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Direct observation of the atomic density fluctuation originating from the first sharp diffraction peak in SiO2 glass 直接观察源自二氧化硅玻璃中第一个尖锐衍射峰的原子密度波动
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-05-10 DOI: 10.1038/s41427-024-00544-w
Akihiko Hirata, Shuya Sato, Motoki Shiga, Yohei Onodera, Koji Kimoto, Shinji Kohara

The intermediate-range order of covalently bonded glasses has been extensively studied in terms of their diffraction peaks observed at low scattering angles; these peaks are called the first sharp diffraction peaks (FSDPs). Although the atomic density fluctuations originating from the quasilattice planes are a critical scientific target, direct experimental observations of these fluctuations are still lacking. Here, we report the direct observation of the atomic density fluctuations in silica glass by energy-filtered angstrom-beam electron diffraction. The correspondence between the local electron diffraction patterns of FSDPs and the atomic configurations constructed based on the X-ray and neutron diffraction results revealed that the local atomic density fluctuations originated from the quasi-periodic alternating arrangements of the columnar chain-like atomic configurations and interstitial tubular voids, as in crystals. We also discovered longer-range fluctuations associated with the shoulder of the FSDP on the low-Q side. The hierarchical fluctuations inherent in materials could aid in the elucidation of their properties and performance.

人们通过在低散射角处观察到的衍射峰,对共价键玻璃的中间阶进行了广泛的研究;这些衍射峰被称为第一尖锐衍射峰(FSDPs)。尽管源于准晶格平面的原子密度波动是一个重要的科学目标,但目前仍缺乏对这些波动的直接实验观测。在此,我们报告了通过能量滤波埃束电子衍射对二氧化硅玻璃中原子密度波动的直接观测。FSDPs的局部电子衍射图案与根据X射线和中子衍射结果构建的原子构型之间的对应关系表明,局部原子密度波动源于柱状链状原子构型和间隙管状空隙的准周期交替排列,就像在晶体中一样。我们还发现了与低 Q 边 FSDP 肩相关的长程波动。材料固有的层次波动有助于阐明其特性和性能。
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引用次数: 0
Phase stabilization of cesium lead iodide perovskites for use in efficient optoelectronic devices 用于高效光电设备的碘化铯铅包晶石的相稳定化
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-05-03 DOI: 10.1038/s41427-024-00540-0
Handong Jin, Yu-Jia Zeng, Julian A. Steele, Maarten B. J. Roeffaers, Johan Hofkens, Elke Debroye

All-inorganic lead halide perovskites (LHPs) and their use in optoelectronic devices have been widely explored because they are more thermally stable than their hybrid organic‒inorganic counterparts. However, the active perovskite phases of some inorganic LHPs are metastable at room temperature due to the critical structural tolerance factor. For example, black phase CsPbI3 is easily transformed back to the nonperovskite yellow phase at ambient temperature. Much attention has been paid to improving the phase stabilities of inorganic LHPs, especially those with high solar cell efficiencies. Herein, we discussed the origin of phase stability for CsPbI3 and the strategies used to stabilize the cubic (α) phase. We also assessed the CsPbI3 black β/γ phases that are relatively stable at nearly room temperature. Furthermore, we determined the relationship between phase stabilization and defect passivation and reviewed the growing trend in solar cell efficiency based on black phase CsPbI3. Finally, we provide perspectives for future research related to the quest for optimum device efficiency and green energy.

