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In Vitro Osteo-Immunological Responses of Bioactive Calcium Phosphate-Containing Urethane Dimethacrylate-Based Composites: A Potential Alternative to Poly(methyl methacrylate) Bone Cement 含生物活性磷酸钙的聚氨酯二甲基丙烯酸酯基复合材料的体外骨免疫反应:聚甲基丙烯酸甲酯骨水泥的潜在替代品
Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-18 DOI: 10.1021/acsmaterialsau.4c00037
Weerachai Singhatanadgit, Piyarat Sungkhaphan, Boonlom Thavornyutikarn, Setthawut Kitpakornsanti, Anne Young, Wanida Janvikul
This investigation developed new composite bone cements using urethane dimethacrylate (UDMA), poly(propylene glycol) dimethacrylate (PPGDMA), and hydroxyethyl methacrylate (HEMA), with micrometer-sized aluminosilicate glass filler. Monocalcium phosphate monohydrate (MCPM) and hydroxyapatite (HA) particles were added to enhance biological performance, particularly osteo-immunomodulation. Free radical polymerization was triggered by mixing two pastes containing either benzoyl peroxide (BPO, an initiator) or N-tolyglycine glycidyl methacrylate (NTGGMA, an activator). Increasing butylated hydroxytoluene (BHT, an inhibitor) enabled a suitable delay after mixing at 25 °C for placement. At 37 °C, the delay time was reduced and the final conversion was enhanced. Findings also demonstrated the biocompatibility of the developed bone cement toward osteo-immunological cell lineages, including mesenchymal stem cells (MSCs), fibroblasts, osteoclast precursor RAW 246.7 cells, and peripheral blood mononuclear cells (PBMCs). Notably, the cement with both MCPM and HA combined facilitated sufficient MSC growth, enabling subsequent mineralization while concurrently suppressing the proliferation of fibroblasts, osteoclast progenitors, and PBMCs. Furthermore, composite cement exhibited the capacity to differentially regulate osteoblast differentiation, cell-(in)dependent mineralization, osteoclastogenesis, and PBMC-mediated inflammatory responses at both cellular and molecular levels in vitro. These observations suggested their potential use for bone repair, especially in cases of inflammation-associated bone defects.
这项研究使用聚氨酯二甲基丙烯酸酯(UDMA)、聚丙二醇二甲基丙烯酸酯(PPGDMA)和甲基丙烯酸羟乙酯(HEMA)以及微米级硅酸铝玻璃填料开发了新型复合骨水泥。此外,还添加了一水磷酸一钙(MCPM)和羟基磷灰石(HA)颗粒,以提高生物性能,尤其是骨免疫调节性能。将两种含有过氧化苯甲酰(BPO,一种引发剂)或 N-聚甘氨酸缩水甘油醚甲基丙烯酸酯(NTGGMA,一种活化剂)的浆料混合,可引发自由基聚合。增加丁基羟基甲苯(BHT,一种抑制剂)可在 25 °C下混合后适当延迟放置时间。37 °C时,延迟时间缩短,最终转化率提高。研究结果还证明了开发的骨水泥对骨免疫细胞系的生物相容性,包括间充质干细胞(MSC)、成纤维细胞、破骨细胞前体 RAW 246.7 细胞和外周血单核细胞(PBMC)。值得注意的是,含有 MCPM 和 HA 的复合水泥能促进间叶干细胞的充分生长,使其随后矿化,同时抑制成纤维细胞、破骨细胞前体细胞和外周血单核细胞的增殖。此外,复合骨水泥还能在体外的细胞和分子水平上对成骨细胞分化、细胞(内)依赖性矿化、破骨细胞生成和 PBMC 介导的炎症反应进行不同程度的调节。这些观察结果表明,它们有可能用于骨修复,尤其是炎症相关的骨缺损。
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引用次数: 0
Embracing Nature’s Clockwork: Crafting Plastics for Degradation in Plant Agricultural Systems 拥抱大自然的发条:在植物农业系统中制作降解塑料
IF 5.7 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsmaterialsau.4c0003110.1021/acsmaterialsau.4c00031
Danila Merino*, 

In the 21st century, global agriculture confronts the urgent challenge of increasing food production by 70% by 2050 while simultaneously addressing environmental and health concerns. Plastics, integral to agricultural innovation, present sustainability challenges due to their non-biodegradable nature and contribution to pollution. This perspective examines the transition to bioplastics, emphasizing their bio-based origin and their crucial characteristic of being readily biodegradable in the soil. Key bioplastics such as poly(lactic acid) (PLA), polyhydroxyalkanoates (PHAs), and biomass-derived polymers are discussed, particularly regarding the microplastic generation in soil resulting from their use in specific applications like mulch films, delivery systems, and soil conditioners. Embracing bioplastics signifies a significant step forward in achieving sustainable agriculture and addressing plastic waste. However, it is highlighted that while some bioplastics can be recovered and recycled, special applications where the plastic is in intimate contact with soil pose challenges for recovery. In these cases, that represent more than the 50% of plastics used in agriculture, meticulous design for biodegradation in soil synchronized with agricultural cycles is necessary. This approach ensures minimal environmental impact and promotes a circular approach to plastic use in agriculture.

