, 10: 442–471

[21] D Xiong, SA Rasaki, Y Li, L Fan, C Liu, Z Chen*, Enhanced cathodic activity by tantalum inclusion at B-site of La0.6Sr0.4CO0.4Fe0.6O3 based on structural property tailored via camphor-assisted solid-state reaction, Journal of Advanced Ceramics, 2022, 11(8): 1130-1342

[22] Z Liu, D Zhao, P Wang, M Yan, C Yang, Z Chen, J Lu, Z Lu, Additive manufacturing of metals: Microstructure evolution and multistage control, Journal of Materials Science & Technology 2022, 100, 224-236

[23] P Wang*, C Lao, Z Chen, Y Liu, H Wang, H Wenrock, J Eckert, S Scudino, Microstructure and mechanical properties of Al-12Si and Al-3.5Cu-1.5Mg-1Si bimetal fabricated by selective laser melting, Journal of Materials Science & Technology 2020, 36: 18-26

[24] S Rasaki, C Liu, C Lao, H Zhang, Z Chen*, The innovative contribution of additive manufacturing towards revolutionizing fuel cell fabrication for clean energy generation: A comprehensive review, Renewable & Sustainable Energy Reviews, 2021, 148: 111369

[25] C Liu*, N Zhao, K Xu, Y Li, JP Mwizerwa, J Shen, Z Chen*, High performance LiFePO4 and SiO@C/graphite interdigitated full lithium-ion battery fabricated via low temperature direct write 3D printing, Materials Today Energy, 2022, 29, 101098

[26] Jean Pierre Mwizerwa, Changyong Liu*, Kun Xu, Ning Zhao, Yide Li, Zhangwei Chen, Jun Shen. Three-dimensional printed Lithium Iron Phosphate coated with Magnesium Oxide cathode with improved areal capacity and ultralong cycling stability for high performance lithium-ion batteries. Journal of Colloid and Interface Science, 2022, 623: 168-181.

[27] Kun Xu, Ning Zhao, Yide Li, Pei Wang, Zhiyuan Liu, Zhangwei Chen, Jun Shen, Changyong Liu*. 3D printing of ultrathick natural graphite anodes for high-performance interdigitated three-dimensional lithium-ion batteries. Electrochemistry Communications, 2022, 139: 107312.

[28] Z Chen*, Z Li, J Li, C Liu, C Lao*, Y Fu, C Liu, Y Li, P Wang, Y He, 3D printing of ceramics: A review, Journal of the European Ceramics Society, 2019, 39(4): 661-687

[29] Changyong Liu#*, Feng Xu#, Yanliang Liu, Jun Ma*, Peiqi Liu, Daming Wang, Changshi Lao, Zhangwei Chen*. High mass loading ultrathick porous Li4Ti5O12 electrodes with improved areal capacity fabricated via low temperature direct writing. Electrochimica Acta, 2019, 314: 81-88.

[30] F Fan, M Jiang*, P Wang, C Liu, Z Liu, Z Chen*, Defect-associated microstructure evolution and deformation heterogeneities in additively manufactured 316L stainless steel, Materials Science and Engineering: A 2023, 861: 144287

[31] D Zhao, Y Guo, R Lai, Y Wen, P Wang, C Liu*, Z Chen, C Yang, S Li, Abnormal three-stage plastic deformation in a 17-4 PH stainless steel fabricated by laser powder bed fusion, Materials Science and Engineering: A 2022, 858, 144160

[32] M Jiang, C Liu, Z Chen*, P Wang, H Liao, D Zhao, Z Liu, X Wang, M Xu*, C Lao*, Enhanced strength-ductility synergy of selective laser melted reduced activation ferritic/martensitic steel via heterogeneous microstructure modification, Materials Science and Engineering A, 2021, 801: 140424

[33] C Liu, J Tong, M Jiang*, Z Chen, X Wu, M Xu, H Liao, P Wang, G Xu, C Lao, Effect of scanning strategy on microstructure and mechanical properties of selective laser melted reduced activation ferritic/martensitic steel, Materials Science and Engineering: A, 2019, 766: 138364

[34] M Jiang, Z Chen*, J Tong, C Liu, G Xu, H Liao, P Wang, X Wang, M Xu, C Lao, Strong and ductile reduced activation ferritic/martensitic steel additively manufactured by selective laser melting. Materials Research Letter, 2019, 7(10): 426-432

作者：徐坤

责任编辑：谢雅洁

责任校对：向映姣

审核：张强

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