Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.08.019
Xinping Luo , Xincong Li , Shiyu Li , Chenxi Zhou , Jing Li , Zhanwei Zhou , Minjie Sun
Aberrant metabolic balance in malignant tumors shapes defensive redox homeostasis and protected tumor cells from oxidative stress damage, consequently impeding clinical transformation process of oxidative stress-dependent anti-tumor therapies represented by chemodynamic therapy and immunotherapy. Herein, a rational designed mitochondria nanomotor was developed by coating a GSH-responsive functional Pt(IV) prodrug layer DP on magnetic iron oxide nanoparticles (MN), which can thoroughly breakdown redox homeostasis by metabolic intervention strategy. Specifically, DP loading two dichloroacetic acid (DCA) axial ligands was stimuli-responsively reduced into Pt(II) and DCA molecules in highly reductive tumor cells, accompanied with glutathione elimination and oxidative stress counteraction weakening. Subsequently, DCA increased pyruvate influx into the mitochondria by pyruvate dehydrogenase activation and enduringly elevated oxidative phosphorylation level, breaking the tumor redox homeostasis thoroughly, contributing to 7.5-fold amplifying hydrogen peroxide production and sensitizing chemodynamic therapy mediated by MN, finally resulting in inspiring 89.5% tumor suppression rate on triple negative breast cancer model. In short, this work realized comprehensive and sustainable oxidative stress elevation of the intracellular environment by metabolic intervention strategy and provided an ingenious perspective of augmenting oxidative stress-dependent anti-tumor therapies.
{"title":"Metabolic intervention mitochondria nanomotors breakdown redox homeostasis for boosting oxidative stress-dependent antitumor therapy","authors":"Xinping Luo , Xincong Li , Shiyu Li , Chenxi Zhou , Jing Li , Zhanwei Zhou , Minjie Sun","doi":"10.1016/j.mattod.2024.08.019","DOIUrl":"10.1016/j.mattod.2024.08.019","url":null,"abstract":"<div><div>Aberrant metabolic balance in malignant tumors shapes defensive redox homeostasis and protected tumor cells from oxidative stress damage, consequently impeding clinical transformation process of oxidative stress-dependent anti-tumor therapies represented by chemodynamic therapy and immunotherapy. Herein, a rational designed mitochondria nanomotor was developed by coating a GSH-responsive functional Pt(IV) prodrug layer DP on magnetic iron oxide nanoparticles (MN), which can thoroughly breakdown redox homeostasis by metabolic intervention strategy. Specifically, DP loading two dichloroacetic acid (DCA) axial ligands was stimuli-responsively reduced into Pt(II) and DCA molecules in highly reductive tumor cells, accompanied with glutathione elimination and oxidative stress counteraction weakening. Subsequently, DCA increased pyruvate influx into the mitochondria by pyruvate dehydrogenase activation and enduringly elevated oxidative phosphorylation level, breaking the tumor redox homeostasis thoroughly, contributing to 7.5-fold amplifying hydrogen peroxide production and sensitizing chemodynamic therapy mediated by MN, finally resulting in inspiring 89.5% tumor suppression rate on triple negative breast cancer model. In short, this work realized comprehensive and sustainable oxidative stress elevation of the intracellular environment by metabolic intervention strategy and provided an ingenious perspective of augmenting oxidative stress-dependent anti-tumor therapies.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 187-200"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721066","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.07.012
Yao Yang , Xiaotong Liang , Qimanguli Saiding , Jiachan Lin , Jinyuan Li , Wenyan Wang , Ping Huang , Li Huang , Wenfeng Zeng , Jinhai Huang , Hongzhong Chen , Wei Tao , Xiaowei Zeng
Photodynamic therapy (PDT) can enhance immune checkpoint blockade (ICB) antitumor immunity. However, PDT can significantly exacerbate the hypoxic tumor microenvironment and stimulate tumor neovascularization, promoting tumor invasion and metastasis. Camptothecin can inhibit angiogenesis by down-regulating hypoxia-inducible factor 1α (HIF-1α). Therefore, this study proposed to combine camptothecin with PDT for the first time to alleviate the disadvantage of PDT, and play its dual role of chemotherapy and antiangiogenesis. Here, a light-activated nanocarrier crosslinked the anti-PD-L1, photosensitizer, and camptothecin prodrug mildly with a thioketal bond for checkpoint blockade immunoregulation was designed. Firstly, photosensitizer-induced PDT and immunogenic cell death effect significantly increase T cell infiltration (33.3 % CD8+ increase), enhancing ICB antitumor immunity. Secondly, the antiangiogenic effect of camptothecin was beneficial for alleviating hypoxic tumor microenvironment exacerbated by PDT (HIF-1α expression decreased in tumor cells). Thirdly, light-activated release facilitates tumor accumulation (3.22 times) and controlled drug release. Thus, the immune checkpoint blockade combined with PDT and an antiangiogenic therapy of camptothecin creates a positive feedback co-delivery platform that exemplifies cascaded synergistic tumor therapy by checkpoint blockade immunoregulation. Besides, it also introduces a new strategy for combining small molecule drugs with macromolecules like proteins to treat various diseases.
