Mengxuan Wang, Wanchao Song, Hua Zou, Guoshuai Liu, Shijie You
The electrocatalytic nitrate reduction reaction (NO 3 RR) to ammonia (NH 3 ) represents a promising strategy for sustainable NH 3 synthesis while mitigating nitrate contamination. However, challenges remain for sluggish kinetics and poor selectivity due to inefficient nitrite (NO 2− ) activation and inadequate generation/utilization of reactive hydrogen species (H*). To address these issues, we design a dual‐atom copper nanozyme anchored on hollow carbon spheres (Cu 2 ‐S 1 N 4 /HCS) by mimicking the enzymatic architecture of copper‐containing nitrite reductases (Cu‐NIRs). Experimental and theoretical investigations reveal that the Cu‐S 1 N 2 site facilitates water dissociation to generate H*, which subsequently spills over to the Cu‐N 3 site. Meanwhile, the electrons are transferred from Cu‐S 1 N 2 to Cu‐N 3 site induced by regulation of coordination environments, resulting in stabilization of the key NO 3 RR intermediates by low‐valent Cu at the Cu‐N 3 site. In this process, the Cu‐N 3 site serves as the catalytic center for inter‐site coupling of H*/e − transfer‐mediated deoxygenation and hydrogenation of NO 3− to NH 3 . The resulting Cu 2 ‐S 1 N 4 /HCS dual‐atom nanozyme delivers a remarkable NO 3− ‐to‐NH 3 Faradaic efficiency (FE, 93.1%) and a high NH 3 yield rate (11.8 mg h −1 cm −2 ) at −0.6 V vs. reversible hydrogen electrode (RHE). This work demonstrates a bioinspired strategy that mimics natural Cu‐NIRs, which offers an efficient and sustainable route for ammonia production from wastewater.
{"title":"Synergistic Dual‐Atom Cu Nanozyme for Efficient Electrocatalytic Nitrate Reduction to Ammonia","authors":"Mengxuan Wang, Wanchao Song, Hua Zou, Guoshuai Liu, Shijie You","doi":"10.1002/adfm.202528731","DOIUrl":"https://doi.org/10.1002/adfm.202528731","url":null,"abstract":"The electrocatalytic nitrate reduction reaction (NO <jats:sub>3</jats:sub> RR) to ammonia (NH <jats:sub>3</jats:sub> ) represents a promising strategy for sustainable NH <jats:sub>3</jats:sub> synthesis while mitigating nitrate contamination. However, challenges remain for sluggish kinetics and poor selectivity due to inefficient nitrite (NO <jats:sub>2</jats:sub> <jats:sup>−</jats:sup> ) activation and inadequate generation/utilization of reactive hydrogen species (H*). To address these issues, we design a dual‐atom copper nanozyme anchored on hollow carbon spheres (Cu <jats:sub>2</jats:sub> ‐S <jats:sub>1</jats:sub> N <jats:sub>4</jats:sub> /HCS) by mimicking the enzymatic architecture of copper‐containing nitrite reductases (Cu‐NIRs). Experimental and theoretical investigations reveal that the Cu‐S <jats:sub>1</jats:sub> N <jats:sub>2</jats:sub> site facilitates water dissociation to generate H*, which subsequently spills over to the Cu‐N <jats:sub>3</jats:sub> site. Meanwhile, the electrons are transferred from Cu‐S <jats:sub>1</jats:sub> N <jats:sub>2</jats:sub> to Cu‐N <jats:sub>3</jats:sub> site induced by regulation of coordination environments, resulting in stabilization of the key NO <jats:sub>3</jats:sub> RR intermediates by low‐valent Cu at the Cu‐N <jats:sub>3</jats:sub> site. In this process, the Cu‐N <jats:sub>3</jats:sub> site serves as the catalytic center for inter‐site coupling of H*/e <jats:sup>−</jats:sup> transfer‐mediated deoxygenation and hydrogenation of NO <jats:sub>3</jats:sub> <jats:sup>−</jats:sup> to NH <jats:sub>3</jats:sub> . The resulting Cu <jats:sub>2</jats:sub> ‐S <jats:sub>1</jats:sub> N <jats:sub>4</jats:sub> /HCS dual‐atom nanozyme delivers a remarkable NO <jats:sub>3</jats:sub> <jats:sup>−</jats:sup> ‐to‐NH <jats:sub>3</jats:sub> Faradaic efficiency (FE, 93.1%) and a high NH <jats:sub>3</jats:sub> yield rate (11.8 mg h <jats:sup>−1</jats:sup> cm <jats:sup>−2</jats:sup> ) at −0.6 V vs. reversible hydrogen electrode (RHE). This work demonstrates a bioinspired strategy that mimics natural Cu‐NIRs, which offers an efficient and sustainable route for ammonia production from wastewater.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"46 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947350","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}
Hyeonjung Jung, Yechan Lee, Kyuri Cho, Tae Yong Kim, Jihyeon Song, Han Sol Jung, Sung Il Park, Yoojin Lee, Jinuk Moon, Wongyu Park, Jaewoo Nam, Sangmin Park, Wooyul Kim, Jeong Woo Han
Seawater Electrolysis
海水电解
{"title":"Strategic Design of Oxophilic Dopants for Active and Durable Alkaline Hydrogen Evolution Reaction Under Seawater (Adv. Funct. Mater. 3/2026)","authors":"Hyeonjung Jung, Yechan Lee, Kyuri Cho, Tae Yong Kim, Jihyeon Song, Han Sol Jung, Sung Il Park, Yoojin Lee, Jinuk Moon, Wongyu Park, Jaewoo Nam, Sangmin Park, Wooyul Kim, Jeong Woo Han","doi":"10.1002/adfm.73578","DOIUrl":"https://doi.org/10.1002/adfm.73578","url":null,"abstract":"<b>Seawater Electrolysis</b>","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"49 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145937934","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}
