Advanced Materials最新文献_第8页

Narrow-Linewidth Emission and Weak Exciton-Phonon Coupling in 2D Layered Germanium Halide Perovskites 二维层状卤化锗钙钛矿的窄线宽发射和弱激子-声子耦合

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-28 DOI: 10.1002/adma.202419879

Zachary A. VanOrman, Benjamin Savinson, Tejas Deshpande, Isaiah W. Gilley, Rosario Scopelliti, Antti-Pekka M. Reponen, Mercouri G. Kanatzidis, Edward H. Sargent, Oleksandr Voznyy, Sascha Feldmann

{"title":"Narrow-Linewidth Emission and Weak Exciton-Phonon Coupling in 2D Layered Germanium Halide Perovskites","authors":"Zachary A. VanOrman, Benjamin Savinson, Tejas Deshpande, Isaiah W. Gilley, Rosario Scopelliti, Antti-Pekka M. Reponen, Mercouri G. Kanatzidis, Edward H. Sargent, Oleksandr Voznyy, Sascha Feldmann","doi":"10.1002/adma.202419879","DOIUrl":"https://doi.org/10.1002/adma.202419879","url":null,"abstract":"The photophysical properties of low-dimensional metal-halide semiconductors and their tunability make them promising candidates for light-absorbing and emitting applications. Yet, the germanium-based halide perovskites to date lack desirable light-emitting properties, with so far only very broad, weak, and unstructured photoluminescence (PL) reported due to significant octahedral distortion. Here, the photophysical properties of the 2D layered Ruddlesden-Popper semiconductors (4F-PMA)2GeI4 and (4F-PMA)2PbI4 (4F-PMA: 4-F-phenylmethylammonium) are characterized and compared. Using a combination of single-crystal X-ray diffraction, variable temperature time-resolved PL, and density functional theory, structure-property relations are correlated. Specifically, the results indicate that (4F-PMA)2PbI4 features stronger coupling to longitudinal optical (LO) phonons, assisting emission from a broad bound-exciton state due to a soft, deformable lattice. In contrast, (4F-PMA)2GeI4, benefitting from intermolecular bonding to scaffold a rigid octahedral structure, shows weaker LO-phonon coupling, resulting in the longest PL lifetime and most narrow linewidth (≈120 meV linewidth at 2 K) reported for a Ge-halide perovskite yet, without the occurrence of any additional bound-state emission at low temperatures. These results highlight the potential of germanium halide perovskite materials for optoelectronic applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"42 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143880298","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

Dual-Scale Hydration-Induced Electrical and Mechanical Torsional Energy Harvesting in Heterophilically Designed CNT Yarns 异亲性设计碳纳米管纱线双尺度水化诱导的机电扭能收集

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-28 DOI: 10.1002/adma.202501111

Jae Myeong Lee, Wonkyeong Son, Myoungeun Oh, Duri Han, Hyunji Seo, Hyeon Jun Sim, Shi Hyeong Kim, Dong-Myeong Shin, Chang-Seok Kim, Seon Jeong Kim, Changsoon Choi

{"title":"Dual-Scale Hydration-Induced Electrical and Mechanical Torsional Energy Harvesting in Heterophilically Designed CNT Yarns","authors":"Jae Myeong Lee, Wonkyeong Son, Myoungeun Oh, Duri Han, Hyunji Seo, Hyeon Jun Sim, Shi Hyeong Kim, Dong-Myeong Shin, Chang-Seok Kim, Seon Jeong Kim, Changsoon Choi","doi":"10.1002/adma.202501111","DOIUrl":"https://doi.org/10.1002/adma.202501111","url":null,"abstract":"Water holds vast potential for a useful energy source, yet traditional approaches capture only a fraction of it. This study introduces a heterophilically designed carbon nanotube (CNT) yarn with an asymmetric configuration. This yarn is capable of both electrical and mechanical torsional energy harvesting through dual-scale hydration. Fabricated via half-electrochemical oxidation, the yarn contains a hydrophilic region enriched with oxygen-containing functional groups and a hydrophobic pristine CNT region. Molecular-scale hydration triggers proton release in the hydrophilic region. Consequently, a concentration gradient is established that generates a peak open-circuit voltage of 106.0 mV and a short-circuit current of 20.6 mA cm−2. Simultaneously, microscale hydration induces water absorption into inter-bundle microchannels, resulting in considerable yarn volume expansion. This process leads to hydro-driven actuation with a torsional stroke of 78.8° mm−1 and a maximum rotational speed of 1012 RPM. The presented simultaneous harvesting results in electrical and mechanical power densities of 3.5 mW m−2 and 34.3 W kg−1, respectively, during a hydration cycle. By integrating molecular and microscale hydrations, the proposed heterophilic CNT yarns establish an unprecedented platform for simultaneous electrical and mechanical energy harvesting from water, representing a groundbreaking development for sustainable applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"91 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143880250","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