21 世纪,全球农业面临着到 2050 年将粮食产量提高 70%,同时解决环境和健康问题的紧迫挑战。塑料是农业创新不可或缺的一部分,但由于其不可生物降解的特性和造成污染的原因,给可持续发展带来了挑战。本视角探讨了向生物塑料过渡的问题,强调了生物塑料的生物基来源及其在土壤中易于生物降解的重要特性。本文讨论了聚乳酸(PLA)、聚羟基烷酸酯(PHAs)和生物质衍生聚合物等主要生物塑料,特别是它们在地膜、输送系统和土壤改良剂等特定应用中使用时在土壤中产生的微塑料。采用生物塑料标志着在实现可持续农业和解决塑料废弃物方面迈出了重要一步。不过,需要强调的是,虽然有些生物塑料可以回收和再循环,但塑料与土壤亲密接触的特殊应用给回收带来了挑战。在这些情况下(占农业塑料用量的 50%以上),有必要进行精心设计,使其在土壤中的生物降解与农业周期同步。这种方法可确保对环境的影响降到最低,并促进塑料在农业中的循环使用。
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引用次数: 0
Embracing Nature’s Clockwork: Crafting Plastics for Degradation in Plant Agricultural Systems 拥抱大自然的发条:在植物农业系统中制作降解塑料
Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsmaterialsau.4c00031
Danila Merino
In the 21st century, global agriculture confronts the urgent challenge of increasing food production by 70% by 2050 while simultaneously addressing environmental and health concerns. Plastics, integral to agricultural innovation, present sustainability challenges due to their non-biodegradable nature and contribution to pollution. This perspective examines the transition to bioplastics, emphasizing their bio-based origin and their crucial characteristic of being readily biodegradable in the soil. Key bioplastics such as poly(lactic acid) (PLA), polyhydroxyalkanoates (PHAs), and biomass-derived polymers are discussed, particularly regarding the microplastic generation in soil resulting from their use in specific applications like mulch films, delivery systems, and soil conditioners. Embracing bioplastics signifies a significant step forward in achieving sustainable agriculture and addressing plastic waste. However, it is highlighted that while some bioplastics can be recovered and recycled, special applications where the plastic is in intimate contact with soil pose challenges for recovery. In these cases, that represent more than the 50% of plastics used in agriculture, meticulous design for biodegradation in soil synchronized with agricultural cycles is necessary. This approach ensures minimal environmental impact and promotes a circular approach to plastic use in agriculture.