Achieving high‐efficiency and low roll‐off red organic light‐emitting diodes (OLEDs) that meet Broadcast Television 2020 (BT. 2020) standards remains a formidable challenge, due to the scarcity of narrowband red emitters exhibiting both short exciton lifetimes and desirable color purity. Herein, three boron‐dipyrromethene (BODIPY)‐derived narrowband red emitters (BDP1P, BDP1TPM, and BDP‐tBu) with high horizontal orientation are developed through vinyl‐bridged conjugation extension achieving bathochromic‐shifted emission (642–652 nm) while maintaining ultra‐narrow emission bandwidth (<30 nm). Furthermore, OLEDs are fabricated using a rational design strategy, employing a low‐polarity tricomponent multi‐sensitization host matrix, doped with BODIPY emitters in the emission layer. This design not only achieves a narrowband electroluminescence with minimal energetic loss during energy transfer but also facilitates accelerated exciton consumption, thereby ameliorating efficiency roll‐off at high luminance levels. Consequently, a remarkable external quantum efficiency (EQE) of 15.6% is achieved for the BDP1P‐based OLED, simultaneously with an ultralow roll‐off (EQE of 15.5% @ 1000 and 13.6% @ 10 000 cd m −2 ) and BT.2020‐compliant color coordinates (CIE: 0.708, 0.292), which represents one of the most advanced performance reported for red OLEDs based on traditional fluorescent emitters.
{"title":"Highly Horizontally Oriented BODIPY Emitters for Efficient BT. 2020 Red OLEDs via Low‐Polarity Multi‐Sensitization Strategy","authors":"Xuewei Nie, Zhizhi Li, Shaofu Chen, Zijian Chen, Yu Fu, Zhihai Yang, Guoxi Yang, Yongxia Ren, Xiangyi Cheng, Yitong Zeng, Yingrui Tian, Denghui Liu, Mengke Li, Junji Kido, Shi‐Jian Su","doi":"10.1002/adfm.202529876","DOIUrl":"https://doi.org/10.1002/adfm.202529876","url":null,"abstract":"Achieving high‐efficiency and low roll‐off red organic light‐emitting diodes (OLEDs) that meet Broadcast Television 2020 (BT. 2020) standards remains a formidable challenge, due to the scarcity of narrowband red emitters exhibiting both short exciton lifetimes and desirable color purity. Herein, three boron‐dipyrromethene (BODIPY)‐derived narrowband red emitters (BDP1P, BDP1TPM, and BDP‐tBu) with high horizontal orientation are developed through vinyl‐bridged conjugation extension achieving bathochromic‐shifted emission (642–652 nm) while maintaining ultra‐narrow emission bandwidth (<30 nm). Furthermore, OLEDs are fabricated using a rational design strategy, employing a low‐polarity tricomponent multi‐sensitization host matrix, doped with BODIPY emitters in the emission layer. This design not only achieves a narrowband electroluminescence with minimal energetic loss during energy transfer but also facilitates accelerated exciton consumption, thereby ameliorating efficiency roll‐off at high luminance levels. Consequently, a remarkable external quantum efficiency (EQE) of 15.6% is achieved for the BDP1P‐based OLED, simultaneously with an ultralow roll‐off (EQE of 15.5% @ 1000 and 13.6% @ 10 000 cd m <jats:sup>−2</jats:sup> ) and BT.2020‐compliant color coordinates (CIE: 0.708, 0.292), which represents one of the most advanced performance reported for red OLEDs based on traditional fluorescent emitters.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"253 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947396","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}
Cheng Zhang, Jia Niu, Mengying Xu, Tianwen Bai, Lei Lu, Shan Ji, Peiyang Gu, Peng Wang
Oxygen vacancy (OV)‐engineered catalysts show promise for lithium sulfur batteries (LSBs) by enhancing polysulfide adsorption and conversion, yet most studies focus on total OV concentration while overlooking spatial distribution effects on local catalytic activity and charge transport. This limitation hinders active site utilization and kinetic improvement. To address these issues, we report the successful synthesis of an olive‐shaped In 2 O x nanocatalyst through a straightforward urea‐assisted precursor engineering strategy. This catalyst exhibits a distinctive non‐uniformly distributed OVs, extending the current insights spatially heterogeneous distribution of OVs. Kinetic analysis demonstrates that this distribution enhances catalytic site density and facilitates optimized electron transport pathways. Capitalizing on the synergistic effects of this gradient OV distribution, LSBs incorporating In 2 O x –L deliver superior performance: an initial capacity of 1171 mAh g −1 (0.2 C), robust high‐rate capability, and extended cyclability under demanding conditions (1 C cycling; E/S = 10 µL mg −1 ). This work demonstrates the precise spatial regulation of OVs in electrocatalysts, thereby advancing design principles for next‐generation vacancy‐engineered catalytic systems.