全无机卤化铅包晶石(LHPs)及其在光电器件中的应用已得到广泛探索,因为它们比有机-无机混合包晶石具有更高的热稳定性。然而,由于临界结构耐受因子的影响,一些无机 LHP 的活性包晶石相在室温下是易陨的。例如,黑相 CsPbI3 在常温下很容易转变回非过氧化物黄相。人们一直在关注如何提高无机 LHP 的相稳定性,尤其是那些具有高太阳能电池效率的 LHP。在此,我们讨论了 CsPbI3 相稳定性的起源以及用于稳定立方(α)相的策略。我们还评估了在接近室温时相对稳定的 CsPbI3 黑色 β/γ 相。此外,我们还确定了相稳定与缺陷钝化之间的关系,并回顾了基于黑相 CsPbI3 的太阳能电池效率的增长趋势。最后,我们展望了与追求最佳器件效率和绿色能源相关的未来研究。
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引用次数: 0
Investigation on mussel periostracum, a viscoelastic-to-poro-gel graded material, as an interface between soft tissue and rigid materials 作为软组织与硬质材料界面的粘弹性-孔凝胶分级材料--贻贝骨膜的研究
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-04-26 DOI: 10.1038/s41427-024-00543-x
Hyungbin Kim, Heejin Lim, Sangsik Kim, Jun Mo Koo, Chanoong Lim, Hojung Kwak, Dongyeop X. Oh, Dong Soo Hwang

Mussel periostracum, a nonliving multifunctional gel that covers the rigid inorganic shells of mussels, provides protection against mechanical impacts, biofouling, and corrosion in harsh ocean environments. The inner part of the periostracum, which emerges from biological tissues, functions as a natural interface between tissue and inorganic materials. The periostracum shows significant potential for application in implantable devices that provide interfaces; however, this system remains unexplored. In this study, we revealed that the inner periostracum performs graded mechanical functions and efficiently dissipates energy to accommodate differences in stiffness and stress types on both sides. On the tissue end, the lightly pigmented periostracum exhibits extensibility and energy dissipation under repetitive tension. This process was facilitated by the slipping and reassembly of β-strands in the discovered major proteins, which we named periostracin proteins. On the shell end, the highly pigmented, mineralized, and porous segment of the periostracum provided stiffness and cushioned against compressive stresses exerted by the shell valves during closure. These findings offer a novel possibilities for the design of interfaces that bridge human tissue and devices.

贻贝骨膜是一种非生物多功能凝胶,覆盖在贻贝坚硬的无机外壳上,可在恶劣的海洋环境中提供保护,防止机械撞击、生物污染和腐蚀。从生物组织中产生的包膜内部是组织与无机材料之间的天然界面。骨膜在提供界面的植入式设备中显示出巨大的应用潜力,但这一系统仍未被开发。在这项研究中,我们发现内骨膜具有分级机械功能,并能有效消散能量,以适应两侧刚度和应力类型的差异。在组织端,轻度色素沉着的骨膜在重复张力作用下表现出伸展性和能量耗散性。这一过程得益于已发现的主要蛋白质(我们将其命名为包膜蛋白)中β-链的滑动和重新组合。在壳的一端,高度色素化、矿化和多孔的壳周膜部分提供了硬度,并缓冲了壳门在闭合过程中施加的压缩应力。这些发现为设计连接人体组织和设备的界面提供了新的可能性。
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引用次数: 0
Formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysis 通过 X 射线多尺度分析法研究铝硅酸盐玻璃初始成核阶段氧化锆晶核的形成
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-04-19 DOI: 10.1038/s41427-024-00542-y
Yohei Onodera, Yasuyuki Takimoto, Hiroyuki Hijiya, Qing Li, Hiroo Tajiri, Toshiaki Ina, Shinji Kohara

Understanding the nucleation mechanism in glass is crucial for the development of new glass-ceramic materials. Herein, we report the structure of a commercially important glass-ceramic ZrO2-doped lithium aluminosilicate system during its initial nucleation stage. We conducted an X-ray multiscale analysis, and this analysis was used to observe the structure from the atomic to the nanometer scale by using diffraction, small-angle scattering, absorption, and anomalous scattering techniques. The inherent phase separation between the Zr-rich and Zr-poor regions in the pristine glass was enhanced by thermal treatment without changing the spatial geometry at the nanoscale. Element-specific pair distribution function analysis using anomalous X-ray scattering data showed the formation of a liquid ZrO2-like local structural motif and edge sharing between the ZrOx polyhedra and (Si/Al)O4 tetrahedra during the initial nucleation stage. Furthermore, the local structure of the Zr4+ ions resembled a cubic or tetragonal ZrO2 crystalline phase and formed after 2 h of annealing the pristine glass. Therefore, the Zr-centric periodic structure formed in the early stage of nucleation was potentially the initial crystal nucleus for the Zr-doped lithium aluminosilicate glass-ceramic.