{"title":"Light-activated polymeric crosslinked nanocarriers as a checkpoint blockade immunoregulatory platform for synergistic tumor therapy","authors":"Yao Yang , Xiaotong Liang , Qimanguli Saiding , Jiachan Lin , Jinyuan Li , Wenyan Wang , Ping Huang , Li Huang , Wenfeng Zeng , Jinhai Huang , Hongzhong Chen , Wei Tao , Xiaowei Zeng","doi":"10.1016/j.mattod.2024.07.012","DOIUrl":"10.1016/j.mattod.2024.07.012","url":null,"abstract":"<div><div>Photodynamic therapy (PDT) can enhance immune checkpoint blockade (ICB) antitumor immunity. However, PDT can significantly exacerbate the hypoxic tumor microenvironment and stimulate tumor neovascularization, promoting tumor invasion and metastasis. Camptothecin can inhibit angiogenesis by down-regulating hypoxia-inducible factor 1α (HIF-1α). Therefore, this study proposed to combine camptothecin with PDT for the first time to alleviate the disadvantage of PDT, and play its dual role of chemotherapy and antiangiogenesis. Here, a light-activated nanocarrier crosslinked the anti-PD-L1, photosensitizer, and camptothecin prodrug mildly with a thioketal bond for checkpoint blockade immunoregulation was designed. Firstly, photosensitizer-induced PDT and immunogenic cell death effect significantly increase T cell infiltration (33.3 % CD8<sup>+</sup> increase), enhancing ICB antitumor immunity. Secondly, the antiangiogenic effect of camptothecin was beneficial for alleviating hypoxic tumor microenvironment exacerbated by PDT (HIF-1α expression decreased in tumor cells). Thirdly, light-activated release facilitates tumor accumulation (3.22 times) and controlled drug release. Thus, the immune checkpoint blockade combined with PDT and an antiangiogenic therapy of camptothecin creates a positive feedback co-delivery platform that exemplifies cascaded synergistic tumor therapy by checkpoint blockade immunoregulation. Besides, it also introduces a new strategy for combining small molecule drugs with macromolecules like proteins to treat various diseases.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 1-22"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142720461","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.09.008
Siyuan Sun , Kun Fan , Jie Yang , Jiaxiang Liu , Xiang Li , Lihua Zhao , Xin He , Xiangyang Liu , Shenli Jia , Qi Li
Polymer materials have played crucial roles in current electrical device/equipment especially in rapidly developed dielectric energy storage field, due to their excellent insulation property, low dielectric loss, lightweight, flexibility and good processability. Typical several strategies including monomer/molecule structure design, aggregation structure regulation and nanocomposite strengthening have acquired numerous processes. However, it is always ignored in existed work that insulation failure of polymer material generally starts from surface, and high-frequency electric field can greatly accelerate this failure process. Here surface modification engineering (SME) on polymer materials with a scalable, rapid and low-cost characteristic presents unique superiority in solving current problems. In this Review, we summarize various SME approaches on polymer materials and discuss introduced variations in surface morphology, physicochemical structure and charge transport behavior. We analyze how particular chemical groups anchoring, organic–inorganic deposition, physicochemical evolution and micro-nano structure design of modification surface can be modulated to obviously enhance multilevel insulation properties (from surface to interior even under high-frequency electric field) and subsequent dielectric energy storage performances. In addition, we highlight the multifunctionality and stability of modification surface on polymer materials, which examines the possibility of synergistically improving other performances like antifouling and anti-corrosion toward complicated/hash insulation scenes and advanced energy storage. Finally, we analyze current challenges in this field and offer a prospect for future development toward high-performance and large-scale practical applications.