氧空位(OV)工程催化剂通过增强多硫化物的吸附和转化,在锂硫电池(LSBs)中表现出了良好的前景,但大多数研究都集中在总氧空位浓度上,而忽视了空间分布对局部催化活性和电荷传输的影响。这一限制阻碍了活性位点的利用和动力学改进。为了解决这些问题,我们报道了通过尿素辅助前驱体工程策略成功合成橄榄形的in2o纳米催化剂。该催化剂表现出独特的非均匀分布的OVs,扩展了目前对OVs空间异质性分布的认识。动力学分析表明,这种分布增强了催化位点密度,有利于优化电子传递途径。利用这种梯度OV分布的协同效应,含有In 2o x -L的lsb提供了卓越的性能:1171 mAh g - 1 (0.2 C)的初始容量,强大的高倍率能力,以及苛刻条件下的扩展可循环性(1c循环;E/S = 10 μ L mg - 1)。这项工作证明了电催化剂中OVs的精确空间调节,从而推进了下一代空位工程催化系统的设计原则。
{"title":"Spatially Heterogeneous Oxygen Vacancy Engineering in Olive‐Shaped In 2 O x for Accelerated Sulfur Redox Kinetics and Long‐Life Lithium–Sulfur Batteries","authors":"Cheng Zhang, Jia Niu, Mengying Xu, Tianwen Bai, Lei Lu, Shan Ji, Peiyang Gu, Peng Wang","doi":"10.1002/adfm.202521294","DOIUrl":"https://doi.org/10.1002/adfm.202521294","url":null,"abstract":"Oxygen vacancy (OV)‐engineered catalysts show promise for lithium sulfur batteries (LSBs) by enhancing polysulfide adsorption and conversion, yet most studies focus on total OV concentration while overlooking spatial distribution effects on local catalytic activity and charge transport. This limitation hinders active site utilization and kinetic improvement. To address these issues, we report the successful synthesis of an olive‐shaped In <jats:sub>2</jats:sub> O <jats:sub>x</jats:sub> nanocatalyst through a straightforward urea‐assisted precursor engineering strategy. This catalyst exhibits a distinctive non‐uniformly distributed OVs, extending the current insights spatially heterogeneous distribution of OVs. Kinetic analysis demonstrates that this distribution enhances catalytic site density and facilitates optimized electron transport pathways. Capitalizing on the synergistic effects of this gradient OV distribution, LSBs incorporating In <jats:sub>2</jats:sub> O <jats:sub>x</jats:sub> –L deliver superior performance: an initial capacity of 1171 mAh g <jats:sup>−1</jats:sup> (0.2 C), robust high‐rate capability, and extended cyclability under demanding conditions (1 C cycling; E/S = 10 µL mg <jats:sup>−1</jats:sup> ). This work demonstrates the precise spatial regulation of OVs in electrocatalysts, thereby advancing design principles for next‐generation vacancy‐engineered catalytic systems.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"53 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947323","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}
Yuxin Zheng, Yifan Yao, Weikong Pang, Zhenxiang Cheng, Huiling Zhao, Ying Bai, Liang Yin, Hong Li
Li‐rich layered oxides (LROs) are promising high‐capacity cathodes for next‐generation Li‐ion batteries, yet suffer from irreversible oxygen release and interfacial degradation, leading to voltage decay, capacity fading, and gas evolution. Herein, we report an i n situ constructed garnet‐type Li 5 La 3 Nb 2 O 12 (LLNO) fast‐ion conductor coating on LRO particles via a sol–gel process using C 4 H 4 NNbO 9 ·nH 2 O as the Nb precursor. During pyrolysis, released NH 3 acts as a mild reducing agent, promoting surface reconstruction accompanied by near‐surface Nb 5+ doping, formation of a spinel transition layer, and a gradient oxygen‐vacancy distribution. The resulting hierarchical architecture integrates: (i) interfacial protection and chemical stability from the LLNO coating, (ii) structural coherence and multidimensional Li + transport from the spinel layer, and (iii) reversible oxygen‐anion redox stabilization enabled by Nb 5+ –O bonding and oxygen vacancies. Benefiting from these cooperative effects, the optimized cathode delivers 281.7 mAh g −1 at 0.1 C and maintains 97.6% capacity retention after 200 cycles at 1 C, outperforming the pristine counterpart. This work demonstrates a multifunctional interfacial‐engineering strategy that unifies coating, doping, and surface reconstruction, providing a generalizable pathway toward durable, high‐energy LROs.