21 世纪,全球农业面临着到 2050 年将粮食产量提高 70%,同时解决环境和健康问题的紧迫挑战。塑料是农业创新不可或缺的一部分,但由于其不可生物降解的特性和造成污染的原因,给可持续发展带来了挑战。本视角探讨了向生物塑料过渡的问题,强调了生物塑料的生物基来源及其在土壤中易于生物降解的重要特性。本文讨论了聚乳酸(PLA)、聚羟基烷酸酯(PHAs)和生物质衍生聚合物等主要生物塑料,特别是它们在地膜、输送系统和土壤改良剂等特定应用中使用时在土壤中产生的微塑料。采用生物塑料标志着在实现可持续农业和解决塑料废弃物方面迈出了重要一步。不过,需要强调的是,虽然有些生物塑料可以回收和再循环,但塑料与土壤亲密接触的特殊应用给回收带来了挑战。在这些情况下(占农业塑料用量的 50%以上),有必要进行精心设计,使其在土壤中的生物降解与农业周期同步。这种方法可确保对环境的影响降到最低,并促进塑料在农业中的循环使用。
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引用次数: 0
Synthesis Route to Single-Walled Zeolite Nanotubes Enabled by Tetrabutylammonium Hydroxide 利用氢氧化四丁基铵合成单壁沸石纳米管的路线
IF 5.7 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-10 DOI: 10.1021/acsmaterialsau.4c0003010.1021/acsmaterialsau.4c00030
Anthony Vallace, Dhrumil R. Shah, Enerelt Burentugs, Atticus J. Tucker, Ashley E. Cavanagh and Christopher W. Jones*, 

Single-walled zeolite nanotubes (ZNT) were recently synthesized in a narrow compositional window. ZNT structural features─thin zeolitic walls and large mesopores─can allow for easy access of small molecules to zeolite micropores, but they also impart processing limitations for these materials, such as challenges with conventional aqueous ion-exchange conditions. Conventional solid- and liquid-phase ion exchange of calcined NaOH-derived ZNT (NaH-ZNT) results in structural degradation to either 2D sheet-like phases, 3D nanocrystals, or amorphous phases, motivating different direct synthesis routes and unconventional ion-exchange procedures of uncalcined ZNT precursors. Here, a modified synthesis route for ZNT synthesis is introduced that facilitates facile ion exchange as well as incorporation of additional non-Al heteroatoms in the zeolite framework. Tetrabutylammonium hydroxide (TBAOH) is used as a hydroxide source and co-OSDA, enabling synthesis of new compositions of ZNT, otherwise unachievable by post-modification of previously reported NaH-ZNT. By varying the gel composition, synthesis temperature, crystallization time, hydroxide source, silicon source, and aluminum source, productive conditions for the new TBAOH synthesis are developed, leading to increased strong acid site density in the ZNT. The collected results demonstrate the sensitivity of the ZNT synthesis to many key parameters and show that the ZNT forms only when Si/(Al + T) ∼ 30 in these synthesis gels and with specific Si and Al sources, and always in the presence of trace Na+. Catalytic testing, via the tandem CO2 hydrogenation to methanol and methanol to aromatics reaction, shows that ZNTs provide adequate catalytic activity (acidity), relative to their conventional 3D counterparts in converting methanol to aromatic compounds.

单壁沸石纳米管(ZNT)是最近在一个狭窄的成分窗口中合成的。ZNT 的结构特征--薄沸石壁和大介孔--可使小分子轻松进入沸石微孔,但也给这些材料的加工带来了限制,例如传统的水相离子交换条件。煅烧过的 NaOH 衍生 ZNT(NaH-ZNT)的传统固相和液相离子交换会导致结构退化为二维片状相、三维纳米晶体或无定形相,这促使人们采用不同的直接合成路线和非煅烧 ZNT 前体的非常规离子交换程序。本文介绍了一种经过改进的 ZNT 合成路线,该路线便于离子交换以及在沸石框架中加入额外的非铝杂质原子。使用四丁基氢氧化铵(TBAOH)作为氢氧化物源和共 OSDA,可以合成新成分的 ZNT,否则无法通过对以前报道过的 NaH-ZNT 进行后修饰来实现。通过改变凝胶成分、合成温度、结晶时间、氢氧化物源、硅源和铝源,开发出了新 TBAOH 合成的生产条件,从而增加了 ZNT 中的强酸位点密度。收集到的结果证明了 ZNT 合成对许多关键参数的敏感性,并表明在这些合成凝胶中,只有当 Si/(Al + T) ∼ 30 时,ZNT 才会形成,并使用特定的硅源和铝源,而且始终存在痕量 Na+。通过串联二氧化碳加氢制甲醇和甲醇制芳烃反应进行的催化测试表明,与传统的三维催化剂相比,ZNT 在将甲醇转化为芳烃化合物方面具有足够的催化活性(酸性)。
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引用次数: 0
Synthesis Route to Single-Walled Zeolite Nanotubes Enabled by Tetrabutylammonium Hydroxide 利用氢氧化四丁基铵合成单壁沸石纳米管的路线
Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-10 DOI: 10.1021/acsmaterialsau.4c00030
Anthony Vallace, Dhrumil R. Shah, Enerelt Burentugs, Atticus J. Tucker, Ashley E. Cavanagh, Christopher W. Jones