高分子材料因其优异的绝缘性能、低介电损耗、轻质、柔性和良好的可加工性，在当前的电气设备中发挥着至关重要的作用，尤其是在快速发展的电介质储能领域。包括单体/分子结构设计、聚集结构调整和纳米复合材料强化在内的几种典型策略已经获得了大量的应用。然而，人们一直忽视了聚合物材料的绝缘失效一般是从表面开始的，而高频电场会大大加速这一失效过程。因此，聚合物材料表面改性工程（SME）具有可扩展、快速和低成本的特点，在解决当前问题方面具有独特的优越性。在本综述中，我们总结了聚合物材料的各种 SME 方法，并讨论了表面形态、物理化学结构和电荷传输行为的变化。我们分析了如何通过调节改性表面的特定化学基团锚定、有机-无机沉积、物理化学演化和微纳结构设计来明显增强多级绝缘特性（即使在高频电场下也能从表面到内部）以及随后的电介质储能性能。此外，我们还强调了改性表面在聚合物材料上的多功能性和稳定性，从而探讨了协同改善防污和防腐蚀等其他性能的可能性，以实现复杂的/短波绝缘场景和先进的储能。最后，我们分析了该领域当前面临的挑战，并展望了未来向高性能和大规模实际应用发展的前景。
{"title":"Surface modification engineering on polymer materials toward multilevel insulation properties and subsequent dielectric energy storage","authors":"Siyuan Sun , Kun Fan , Jie Yang , Jiaxiang Liu , Xiang Li , Lihua Zhao , Xin He , Xiangyang Liu , Shenli Jia , Qi Li","doi":"10.1016/j.mattod.2024.09.008","DOIUrl":"10.1016/j.mattod.2024.09.008","url":null,"abstract":"<div><div>Polymer materials have played crucial roles in current electrical device/equipment especially in rapidly developed dielectric energy storage field, due to their excellent insulation property, low dielectric loss, lightweight, flexibility and good processability. Typical several strategies including monomer/molecule structure design, aggregation structure regulation and nanocomposite strengthening have acquired numerous processes. However, it is always ignored in existed work that insulation failure of polymer material generally starts from surface, and high-frequency electric field can greatly accelerate this failure process. Here surface modification engineering (SME) on polymer materials with a scalable, rapid and low-cost characteristic presents unique superiority in solving current problems. In this Review, we summarize various SME approaches on polymer materials and discuss introduced variations in surface morphology, physicochemical structure and charge transport behavior. We analyze how particular chemical groups anchoring, organic–inorganic deposition, physicochemical evolution and micro-nano structure design of modification surface can be modulated to obviously enhance multilevel insulation properties (from surface to interior even under high-frequency electric field) and subsequent dielectric energy storage performances. In addition, we highlight the multifunctionality and stability of modification surface on polymer materials, which examines the possibility of synergistically improving other performances like antifouling and anti-corrosion toward complicated/hash insulation scenes and advanced energy storage. Finally, we analyze current challenges in this field and offer a prospect for future development toward high-performance and large-scale practical applications.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 758-823"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142720917","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.09.016
Xiaobing Yan , Jiangzhen Niu , Ziliang Fang , Jikang Xu , Changlin Chen , Yufei Zhang , Yong Sun , Liang Tong , Jianan Sun , Saibo Yin , Yiduo Shao , Shiqing Sun , Jianhui Zhao , Mario Lanza , Tianling Ren , Jingsheng CHEN , Peng Zhou
Next-generation synaptic devices with multiple non-volatile states, high endurance and high-temperature operation are highly desired in the era of big data. Here, high-performance memristors are fabricated using La: HfO2(HLO)/La2/3Sr1/3MnO3(LSMO) heterostructures on Si substrate, with domain matching epitaxial structure using SrTiO3(STO) as buffer layer. The devices possess high reliability, nonvolatility, low fluctuation rate (<2.5 %) and the highest number of states per cell (32 states or 5 bits) among the reported Hf-based ferroelectric memories at room temperature (25 °C) and high temperature (85 °C). Moreover, the device exhibits high endurance of 109 cycles and excellent uniformity at the room and high temperatures. The functionality of long-term plasticity in the synaptic device is obtained with high precision (128 states), reproducibility (cycle-to-cycle variation, ∼4.7 %) and linearity. Then, we simulate one system using the stable performance at high temperature that detects the speed of moving targets, which achieves high accuracy of 98 % and 99 % on Human Motion and MNIST datasets, respectively. Furthermore, we have built a hardware circuit to realize a spiking neural network (SNN) system for digital pattern online learning, which demonstrates the capability of the device in brain-like computing applications.