富锂层状氧化物(LROs)是下一代锂离子电池极具潜力的高容量阴极材料,但其存在不可逆的氧释放和界面降解问题,导致电压衰减、容量衰减和气体析出。本文以c4h4nnbo 9·nh2o为Nb前驱体,采用溶胶-凝胶法在LRO颗粒上原位构建了石榴石型Li 5la3nb 2o12 (LLNO)快离子导体涂层。在热解过程中,释放的nh3作为温和还原剂,促进了表面重构,伴随近表面Nb 5+掺杂,尖晶石过渡层的形成,以及梯度氧空位分布。由此产生的分层结构集成了:(i) LLNO涂层的界面保护和化学稳定性,(ii)尖晶石层的结构一致性和多维Li +传输,以及(iii) Nb 5+ -O键和氧空位实现的可逆氧-阴离子氧化还原稳定性。得益于这些协同效应,优化后的阴极在0.1℃下可提供281.7 mAh g - 1,在1c下循环200次后仍能保持97.6%的容量,优于原始阴极。这项工作展示了一种多功能的界面工程策略,它将涂层、掺杂和表面重建结合起来,为实现持久、高能的lro提供了一条可推广的途径。
{"title":"Hierarchical Garnet‐Type Interfacial Engineering Enables Reversible Oxygen Redox in Li‐Rich Layered Cathodes","authors":"Yuxin Zheng, Yifan Yao, Weikong Pang, Zhenxiang Cheng, Huiling Zhao, Ying Bai, Liang Yin, Hong Li","doi":"10.1002/adfm.202530416","DOIUrl":"https://doi.org/10.1002/adfm.202530416","url":null,"abstract":"Li‐rich layered oxides (LROs) are promising high‐capacity cathodes for next‐generation Li‐ion batteries, yet suffer from irreversible oxygen release and interfacial degradation, leading to voltage decay, capacity fading, and gas evolution. Herein, we report an i <jats:italic>n situ</jats:italic> constructed garnet‐type Li <jats:sub>5</jats:sub> La <jats:sub>3</jats:sub> Nb <jats:sub>2</jats:sub> O <jats:sub>12</jats:sub> (LLNO) fast‐ion conductor coating on LRO particles via a sol–gel process using C <jats:sub>4</jats:sub> H <jats:sub>4</jats:sub> NNbO <jats:sub>9</jats:sub> ·nH <jats:sub>2</jats:sub> O as the Nb precursor. During pyrolysis, released NH <jats:sub>3</jats:sub> acts as a mild reducing agent, promoting surface reconstruction accompanied by near‐surface Nb <jats:sup>5+</jats:sup> doping, formation of a spinel transition layer, and a gradient oxygen‐vacancy distribution. The resulting hierarchical architecture integrates: (i) interfacial protection and chemical stability from the LLNO coating, (ii) structural coherence and multidimensional Li <jats:sup>+</jats:sup> transport from the spinel layer, and (iii) reversible oxygen‐anion redox stabilization enabled by Nb <jats:sup>5+</jats:sup> –O bonding and oxygen vacancies. Benefiting from these cooperative effects, the optimized cathode delivers 281.7 mAh g <jats:sup>−1</jats:sup> at 0.1 C and maintains 97.6% capacity retention after 200 cycles at 1 C, outperforming the pristine counterpart. This work demonstrates a multifunctional interfacial‐engineering strategy that unifies coating, doping, and surface reconstruction, providing a generalizable pathway toward durable, high‐energy LROs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"46 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947326","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}
Xuan Ding, Wen He, Daijun Meng, Ali A. AL‐Thuraya, Bizi Yu, Yuting Zhang, Ayan Yao, Yumo Fan, Jian Guan, Pengbo Liao, Hongjun Zhang, Jiangtao Liu
The development of conjugated microporous polymers (CMPs) with extended π ‐conjugation has positioned them as promising candidates for advanced gas separation membranes. Realizing their superior performance hinges on the rational design of their porous frameworks. Herein, we report a novel strategy to create tunable localized electric fields within CMPs by incorporating triazine rings at varied molecular positions, thereby achieving highly efficient CO 2 separation in Pebax‐based mixed matrix membranes (MMMs). As designed, the fine‐tuning of the triazine units enables the construction of an optimized donor‐ π ‐acceptor (D‐ π ‐A) electronic structure in the CMP‐PT framework. This tailored structure enhances intermolecular interactions, confers a larger dipole moment, improves coordination capability, and ultimately optimizes the microporous environment of the resultant MMM. Compared to the pristine Pebax membrane, the optimal Pebax‐CMP‐PT‐1% MMM exhibits a remarkable 83.4% enhancement in CO 2 permeability and a CO 2 /N 2 selectivity of 167.31 at 20 bar, surpassing the 2019 Robeson upper bound. This work provides a valuable strategy for the development of next‐generation high‐performance CO 2 separation membranes.
