Advanced Materials最新文献

Clarifying the Active Structure and Reaction Mechanism of Atomically Dispersed Metal and Nonmetal Sites with Enhanced Activity for Oxygen Reduction Reaction

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-24 DOI: 10.1002/adma.202416126

Hui Hu, Jiajun Wang, Kang Liao, Zanyu Chen, Shiyu Zhang, Buwei Sun, Xin Wang, Xixi Ren, Jianguo Lin, Xiaopeng Han

{"title":"Clarifying the Active Structure and Reaction Mechanism of Atomically Dispersed Metal and Nonmetal Sites with Enhanced Activity for Oxygen Reduction Reaction","authors":"Hui Hu, Jiajun Wang, Kang Liao, Zanyu Chen, Shiyu Zhang, Buwei Sun, Xin Wang, Xixi Ren, Jianguo Lin, Xiaopeng Han","doi":"10.1002/adma.202416126","DOIUrl":"https://doi.org/10.1002/adma.202416126","url":null,"abstract":"Atomically dispersed transition metal (ADTM) catalysts are widely implemented in energy conversion reactions, while the similar properties of TMs make it difficult to continuously improve the activity of ADTMs via tuning the composition of metals. Introducing nonmetal sites into ADTMs may help to effectively modulate the electronic structure of metals and significantly improve the activity. However, it is difficult to achieve the co-existence of ADTMs with nonmetal atoms and clarify their synergistic effect on the catalytic mechanism. Therefore, elucidating the active sites within atomically dispersed metal-nonmetal materials and unveiling catalytic mechanism is highly important. Herein, a novel hybrid catalyst, with coexistence of Co single-atoms and Co─Se dual-atom sites (Co─Se/Co/NC), is successfully synthesized and exhibits remarkable performance for oxygen reduction reaction (ORR). Theoretical results demonstrate that the Se sites can effectively modulate the charge redistribution at Co active sites. Furthermore, the synergistic effect between Co single-atom sites and Co─Se dual-atom sites can further adjust the d-band center, optimize the adsorption/desorption behavior of intermediates, and finally accelerate the ORR kinetics. This work has clearly clarified the reaction mechanism and shows the great potential of atomically dispersed metal-nonmetal nanomaterials for energy conversion and storage applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"137 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142880139","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}

引用次数: 0

Rationally Engineering Pro‐Proteins and Membrane‐Penetrating α‑Helical Polypeptides for Genome Editing Toward Choroidal Neovascularization Treatment

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-24 DOI: 10.1002/adma.202412366

Xun Liu, Ziyin Zhao, Wei Li, Mengyao Ren, Haoyu Zhang, Desheng Cao, Yehan Wang, He Yang, Yajie Li, Manhui Zhu, Laiqing Xie, Lichen Yin

{"title":"Rationally Engineering Pro‐Proteins and Membrane‐Penetrating α‑Helical Polypeptides for Genome Editing Toward Choroidal Neovascularization Treatment","authors":"Xun Liu, Ziyin Zhao, Wei Li, Mengyao Ren, Haoyu Zhang, Desheng Cao, Yehan Wang, He Yang, Yajie Li, Manhui Zhu, Laiqing Xie, Lichen Yin","doi":"10.1002/adma.202412366","DOIUrl":"https://doi.org/10.1002/adma.202412366","url":null,"abstract":"Ribonucleoprotein (RNP)‐based CRISPR/Cas9 genome editing holds great potential for the treatment of choroidal neovascularization (CNV), which however, is challenged by the lack of efficient cytosolic protein delivery tools. Herein, reversibly‐phosphorylated pro‐proteins (P‐proteins) with conjugated adenosine triphosphate (ATP) tags are engineered and coupled with a membrane‐penetrating, guanidine‐enriched, α‐helical polypeptide (LGP) to mediate robust and universal cytosolic delivery. LGP forms salt‐stable nanocomplexes (NCs) with P‐proteins via electrostatic interaction and salt bridging, and the helix‐assisted, strong membrane activities of LGP enabled efficient cellular internalization and endolysosomal escape of NCs. Therefore, this approach allows efficient cytosolic delivery of a wide range of protein cargoes and maintains their bioactivities due to endolysosomal acidity‐triggered traceless restoration of P‐proteins. Notably, intravitreally delivered LGP/P‐RNP NCs targeting hypoxia‐inducible factor‐1α (HIF‐1α) induce pronounced gene disruption to downregulate pro‐angiogenic factors and alleviate subretinal fibrosis, ultimately provoking robust therapeutic efficacy in CNV mice. Such a facile and versatile platform provides a powerful tool for cytosolic protein delivery and genome editing, and it holds promising potential for the treatment of CNV‐associated diseases, such as age‐related macular degeneration.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"12 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142880043","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}