Luminescent Liquid Crystalline Elastomer Promoted Self-Adaptive Smart Active Optical Waveguide with Ultra-Low Optical Loss 发光液晶弹性体推进的超低光损耗自适应智能有源光波导

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-28 DOI: 10.1002/adma.202504256

Tian-Tian Hao, Yan Guan, Akhila Joy, Jie Li, Wei Xia, Yi Chen, Qi Lin, Xiao Li, Zhi-Wang Luo, Pengfei Duan, Er-Qiang Chen, He-Lou Xie

{"title":"Luminescent Liquid Crystalline Elastomer Promoted Self-Adaptive Smart Active Optical Waveguide with Ultra-Low Optical Loss","authors":"Tian-Tian Hao, Yan Guan, Akhila Joy, Jie Li, Wei Xia, Yi Chen, Qi Lin, Xiao Li, Zhi-Wang Luo, Pengfei Duan, Er-Qiang Chen, He-Lou Xie","doi":"10.1002/adma.202504256","DOIUrl":"https://doi.org/10.1002/adma.202504256","url":null,"abstract":"Currently, optical waveguides show extensive application in photonics and optoelectronic devices due to their high information capacity and transmission capabilities. However, developing self-adaptive, smart optical waveguide materials with ultra-low optical loss remains a significant challenge. To address this issue, luminescent liquid crystalline elastomers (LLCEs) with remarkable flexibility and minimal optical loss through one-pot synthetic method is synthesized, marking the first example of such an approach. The resultant organic optical waveguide materials (OOWMs) demonstrate exceptional mechanical performance and low optical loss, even under significant deformation. An optical loss coefficient of 0.0375 dB mm−1 has been achieved in LLCE-based OOWMs through synergistic Förster resonance energy transfer. Additionally, these flexible OOWMs can endure large deformations and be shaped into arbitrary forms within macro-scale dimensions. Notably, LLCE-based OOWMs demonstrate smart, self-adaptive behavior with ultra-low optical loss when exposed to heat or light. Consequently, these OOWMs can be used to fabricate photo switches of various shapes. This work provides a feasible approach to achieving integrated photonic systems with low optical loss for intelligent high-speed data transmission.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"42 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143880253","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

Material Selection and Device Design of Scalable Flexible Brain-Computer Interfaces: A Balance Between Electrical and Mechanical Performance 可扩展柔性脑机接口的材料选择和器件设计：电气和机械性能之间的平衡

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-28 DOI: 10.1002/adma.202413938

Xinyi Lin, Xuyue Zhang, Juntao Chen, Jia Liu

{"title":"Material Selection and Device Design of Scalable Flexible Brain-Computer Interfaces: A Balance Between Electrical and Mechanical Performance","authors":"Xinyi Lin, Xuyue Zhang, Juntao Chen, Jia Liu","doi":"10.1002/adma.202413938","DOIUrl":"https://doi.org/10.1002/adma.202413938","url":null,"abstract":"Brain-computer interfaces (BCIs) hold the potential to revolutionize brain function restoration, enhance human capability, and advance our understanding of cognitive mechanisms by directly linking neural signals with hardware. However, the mechanical mismatch between conventional rigid BCIs and soft brain tissue limits long-term interface stability. Next-generation BCIs must achieve long-term biocompatibility while maintaining high performance, enabling the integration of millions of sensors within tissue-level flexible and soft, stable neural interfaces. Lithographic fabrication techniques provide scalable thin-film flexible electronics, but traditional electronic materials often fail to meet the unique requirements of BCIs. This review examines the selection of materials and device design for flexible BCIs, starting with an analysis of intrinsic material properties—Young's modulus, electrical conductivity and dielectric constant. It then explores the integration of material selection with electrode design to optimize electrical circuits and assess key mechanical factors. Next, the correlation between electrical and mechanical performance is analyzed to guide material selection and device design. Finally, recent advances in neural probes are reviewed, highlighting improvements in signal quality, recording stability, and scalability. This review focuses on scalable, lithography-based BCIs, aiming to identify optimal materials and designs for long-term, reliable neural recordings.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"33 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143880254","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

eg Electron Occupancy as a Descriptor for Designing Iron Single-Atom Electrocatalysts 电子占位作为设计铁单原子电催化剂的描述符