{"title":"Electron‐Donating Conjugated Microporous Polymer Membranes for Enhanced CO 2 Capture","authors":"Xuan Ding, Wen He, Daijun Meng, Ali A. AL‐Thuraya, Bizi Yu, Yuting Zhang, Ayan Yao, Yumo Fan, Jian Guan, Pengbo Liao, Hongjun Zhang, Jiangtao Liu","doi":"10.1002/adfm.202528057","DOIUrl":"https://doi.org/10.1002/adfm.202528057","url":null,"abstract":"The development of conjugated microporous polymers (CMPs) with extended <jats:italic>π</jats:italic> ‐conjugation has positioned them as promising candidates for advanced gas separation membranes. Realizing their superior performance hinges on the rational design of their porous frameworks. Herein, we report a novel strategy to create tunable localized electric fields within CMPs by incorporating triazine rings at varied molecular positions, thereby achieving highly efficient CO <jats:sub>2</jats:sub> separation in Pebax‐based mixed matrix membranes (MMMs). As designed, the fine‐tuning of the triazine units enables the construction of an optimized donor‐ <jats:italic>π</jats:italic> ‐acceptor (D‐ <jats:italic>π</jats:italic> ‐A) electronic structure in the CMP‐PT framework. This tailored structure enhances intermolecular interactions, confers a larger dipole moment, improves coordination capability, and ultimately optimizes the microporous environment of the resultant MMM. Compared to the pristine Pebax membrane, the optimal Pebax‐CMP‐PT‐1% MMM exhibits a remarkable 83.4% enhancement in CO <jats:sub>2</jats:sub> permeability and a CO <jats:sub>2</jats:sub> /N <jats:sub>2</jats:sub> selectivity of 167.31 at 20 bar, surpassing the 2019 Robeson upper bound. This work provides a valuable strategy for the development of next‐generation high‐performance CO <jats:sub>2</jats:sub> separation membranes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"81 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947397","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}
Advancing space thermal management requires radiative cooling materials with ultralow solar absorptance and exceptional irradiation resistance, yet conventional coatings fall short due to intrinsic UV absorption, suboptimal material, and structural design. Here, bandgap engineering is integrated with photonic structure optimization to develop all‐inorganic metacoatings that overcome these issues. Density functional theory identifies La as ideal dopant for ZrO 2 , as it enlarges the bandgap and enhances lattice stability, suppressing UV absorption and irradiation‐induced defect formation. Monte Carlo simulations determine the optimal submicrosphere diameter (∼0.7 µm) and volume fraction (35%) for maximal solar backscattering. Then we successfully and controllably synthesized the designed La‐doped ZrO 2 submicrospheres and fabricated metacoatings via scalable spray‐coating. The metacoating achieves ultralow solar absorptance ( α s = 0.061) and high thermal emittance ( ε = 0.941) at ∼100 µm, yielding the lowest αs / ε value among the commercial and reported coatings. Under AM0 illumination, it delivers a net cooling power of 280 W·m −2 and reduces temperature by 78°C relative to uncoated Al substrate. The metacoating exhibits excellent irradiation stability with minimal optical degradation after proton, electron, atomic oxygen, and UV exposures, and remains stable after 50 thermal cycles (−196°C to 150°C). This work offers a general strategy for high‐performance radiative cooling materials in extreme space environments.