了解玻璃中的成核机制对于开发新型玻璃陶瓷材料至关重要。在此,我们报告了一种具有重要商业价值的玻璃陶瓷 ZrO2 掺杂铝硅酸锂体系在其初始成核阶段的结构。我们进行了 X 射线多尺度分析,并利用衍射、小角散射、吸收和反常散射技术观察了从原子到纳米尺度的结构。原始玻璃中富锆区和贫锆区之间的固有相分离通过热处理得到了加强,但并没有改变纳米尺度的空间几何结构。利用反常 X 射线散射数据进行的元素特异对分布函数分析表明,在初始成核阶段形成了类似 ZrO2 的液态局部结构图案,ZrOx 多面体和(Si/Al)O4 四面体之间实现了边缘共享。此外,Zr4+ 离子的局部结构类似于立方或四方 ZrO2 结晶相,并在原始玻璃退火 2 小时后形成。因此,成核初期形成的以 Zr 为中心的周期性结构可能是掺杂 Zr 的锂铝硅酸盐玻璃陶瓷的初始晶核。
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引用次数: 0
A bone adhesive enhances osteoporotic fracture repair by regulating bone homeostasis 骨粘合剂通过调节骨平衡增强骨质疏松性骨折的修复能力
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-04-12 DOI: 10.1038/s41427-024-00539-7
Shenghui Su, Jiajun Xie, Jian Gao, Shencai Liu, Xieping Dong, Jianwei Li, Zhong Feng Gao, Keyuan Chen, Weilu Liu

Patients suffering from osteoporotic fractures often require effective fixation and subsequent bone repair. However, the currently available materials are functionally limited and often fail to improve outcomes in this patient population. In this study, we developed orthopedic adhesives doped with romosozumab-loaded mesoporous bioactive glass nanoparticles to aid in osteoporotic fracture fixation and restore dysregulated bone homeostasis. These adhesives were designed to promote osteoblast formation while simultaneously inhibiting osteoclastic bone-resorbing activity, thus working synergistically to promote the healing of osteoporotic fractures. Orthopedic adhesives exhibit injectability, reversible adhesiveness, and malleability, enhancing their adaptability to complex clinical scenarios. Furthermore, the release of romosozumab from mesoporous bioactive glass nanoparticles accelerated osteogenesis and inhibited osteoclastogenesis, delaying the bone resorption process. This dual action contributes to the regulation of bone regeneration and remodeling. Notably, our orthopedic adhesive could restore the disrupted bone homeostasis associated with osteoporotic fractures.

骨质疏松性骨折患者往往需要有效的固定和后续骨修复。然而,目前可用的材料功能有限,往往无法改善这类患者的治疗效果。在这项研究中,我们开发了掺杂有罗莫单抗的介孔生物活性玻璃纳米颗粒的骨科粘合剂,以帮助骨质疏松性骨折的固定和恢复失调的骨平衡。这些粘合剂旨在促进成骨细胞的形成,同时抑制破骨细胞的骨吸收活性,从而协同促进骨质疏松性骨折的愈合。骨科粘合剂具有可注射性、可逆粘合性和延展性,能更好地适应复杂的临床情况。此外,介孔生物活性玻璃纳米粒子释放的罗莫索单抗可加速骨生成,抑制破骨细胞生成,延缓骨吸收过程。这种双重作用有助于调节骨再生和重塑。值得注意的是,我们的骨科粘合剂可以恢复与骨质疏松性骨折相关的骨平衡紊乱。
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引用次数: 0
Recent advances in functional materials and devices for Zn-Ion hybrid supercapacitors 用于锌离子混合超级电容器的功能材料和器件的最新进展
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-04-05 DOI: 10.1038/s41427-024-00537-9
Weijia Fan, Faxing Wang, Xiaosong Xiong, Bingyan Song, Tao Wang, Xinbing Cheng, Zhi Zhu, Jiarui He, Yankai Liu, Yuping Wu