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-28 DOI: 10.1002/adma.202504852

Chun Pei, Guohua Yao, Ziguang Zhao, Yafei Sun, Qin Wang, Tongxin Shang, Ying Wan

引用次数: 0

Microbial Photosynthetic Oxygenation and Radiotherapeutic Sensitization Enables Pyroptosis Induction for Combinatorial Cancer Therapy 微生物光合氧化和放射治疗致敏使热亡诱导联合癌症治疗

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-26 DOI: 10.1002/adma.202503138

Tianyu Li, Ya Zhang, Cong Li, Yanwei Song, Tiaoyan Jiang, Yipengchen Yin, Meiqi Chang, Xinran Song, Xiaojun Zheng, Wenqing Zhang, Zhongdan Yu, Wei Feng, Qin Zhang, Li Ding, Yu Chen, Sheng Wang

{"title":"Microbial Photosynthetic Oxygenation and Radiotherapeutic Sensitization Enables Pyroptosis Induction for Combinatorial Cancer Therapy","authors":"Tianyu Li, Ya Zhang, Cong Li, Yanwei Song, Tiaoyan Jiang, Yipengchen Yin, Meiqi Chang, Xinran Song, Xiaojun Zheng, Wenqing Zhang, Zhongdan Yu, Wei Feng, Qin Zhang, Li Ding, Yu Chen, Sheng Wang","doi":"10.1002/adma.202503138","DOIUrl":"https://doi.org/10.1002/adma.202503138","url":null,"abstract":"Rectal cancer surgery is challenging due to the complex anatomy, making it difficult to achieve clear surgical margins. Radiotherapy (RT) plays a crucial role, especially in treating locally recurrent rectal cancer and preserving anal function. However, its effectiveness is often limited by tumor hypoxia, particularly prevalent in hypoxic regions near the bowel wall in colorectal cancer. Hypoxia contributes to both radiation resistance and apoptosis resistance, compromising RT outcomes. To overcome hypoxia‐driven radiotherapy resistance, this work designs and engineers a radiotherapy‐sensitizing bioplatform for efficient cancer RT. It combines lanthanum oxide nanoparticles (La2O3 NPs) with cyanobacteria, which produces oxygen through photosynthesis. This bioplatform uniquely reduces tumor hypoxia, enhances radiation deposition, and improves RT efficacy. La2O3 NPs further enhance reactive oxygen species (ROS) production induced by radiation, triggering pyroptosis via the ROS‐NLRP3‐GSDMD pathway, while RT amplifies pyroptosis through GSDME, circumventing tumor apoptosis resistance. The further integrated thermosensitive hydrogels ensure precise localization of the bioplatform, reducing systemic toxicity and improving therapeutic specificity. Compared to conventional therapies, this dual‐action system addresses hypoxia, RT resistance, and apoptosis resistance more effectively. In vivo and in vitro hypoxia models validate its potent anti‐tumor efficacy, offering valuable insights for refining clinical treatment paradigms.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"130 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875843","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

Screening Natural Cholesterol Analogs to Assemble Self‐Adjuvant Lipid Nanoparticles for Antigens Tagging Guided Therapeutic Tumor Vaccine 筛选天然胆固醇类似物组装自佐剂脂质纳米颗粒用于抗原标记引导治疗性肿瘤疫苗

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-26 DOI: 10.1002/adma.202419182

Shuang Liang, Shuying Gao, Shunli Fu, Shijun Yuan, Jinhu Liu, Man Liang, Leiqiang Han, Zipeng Zhang, Yongjun Liu, Na Zhang