Single-walled zeolite nanotubes (ZNT) were recently synthesized in a narrow compositional window. ZNT structural features─thin zeolitic walls and large mesopores─can allow for easy access of small molecules to zeolite micropores, but they also impart processing limitations for these materials, such as challenges with conventional aqueous ion-exchange conditions. Conventional solid- and liquid-phase ion exchange of calcined NaOH-derived ZNT (NaH-ZNT) results in structural degradation to either 2D sheet-like phases, 3D nanocrystals, or amorphous phases, motivating different direct synthesis routes and unconventional ion-exchange procedures of uncalcined ZNT precursors. Here, a modified synthesis route for ZNT synthesis is introduced that facilitates facile ion exchange as well as incorporation of additional non-Al heteroatoms in the zeolite framework. Tetrabutylammonium hydroxide (TBAOH) is used as a hydroxide source and co-OSDA, enabling synthesis of new compositions of ZNT, otherwise unachievable by post-modification of previously reported NaH-ZNT. By varying the gel composition, synthesis temperature, crystallization time, hydroxide source, silicon source, and aluminum source, productive conditions for the new TBAOH synthesis are developed, leading to increased strong acid site density in the ZNT. The collected results demonstrate the sensitivity of the ZNT synthesis to many key parameters and show that the ZNT forms only when Si/(Al + T) ∼ 30 in these synthesis gels and with specific Si and Al sources, and always in the presence of trace Na+. Catalytic testing, via the tandem CO2 hydrogenation to methanol and methanol to aromatics reaction, shows that ZNTs provide adequate catalytic activity (acidity), relative to their conventional 3D counterparts in converting methanol to aromatic compounds.
单壁沸石纳米管(ZNT)是最近在一个狭窄的成分窗口中合成的。ZNT 的结构特征--薄沸石壁和大介孔--可使小分子轻松进入沸石微孔,但也给这些材料的加工带来了限制,例如传统的水相离子交换条件。煅烧过的 NaOH 衍生 ZNT(NaH-ZNT)的传统固相和液相离子交换会导致结构退化为二维片状相、三维纳米晶体或无定形相,这促使人们采用不同的直接合成路线和非煅烧 ZNT 前体的非常规离子交换程序。本文介绍了一种经过改进的 ZNT 合成路线,该路线便于离子交换以及在沸石框架中加入额外的非铝杂质原子。使用四丁基氢氧化铵(TBAOH)作为氢氧化物源和共 OSDA,可以合成新成分的 ZNT,否则无法通过对以前报道过的 NaH-ZNT 进行后修饰来实现。通过改变凝胶成分、合成温度、结晶时间、氢氧化物源、硅源和铝源,开发出了新 TBAOH 合成的生产条件,从而增加了 ZNT 中的强酸位点密度。收集到的结果证明了 ZNT 合成对许多关键参数的敏感性,并表明在这些合成凝胶中,只有当 Si/(Al + T) ∼ 30 时,ZNT 才会形成,并使用特定的硅源和铝源,而且始终存在痕量 Na+。通过串联二氧化碳加氢制甲醇和甲醇制芳烃反应进行的催化测试表明,与传统的三维催化剂相比,ZNT 在将甲醇转化为芳烃化合物方面具有足够的催化活性(酸性)。
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引用次数: 0
Viscoelasticity in 3D Cell Culture and Regenerative Medicine: Measurement Techniques and Biological Relevance 三维细胞培养和再生医学中的粘弹性:测量技术和生物学相关性
IF 5.7 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-18 DOI: 10.1021/acsmaterialsau.3c00038
Payam Eliahoo, Hesam Setayesh, Tyler Hoffman, Yifan Wu, Song Li and Jennifer B. Treweek*, 

The field of mechanobiology is gaining prominence due to recent findings that show cells sense and respond to the mechanical properties of their environment through a process called mechanotransduction. The mechanical properties of cells, cell organelles, and the extracellular matrix are understood to be viscoelastic. Various technologies have been researched and developed for measuring the viscoelasticity of biological materials, which may provide insight into both the cellular mechanisms and the biological functions of mechanotransduction. Here, we explain the concept of viscoelasticity and introduce the major techniques that have been used to measure the viscoelasticity of various soft materials in different length- and timescale frames. The topology of the material undergoing testing, the geometry of the probe, the magnitude of the exerted stress, and the resulting deformation should be carefully considered to choose a proper technique for each application. Lastly, we discuss several applications of viscoelasticity in 3D cell culture and tissue models for regenerative medicine, including organoids, organ-on-a-chip systems, engineered tissue constructs, and tunable viscoelastic hydrogels for 3D bioprinting and cell-based therapies.