Zinc-ion hybrid supercapacitors (ZHSCs) are attracting significant attention due to their high energies/power densities, safety, and low cost. In this review, recent advances in the development of ZHSCs are summarized. Particular emphasis is placed on state-of-the-art cathodes (including carbon, metal oxides, MXenes, and redox-active polymers), anodes (including Zn-based composites and Zn-free materials) and electrolytes for ZHSCs. Furthermore, the latest research on functional ZHSC devices with miniaturized ZHSCs, fiber-shaped ZHSCs, self-chargeable ZHSCs and self-healing devices is reported. Finally, further developments with ZHSCs are envisaged for future research in this thriving field.

锌离子混合超级电容器(ZHSCs)因其高能量/功率密度、安全性和低成本而备受关注。本综述总结了锌离子混合超级电容器的最新研发进展。其中特别强调了用于 ZHSCs 的最先进阴极(包括碳、金属氧化物、MXenes 和氧化还原活性聚合物)、阳极(包括锌基复合材料和无锌材料)和电解质。此外,报告还介绍了有关微型 ZHSC、纤维状 ZHSC、可自充电 ZHSC 和自修复器件等功能 ZHSC 器件的最新研究。最后,还展望了 ZHSCs 在这一蓬勃发展的研究领域的未来发展。
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引用次数: 0
Giant gate modulation of antiferromagnetic spin reversal by the magnetoelectric effect 磁电效应对反铁磁自旋反转的巨门调制
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-04-05 DOI: 10.1038/s41427-024-00541-z
Kakeru Ujimoto, Hiroki Sameshima, Kentaro Toyoki, Takahiro Moriyama, Kohji Nakamura, Yoshinori Kotani, Motohiro Suzuki, Ion Iino, Naomi Kawamura, Ryoichi Nakatani, Yu Shiratsuchi

In this study, using the Pt/Cr2O3/Pt epitaxial trilayer, we demonstrate the giant voltage modulation of the antiferromagnetic spin reversal and the voltage-induced 180° switching of the Néel vector in maintaining a permanent magnetic field. We obtained a significant modulation efficiency of the switching field, Δμ0HSWVμ0HSWE), reaching a maximum of −500 mT/V (−4.80 T nm/V); this value was more than 50 times greater than that of the ferromagnetic-based counterparts. From the temperature dependence of the modulation efficiency, X-ray magnetic circular dichroism measurements and first-principles calculations, we showed that the origin of the giant modulation efficiency relied on the electric field modulation of the net magnetization due to the magnetoelectric effect. From the first-principles calculation and the thickness effect on the offset electric field, we found that the interfacial magnetoelectric effect emerged. Our demonstration reveals the energy-efficient and widely applicable operation of an antiferromagnetic spin based on a mechanism distinct from magnetic anisotropy control.

在这项研究中,我们利用 Pt/Cr2O3/Pt 外延三层,展示了反铁磁性自旋反转的巨电压调制,以及在维持永久磁场时电压诱导的奈尔矢量 180° 切换。我们获得了开关磁场的显著调制效率Δμ0HSW/ΔV(Δμ0HSW/ΔE),最大值为-500 mT/V (-4.80 T nm/V);该值比铁磁基对应物高出 50 多倍。从调制效率的温度依赖性、X 射线磁圆二色性测量和第一性原理计算中,我们发现巨调制效率的起源依赖于磁电效应对净磁化的电场调制。通过第一原理计算和厚度对偏移电场的影响,我们发现出现了界面磁电效应。我们的演示揭示了基于不同于磁各向异性控制机制的反铁磁自旋的高能效和广泛应用。
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引用次数: 0
Bayesian optimization-driven enhancement of the thermoelectric properties of polycrystalline III-V semiconductor thin films 贝叶斯优化驱动的多晶 III-V 族半导体薄膜热电性能增强技术
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-03-29 DOI: 10.1038/s41427-024-00536-w
Takamitsu Ishiyama, Koki Nozawa, Takeshi Nishida, Takashi Suemasu, Kaoru Toko

