Advanced Materials最新文献_第3页

Engineering Flow-Through Hollow Fiber Gas-Diffusion Electrodes for Unlocking High-Rate Gas-Phase Electrochemical Conversion 工程流经中空纤维气体扩散电极解锁高速率气相电化学转化

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202420391

Guoliang Chen, Hesamoddin Rabiee, Mengran Li, Beibei Ma, Yizhu Kuang, Fatereh Dorosti, Zhonghua Zhu, Hao Wang, Lei Ge

{"title":"Engineering Flow-Through Hollow Fiber Gas-Diffusion Electrodes for Unlocking High-Rate Gas-Phase Electrochemical Conversion","authors":"Guoliang Chen, Hesamoddin Rabiee, Mengran Li, Beibei Ma, Yizhu Kuang, Fatereh Dorosti, Zhonghua Zhu, Hao Wang, Lei Ge","doi":"10.1002/adma.202420391","DOIUrl":"https://doi.org/10.1002/adma.202420391","url":null,"abstract":"Designing advanced electrodes with efficient contact with gas, electrolytes, and catalysts presents significant opportunities to enhance the accessibility of concentrated gas molecules to the catalytic sites while mitigating undesirable side reactions such as the hydrogen evolution reaction (HER), which advances the gas-phase electrochemical reduction toward industrial-scale applications. Traditional planar electrodes face challenges, including limited gas solubility and restricted mass transport. Although commercial flow-by gas-diffusion electrodes can reduce mass transfer resistance by enabling direct diffusion of gas molecules to active sites, the reliance on diffusive gas flow becomes insufficient to meet the rapid consumption demands of gas reactants at high current density. Flow-through hollow fiber gas-diffusion electrodes (HFGDEs) or hollow fiber gas penetration electrodes (HFGPEs) provide a promising solution by continuously delivering convective gas flow to active sites, resulting in enhanced mass transport and superior gas accessibility near the catalytic sites. Notably, HFGDEs have demonstrated the ability to achieve current densities exceeding multiple amperes per square centimeter in liquid electrolytes. This review provides a comprehensive overview of the design criteria, fabrication methods, and design strategies for porous metallic HFGDEs. It highlights the state-of-the-art advancements in HFGDEs composed of various metals (e.g., Cu, Ni, Ag, Bi, Ti, and Zn), with a particular focus on their utilization in the electrochemical conversion of CO2. Finally, future research directions are discussed, underscoring the potential of porous metallic HFGDEs as a versatile and scalable electrode architecture for diverse electrochemical applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"139 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910590","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

Active Hydrogen Enrichment on Cu6Sn5-type High Entropy Intermetallics for Efficient Nitrate Reduction Reaction cu6sn5型高熵金属间化合物的富氢高效硝酸还原反应

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202501886

Ziwei Xiang, Ying-Rui Lu, Linghu Meng, Jiao Lan, Feng Xie, Shanqiang Gao, Jilong Li, Min Luo, Ming Peng, Yongwen Tan

{"title":"Active Hydrogen Enrichment on Cu6Sn5-type High Entropy Intermetallics for Efficient Nitrate Reduction Reaction","authors":"Ziwei Xiang, Ying-Rui Lu, Linghu Meng, Jiao Lan, Feng Xie, Shanqiang Gao, Jilong Li, Min Luo, Ming Peng, Yongwen Tan","doi":"10.1002/adma.202501886","DOIUrl":"https://doi.org/10.1002/adma.202501886","url":null,"abstract":"Electrocatalytic nitrate reduction reaction (NO3RR) provides a feasible strategy for green ammonia production and the treatment of nitrate pollution in wastewater. The generation of active hydrogen (H*) plays an important role in improving the selectivity, yield rate, and Faradaic efficiency of ammonia products. Here, structurally ordered nanoporous Cu6Sn5-type high entropy intermetallics (HEI) with extremely superior performance toward NO3RR is demonstrated. The optimal nanoporous (Cu0.25Ni0.25Fe0.25Co0.25)6Sn5 HEI delivers a high NH3 Faradaic efficiency of 97.09 ± 1.15% and excellent stability of 120 h at the industrial level current density of 1 A cm−2, accordingly directly converting NO3‒ to high-purity (NH4)2HPO4 with near-unity efficiency. Theoretical calculations combined with experimental results reveal that the ordered multi-site nature of the nanoporous HEI can simultaneously promote water dissociation, reduce the reaction-free energy of the hydrogenation process, and suppress hydrogen evolution. This work provides the design of the precious-metal-free HEI for sustainable NH3 synthesis and paves insights into the H* enrichment mechanism.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"24 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910591","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