引用次数: 0

Ionic Diode-Based Drug Delivery System

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-24 DOI: 10.1002/adma.202412377

Hyunjae Yoo, Soon-Bo Kang, Jeongsoo Kim, Wonkyung Cho, Hyojeong Ha, Seyoung Oh, Seol-Ha Jeong, Sihwan Lee, Hyemin Lee, Chang Seo Park, Dong-yup Lee, Taek Dong Chung, Kyung-Mi Lee, Jeong-Yun Sun

{"title":"Ionic Diode-Based Drug Delivery System","authors":"Hyunjae Yoo, Soon-Bo Kang, Jeongsoo Kim, Wonkyung Cho, Hyojeong Ha, Seyoung Oh, Seol-Ha Jeong, Sihwan Lee, Hyemin Lee, Chang Seo Park, Dong-yup Lee, Taek Dong Chung, Kyung-Mi Lee, Jeong-Yun Sun","doi":"10.1002/adma.202412377","DOIUrl":"https://doi.org/10.1002/adma.202412377","url":null,"abstract":"Drug delivery systems hold promise for delivering cytotoxic drugs by controlling the timing and location of the drug release. However, conventional delivery mechanisms often fall short of achieving spatiotemporally controlled yet sustained release, which is crucial for ensuring drug efficacy and minimizing impact on surrounding tissues. Here, an ionic diode-based drug delivery system is reported that is controlled by an electric potential and capable of releasing drugs at scales ranging from nanogram to microgram. The migrated drug is slowly but continuously diffused to the lesion through the hydrogel at the desired rate. The ionic diode provides flow-free drug delivery while minimizing unintended drug leakage over prolonged periods. Implanted in a freely moving tumor-bearing mouse model, the system filled with doxorubicin demonstrated superior anti-tumor efficacy and minimal off-target immune toxicity compared to the intratumoral injection of free doxorubicin. With its mechanically compliant and biocompatible components, the system offers a safe and readily translatable approach to patients with surgically unresectable tumors.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"42 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142880243","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}

引用次数: 0

Flexible Photonic Materials and Devices: Synthetic Strategies, Sensing Properties, and Wearable Applications

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-24 DOI: 10.1002/adma.202415856

Chunhuan Zhang, Yong Sheng Zhao

引用次数: 0

Self-Wrinkling-Induced Mechanically Adaptive Patterned Surface of Photocuring Coating for Abrasion Resistance

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-24 DOI: 10.1002/adma.202414352

Yi Zhu, Jin Li, Tianjiao Ma, Xiaxin Gao, Kexing Li, Xiaodong Ma, Xuesong Jiang

{"title":"Self-Wrinkling-Induced Mechanically Adaptive Patterned Surface of Photocuring Coating for Abrasion Resistance","authors":"Yi Zhu, Jin Li, Tianjiao Ma, Xiaxin Gao, Kexing Li, Xiaodong Ma, Xuesong Jiang","doi":"10.1002/adma.202414352","DOIUrl":"https://doi.org/10.1002/adma.202414352","url":null,"abstract":"Providing mechanically adaptive performance to surfaces is significant in preserving materials from damage in variable environments, however, it has rarely been studied. Inspired by the mechanically adaptive behaviors of the surface microstructure on the carapace of desert scorpions and bark of desert tamarisks, a self-wrinkled mechanically adaptive patterned surface (SWMAPS) using one-step UV-curing and self-wrinkling technique is reported. Because of the fluorinated polyurethane photo-initiator formed by self-assembly at the top surface, UV-induced photo-crosslinking can spontaneously generate a gradient-crosslinked structure and wrinkled patterns with different morphology. With mechanically adaptive behavior originating from self-assembled fluorinated polyurethane photo-initiators, gradient-crosslinked structures, and self-wrinkled patterns, the SWMAPS remains intact under 600 cycles of reciprocating friction with little variation in the coefficient of friction and water contact angle. The SWMAPS prepared by programmable UV irradiation maintains integral under 1800 cycles of reciprocating friction with a stable friction coefficient. Furthermore, the SWMAPS is fabricated with high efficiency, regulated morphology, good surface mechanical properties, and self-recovery performance. This strategy establishes a new field of mechanically adaptive patterned surfaces, which significantly improves durability and prolongs the service life of materials in variable environments.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"11 12 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142880140","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}