推进空间热管理需要具有超低太阳吸收率和卓越的抗辐照性的辐射冷却材料,然而传统涂层由于固有的紫外线吸收、不理想的材料和结构设计而不足。在这里,带隙工程与光子结构优化相结合,开发出克服这些问题的全无机超镀膜。密度泛函理论认为,La是ZrO - 2的理想掺杂剂,因为它扩大了带隙,增强了晶格稳定性,抑制了紫外线吸收和辐照诱导的缺陷形成。蒙特卡罗模拟确定了最大太阳后向散射的最佳亚微球直径(~ 0.7µm)和体积分数(35%)。然后,我们成功地、可控地合成了设计的La掺杂zro2亚微球,并通过可扩展喷涂制备了亚涂层。该涂层在~ 100µm处实现了超低的太阳吸收率(α s = 0.061)和高热发射率(ε = 0.941),在商业和报道的涂层中产生了最低的α s / ε值。在AM0照明下,它提供了280 W·m−2的净冷却功率,相对于未涂层的Al基底降低了78°C的温度。在质子、电子、原子氧和紫外线照射后,稳镀膜具有优异的辐照稳定性,光学降解最小,并且在50个热循环(- 196°C至150°C)后保持稳定。这项工作为极端空间环境下的高性能辐射冷却材料提供了一种通用策略。
{"title":"Material and Structure Tailored La‐Doped ZrO 2 Submicrosphere Metacoatings for High‐Performance Space Radiative Cooling","authors":"Hao Gong, Liping Tong, Zhongyang Wang, Xiaokun Song, Hongchao Li, Zhiyuan Zhao, Yan Zheng, Gang Liu, Hao Luan, Shuqiang Xiong, Tongxiang Fan, Xiao Zhou","doi":"10.1002/adfm.202528343","DOIUrl":"https://doi.org/10.1002/adfm.202528343","url":null,"abstract":"Advancing space thermal management requires radiative cooling materials with ultralow solar absorptance and exceptional irradiation resistance, yet conventional coatings fall short due to intrinsic UV absorption, suboptimal material, and structural design. Here, bandgap engineering is integrated with photonic structure optimization to develop all‐inorganic metacoatings that overcome these issues. Density functional theory identifies La as ideal dopant for ZrO <jats:sub>2</jats:sub> , as it enlarges the bandgap and enhances lattice stability, suppressing UV absorption and irradiation‐induced defect formation. Monte Carlo simulations determine the optimal submicrosphere diameter (∼0.7 µm) and volume fraction (35%) for maximal solar backscattering. Then we successfully and controllably synthesized the designed La‐doped ZrO <jats:sub>2</jats:sub> submicrospheres and fabricated metacoatings via scalable spray‐coating. The metacoating achieves ultralow solar absorptance ( <jats:italic> α <jats:sub>s</jats:sub> </jats:italic> = 0.061) and high thermal emittance ( <jats:italic>ε </jats:italic> = 0.941) at ∼100 µm, yielding the lowest <jats:italic>α</jats:italic> <jats:sub>s</jats:sub> / <jats:italic>ε</jats:italic> value among the commercial and reported coatings. Under AM0 illumination, it delivers a net cooling power of 280 W·m <jats:sup>−2</jats:sup> and reduces temperature by 78°C relative to uncoated Al substrate. The metacoating exhibits excellent irradiation stability with minimal optical degradation after proton, electron, atomic oxygen, and UV exposures, and remains stable after 50 thermal cycles (−196°C to 150°C). This work offers a general strategy for high‐performance radiative cooling materials in extreme space environments.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"253 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947322","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}
The multi‐electron transfer capability of iodine renders it a promising conversion‐type cathode for aluminum‐ion batteries. However, conventional aluminum/iodine (Al/I 2 ) batteries typically operate via the I 0 (or I 3− )/I − redox couple at low voltages, leaving the high‐potential I + /I 0 redox largely unexplored and limiting both capacity and energy density. Herein, we develop high‐performance Al/I 2 batteries by employing iodine‐rich 1D perovskite cathodes that leverage the thermodynamically favorable ionic liquid electrolyte environment to achieve a four‐electron I + /I 0 /I − redox process. These perovskite cathodes lower the reaction barrier for I + /I 0 conversion and suppress the shuttle effect of iodine species through hydrogen bonding and halogen bonding interactions, ensuring cycling stability and a stable environment for four‐electron transfer reaction. The I + formed can be effectively stabilized by AlCl 4− , further accelerating the reaction kinetics. Through organic and metal cation engineering to modulate bonding interactions and electronic properties, the benzamidinium and Bi 3+ ‐based perovskite (PFABiI 4 ) cathode achieves a high specific capacity of 311.2 mAh g −1I at 0.2 A g −1 and exceptional cycling stability, with a capacity decay rate of only 0.0056% per cycle over 8000 cycles at 2 A g −1 . This work opens an avenue for designing high‐voltage, high‐energy‐density, and long‐cycle‐life Al/I 2 batteries.