{"title":"High-performance in domain matching epitaxial La:HfO2 film memristor for spiking neural network system application","authors":"Xiaobing Yan , Jiangzhen Niu , Ziliang Fang , Jikang Xu , Changlin Chen , Yufei Zhang , Yong Sun , Liang Tong , Jianan Sun , Saibo Yin , Yiduo Shao , Shiqing Sun , Jianhui Zhao , Mario Lanza , Tianling Ren , Jingsheng CHEN , Peng Zhou","doi":"10.1016/j.mattod.2024.09.016","DOIUrl":"10.1016/j.mattod.2024.09.016","url":null,"abstract":"<div><div>Next-generation synaptic devices with multiple non-volatile states, high endurance and high-temperature operation are highly desired in the era of big data. Here, high-performance memristors are fabricated using La: HfO<sub>2</sub>(HLO)/La<sub>2/3</sub>Sr<sub>1/3</sub>MnO<sub>3</sub>(LSMO) heterostructures on Si substrate, with domain matching epitaxial structure using SrTiO<sub>3</sub>(STO) as buffer layer. The devices possess high reliability, nonvolatility, low fluctuation rate (<2.5 %) and the highest number of states per cell (32 states or 5 bits) among the reported Hf-based ferroelectric memories at room temperature (25 °C) and high temperature (85 °C). Moreover, the device exhibits high endurance of 10<sup>9</sup> cycles and excellent uniformity at the room and high temperatures. The functionality of long-term plasticity in the synaptic device is obtained with high precision (128 states), reproducibility (cycle-to-cycle variation, ∼4.7 %) and linearity. Then, we simulate one system using the stable performance at high temperature that detects the speed of moving targets, which achieves high accuracy of 98 % and 99 % on Human Motion and MNIST datasets, respectively. Furthermore, we have built a hardware circuit to realize a spiking neural network (SNN) system for digital pattern online learning, which demonstrates the capability of the device in brain-like computing applications.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 365-373"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142720920","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.08.026
Jiaming Sun , Shanyu Zhao , Xiangsong Wang , Weiqing Kong , Wei Li , Shuangfei Wang , Shouxin Liu , Shuangxi Nie
Solar steam generation presents a promising solution to address water shortages in an eco-friendly and low-cost manner. Numerous broad-band light absorbers and topological designs have been developed to enhance the evaporation rate. However, when considering solely solar energy input, the evaporation rate faces theoretically limitations, assuming 100 % energy conversion efficiency, due to the latent heat requirement for water vaporization. As material selection and structural design reach the saturation of novelty, researchers are increasingly focusing on the enthalpy of evaporation of water (EEW). In this review, we briefly outline factors influencing net heat input, taking note of the influence of environmental energy, and then delve into the concept of EEW in evaporators, elucidating regulation principle, characterization and analysis methods related to EEW systematically. Subsequently, we review the latest research progress on optimization strategies aimed at minimizing EEW, including the modulation of hydration state and the adjustment of pore structure in evaporators. Finally, we discuss current challenges and future research opportunities in minimizing EEW in solar steam generation.
{"title":"Minimizing enthalpy of evaporation in solar steam generation: An emerging strategy beyond theoretical evaporation limitation","authors":"Jiaming Sun , Shanyu Zhao , Xiangsong Wang , Weiqing Kong , Wei Li , Shuangfei Wang , Shouxin Liu , Shuangxi Nie","doi":"10.1016/j.mattod.2024.08.026","DOIUrl":"10.1016/j.mattod.2024.08.026","url":null,"abstract":"<div><div>Solar steam generation presents a promising solution to address water shortages in an eco-friendly and low-cost manner. Numerous broad-band light absorbers and topological designs have been developed to enhance the evaporation rate. However, when considering solely solar energy input, the evaporation rate faces theoretically limitations, assuming 100 % energy conversion efficiency, due to the latent heat requirement for water vaporization. As material selection and structural design reach the saturation of novelty, researchers are increasingly focusing on the enthalpy of evaporation of water (EEW). In this review, we briefly outline factors influencing net heat input, taking note of the influence of environmental energy, and then delve into the concept of EEW in evaporators, elucidating regulation principle, characterization and analysis methods related to EEW systematically. Subsequently, we review the latest research progress on optimization strategies aimed at minimizing EEW, including the modulation of hydration state and the adjustment of pore structure in evaporators. Finally, we discuss current challenges and future research opportunities in minimizing EEW in solar steam generation.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 619-647"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142720960","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.08.028
Siyu Liu, Tongqi Wen, A.S.L. Subrahmanyam Pattamatta, David J. Srolovitz
Large language models (LLMs) have demonstrated rapid progress across a wide array of domains. Owing to the very large number of parameters and training data in LLMs, these models inherently encompass an expansive and comprehensive materials knowledge database, far exceeding the capabilities of individual researcher. Nonetheless, devising methods to harness the knowledge embedded within LLMs for the design and discovery of novel materials remains a formidable challenge. We introduce a general approach for addressing materials classification problems, which incorporates LLMs, prompt engineering, and deep learning. Utilizing a dataset of metallic glasses as a case study, our methodology achieved an improvement of up to 463% in prediction accuracy compared to conventional classification models. These findings underscore the potential of leveraging textual knowledge generated by LLMs for materials especially in the common situation where datasets are sparse, thereby promoting innovation in materials discovery and design.