Studying the properties of thermoelectric materials needs substantial effort owing to the interplay of the trade-off relationships among the influential parameters. In view of this issue, artificial intelligence has recently been used to investigate and optimize thermoelectric materials. Here, we used Bayesian optimization to improve the thermoelectric properties of multicomponent III–V materials; this domain warrants comprehensive investigation due to the need to simultaneously control multiple parameters. We designated the figure of merit ZT as the objective function to improve and search for a five-dimensional space comprising the composition of InGaAsSb thin films, dopant concentration, and film-deposition temperatures. After six Bayesian optimization cycles, ZT exhibited an approximately threefold improvement compared to its values obtained in the random initial experimental trials. Additional analysis employing Gaussian process regression elucidated that a high In composition and low substrate temperature were particularly effective at increasing ZT. The optimal substrate temperature (205 °C) demonstrated the potential for depositing InGaAsSb thermoelectric thin films onto plastic substrates. These findings not only promote the development of thermoelectric devices based on III–V semiconductors but also highlight the effectiveness of using Bayesian optimization for multicomponent materials.

由于各影响参数之间存在相互影响的权衡关系,因此研究热电材料的特性需要投入大量精力。有鉴于此,人工智能最近被用于研究和优化热电材料。在此,我们使用贝叶斯优化法来改善多组分 III-V 材料的热电特性;由于需要同时控制多个参数,这一领域值得全面研究。我们将功勋值 ZT 指定为需要改进的目标函数,并搜索由 InGaAsSb 薄膜成分、掺杂浓度和薄膜沉积温度组成的五维空间。经过六个贝叶斯优化周期后,ZT 与随机初始实验试验中获得的值相比提高了约三倍。利用高斯过程回归进行的其他分析表明,高 In 成分和低衬底温度对提高 ZT 特别有效。最佳衬底温度(205 °C)证明了在塑料衬底上沉积 InGaAsSb 热电薄膜的潜力。这些发现不仅促进了基于 III-V 族半导体的热电设备的开发,而且凸显了使用贝叶斯优化技术对多组分材料进行优化的有效性。
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引用次数: 0
Formulation of energy loss due to magnetostriction to design ultraefficient soft magnets 计算磁致伸缩导致的能量损失,设计超高效软磁体
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-03-26 DOI: 10.1038/s41427-024-00538-8
Hiroshi Tsukahara, Haodong Huang, Kiyonori Suzuki, Kanta Ono

The mechanism of energy loss due to magnetostriction in soft magnetic materials was analytically formulated, and our experiments validated this formulation. The viscosity of magnetic materials causes the resistive force acting on magnetic domain walls through strain due to magnetostriction, and magnetic energy is eventually dissipated by friction even without eddy currents. This energy loss mechanism explains the frequency dependence of the excess loss observed in the experiments, and the excess loss is dominated by the contribution of magnetostriction when the magnetostriction constant exceeds approximately 20 ppm. The random anisotropy model was extended by considering the effect of local magnetostriction as a correction to the magnetocrystalline anisotropy. The effect of magnetostriction was considerably suppressed by the exchange-averaging effect. The estimated effective random magnetoelastic anisotropy for nanocrystalline α-Fe reached as low as 18.6 J/m3, but this static effect could not explain the high excess loss at high frequencies observed in the experiments. The results of this research could provide new design criteria for high-performance soft magnetic materials based on low magnetostriction to reduce the excess loss.