碘的多电子转移能力使其成为一种很有前途的铝离子电池转换型阴极。然而,传统的铝/碘(Al/ i2)电池通常在低电压下通过i0(或i3 -)/I -氧化还原对工作,使得高电位的I + / i0氧化还原在很大程度上未被开发,并且限制了容量和能量密度。本文中,我们开发了高性能的Al/ i2电池,采用富碘的1D钙钛矿阴极,利用有利的热动力学离子液体电解质环境来实现四电子I + /I 0 /I−氧化还原过程。这些钙钛矿阴极降低了I + /I 0转化的反应势垒,抑制了碘物质通过氢键和卤素键相互作用的穿梭效应,确保了循环稳定性和四电子转移反应的稳定环境。AlCl -可以有效地稳定生成的I +,进一步加快反应动力学。通过有机和金属阳离子工程来调节键的相互作用和电子性能,苯偕胺和bi3 +基钙钛矿(pfabi4)阴极在0.2 a g−1时获得了311.2 mAh g−1 I的高比容量和出色的循环稳定性,在2 a g−1的8000次循环中,每循环的容量衰减率仅为0.0056%。这项工作为设计高电压、高能量密度、长循环寿命的Al/ i2电池开辟了一条道路。
{"title":"Iodide Perovskites Leveraging Ionic Liquid Electrolytes Activate I + /I 0 /I − Four‐Electron Redox for Long‐Life and High‐Voltage Aluminum/Iodine Batteries","authors":"Xin Fu, Pengyun Liu, Xueru Wang, Yanfu Tong, Yiting Li, Xuejin Li, Tonghui Cai, Yongpeng Cui, Zifeng Yan, Lianming Zhao, Wei Xing","doi":"10.1002/adfm.202531085","DOIUrl":"https://doi.org/10.1002/adfm.202531085","url":null,"abstract":"The multi‐electron transfer capability of iodine renders it a promising conversion‐type cathode for aluminum‐ion batteries. However, conventional aluminum/iodine (Al/I <jats:sub>2</jats:sub> ) batteries typically operate via the I <jats:sup>0</jats:sup> (or I <jats:sub>3</jats:sub> <jats:sup>−</jats:sup> )/I <jats:sup>−</jats:sup> redox couple at low voltages, leaving the high‐potential I <jats:sup>+</jats:sup> /I <jats:sup>0</jats:sup> redox largely unexplored and limiting both capacity and energy density. Herein, we develop high‐performance Al/I <jats:sub>2</jats:sub> batteries by employing iodine‐rich 1D perovskite cathodes that leverage the thermodynamically favorable ionic liquid electrolyte environment to achieve a four‐electron I <jats:sup>+</jats:sup> /I <jats:sup>0</jats:sup> /I <jats:sup>−</jats:sup> redox process. These perovskite cathodes lower the reaction barrier for I <jats:sup>+</jats:sup> /I <jats:sup>0</jats:sup> conversion and suppress the shuttle effect of iodine species through hydrogen bonding and halogen bonding interactions, ensuring cycling stability and a stable environment for four‐electron transfer reaction. The I <jats:sup>+</jats:sup> formed can be effectively stabilized by AlCl <jats:sub>4</jats:sub> <jats:sup>−</jats:sup> , further accelerating the reaction kinetics. Through organic and metal cation engineering to modulate bonding interactions and electronic properties, the benzamidinium and Bi <jats:sup>3+</jats:sup> ‐based perovskite (PFABiI <jats:sub>4</jats:sub> ) cathode achieves a high specific capacity of 311.2 mAh g <jats:sup>−1</jats:sup> <jats:sub>I</jats:sub> at 0.2 A g <jats:sup>−1</jats:sup> and exceptional cycling stability, with a capacity decay rate of only 0.0056% per cycle over 8000 cycles at 2 A g <jats:sup>−1</jats:sup> . This work opens an avenue for designing high‐voltage, high‐energy‐density, and long‐cycle‐life Al/I <jats:sub>2</jats:sub> batteries.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"240 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947324","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}
Kyeong Seob Hwang, Hui‐Wen Liu, Hyogeun Shin, Hyun Wook Kang, Minjin Kang, Jongbaeg Kim, Il‐Joo Cho, Nakwon Choi, Seok Chung, Hong Nam Kim
In the human brain, neurons establish long‐range, unidirectional connections between distinct regions, allowing directional transmission of neuronal signals and the transport of neurotoxic proteins. In this study, a region‐to‐region unidirectional connection in an in vitro brain model that enables the one‐way transfer of signals and molecules is reconstructed. By embedding one brain organoid in hydrogel earlier than the other and promoting neurite outgrowth, it is induced preferential axonal extension toward the later‐seeded organoid, where synaptic connections are formed. This structurally defined unidirectional linkage demonstrated functional unidirectionality, as verified by direction‐specific propagation of electrical activity using dual neural probe monitoring. The model also reproduced directional neuroinflammatory spread following region‐specific introduction of activated microglia. Furthermore, it permitted unidirectional transfer of neurotoxic proteins, including amyloid beta (Aβ), Tau, and alpha‐synuclein (α‐synuclein). Owing to its ability to recapitulate in vivo‐like neuronal functionality, this in vitro brain model provides a valuable experimental platform for elucidating the directional propagation of neuropathological processes.