{"title":"A prompt-engineered large language model, deep learning workflow for materials classification","authors":"Siyu Liu, Tongqi Wen, A.S.L. Subrahmanyam Pattamatta, David J. Srolovitz","doi":"10.1016/j.mattod.2024.08.028","DOIUrl":"10.1016/j.mattod.2024.08.028","url":null,"abstract":"<div><div>Large language models (LLMs) have demonstrated rapid progress across a wide array of domains. Owing to the very large number of parameters and training data in LLMs, these models inherently encompass an expansive and comprehensive materials knowledge database, far exceeding the capabilities of individual researcher. Nonetheless, devising methods to harness the knowledge embedded within LLMs for the design and discovery of novel materials remains a formidable challenge. We introduce a general approach for addressing materials classification problems, which incorporates LLMs, prompt engineering, and deep learning. Utilizing a dataset of metallic glasses as a case study, our methodology achieved an improvement of up to 463% in prediction accuracy compared to conventional classification models. These findings underscore the potential of leveraging textual knowledge generated by LLMs for materials especially in the common situation where datasets are sparse, thereby promoting innovation in materials discovery and design.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 240-249"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721070","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.08.020
Voichita Mihali , Piotr Jasko , Michal Skowicki , Cornelia G. Palivan
Compartmentalization is essential in nature for precisely controlling metabolic reactions, exchange of molecules and signals with the environment and inter-cell communication. While artificial organelles and cells offer simplified conditions for studying enzymatic reactions, it is still challenging to spatially and directionally control them. Here we present self-organized clusters combining catalytic nanocompartments (CNCs) loaded with different enzymes that are specifically attached to Janus nanoparticles (JNPs). The clusters are modularly assembled through programmed DNA hybridization. The asymmetry of the JNPs has unique advantages by allowing a precise arrangement of the CNCs and enabling, in a modular manner, various reaction configurations, including single, parallel and cascade enzymatic reactions. Additionally, JNP-CNCs clusters integrating imaging and therapeutic nanocompartments support nanotheranostic applications by simultaneous precise detection of their in vitro position and production of reactive oxygen species (ROS) that induce apoptosis. Such JNP-CNCs clusters provide both spatial and directional control of enzymatic reactions at the nanoscale and have high potential in biomedical applications, including protein therapy and theranostics.
{"title":"Controlled enzymatic reactions by programmed confinement in clusters of polymersomes and Janus nanoparticles","authors":"Voichita Mihali , Piotr Jasko , Michal Skowicki , Cornelia G. Palivan","doi":"10.1016/j.mattod.2024.08.020","DOIUrl":"10.1016/j.mattod.2024.08.020","url":null,"abstract":"<div><div>Compartmentalization is essential in nature for precisely controlling metabolic reactions, exchange of molecules and signals with the environment and inter-cell communication. While artificial organelles and cells offer simplified conditions for studying enzymatic reactions, it is still challenging to spatially and directionally control them. Here we present self-organized clusters combining catalytic nanocompartments (CNCs) loaded with different enzymes that are specifically attached to Janus nanoparticles (JNPs). The clusters are modularly assembled through programmed DNA hybridization. The asymmetry of the JNPs has unique advantages by allowing a precise arrangement of the CNCs and enabling, in a modular manner, various reaction configurations, including single, parallel and cascade enzymatic reactions. Additionally, JNP-CNCs clusters integrating imaging and therapeutic nanocompartments support nanotheranostic applications by simultaneous precise detection of their <em>in vitro</em> position and production of reactive oxygen species (ROS) that induce apoptosis. Such JNP-CNCs clusters provide both spatial and directional control of enzymatic reactions at the nanoscale and have high potential in biomedical applications, including protein therapy and theranostics.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 201-217"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721067","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.08.009
Haiyue Zu , Lizhen Zheng , Mengke Huo , Kevin Liu , Chris Halling Dreyer , Yuantao Zhang , Xuan He , Ye Li , Li Zou , Le Huang , Xueting Yi , Antonia Rujia Sun , Xiangbo Meng , Keda Shi , Huijuan Cao , Xiaoshui Zu , Wenxue Tong , Dick Hokiu Chow , Xinluan Wang , Yuxiao Lai , Ling Qin
Biodegradable magnesium (Mg)-based materials show promise in managing musculoskeletal diseases, attributed to their desired proper mechanical strength, and facilitating self-regenerative processes via spatiotemporal degradation during treatments for non-weight-bearing skeletal sites. However, to achieve a long-term steady state of the local biomechanical environment, it is essential to coupling implant degeneration and neo-tissue ingrowth without sacrificing local mechanical integrity. Steroid-associated osteonecrosis (SAON) presents a formidable clinical challenge, necessitating robust mechanical support to prevent collapse of weight-bearing hip joints while reversing pathological progression. Herein, a novel tree-inspired Mg hybrid column (Mg + BC) incorporating cannulated Mg screw and injectable Mg-containing bone cement (BC) is reported. Mg + BC tuned the gradual release of mineral ions (Mg, Ca, P), OH– and H2 via electrochemical suppression and crystal re-deposition during degradation. Finite element analysis demonstrated that Mg + BC significantly reduced the proportion of relatively high load-bearing regions (CD: 26.0 %, Mg: 26.6 %, BC: 18.2 %, Mg + BC: 17.5 %) and effectively shifted the predominant loading from subchondral trabeculae to the femoral shaft cortex. The efficacy of the tree-inspired Mg hybrid column was validated in a clinically relevant bipedal emu model of SAON. Compared to standalone Mg screws, Mg + BC exhibited sustained degradation and enhanced bone-implant contact, indicating improved alignment between material degradation and tissue regeneration. After 6 months in vivo, the implant residue volume was significantly higher in the Mg + BC group (73.53 ± 10.90 %) compared to the Mg screw group (39.10 ± 11.31 %). The optimized degradation pattern of Mg + BC facilitated bone regeneration through modulation of macrophage recruitment and M1-to-M2 polarization shift. Notably, Mg + BC treatment significantly reduced hip joint collapse incidence (1/10) compared to CD group (7/10). The Mg + BC group maintained greater articular cartilage thickness in the intact region (1.74 ± 0.25 mm) compared to CD group (0.71 ± 0.15 mm). Gait analysis revealed substantial improvement in stride length for the Mg + BC group (87.14 ± 2.29 cm) compared to CD group (60.03 ± 1.31 cm), indicating maintenance of the hip anatomical structure and functional performance. Taken together, the tree-inspired Mg hybrid column is expected to be a unique hybrid system for bone tissue regeneration and prevention of joint collapse in weight-bearing regions affected by SAON, offering promising translational potential for clinical application.