最近的研究结果表明,细胞通过一种叫做机械传导的过程来感知和响应周围环境的机械特性,因此机械生物学领域正变得越来越重要。据了解,细胞、细胞器和细胞外基质的机械特性具有粘弹性。目前已研究和开发出多种测量生物材料粘弹性的技术,这些技术可帮助人们深入了解机械传导的细胞机制和生物功能。在此,我们将解释粘弹性的概念,并介绍用于测量各种软材料在不同长度和时间范围内的粘弹性的主要技术。应仔细考虑测试材料的拓扑结构、探针的几何形状、施加应力的大小以及由此产生的变形,以便为每种应用选择合适的技术。最后,我们讨论了粘弹性在三维细胞培养和再生医学组织模型中的几种应用,包括有机体、片上器官系统、工程组织结构以及用于三维生物打印和细胞疗法的可调粘弹性水凝胶。
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引用次数: 0
Impact of Nickel on Iridium–Ruthenium Structure and Activity for the Oxygen Evolution Reaction under Acidic Conditions 镍对酸性条件下铱-钌结构和氧进化反应活性的影响
IF 5.7 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-15 DOI: 10.1021/acsmaterialsau.4c0002510.1021/acsmaterialsau.4c00025
Erlend Bertheussen, Simon Pitscheider, Susan R. Cooper, Rebecca Pittkowski, Katrine L. Svane, Aline Bornet, Erik M. Wisaeus, Kirsten M. Ø. Jensen, Jan Rossmeisl, Matthias Arenz, Christian Kallesøe and Christoffer M. Pedersen*, 

Proton exchange membrane water electrolysis (PEMWE) is a promising technology to produce hydrogen directly from renewable electricity sources due to its high power density and potential for dynamic operation. Widespread application of PEMWE is, however, currently limited due to high cost and low efficiency, for which high loading of expensive iridium catalyst and high OER overpotential, respectively, are important reasons. In this study, we synthesize highly dispersed IrRu nanoparticles (NPs) supported on antimony-doped tin oxide (ATO) to maximize catalyst utilization. Furthermore, we study the effect of adding various amounts of Ni to the synthesis, both in terms of catalyst structure and OER activity. Through characterization using various X-ray techniques, we determine that the presence of Ni during synthesis yields significant changes in the structure of the IrRu NPs. With no Ni present, metallic IrRu NPs were synthesized with Ir-like structure, while the presence of Ni leads to the formation of IrRu oxide particles with rutile/hollandite structure. There are also clear indications that the presence of Ni yields smaller particles, which can result in better catalyst dispersion. The effect of these differences on OER activity was also studied through rotating disc electrode measurements. The IrRu-supported catalyst synthesized with Ni exhibited OER activity of up to 360 mA mgPGM–1 at 1.5 V vs RHE. This is ∼7 times higher OER activity than the best-performing IrOx benchmark reported in the literature and more than twice the activity of IrRu-supported catalyst synthesized without Ni. Finally, density functional theory (DFT) calculations were performed to further elucidate the origin of the observed activity enhancement, showing no improvement in intrinsic OER activity for hollandite Ir and Ru compared to the rutile structures. We, therefore, hypothesize that the increased activity measured for the IrRu supported catalyst synthesized with Ni present is instead due to increased electrochemical surface area.

