{"title":"Vertically Arrayed Co4N/MoN Nanosheets for Robust Alkaline Electrocatalytic Hydrogen Evolution at Ampere-Level Current Density","authors":"Can Li, Ningning Wang, Shuo Wang, Chenyang Li, Wenjun Fan, Taifeng Liu, Shanshan Chen, Fuxiang Zhang","doi":"10.1002/adfm.202423856","DOIUrl":"https://doi.org/10.1002/adfm.202423856","url":null,"abstract":"Metal nitride electrocatalysts have been extensively developed for efficient alkaline water splitting, but it still remains a huge challenge in improving their stability especially at high current density of over 500 mA cm<sup>−2</sup>. Herein the Co<sub>4</sub>N/MoN electrocatalyst with hierarchical nanoparticle-assembled nanosheet arrays is fabricated by a facile electrodeposition-nitridation method for alkaline hydrogen evolution reaction (HER). Results show that it exhibits an impressively low overpotential of 238 mV and high durability at 1.0 A cm<sup>−2</sup> for over 100 h, which is the best among the reported cobalt-based nitride electrocatalysts with both excellent HER activity and robust stability at ampere-level current density. The superior intrinsic HER activity is mainly ascribed to the synergistic effect of Co<sub>4</sub>N and MoN, which can effectively reduce the H<sub>2</sub>O dissociation energy barrier and accelerate the alkaline HER kinetics. Moreover, benefiting from the vertically arrayed nanosheet structure with a solid framework and excellent mechanical strength, robust water electrolysis even at ampere-level current density can be achieved. This work provides an alternative way to develop metal nitride electrocatalysts via fabricating hierarchical heterostructure for efficient and stable industrial water splitting.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"129 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418242","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}
Bo Zhao, Lixian Song, Zhijuan Zou, Zhu Xiong, Yunfeng Zhang, Qin Yang, Zixiong Shi, Yaping Zhang, Yingze Song
{"title":"Electrospun Ti3C2 MXene Fiber-Decorated Interlayer for Synchronous Sulfur Activation and Lithium Stabilization","authors":"Bo Zhao, Lixian Song, Zhijuan Zou, Zhu Xiong, Yunfeng Zhang, Qin Yang, Zixiong Shi, Yaping Zhang, Yingze Song","doi":"10.1002/adfm.202500079","DOIUrl":"https://doi.org/10.1002/adfm.202500079","url":null,"abstract":"Concurrent regulation of sulfur redox kinetics and lithium deposition homogeneity is a key prerequisite for achieving high-performance lithium–sulfur (Li–S) batteries. To this end, rational design of dual-functional interlayers is recognized as a feasible yet promising approach. Herein, few-layered Ti<sub>3</sub>C<sub>2</sub> MXene flakes are uniformly decorated into the porous carbon nanofiber film via a straightforward electrostatic spinning technique, wherein the Ti<sub>3</sub>C<sub>2</sub> MXene content is fine-tuned to maximum sulfur utilization and stabilize lithium anode. For one thing, it is revealed by synchrotron radiation X-ray three-dimensional nano-computed tomography that Ti<sub>3</sub>C<sub>2</sub> MXene-decorated fiber can expedite polysulfide conversion and induce favorable Li<sub>2</sub>S nucleation. For another, small-angle neutron scattering evidence substantiates that abundant lithiophilic sites are conducive to homogenizing Li-ion flux and promoting lithium deposition during cycling procedure. As a consequence, Li–S batteries maintain a stable operation at 2.0 C over 1000 cycles with a low-capacity degeneration rate of 0.057% per cycle, accompanied by a superior areal capacity of 7.5 mAh cm<sup>−2</sup> when the sulfur loading is increased to 9.5 mg cm<sup>−2</sup>. More encouragingly, the as-assembled multi-layer Li–S pouch cell deliver an impressive cell energy density of 342.3 Wh kg<sup>−1</sup> with smooth cyclic operation.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418321","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}