{"title":"Region‐to‐Region Unidirectional Connection In Vitro Brain Model for Studying Directional Propagation of Neuropathologies","authors":"Kyeong Seob Hwang, Hui‐Wen Liu, Hyogeun Shin, Hyun Wook Kang, Minjin Kang, Jongbaeg Kim, Il‐Joo Cho, Nakwon Choi, Seok Chung, Hong Nam Kim","doi":"10.1002/adfm.202516238","DOIUrl":"https://doi.org/10.1002/adfm.202516238","url":null,"abstract":"In the human brain, neurons establish long‐range, unidirectional connections between distinct regions, allowing directional transmission of neuronal signals and the transport of neurotoxic proteins. In this study, a region‐to‐region unidirectional connection in an in vitro brain model that enables the one‐way transfer of signals and molecules is reconstructed. By embedding one brain organoid in hydrogel earlier than the other and promoting neurite outgrowth, it is induced preferential axonal extension toward the later‐seeded organoid, where synaptic connections are formed. This structurally defined unidirectional linkage demonstrated functional unidirectionality, as verified by direction‐specific propagation of electrical activity using dual neural probe monitoring. The model also reproduced directional neuroinflammatory spread following region‐specific introduction of activated microglia. Furthermore, it permitted unidirectional transfer of neurotoxic proteins, including amyloid beta (Aβ), Tau, and alpha‐synuclein (α‐synuclein). Owing to its ability to recapitulate in vivo‐like neuronal functionality, this in vitro brain model provides a valuable experimental platform for elucidating the directional propagation of neuropathological processes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"46 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947325","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}
This study presents a sustainable strategy to transform iron‐accumulating algae—an environmental nuisance—into high‐performance iron single‐atom catalysts (Fe‐SACs), enabling efficient Fenton‐like catalysis with full lifecycle sustainability. We selected 16 distinct polluting algal species, including eleven iron‐accumulating types with varying iron contents and five iron‐free species for comparison. Iron contents with a range of 0.022–1.56 wt.% could be achieved in the Fe‐SACs derived from iron‐accumulating algae using a tailored pyrolysis approach after urea treatment for increasing nitrogen content to coordinate with the iron atom. We found that the iron species after transferring into single‐atom iron could promote the catalytic activity based on the catalytic roles of fundamental compositions in these algae and urea‐derived nitrogen species. A certain correlation ( R2 = 0.69) was observed between the iron contents in these iron‐accumulating catalysts and the resulting catalytic performances for pollutant degradation. A full lifecycle assessment (LCA) was further conducted to quantitatively evaluate the environmental benefits of this “waste‐to‐wealth” strategy compared to the conventional algae disposal method. Importantly, the principle established here—using naturally iron‐enriched biomass, such as iron‐accumulating plants grown in distinctive soils like the red soils of Southern China, or iron‐rich sewage sludge, as precursors—exhibits broad applicability for water purification.
{"title":"From Algal Threat to Fe/N‐Rich Single‐Atom Catalyst: Engineering Iron‐Accumulating Algae for High‐Performance Fenton‐Like Chemistry and Lifecycle Sustainability","authors":"Dengzheng Zhang, Zhengheng Xu, Xing Xu, Tongtong Wang, Weixuan Huang, Binrong Li, Yali Guo, Hanghang Zhao","doi":"10.1002/adfm.202529134","DOIUrl":"https://doi.org/10.1002/adfm.202529134","url":null,"abstract":"This study presents a sustainable strategy to transform iron‐accumulating algae—an environmental nuisance—into high‐performance iron single‐atom catalysts (Fe‐SACs), enabling efficient Fenton‐like catalysis with full lifecycle sustainability. We selected 16 distinct polluting algal species, including eleven iron‐accumulating types with varying iron contents and five iron‐free species for comparison. Iron contents with a range of 0.022–1.56 wt.% could be achieved in the Fe‐SACs derived from iron‐accumulating algae using a tailored pyrolysis approach after urea treatment for increasing nitrogen content to coordinate with the iron atom. We found that the iron species after transferring into single‐atom iron could promote the catalytic activity based on the catalytic roles of fundamental compositions in these algae and urea‐derived nitrogen species. A certain correlation ( <jats:italic>R</jats:italic> <jats:sup>2</jats:sup> = 0.69) was observed between the iron contents in these iron‐accumulating catalysts and the resulting catalytic performances for pollutant degradation. A full lifecycle assessment (LCA) was further conducted to quantitatively evaluate the environmental benefits of this “waste‐to‐wealth” strategy compared to the conventional algae disposal method. Importantly, the principle established here—using naturally iron‐enriched biomass, such as iron‐accumulating plants grown in distinctive soils like the red soils of Southern China, or iron‐rich sewage sludge, as precursors—exhibits broad applicability for water purification.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"29 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947328","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}