质子交换膜水电解法(PEMWE)具有高功率密度和动态运行的潜力,是一种利用可再生能源直接制氢的前景广阔的技术。然而,由于成本高、效率低,质子交换膜水电解法的广泛应用目前受到了限制,其中昂贵的铱催化剂的高负载量和高OER过电位分别是重要原因。在本研究中,我们在掺锑氧化锡(ATO)上合成了高度分散的铱钌纳米粒子(NPs),以最大限度地提高催化剂的利用率。此外,我们还研究了在合成过程中添加不同量的 Ni 对催化剂结构和 OER 活性的影响。通过使用各种 X 射线技术进行表征,我们确定合成过程中镍的存在会使 IrRu NPs 的结构发生显著变化。在没有镍存在的情况下,合成的金属 IrRu NPs 具有类似于铁的结构,而镍的存在则导致形成具有金红石/荷兰石结构的 IrRu 氧化物颗粒。还有明显的迹象表明,镍的存在会产生更小的颗粒,从而使催化剂的分散性更好。我们还通过旋转圆盘电极测量研究了这些差异对 OER 活性的影响。用镍合成的 IrRu 支承催化剂在 1.5 V 对比 RHE 时的 OER 活性高达 360 mA mgPGM-1。这比文献报道的性能最好的 IrOx 基准催化剂的 OER 活性高出 7 倍,是不含 Ni 的 IrRu 支持催化剂活性的两倍多。最后,我们进行了密度泛函理论(DFT)计算,以进一步阐明所观察到的活性增强的原因,结果显示与金红石结构相比,荷兰石 Ir 和 Ru 的固有 OER 活性没有提高。因此,我们推测,在含有镍的情况下合成的 IrRu 支承催化剂活性的提高是由于电化学表面积的增加。
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引用次数: 0
In Vivo Assessment of a Triple Periodic Minimal Surface Based Biomimmetic Gyroid as an Implant Material in a Rabbit Tibia Model 在兔胫骨模型中对作为植入材料的三周期极小表面生物仿生陀螺仪进行体内评估
IF 5.7 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-12 DOI: 10.1021/acsmaterialsau.4c0001610.1021/acsmaterialsau.4c00016
Pearlin Amaan Khan, Ansheed Raheem, Cheirmadurai Kalirajan, Konda Gokuldoss Prashanth and Geetha Manivasagam*, 

Biomimetic approaches to implant construction are a rising frontier in implantology. Triple Periodic Minimal Surface (TPMS)-based additively manufactured gyroid structures offer a mean curvature of zero, rendering this structure an ideal porous architecture. Previous studies have demonstrated the ability of these structures to effectively mimic the mechanical cues required for optimal implant construction. The porous nature of gyroid materials enhances bone ingrowth, thereby improving implant stability within the body. This enhancement is attributed to the increased surface area of the gyroid structure, which is approximately 185% higher than that of a dense material of the same form factor. This larger surface area allows for enhanced cellular attachment and nutrient circulation facilitated by the porous channels. This study aims to evaluate the biological performance of a gyroid-based Ti6Al-4V implant material compared to a dense alloy counterpart. Cellular viability was assessed using the lactate dehydrogenase (LDH) assay, which demonstrated that the gyroid surface allowed marginally higher viability than dense material. The in vivo integration was studied over 6 weeks using a rabbit tibia model and characterized using X-ray, micro-CT, and histopathological examination. With a metal volume of 8.1%, the gyroid exhibited a bone volume/total volume (BV/TV) ratio of 9.6%, which is 11-fold higher than that of dense metal (0.8%). Histological assessments revealed neovascularization, in-bone growth, and the presence of a Haversian system in the gyroid structure, hinting at superior osteointegration.