Understanding Multi-Stage Charge Storage on Nanoporous Carbons in Zn-Ion Hybrid Capacitors 锌离子杂化电容器中纳米孔碳的多级电荷存储研究

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202502422

Jiaxin Li, Kangkang Ge, Anastatios Orestis Grammenos, Pierre-Louis Taberna, Patrice Simon, Markus Antonietti, Mateusz Odziomek

{"title":"Understanding Multi-Stage Charge Storage on Nanoporous Carbons in Zn-Ion Hybrid Capacitors","authors":"Jiaxin Li, Kangkang Ge, Anastatios Orestis Grammenos, Pierre-Louis Taberna, Patrice Simon, Markus Antonietti, Mateusz Odziomek","doi":"10.1002/adma.202502422","DOIUrl":"https://doi.org/10.1002/adma.202502422","url":null,"abstract":"Zn-ion hybrid capacitors (ZIHCs) are promising high-power energy storage devices. However, the underlying charge storage mechanisms, especially the influence of proton storage, remain poorly understood. Herein, the model porous carbons are synthesized having similar specific surface areas (SSAs) and surface chemistry but different pore sizes. They highlight the role of supermicropores and small mesopores (0.86–4 nm) enabling a high capacity of 198 mAh g−1 (capacitance of 446 F g−1), while larger mesopores (4–13 nm) significantly enhance cycling stability, exceeding 0.6 million cycles. Electrochemical studies, including EQCM analysis, reveal a 4-stage charge-storage process under cathodic polarization, comprising adsorption and desolvation of hydrated Zn2+ ions, followed by water reduction, catalyzed by Zn2+, and formation of Had. The rising pH leads to the formation of insoluble zinc hydroxysulfate hydrates (ZHS). Depending on the pore architecture, the precipitation of ZHS has different effects on the overall stability of cycling. The study overall: (i) presents a simplified method for pore control in carbon synthesis; (ii) discuss the effect of pore size on charge storage and cycling stability in respect of ZHS formation; (iii) sheds light on the charge storage mechanism indicating the important contribution of cation effect known from electrocatalysis on faradaic charge storage mechanism.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"139 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910657","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

Reconstruction of the Buried Interface of Triple-Halide Wide-Bandgap Perovskite for All-Perovskite Tandems 全钙钛矿串联中三卤化物宽禁带钙钛矿埋藏界面的重建

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202502450

Chen Wang, Guang Li, Hongsen Cui, Yansong Ge, Shiqiang Fu, Hongling Guan, Shun Zhou, Xuzhi Hu, Wenlong Shao, Peng Jia, Guoyi Chen, Shengjie Du, Weijun Ke, Guojia Fang

{"title":"Reconstruction of the Buried Interface of Triple-Halide Wide-Bandgap Perovskite for All-Perovskite Tandems","authors":"Chen Wang, Guang Li, Hongsen Cui, Yansong Ge, Shiqiang Fu, Hongling Guan, Shun Zhou, Xuzhi Hu, Wenlong Shao, Peng Jia, Guoyi Chen, Shengjie Du, Weijun Ke, Guojia Fang","doi":"10.1002/adma.202502450","DOIUrl":"https://doi.org/10.1002/adma.202502450","url":null,"abstract":"All-perovskite tandem solar cells (TSCs) paired by wide-bandgap (WBG) perovskites with narrow-bandgap perovskites holds the potential to overcome the Shockley-Queisser limitation. However, the severe phase segregation and non-radiative recombination of WBG perovskite put on a shadow for their power conversion efficiency and stability. Here, an interfacial engineering strategy is introduced into the triple-halide WBG perovskite. Potassium trifluoromethanesulfonate (TfOK) is utilized to reconstruct the buried interface of the triple-halide WBG perovskite. The distribution of (chlorine) Cl− changes from perovskite bulk toward the buried interface due to the TfOK addition. Therefore, a wider bandgap perovskite thin layer is formed at buried layer, which can form a graded heterojunction with bulk WBG perovskite to improve carrier separation and transfer. Meanwhile, the (potassium) K+ of TfOK diffuses into WBG perovskite bulk to suppress halide phase segregation. Consequently, the 1.78 eV WBG PSCs deliver an impressive power conversion efficiency of 20.47% and an extremely high fill factor over 85%. Furthermore, the resultant two-terminal all-perovskite TSCs achieves a champion efficiency of 28.30%. This strategy provides a unique avenue to improve performance and photostability of WBG PSCs, a new function of Cl− in triple-halide is illustrated.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"18 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910788","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