可生物降解的镁（Mg）基材料在治疗肌肉骨骼疾病方面大有可为，因为它们具有理想的适当机械强度，并能在治疗非承重骨骼部位的过程中通过时空降解促进自我再生过程。然而，要实现局部生物力学环境的长期稳定状态，必须在不牺牲局部机械完整性的前提下将植入物退化和新组织生长耦合起来。类固醇相关性骨坏死（SAON）是一项严峻的临床挑战，需要强有力的机械支持来防止负重髋关节的塌陷，同时逆转病理进展。本文报告了一种新型树状镁混合柱（Mg + BC），它结合了插管镁螺钉和可注射的含镁骨水泥（BC）。Mg + BC 可在降解过程中通过电化学抑制和晶体再沉积作用逐步释放矿物质离子（Mg、Ca、P）、OH- 和 H2。有限元分析表明，Mg + BC 显著降低了相对高承重区域的比例（CD：26.0%，Mg：26.6%，BC：18.2%，Mg + BC：17.5%），并有效地将主要承重从软骨下小梁转移到股骨干皮层。在临床相关的 SAON 双足鸸鹋模型中验证了树状镁混合柱的功效。与独立的镁螺钉相比，镁+BC具有持续降解和增强骨与植入物接触的特性，这表明材料降解与组织再生之间的一致性得到了改善。在体内使用 6 个月后，与镁螺钉组（39.10 ± 11.31 %）相比，镁 + BC 组的植入物残留量（73.53 ± 10.90 %）明显更高。镁+BC的优化降解模式通过调节巨噬细胞招募和M1-M2极化转变促进了骨再生。值得注意的是，与 CD 组（7/10）相比，Mg + BC 治疗显著降低了髋关节塌陷发生率（1/10）。与CD组（0.71 ± 0.15 mm）相比，Mg + BC组在完整区域保持了更大的关节软骨厚度（1.74 ± 0.25 mm）。步态分析表明，与 CD 组（60.03 ± 1.31 厘米）相比，Mg + BC 组的步长（87.14 ± 2.29 厘米）有了显著改善，这表明髋关节的解剖结构和功能表现得到了维持。综上所述，受树启发的镁混合柱有望成为一种独特的混合系统，用于骨组织再生和防止受SAON影响的负重区域的关节塌陷，为临床应用提供了广阔的转化潜力。
{"title":"Tree-inspired magnesium hybrid column for preventing hip collapse in steroid-associated osteonecrosis in bipedal emus","authors":"Haiyue Zu , Lizhen Zheng , Mengke Huo , Kevin Liu , Chris Halling Dreyer , Yuantao Zhang , Xuan He , Ye Li , Li Zou , Le Huang , Xueting Yi , Antonia Rujia Sun , Xiangbo Meng , Keda Shi , Huijuan Cao , Xiaoshui Zu , Wenxue Tong , Dick Hokiu Chow , Xinluan Wang , Yuxiao Lai , Ling Qin","doi":"10.1016/j.mattod.2024.08.009","DOIUrl":"10.1016/j.mattod.2024.08.009","url":null,"abstract":"<div><div>Biodegradable magnesium (Mg)-based materials show promise in managing musculoskeletal diseases, attributed to their desired proper mechanical strength, and facilitating self-regenerative processes via spatiotemporal degradation during treatments for non-weight-bearing skeletal sites. However, to achieve a long-term steady state of the local biomechanical environment, it is essential to coupling implant degeneration and neo-tissue ingrowth without sacrificing local mechanical integrity. Steroid-associated osteonecrosis (SAON) presents a formidable clinical challenge, necessitating robust mechanical support to prevent collapse of weight-bearing hip joints while reversing pathological progression. Herein, a novel tree-inspired Mg hybrid column (Mg + BC) incorporating cannulated Mg screw and injectable Mg-containing bone cement (BC) is reported. Mg + BC tuned the gradual release of mineral ions (Mg, Ca, P), OH<sup>–</sup> and H<sub>2</sub> via electrochemical suppression and crystal re-deposition during degradation. Finite element analysis demonstrated that Mg + BC significantly reduced the proportion of relatively high load-bearing regions (CD: 26.0 %, Mg: 26.6 %, BC: 18.2 %, Mg + BC: 17.5 %) and effectively shifted the predominant loading from subchondral trabeculae to the femoral shaft cortex. The efficacy of the tree-inspired Mg hybrid column was validated in a clinically relevant bipedal emu model of SAON. Compared to standalone Mg screws, Mg + BC exhibited sustained degradation and enhanced bone-implant contact, indicating improved alignment between material degradation and tissue regeneration. After 6 months <em>in vivo</em>, the implant residue volume was significantly higher in the Mg + BC group (73.53 ± 10.90 %) compared to the Mg screw group (39.10 ± 11.31 %). The optimized degradation pattern of Mg + BC facilitated bone regeneration through modulation of macrophage recruitment and M1-to-M2 polarization shift. Notably, Mg + BC treatment significantly reduced hip joint collapse incidence (1/10) compared to CD group (7/10). The Mg + BC group maintained greater articular cartilage thickness in the intact region (1.74 ± 0.25 mm) compared to CD group (0.71 ± 0.15 mm). Gait analysis revealed substantial improvement in stride length for the Mg + BC group (87.14 ± 2.29 cm) compared to CD group (60.03 ± 1.31 cm), indicating maintenance of the hip anatomical structure and functional performance. Taken together, the tree-inspired Mg hybrid column is expected to be a unique hybrid system for bone tissue regeneration and prevention of joint collapse in weight-bearing regions affected by SAON, offering promising translational potential for clinical application.