引用次数: 0

In Situ Reconstructed Hydroxyl‐Rich Atomic‐Thin Bi2O2CO3 Enables Ampere‐Scale Synthesis of Formate from CO2 with Activated Water Dissociation

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-23 DOI: 10.1002/adma.202415639

Qizheng Huang, Zhengyi Qian, Na Ye, Yingjun Tan, Menggang Li, Mingchuan Luo, Shaojun Guo

{"title":"In Situ Reconstructed Hydroxyl‐Rich Atomic‐Thin Bi2O2CO3 Enables Ampere‐Scale Synthesis of Formate from CO2 with Activated Water Dissociation","authors":"Qizheng Huang, Zhengyi Qian, Na Ye, Yingjun Tan, Menggang Li, Mingchuan Luo, Shaojun Guo","doi":"10.1002/adma.202415639","DOIUrl":"https://doi.org/10.1002/adma.202415639","url":null,"abstract":"Renewable electricity‐driven CO2 electroreduction provides a promising route toward carbon neutrality and sustainable chemical production. Nevertheless, the viability of this route faces constraints of catalytic efficiency and durability in near‐neutral electrolytes at industrial‐scale current densities, mechanistically originating from unfavorable accommodation of *H species from water dissociation. Herein, a new strategy is reported to accelerate water dissociation by the rich surface hydroxyl on bismuth subcarbonate nanosheets in situ electrochemical transformed from bismuth hydroxide nanotube precursors. This catalyst enables the electrosynthesis of formate at current densities up to 1000 mA cm−2 with >96% faradaic efficiencies in flow cells, and a 200 h durable membrane electrode assembly in a dilute near‐neutral environment. Combined kinetic studies, in situ characterizations, and theoretical calculations reveal that the atomic thickness strengthens the hydroxyl adsorption, and with a highly localized electron configuration, the hydroxyl‐functionalized surface is more affinitive to oxygenated species, thus lowering the barrier for water dissociation and the crucial hydrogenation step in the proton‐coupled electron transfer from *OCHO to *HCOOH.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"3 131 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874226","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}

引用次数: 0

STING‐Activating Polymers Boost Lymphatic Delivery of mRNA Vaccine to Potentiate Cancer Immunotherapy

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-23 DOI: 10.1002/adma.202412654

Miao Zhang, Yongling Wang, Benhao Li, Bowei Yang, Mengyao Zhao, Bingyu Li, Jianping Liu, Yaxin Hu, Zhaoming Wu, Yenhui Ong, Xiaolin Han, Lingwen Ding, Kongfu Zhu, Jianwei Li, Min Luo, Shengqi Chen, Ling Peng, Longjiang Zhang, Xiaoyuan Chen, Qianqian Ni

{"title":"STING‐Activating Polymers Boost Lymphatic Delivery of mRNA Vaccine to Potentiate Cancer Immunotherapy","authors":"Miao Zhang, Yongling Wang, Benhao Li, Bowei Yang, Mengyao Zhao, Bingyu Li, Jianping Liu, Yaxin Hu, Zhaoming Wu, Yenhui Ong, Xiaolin Han, Lingwen Ding, Kongfu Zhu, Jianwei Li, Min Luo, Shengqi Chen, Ling Peng, Longjiang Zhang, Xiaoyuan Chen, Qianqian Ni","doi":"10.1002/adma.202412654","DOIUrl":"https://doi.org/10.1002/adma.202412654","url":null,"abstract":"The unprecedented success of mRNA vaccines against COVID‐19 has inspired scientists to develop mRNA vaccines for cancer immunotherapy. However, using nucleoside modified mRNA as vaccine, though evading innate immune toxicity, diminishes its therapeutic efficacy for cancers. Here, we report a polyvalent stimulator of interferon genes (STING) activating polymer (termed as PD) to bolster the immunogenicity of mRNA vaccine. PD is made of tertiary amine units and conjugated with a biodegradable alkyl chain. Co‐formulation of PDs bearing different number of tertiary amines with lipid materials and mRNA resulted in the lipid‐like nanoparticles (PD LNPs) which effectively promoted lymphatic delivery and elicited robust immune activation via the STING signaling pathway. Notably, PD with eighteen tertiary amines (PD18) is predominant in balancing immune activity and tolerability. Subcutaneous administration of PD18 LNPs containing ovalbumin (OVA) mRNA enhanced the frequency of antigen specific CD8+ T cell with immune memory, leading to potent anticancer efficacy that surpassed 2′3’‐cGAMP in both prophylactic and therapeutic cancer models. Additionally, PD18 LNP‐based mRNA vaccine showed conferred resistance to cancer challenge for up to 60 days. Overall, this study offers a new perspective of using STING‐ activating polymer for imparting synergistic activity in mRNA vaccine‐based cancer immunotherapy.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"23 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874231","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}