Atomically Dispersed Sn on Core‐Shell MoS2 Nanoreactors as Mott‐Schottky Phase Junctions for Efficient Electrocatalytic Hydrogen Evolution 原子分散Sn在MoS2纳米反应器上作为Mott - Schottky相结的高效电催化析氢

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202502977

Hao Jin, Yan Zhang, Zhuwei Cao, Jian Liu, Sheng Ye

{"title":"Atomically Dispersed Sn on Core‐Shell MoS2 Nanoreactors as Mott‐Schottky Phase Junctions for Efficient Electrocatalytic Hydrogen Evolution","authors":"Hao Jin, Yan Zhang, Zhuwei Cao, Jian Liu, Sheng Ye","doi":"10.1002/adma.202502977","DOIUrl":"https://doi.org/10.1002/adma.202502977","url":null,"abstract":"The electrocatalytic hydrogen evolution reaction (HER) plays a pivotal role in electrochemical energy conversion and storage. However, traditional HER catalysts still face significant challenges, including limited activity, poor acid resistance, and high costs. To address these issues, a hollow core‐shell structured 2H@1T‐MoS2‐Sn1 nanoreactor is designed for acidic HER, where Sn single atoms are anchored on the shell of 2H@1T‐MoS2 Mott‐Schottky phase junction. The 2H@1T‐MoS2‐Sn1 catalyst demonstrates exceptional HER performance, achieving an ultralow overpotential of 9 mV at 10 mA cm−2 and a Tafel slope of 16.3 mV dec−1 in acidic media—the best performance reported to date among MoS2‐based electrocatalysts. The enhanced performance is attributed to the internal electric field at the Mott‐Schottky phase junction, which facilitates efficient electron transfer. Additionally, the Sn single atoms modulate the electronic structure of Mo atoms within the Sn‐S2‐Mo motif, inducing a significant shift in the d‐band center and thereby optimizing the dehydrogenation process. This work presents a novel electrocatalyst design strategy that simultaneously engineers interfacial charge transfer and surface catalysis, offering a promising approach for advancing energy conversion technologies.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"19 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910395","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

Layer-by-Layer Deposition of Antigen Peptides on Bifidobacterium for Subintestinal Lymphatic System-Guided Personalized Tumor Immunotherapy 抗原肽在双歧杆菌上的逐层沉积用于肠下淋巴系统引导的个性化肿瘤免疫治疗

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202503571

Zhu Chen, You-Teng Qin, Qian-Ru Li, Jin-Lian He, Xin-Chen Deng, Yun Zhang, Hao-Dong Yang, Jun Feng, Yun-Xia Sun, Xian-Zheng Zhang

{"title":"Layer-by-Layer Deposition of Antigen Peptides on Bifidobacterium for Subintestinal Lymphatic System-Guided Personalized Tumor Immunotherapy","authors":"Zhu Chen, You-Teng Qin, Qian-Ru Li, Jin-Lian He, Xin-Chen Deng, Yun Zhang, Hao-Dong Yang, Jun Feng, Yun-Xia Sun, Xian-Zheng Zhang","doi":"10.1002/adma.202503571","DOIUrl":"https://doi.org/10.1002/adma.202503571","url":null,"abstract":"Gut-associated lymphoid tissue (GALT) possesses a highly specialized immune system and is rational as a foothold for oral tumor vaccines. Here, a noninvasive oral vaccine (Bif-OVA-Ocur) is designed to engage GALT, inducing both intestinal mucosal and systemic immunity for tumor therapeutics. The vaccine uses Bifidobacterium (Bif) as a delivery vehicle for tumor antigen peptides, which are coated with antigen peptides (OVA) and oxidized curdlan (Ocur) in a layer-by-layer (LBL) manner. Upon oral administration, Bif-OVA-Ocur is efficiently directed to Peyer's patches (PPs) in the intestines and further presented to antigen-presenting cells (APCs), which then migrate to the mesenteric lymph nodes (MLNs) to evoke specific T cell responses. In mouse models, Bif-OVA-Ocur effectively boosts the production of secretory immunoglobin A (SIgA) and promotes a strong mucosal and systemic immune response, leading to significant tumor suppression and resistance to tumor challenges. Importantly, the vaccine shows no systemic toxicity. This approach to harnessing the intestinal mucosal immune system offers valuable insights for the development of other non-invasive oral vaccines and therapeutic agents.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"15 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910587","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

Artificial Cells Capable of NO Generation with Light Controllable Membraneless Organelles for Melanoma Therapy 光可控无膜细胞器产生NO的人造细胞用于黑色素瘤治疗