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 113-138"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142720924","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Twisted stacking-induced moiré superlattice of two-dimensional (2D) materials have aroused surging interest due to their novel properties and promising applications in quantum technologies. However, problems such as unavoidable interfacial contamination in the prevailing mechanically transferred method, and limited members of 2D materials for constructing twisted homostructures/heterostructures impede the advance of 2D moiré superlattice. Here, bottom-up growth of high-quality bismuth oxychloride twisted homostructures (BiOCl THS) is achieved by a precursor-regulated chemical vapor deposition (CVD) method. In contrast to the conventional screw-dislocation-driven growth of spiral-like nanosheets, the as-prepared BiOCl THSs show a wide range of twist angles and large lateral sizes. A unique secondary twisted nucleation growth mechanism is revealed by multiple characterizations and theoretical calculations. It is demonstrated that the adsorption of polar H2O molecule on BiOCl can lead to a stable nucleation with rotation angles. Furthermore, benefitting from the bottom-up growth of the twisted homostructures, clear moiré patterns and moiré potential induced variation of interlayer coupling and exciton resonances were observed in the BiOCl THS. Our work provides a promising strategy for controllable preparation of high-quality 2D moiré superlattice.
{"title":"Bottom-up growth of high-quality BiOCl twisted homostructures via a precursor regulation strategy","authors":"Pengfei Liu, Li-ping Feng, Xiaodong Zhang, Yulong Yang, Xiaoqi Zheng, Xitong Wang","doi":"10.1016/j.mattod.2024.07.014","DOIUrl":"10.1016/j.mattod.2024.07.014","url":null,"abstract":"<div><div>Twisted stacking-induced moiré superlattice of two-dimensional (2D) materials have aroused surging interest due to their novel properties and promising applications in quantum technologies. However, problems such as unavoidable interfacial contamination in the prevailing mechanically transferred method, and limited members of 2D materials for constructing twisted homostructures/heterostructures impede the advance of 2D moiré superlattice. Here, bottom-up growth of high-quality bismuth oxychloride twisted homostructures (BiOCl THS) is achieved by a precursor-regulated chemical vapor deposition (CVD) method. In contrast to the conventional screw-dislocation-driven growth of spiral-like nanosheets, the as-prepared BiOCl THSs show a wide range of twist angles and large lateral sizes. A unique secondary twisted nucleation growth mechanism is revealed by multiple characterizations and theoretical calculations. It is demonstrated that the adsorption of polar H<sub>2</sub>O molecule on BiOCl can lead to a stable nucleation with rotation angles. Furthermore, benefitting from the bottom-up growth of the twisted homostructures, clear moiré patterns and moiré potential induced variation of interlayer coupling and exciton resonances were observed in the BiOCl THS. Our work provides a promising strategy for controllable preparation of high-quality 2D moiré superlattice.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 40-49"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142720462","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.mattod.2024.09.015
Xinhua Zheng , Ruihao Luo , Zaichun Liu , Mingming Wang , Muhammad Sajid , Zehui Xie , Jifei Sun , Kui Xu , Li Song , Yuan Yuan , Taoli Jiang , Shuang Liu , Na Chen , Wei Chen