引用次数: 0

Self-Assembled Metal Complexes in Biomedical Research

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-23 DOI: 10.1002/adma.202416122

Wenting Wang, Yang Xu, Yuqi Tang, Quan Li

引用次数: 0

Renal Clearable Chiral Manganese Oxide Supraparticles for In Vivo Detection of Metalloproteinase‐9 in Early Cancer Diagnosis

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-23 DOI: 10.1002/adma.202415656

Hongyu Zhang, Panpan Chen, Wenxiong Shi, Aihua Qu, Maozhong Sun, Hua Kuang

{"title":"Renal Clearable Chiral Manganese Oxide Supraparticles for In Vivo Detection of Metalloproteinase‐9 in Early Cancer Diagnosis","authors":"Hongyu Zhang, Panpan Chen, Wenxiong Shi, Aihua Qu, Maozhong Sun, Hua Kuang","doi":"10.1002/adma.202415656","DOIUrl":"https://doi.org/10.1002/adma.202415656","url":null,"abstract":"In this study, polypeptide TGGGPLGVARGKGGC‐induced chiral manganese dioxide supraparticles (MnO2 SPs) are prepared for sensitive quantification of matrix metalloproteinase‐9 (MMP‐9) in vitro and in vivo. The results show that L‐type manganese dioxide supraparticles (L‐MnO2 SPs) exhibited twice the affinity for the cancer cell membrane receptor CD47 (cluster of differentiation, integrin‐associated protein) than D‐type manganese dioxide supraparticles (D‐MnO2 SPs) to accumulate at the tumor site after surface modification of the internalizing arginine‐glycine‐aspartic acid (iRGD) ligand, specifically reacting with the MMP‐9, disassembling into ultrasmall nanoparticles (NPs), and efficiently underwent renal clearance. Furthermore, L‐MnO2 facilitates the quantification of MMP‐9 in mouse tumor xenografts, as demonstrated by circular dichroism (CD) and magnetic resonance imaging (MRI) within 2 h. A strong linear relationship is observed between MMP‐9 concentration and both CD and MRI intensity, ranging from 0.01 to 10 ng mL−1. The corresponding limits of detection (LOD) are 0.0054 ng mL−1 for CD and 0.0062 ng mL−1 for MRI, respectively. hese SPs provide a new approach for exploring chiral advanced biosensors for early diagnosis of cancer.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"111 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874236","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}

引用次数: 0

HClO-Activated Near-Infrared Chemiluminescent Probes with a Malononitrile Group for In-Vivo Imaging

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2024-12-23 DOI: 10.1002/adma.202408941

Yalei Cao, Juqing Gu, Zhijian Chen, Jucai Gao, Jie Yang, Wenbo Wu, Manman Fang, Qianqian Li, Bin Liu, Zhen Li

{"title":"HClO-Activated Near-Infrared Chemiluminescent Probes with a Malononitrile Group for In-Vivo Imaging","authors":"Yalei Cao, Juqing Gu, Zhijian Chen, Jucai Gao, Jie Yang, Wenbo Wu, Manman Fang, Qianqian Li, Bin Liu, Zhen Li","doi":"10.1002/adma.202408941","DOIUrl":"https://doi.org/10.1002/adma.202408941","url":null,"abstract":"Chemiluminescence (CL) imaging has emerged as a powerful approach to molecular imaging that allows exceptional sensitivity with virtually no background interference because of its unique capacity to emit photons without an external excitation source. Despite its high potential, the application of this nascent technique faces challenges because the current chemiluminescent agents have limited reactive sites, require complex synthesis, are insufficiently bright, and lack near-infrared emission. Herein, a series of HClO-activated chemiluminescent probes that exhibit robust near-infrared emission are studied. Specifically engineered to respond to HClO, a known biomarker of acute inflammation, these probes achieve high-contrast in vivo imaging by eliminating the need for constant external excitation. Comprehensive experimental and theoretical investigations demonstrate that the CL of the probes depends on the reactivity of the vinylene bonds, following a concerted decomposition of the oxidized chemiluminescent molecule. The application of these chemiluminescent nanoparticles in vivo facilitates high-contrast imaging of acute inflammation, providing real-time, high-contrast visualization of inflammatory conditions. This advancement signifies a leap forward for chemiluminescent nanoplatforms in biomedical imaging and expands the available methodologies in this field.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"17 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874374","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}

引用次数: 0