{"title":"Screening Natural Cholesterol Analogs to Assemble Self‐Adjuvant Lipid Nanoparticles for Antigens Tagging Guided Therapeutic Tumor Vaccine","authors":"Shuang Liang, Shuying Gao, Shunli Fu, Shijun Yuan, Jinhu Liu, Man Liang, Leiqiang Han, Zipeng Zhang, Yongjun Liu, Na Zhang","doi":"10.1002/adma.202419182","DOIUrl":"https://doi.org/10.1002/adma.202419182","url":null,"abstract":"The clinical progress of tumor nucleotide vaccines is limited due to insufficient recognition and killing of tumor cells with low antigen expression by cytotoxic T lymphocytes (CTL). Here, natural cholesterol analogs are screened to assemble self‐adjuvant lipid nanoparticles (LNPs) for antigens tagging tumor cells and dendritic cells (DC) activation. First, a library of ginsenosides are collected, and then screened according to their anti‐tumor immunity. Then, ginsenoside‐Rg3 based‐LNPs loaded with antigens (Rg3‐LNPs) are identified as the optimal formulation by investigating the physicochemical and biological properties. Finally, Rg3‐LNPs and granulocyte‐macrophage colony‐stimulating factor (GM‐CSF) are co‐loaded into a macroporous hydrogel for long‐term immune response. Rg3‐LNPs could accumulate into both tumors and LNs. Rg3‐LNPs targeted tumor cells with high glucose transporter‐1 expression via the targeting ligand Rg3, and anchored antigens on the tumor cell surface, thus promoting the recognition of CTL to tumor cells; Rg3‐LNPs can accumulate into the LNs to promote DC activation and antigen presentation, thus stimulating CTL activation. Besides, Rg3, as an adjuvant, cooperated with GM‐CSF to remodel the tumor microenvironment, thus promoting the killing of CTL to tumor cells. Collectively, this work highlights the importance of tagging antigens to tumor cells in tumor vaccine and has great clinical value for immune‐escaping tumors.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"4 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876117","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

Biomimetic Dynamics of Nanoscale Groove and Ridge Topography for Stem Cell Regulation 用于干细胞调控的纳米级槽脊形貌的仿生动力学原理

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-26 DOI: 10.1002/adma.202419416

Hyunsik Hong, Dahee Kim, Hwapyung Jung, Seongyeol Kim, Sunhong Min, Chowon Kim, Kanghyeon Kim, Hyunji Rha, Heemin Kang

{"title":"Biomimetic Dynamics of Nanoscale Groove and Ridge Topography for Stem Cell Regulation","authors":"Hyunsik Hong, Dahee Kim, Hwapyung Jung, Seongyeol Kim, Sunhong Min, Chowon Kim, Kanghyeon Kim, Hyunji Rha, Heemin Kang","doi":"10.1002/adma.202419416","DOIUrl":"https://doi.org/10.1002/adma.202419416","url":null,"abstract":"Native extracellular matrix exhibits multiscale groove and ridge structures that continuously change, such as collagen fibril‐based nanogrooves in bone tissue, and regulate cellular responses. However, dynamic switching between groove and ridge nanostructures at the molecular level has not been demonstrated. Herein, materials capable of dynamic groove‐ridge switching at tens‐of‐nanometers scale are developed by flexibly conjugating RGD‐magnetically activatable nanoridges (MANs) to non‐magnetic nanogrooves with independently tuned widths comparable to the sizes of integrin‐presenting filopodia by modulating hydrophobicity in bicontinuous microemulsion, allowing for cyclic modulation of RGD accessibility and cellular adhesion. Nanogrooves with medium width restrict RGD accessibility in the “groove” state in which the RGD‐MANs are buried, which is reversed by magnetically raising them to protrude and form the “ridge” state that fully exposes the RGDs. This reversibly stimulates integrin recruitment, focal adhesion complex assembly, mechanotransduction, and differentiation of stem cells in vivo. This is the first demonstration of molecular‐level groove and ridge nanostructures that exhibit unprecedented switchability between groove and ridge nanostructures. Versatile tuning of the width, height, pitch, and shape of intricate nanogroove structures with remote manipulability can enlighten the understanding of molecular‐scale cell–ligand interactions for stem cell engineering‐based treatment of aging, injuries, and stress‐related diseases.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"41 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876119","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

Hybrid Additive Manufacturing of Shear‐Stiffening Elastomer Composites for Enhanced Mechanical Properties and Intelligent Wearable Applications 用于增强机械性能和智能可穿戴应用的剪切增强弹性体复合材料的混合增材制造