仿生植入物制造方法是植入学的一个新兴前沿领域。基于三周期最小表面(TPMS)的添加剂制造陀螺结构的平均曲率为零,使这种结构成为理想的多孔结构。之前的研究已经证明,这些结构能够有效模拟最佳种植体结构所需的机械线索。陀螺状材料的多孔性能促进骨的生长,从而提高植入物在体内的稳定性。这种提高归功于陀螺结构表面积的增加,与相同形状系数的致密材料相比,陀螺结构的表面积增加了约 185%。更大的表面积可通过多孔通道促进细胞附着和营养循环。本研究旨在评估基于陀螺结构的 Ti6Al-4V 植入材料与致密合金植入材料相比的生物性能。使用乳酸脱氢酶(LDH)检测法评估了细胞存活率,结果表明陀螺表面的细胞存活率略高于致密材料。使用兔子胫骨模型对体内整合情况进行了为期 6 周的研究,并使用 X 射线、显微 CT 和组织病理学检查对其进行了鉴定。在金属体积为 8.1% 的情况下,陀螺表面的骨体积/总体积(BV/TV)比为 9.6%,是致密金属(0.8%)的 11 倍。组织学评估显示,陀螺结构中出现了新生血管、骨内生长和哈弗系统,这表明其骨整合性极佳。
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引用次数: 0
Electrocatalytic and Selective Oxidation of Glycerol to Formate on 2D 3d-Metal Phosphate Nanosheets and Carbon-Negative Hydrogen Generation 二维 3d 磷酸盐金属纳米片上甘油到甲酸盐的电催化和选择性氧化及负碳制氢
IF 5.7 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-04 DOI: 10.1021/acsmaterialsau.4c0002410.1021/acsmaterialsau.4c00024
Inderjeet Chauhan, Pothoppurathu M. Vijay, Ravi Ranjan, Kshirodra Kumar Patra and Chinnakonda S. Gopinath*, 

In the landscape of green hydrogen production, alkaline water electrolysis is a well-established, yet not-so-cost-effective, technique due to the high overpotential requirement for the oxygen evolution reaction (OER). A low-voltage approach is proposed to overcome not only the OER challenge by favorably oxidizing abundant feedstock molecules with an earth-abundant catalyst but also to reduce the energy input required for hydrogen production. This alternative process not only generates carbon-negative green H2 but also yields concurrent value-added products (VAPs), thereby maximizing economic advantages and transforming waste into valuable resources. The essence of this study lies in a novel electrocatalyst material. In the present study, unique and two-dimensional (2D) ultrathin nanosheet phosphates featuring first-row transition metals are synthesized by a one-step solvothermal method, and evaluated for the electrocatalytic glycerol oxidation reaction (GLYOR) in an alkaline medium and simultaneous H2 production. Co3(PO4)2 (CoP), Cu3(PO4)2 (CuP), and Ni3(PO4)2 (NiP) exhibit 2D sheet morphologies, while FePO4 (FeP) displays an entirely different snowflake-like morphology. The 2D nanosheet morphology provides a large surface area and a high density of active sites. As a GLYOR catalyst, CoP ultrathin (∼5 nm) nanosheets exhibit remarkably low onset potential at 1.12 V (vs RHE), outperforming that of NiP, FeP, and CuP around 1.25 V (vs RHE). CoP displays 82% selective formate production, indicating a superior capacity for C–C cleavage and concurrent oxidation; this property could be utilized to valorize larger molecules. CoP also exhibits highly sustainable electrochemical stability for a continuous 200 h GLYOR operation, yielding 6.5 L of H2 production with a 4 cm2 electrode and 98 ± 0.5% Faradaic efficiency. The present study advances our understanding of efficient GLYOR catalysts and underscores the potential of sustainable and economically viable green hydrogen production methodologies.

在绿色制氢领域,碱性水电解是一种成熟但成本效益不高的技术,原因是氧进化反应(OER)需要较高的过电位。我们提出了一种低电压方法,不仅可以通过使用富土催化剂有利地氧化丰富的原料分子来克服氧进化反应的挑战,还可以减少制氢所需的能量输入。这种替代工艺不仅能产生负碳绿色氢气,还能同时产生增值产品 (VAP),从而最大限度地发挥经济优势,变废为宝。这项研究的精髓在于一种新型电催化剂材料。本研究采用一步溶热法合成了独特的二维(2D)超薄纳米片磷酸盐,其中含有第一排过渡金属,并对其在碱性介质中的甘油氧化反应(GLYOR)以及同时产生 H2 的电催化性能进行了评估。Co3(PO4)2 (CoP)、Cu3(PO4)2 (CuP) 和 Ni3(PO4)2 (NiP) 呈现出二维片状形态,而 FePO4 (FeP) 则呈现出完全不同的雪花状形态。二维纳米片形态提供了较大的表面积和高密度的活性位点。作为一种 GLYOR 催化剂,CoP 超薄(∼5 nm)纳米片的起始电位非常低,仅为 1.12 V(相对于 RHE),超过了 NiP、FeP 和 CuP 在 1.25 V 左右的起始电位(相对于 RHE)。CoP 显示出 82% 的甲酸选择性生成,表明其具有卓越的 C-C 裂解和同步氧化能力;这一特性可用于较大分子的估值。CoP 还在连续 200 小时的 GLYOR 操作中表现出高度可持续的电化学稳定性,4 平方厘米的电极可产生 6.5 升 H2,法拉第效率为 98 ± 0.5%。本研究加深了我们对高效 GLYOR 催化剂的了解,并强调了可持续且经济可行的绿色制氢方法的潜力。