我们分析了软磁材料中磁致伸缩导致能量损耗的机理,并通过实验验证了这一机理。磁性材料的粘度通过磁致伸缩引起的应变作用于磁畴壁上的阻力,即使没有涡流,磁能最终也会通过摩擦耗散。这种能量损耗机制解释了实验中观察到的过量损耗的频率依赖性,当磁致伸缩常数超过约 20 ppm 时,过量损耗主要由磁致伸缩贡献。将局部磁致伸缩的影响视为对磁晶各向异性的修正,从而扩展了随机各向异性模型。磁致伸缩效应在很大程度上被交换平均效应所抑制。纳米晶 α-Fe 的有效随机磁弹性各向异性估计值低至 18.6 J/m3,但这种静态效应无法解释实验中观察到的高频率下的高过量损耗。这项研究的结果可为基于低磁致伸缩的高性能软磁材料提供新的设计标准,以降低过量损耗。
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引用次数: 0
Nanocomposite magnetic hydrogel with dual anisotropic properties induces osteogenesis through the NOTCH-dependent pathways 具有双重各向异性的纳米复合磁性水凝胶通过 NOTCH 依赖性途径诱导骨生成
IF 9.7 2区 材料科学 Q1 Mathematics Pub Date : 2024-03-22 DOI: 10.1038/s41427-024-00535-x
Shijia Tang, Yue Yan, Xiaoli Lu, Peng Wang, Xueqin Xu, Ke Hu, Sen Yan, Zhaobin Guo, Xiao Han, Feimin Zhang, Ning Gu

Physical factors in the cellular microenvironment have critical effects on stem cell differentiation. The utilization of physical factors to promote the osteogenic differentiation of stem cells has been established as a new strategy for developing bone tissue engineering scaffolds. In this context, scaffolds with multiscale anisotropy are considered to possess biomimetic properties, which are advantageous for their biological performance. In the present study, a novel magnetic anisotropic hydrogel (MAH) with magnetic and topographic anisotropy was designed by combining static magnetic field-induced magnetic nanomaterials and a hydrogel. In in vitro studies, the MAH exhibited excellent biocompatibility and osteogenic bioactivity. The alkaline phosphatase activity and the expression of osteogenic-related genes and proteins induced by the MAH were greater than those induced by the pure PEGDA–GelMA hydrogel (PGH) and the magnetic isotropic hydrogel (MIH). In addition, the present study revealed that the dual anisotropic properties of the MAH activated the NOTCH1/2 pathway by upregulating SNHG5 and downstream SIRT6, which modulates the level of NOTCH1/2 by antagonizing DNMT1 protein stability, ultimately inducing the osteogenic differentiation of bone marrow mesenchymal stem cells (BMSCs). Furthermore, the MAH, MIH, and PGH were tested for in vivo bone regeneration in rabbits with femur defects, and the results demonstrated that the MAH effectively stimulated bone regeneration. Taken together, these findings suggest that this magnetically and topographically anisotropic biomimetic hydrogel might be a promising candidate for application in the field of bone tissue regeneration.

细胞微环境中的物理因素对干细胞分化有至关重要的影响。利用物理因素促进干细胞成骨分化已被确立为开发骨组织工程支架的新策略。在这种情况下,具有多尺度各向异性的支架被认为具有生物仿生特性,这对其生物学性能十分有利。在本研究中,通过将静态磁场诱导的磁性纳米材料与水凝胶相结合,设计出了一种具有磁性和地形各向异性的新型磁性各向异性水凝胶(MAH)。在体外研究中,MAH 表现出优异的生物相容性和成骨生物活性。与纯 PEGDA-GelMA 水凝胶(PGH)和磁性各向同性水凝胶(MIH)相比,MAH 诱导的碱性磷酸酶活性以及成骨相关基因和蛋白质的表达量更高。此外,本研究还发现,MAH的双重各向异性特性通过上调SNHG5和下游SIRT6激活了NOTCH1/2通路,而SIRT6则通过拮抗DNMT1蛋白的稳定性调节NOTCH1/2的水平,最终诱导骨髓间充质干细胞(BMSCs)的成骨分化。此外,还对 MAH、MIH 和 PGH 在股骨缺损家兔体内的骨再生进行了测试,结果表明 MAH 能有效刺激骨再生。综上所述,这些研究结果表明,这种具有磁性和地形各向异性的仿生水凝胶有望应用于骨组织再生领域。
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引用次数: 0
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