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-26 DOI: 10.1002/adma.202419096

Junjie Yang, Chunyu Zhao, Shuyu Lai, Dongpeng Wang, Xinglong Gong

{"title":"Hybrid Additive Manufacturing of Shear‐Stiffening Elastomer Composites for Enhanced Mechanical Properties and Intelligent Wearable Applications","authors":"Junjie Yang, Chunyu Zhao, Shuyu Lai, Dongpeng Wang, Xinglong Gong","doi":"10.1002/adma.202419096","DOIUrl":"https://doi.org/10.1002/adma.202419096","url":null,"abstract":"Shear‐stiffening materials, renowned for their rate‐dependent behavior, hold immense potential for impact‐resistant applications but are often constrained by limited load‐bearing capacity under extreme conditions. In this study, a novel hybrid additive manufacturing strategy that successfully achieves anisotropic structural design of shear‐stiffening materials is proposed. In this strategy, fused deposition modeling (FDM) is synergistically combined with direct ink writing (DIW) to fabricate lattice‐structured soft‐hard phase elastomer composites (TPR‐SSE composites) with enhanced mechanical properties. Through quasistatic characterization and dynamic impact experiments, complemented by noncontact optical measurement and finite element simulation, the mechanical enhancement mechanisms imparted by the lattice architecture are systematically uncovered. The resulting composites exhibit exceptional load‐bearing capacity under quasistatic conditions and superior energy dissipation under dynamic impacts, making them ideal for advanced protective systems. Building on this, smart sports shoes featuring a deep‐learning‐based smart sensing module that integrates structural customizability, buffering capacity, and gait recognition, are developed. This work provides a transformative structure design approach to shear‐stiffening materials systems, paving the way for next‐generation intelligent wearable protection applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"48 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876116","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

Rational Ligand Design of Conjugated Coordination Polymers for Efficient and Selective Nitrate Electroreduction to Ammonia 合理配体设计共轭配位聚合物，实现高效和选择性硝酸盐电还原成氨气

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-04-26 DOI: 10.1002/adma.202418681

Shouhan Zhang, Yan Liu, Yidan Ding, Hangjuan Wu, Li Qing, Jiexin Zhu, Shenghua Chen, Ziyun Wang, Longsheng Zhang, Tianxi Liu

{"title":"Rational Ligand Design of Conjugated Coordination Polymers for Efficient and Selective Nitrate Electroreduction to Ammonia","authors":"Shouhan Zhang, Yan Liu, Yidan Ding, Hangjuan Wu, Li Qing, Jiexin Zhu, Shenghua Chen, Ziyun Wang, Longsheng Zhang, Tianxi Liu","doi":"10.1002/adma.202418681","DOIUrl":"https://doi.org/10.1002/adma.202418681","url":null,"abstract":"Electrocatalytic nitrate reduction to ammonia (NRA) offers an attractive route for converting nitrate pollutants to ammonia under mild conditions. Among other catalysts, single‐atom catalysts (SACs) with high metal‐atom‐utilization efficiency and low‐coordinated metal sites hold immense potential to be extensively applied, which unfortunately encounter a formidable challenge to obtain simultaneous improvement of NRA activity and selectivity. Here, a novel and general strategy is reported to achieve efficient and selective NRA catalysis on conjugated coordination polymers featuring with high‐density and well‐defined nitrogen (N)‐coordinated single‐atom metal sites via precise regulation of N‑heterocyclic ligands toward accelerating the hydrogenation kinetics necessitated in the NRA pathway. Taking cobalt (Co) as an example, two CoN4‐centered conjugated coordination polymer electrocatalysts (CoN4‐pyrr and CoN4‐pyri) are synthesized with pyrrole and pyridine ligands are investigated as a proof‐of‐concept study. As revealed, the CoN4‐pyrr can markedly outperform the CoN4‐pyri toward NRA electrocatalysis. Experimental and theoretical results suggest that, relative to the N atoms of pyridine ligand in CoN4‐pyri, the N atoms of pyrrole ligand in CoN4‐pyrr can enable a faster transfer of hydrogen radicals to the Co active sites for accelerating the hydrogenation kinetics of *NO intermediate at the rate‐determining step of NRA pathway.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"1 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876120","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