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202500242

Yingming Zhao, Shubin Li, Yanhao Liu, Chao Li, Jingjing Zhao, Yongshuo Ren, Wan Zhao, Xiangxiang Zhang, Xinyu Cui, Xuefeng Tang, Peipei Ren, Xiaojun Han

{"title":"Artificial Cells Capable of NO Generation with Light Controllable Membraneless Organelles for Melanoma Therapy","authors":"Yingming Zhao, Shubin Li, Yanhao Liu, Chao Li, Jingjing Zhao, Yongshuo Ren, Wan Zhao, Xiangxiang Zhang, Xinyu Cui, Xuefeng Tang, Peipei Ren, Xiaojun Han","doi":"10.1002/adma.202500242","DOIUrl":"https://doi.org/10.1002/adma.202500242","url":null,"abstract":"Membraneless organelles (MLOs) formed by liquid–liquid phase separation exhibit diverse important biofunctions in cells. The construction of artificial cells containing MLOs with enhanced complexity and functions is still challenging. Here a light-responsive protein, Cry2olig-IDRs, is designed and purified to form MLOs upon light (488 nm) irradiation. They are capable of rapidly recruiting positively charged inducible nitric oxide synthase (iNOS+) from surroundings to regulate its activity for NO production. NO-artificial cells are constructed by encapsulating Cry2olig-IDRs and iNOS+ into giant unilamellar vesicles, which are capable of rapid production of NO with high concentration due to the formation of MLOs upon light irradiation. NO-artificial cells are confirmed to possess the ability for melanoma tumor therapy in mice. These findings provide an efficient method for remotely regulating enzyme activity inside artificial cells, paving the path to build more sophisticated artificial cells for their biomedical applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"143 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910589","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

Disordered Rocksalts as High-Energy and Earth-Abundant Li-Ion Cathodes 无序岩盐作为高能和地球丰富的锂离子阴极

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202502766

Han-Ming Hau, Tucker Holstun, Eunryeol Lee, Bernardine L. D. Rinkel, Tara P. Mishra, Max Markuson DiPrince, Rohith Srinivaas Mohanakrishnan, Ethan C. Self, Kristin A. Persson, Bryan D. McCloskey, Gerbrand Ceder

{"title":"Disordered Rocksalts as High-Energy and Earth-Abundant Li-Ion Cathodes","authors":"Han-Ming Hau, Tucker Holstun, Eunryeol Lee, Bernardine L. D. Rinkel, Tara P. Mishra, Max Markuson DiPrince, Rohith Srinivaas Mohanakrishnan, Ethan C. Self, Kristin A. Persson, Bryan D. McCloskey, Gerbrand Ceder","doi":"10.1002/adma.202502766","DOIUrl":"https://doi.org/10.1002/adma.202502766","url":null,"abstract":"To address the growing demand for energy and support the shift toward transportation electrification and intermittent renewable energy, there is an urgent need for low-cost, energy-dense electrical storage. Research on Li-ion electrode materials has predominantly focused on ordered materials with well-defined lithium diffusion channels, limiting cathode design to resource-constrained Ni- and Co-based oxides and lower-energy polyanion compounds. Recently, disordered rocksalts with lithium excess (DRX) have demonstrated high capacity and energy density when lithium excess and/or local ordering allow statistical percolation of lithium sites through the structure. This cation disorder can be induced by high temperature synthesis or mechanochemical synthesis methods for a broad range of compositions. DRX oxides and oxyfluorides containing Earth-abundant transition metals have been prepared using various synthesis routes, including solid-state, molten-salt, and sol-gel reactions. This review outlines DRX design principles and explains the effect of synthesis conditions on cation disorder and short-range cation ordering (SRO), which determines the cycling stability and rate capability. In addition, strategies to enhance Li transport and capacity retention with Mn-rich DRX possessing partial spinel-like ordering are discussed. Finally, the review considers the optimization of carbon and electrolyte in DRX materials and addresses key challenges and opportunities for commercializing DRX cathodes.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"15 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910594","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

Entropy-Driven Stabilization of Noble Metal Single Atoms: Advancing Ammonia Synthesis and Energy Output in Zinc-Nitrate Batteries 贵金属单原子的熵驱动稳定：推进氨合成和硝酸锌电池的能量输出

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202500224

Hele Guo, Zhongyuan Guo, Guohao Xue, Haifeng Wang, Jiaming Gong, Kaibin Chu, Jingjing Qin, Yawen Guan, Hongliang Dong, Yujie Chen, Yue-E Miao, Chao Zhang, Hezhou Liu, Tianxi Liu, Johan Hofkens, Feili Lai