The next-generation high-performance batteries for large-scale energy storage should meet the requirements of low cost, high safety, long life and reasonable energy density. Here, we report a practical Ah-level zinc-bromine (Zn-Br2) pouch cell, which operates stably over 3400 h at 100 % depth of discharge and shows an attractive energy density of 76 Wh kg−1. The Zn-Br2 battery is achieved by in-situ electrolyte dynamic stabilizer (EDS) regulation using quaternary ammonium salts on both solid bromine cathode and Zn anode chemistries, whose energy storage mechanisms are comprehensively revealed through in-situ optical microscopy, electrochemical analyses, and simulations. The EDS prevents bromine cathodes from dissolution and diffusion into electrolyte while regulating uniform Zn nucleation and plating through electrostatic shielding. Benefiting from the EDS regulation, the bromine cathode displays a high areal capacity of 40 mAh cm−2 and can stably operate for 1200 cycles at an areal capacity of 15 mAh cm−2. The Zn anode exhibits excellent performance with dendrite-free Zn plating/stripping at a high areal capacity of 100 mAh cm−2 for 400 h and at 10 mAh cm−2 over 1500 h in an anode-free electrode design. The excellent performance of our Zn-Br2 batteries opens up new opportunities for practical large-scale energy storage applications.
用于大规模储能的下一代高性能电池应满足低成本、高安全性、长寿命和合理能量密度的要求。在此，我们报告了一种实用的 Ah 级锌溴 (Zn-Br2) 袋式电池，该电池在 100 % 放电深度下可稳定运行 3400 小时，能量密度高达 76 Wh kg-1。Zn-Br2 电池是通过使用季铵盐对固体溴阴极和锌阳极化学物质进行原位电解质动态稳定剂（EDS）调节实现的，其储能机制通过原位光学显微镜、电化学分析和模拟得到了全面揭示。EDS 可防止溴阴极溶解和扩散到电解液中，同时通过静电屏蔽调节锌的均匀成核和电镀。得益于 EDS 的调节，溴阴极显示出 40 mAh cm-2 的高磁场容量，并能以 15 mAh cm-2 的磁场容量稳定运行 1200 个循环。锌阳极在无树枝状晶粒的锌镀层/剥离下表现出卓越的性能，在无阳极电极设计中，400 小时的高磁通量为 100 mAh cm-2，1500 小时的高磁通量为 10 mAh cm-2。我们的 Zn-Br2 电池的优异性能为实际大规模储能应用提供了新的机遇。
{"title":"A practical zinc-bromine pouch cell enabled by electrolyte dynamic stabilizer","authors":"Xinhua Zheng , Ruihao Luo , Zaichun Liu , Mingming Wang , Muhammad Sajid , Zehui Xie , Jifei Sun , Kui Xu , Li Song , Yuan Yuan , Taoli Jiang , Shuang Liu , Na Chen , Wei Chen","doi":"10.1016/j.mattod.2024.09.015","DOIUrl":"10.1016/j.mattod.2024.09.015","url":null,"abstract":"<div><div>The next-generation high-performance batteries for large-scale energy storage should meet the requirements of low cost, high safety, long life and reasonable energy density. Here, we report a practical Ah-level zinc-bromine (Zn-Br<sub>2</sub>) pouch cell, which operates stably over 3400 h at 100 % depth of discharge and shows an attractive energy density of 76 Wh kg<sup>−1</sup>. The Zn-Br<sub>2</sub> battery is achieved by in-situ electrolyte dynamic stabilizer (EDS) regulation using quaternary ammonium salts on both solid bromine cathode and Zn anode chemistries, whose energy storage mechanisms are comprehensively revealed through in-situ optical microscopy, electrochemical analyses, and simulations. The EDS prevents bromine cathodes from dissolution and diffusion into electrolyte while regulating uniform Zn nucleation and plating through electrostatic shielding. Benefiting from the EDS regulation, the bromine cathode displays a high areal capacity of 40 mAh cm<sup>−2</sup> and can stably operate for 1200 cycles at an areal capacity of 15 mAh cm<sup>−2</sup>. The Zn anode exhibits excellent performance with dendrite-free Zn plating/stripping at a high areal capacity of 100 mAh cm<sup>−2</sup> for 400 h and at 10 mAh cm<sup>−2</sup> over 1500 h in an anode-free electrode design. The excellent performance of our Zn-Br<sub>2</sub> batteries opens up new opportunities for practical large-scale energy storage applications.</div></div>","PeriodicalId":387,"journal":{"name":"Materials Today","volume":"80 ","pages":"Pages 353-364"},"PeriodicalIF":21.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142720918","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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