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引用次数: 0
Electrocatalytic and Selective Oxidation of Glycerol to Formate on 2D 3d-Metal Phosphate Nanosheets and Carbon-Negative Hydrogen Generation 二维 3d 磷酸盐金属纳米片上甘油到甲酸盐的电催化和选择性氧化及负碳制氢
Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-04 DOI: 10.1021/acsmaterialsau.4c00024
Inderjeet Chauhan, Pothoppurathu M. Vijay, Ravi Ranjan, Kshirodra Kumar Patra, Chinnakonda S. Gopinath
In the landscape of green hydrogen production, alkaline water electrolysis is a well-established, yet not-so-cost-effective, technique due to the high overpotential requirement for the oxygen evolution reaction (OER). A low-voltage approach is proposed to overcome not only the OER challenge by favorably oxidizing abundant feedstock molecules with an earth-abundant catalyst but also to reduce the energy input required for hydrogen production. This alternative process not only generates carbon-negative green H2 but also yields concurrent value-added products (VAPs), thereby maximizing economic advantages and transforming waste into valuable resources. The essence of this study lies in a novel electrocatalyst material. In the present study, unique and two-dimensional (2D) ultrathin nanosheet phosphates featuring first-row transition metals are synthesized by a one-step solvothermal method, and evaluated for the electrocatalytic glycerol oxidation reaction (GLYOR) in an alkaline medium and simultaneous H2 production. Co3(PO4)2 (CoP), Cu3(PO4)2 (CuP), and Ni3(PO4)2 (NiP) exhibit 2D sheet morphologies, while FePO4 (FeP) displays an entirely different snowflake-like morphology. The 2D nanosheet morphology provides a large surface area and a high density of active sites. As a GLYOR catalyst, CoP ultrathin (∼5 nm) nanosheets exhibit remarkably low onset potential at 1.12 V (vs RHE), outperforming that of NiP, FeP, and CuP around 1.25 V (vs RHE). CoP displays 82% selective formate production, indicating a superior capacity for C–C cleavage and concurrent oxidation; this property could be utilized to valorize larger molecules. CoP also exhibits highly sustainable electrochemical stability for a continuous 200 h GLYOR operation, yielding 6.5 L of H2 production with a 4 cm2 electrode and 98 ± 0.5% Faradaic efficiency. The present study advances our understanding of efficient GLYOR catalysts and underscores the potential of sustainable and economically viable green hydrogen production methodologies.
在绿色制氢领域,碱性水电解是一种成熟但成本效益不高的技术,原因是氧进化反应(OER)需要较高的过电位。我们提出了一种低电压方法,不仅可以通过使用富土催化剂有利地氧化丰富的原料分子来克服氧进化反应的挑战,还可以减少制氢所需的能量输入。这种替代工艺不仅能产生负碳绿色氢气,还能同时产生增值产品 (VAP),从而最大限度地发挥经济优势,变废为宝。这项研究的精髓在于一种新型电催化剂材料。本研究采用一步溶热法合成了独特的二维(2D)超薄纳米片磷酸盐,其中含有第一排过渡金属,并对其在碱性介质中的甘油氧化反应(GLYOR)以及同时产生 H2 的电催化性能进行了评估。Co3(PO4)2 (CoP)、Cu3(PO4)2 (CuP) 和 Ni3(PO4)2 (NiP) 呈现出二维片状形态,而 FePO4 (FeP) 则呈现出完全不同的雪花状形态。二维纳米片形态提供了较大的表面积和高密度的活性位点。作为一种 GLYOR 催化剂,CoP 超薄(∼5 nm)纳米片的起始电位非常低,仅为 1.12 V(相对于 RHE),超过了 NiP、FeP 和 CuP 在 1.25 V 左右的起始电位(相对于 RHE)。CoP 显示出 82% 的甲酸选择性生成,表明其具有卓越的 C-C 裂解和同步氧化能力;这一特性可用于较大分子的估值。CoP 还在连续 200 小时的 GLYOR 操作中表现出高度可持续的电化学稳定性,4 平方厘米的电极可产生 6.5 升 H2,法拉第效率为 98 ± 0.5%。本研究加深了我们对高效 GLYOR 催化剂的了解,并强调了可持续且经济可行的绿色制氢方法的潜力。
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引用次数: 0
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