{"title":"Entropy-Driven Stabilization of Noble Metal Single Atoms: Advancing Ammonia Synthesis and Energy Output in Zinc-Nitrate Batteries","authors":"Hele Guo, Zhongyuan Guo, Guohao Xue, Haifeng Wang, Jiaming Gong, Kaibin Chu, Jingjing Qin, Yawen Guan, Hongliang Dong, Yujie Chen, Yue-E Miao, Chao Zhang, Hezhou Liu, Tianxi Liu, Johan Hofkens, Feili Lai","doi":"10.1002/adma.202500224","DOIUrl":"https://doi.org/10.1002/adma.202500224","url":null,"abstract":"Noble metal single atoms (NMSA) offer exceptional atom utilization and catalytic activity but face challenges like limited stability, low atomic loading, and complex synthesis. This study presents an innovative entropy-driven strategy to stabilize Ru single atoms (SA) on a (CePrYZrHf)Ox high-entropy oxide substrate (Ruα%-HEO). Due to their defect-rich structure and significant lattice distortion, HEO substrates can accommodate and stabilize more Ru SA than traditional low-entropy oxides (LEO) like CeO2. This strategy is also effective for achieving high loadings of other NMSAs, such as Pd and Pt. Ru3%-HEO, as an electrocatalyst for nitrate reduction, achieves a high ammonia yield (5.79 mg h−1 mgcat.−1) and a Faradaic efficiency (FE) of 91.3%. Density functional theory (DFT) calculations reveal that Ru3%-HEO exhibits favorable thermodynamics for nitrate reduction, with a lower energy barrier for the rate-determining step of first hydrogenation (*NO + H+ + e⁻ → *NOH) and stronger intermediates adsorption compared to RuO2, enhancing its catalytic efficiency. As a cathode material in a zinc-nitrate battery, Ru3%-HEO demonstrates a high NH3 yield rate (1.11 mg h−1 cm−2) and FE value (93.4%). This study provides an efficient strategy to produce stable and high-loading SA using high-entropy materials, showcasing their broad applicability in advanced electrocatalysis.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"8 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910838","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

Parallel Regulation of Charge Dynamics on Bipolar Ferroelectric Surfaces Breaks the Limits for Water Splitting Efficiency 双极铁电表面电荷动力学的平行调节打破了水分解效率的极限

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-05-06 DOI: 10.1002/adma.202501875

Jie Zhang, Thomas Dittrich, Qian Li, Chenwei Ni, Zhongrui Min, Lingcong Zhang, Jiangshan Qu, Mingrun Li, Xiuli Wang, Can Li, Fengtao Fan

{"title":"Parallel Regulation of Charge Dynamics on Bipolar Ferroelectric Surfaces Breaks the Limits for Water Splitting Efficiency","authors":"Jie Zhang, Thomas Dittrich, Qian Li, Chenwei Ni, Zhongrui Min, Lingcong Zhang, Jiangshan Qu, Mingrun Li, Xiuli Wang, Can Li, Fengtao Fan","doi":"10.1002/adma.202501875","DOIUrl":"https://doi.org/10.1002/adma.202501875","url":null,"abstract":"Ferroelectric materials, known for their non-inversion symmetry, show promise as photocatalysts due to their unique asymmetric charge separation, which separates hydrogen and oxygen evolution sites. However, the strong depolarized field induces a relaxed surface structure, which in turn directly leads to slow hole charge transfer dynamics, hindering their efficiency in water splitting. In this study, a fundamental breakthrough in dramatically enhancing the overall water-splitting activity is presented, through the synergistically regulating of the surface behaviors of photogenerated carriers, resulting in nearly perfect parallel dynamics and balanced amounts. By depositing atomic layers of TiO2 onto the surface of PbTiO3, surface vacancies are effectively passivated, significantly prolonging the hole lifetime from 10−6 to 10−3 s. Spatially resolved transient photovoltage spectroscopy showed that improved hole dynamics led to a 180° phase shift between photogenerated electrons and holes, indicating nearly identical extraction dynamics. Notably, hole and electron concentrations increased to equivalent levels. This leads to a nearly 578-fold increment in the apparent quantum yield, resulting in significantly increased overall water-splitting rates, with a quantum yield of 5.78% at 365 nm. The strategy is also effective with Al2O3 and SiO2, demonstrating its versatility across varied materials, providing a valuable method for creating high-performance ferroelectric photocatalysts.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"2 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910593","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