{"title":"Interlayer Assembly of Thin-Film Composite Membranes With Ultra-Interfacial Adhesion","authors":"Chao Sang, Siyuan Zhang, Geng Li, Hanzhu Wu, Siyu Pang, Yan Zhuang, Lankun Wang, Shilong Dong, Songyuan Yao, Lu Lu, Zhihao Si, Peng-Fei Cao, Peiyong Qin","doi":"10.1002/adfm.202420130","DOIUrl":"https://doi.org/10.1002/adfm.202420130","url":null,"abstract":"Thin-film composite (TFC) membranes are considered as an effective architecture to achieve selective separation for various application scenarios. However, most polymeric separation layers are in physically contacted with an underlying porous substrate, where the physical exfoliation or over-swelling of the selective layer severely shortens the usage lifespan. In this work, a novel interlayer assembly design is proposed to realize a polydimethylsiloxane (PDMS)/polyvinylidene fluoride (PVDF) TFC membrane with ultra-interfacial adhesion via the UV-triggered covalent attachment. Especially, by overcoming the chemical inertness of PVDF, the synthetic methacrylate-functionalized PVDF substrate is rapidly copolymerized with the methacrylate-functionalized PDMS layer. It shows that the critical load for selective layer failure is 56.92 mN with applied nano-scratch, 59% higher than the pristine one and also being the highest interfacial strength among the reported state-of-the-art ones. The resulting membrane also shows an excellent pervaporation performance for phenol than the pristine one, and a stable running with an average separation factor of 7.3 and membrane flux of 3142 g m<sup>−2</sup> h<sup>−1</sup> under extreme conditions (e.g., high phenol concentration of 20 wt.% and high temperature of 80 °C). This interlayer chemically bonded design principle provides a scalable approach to develop ultra-stable and efficient-separation TFC membranes adaptable to various separation purposes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"11 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418323","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}
{"title":"Regulating the Mott–Hubbard Splitting for High-Performance Co-Free Li-Rich Mn-Based Oxide Cathode","authors":"Tianyu Wang, Ruoyu Wang, Jicheng Zhang, Guangxue Zhao, Wen Yin, Nian Zhang, Lirong Zheng, Xiangfeng Liu","doi":"10.1002/adfm.202423843","DOIUrl":"https://doi.org/10.1002/adfm.202423843","url":null,"abstract":"Co-free Li-rich Mn-based layered oxides attract great attention as next-generation cathodes due to high specific capacity and low cost. However, their practical applications are hindered by the structural damage and poor cycling stability caused by the irreversible oxygen anion redox (OAR). Herein, a distinct strategy for regulating Mott–Hubbard splitting to address the detrimental issues is proposed. Introducing cations with specific electronic properties into the Li layer and transition metal (TM) layer decreases the Mott–Hubbard splitting energy (U) of TM cations, which promotes the electron removal and optimizes the band structure. This causes the antibonding band (M─O)* to rise and reduces its overlap with O2p band, thereby simultaneously enhancing the redox activity of TMs and the reversibility of OAR. The specific capacity, rate capability, and capacity retention are all significantly improved (255 mAh g<sup>−1</sup> vs 223 mAh g<sup>−1</sup> at 0.1C;197 mAh g<sup>−1</sup> vs168 mAh g<sup>−1</sup> at 1C;147 mAh g<sup>−1</sup> vs115 mAh g<sup>−1</sup> at 5 C; 93.2% vs 75.5% at 1C after 400 cycles). The oxygen release and voltage decay are also mitigated (92.4% vs 85.6% at 1C after 400 cycles). Moreover, a quantitative method to estimate U value is established for the first time. These findings provide insights into the intrinsic interaction mechanism of anions and cations redox and provide guidance for designing high-performance cathodes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"135 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418383","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}
{"title":"Controllable Growth of Monocrystalline MoS2/Polycrystalline ReS2 Lateral Heterojunction for High Quantum Efficiency Photodetector","authors":"Jiaxi Li, Jinrong Chen, Yixun He, Jiaying Xiao, Guoqiang Li, Wenliang Wang","doi":"10.1002/adfm.202421508","DOIUrl":"https://doi.org/10.1002/adfm.202421508","url":null,"abstract":"Photodetectors (PDs) based on 2D transition metal dichalcogenides (2D TMDCs) heterojunction have become a potential candidate for frontier technology applications such as visible light communication (VLC). However, the conventional 2D TMDCs heterojunction PDs are facing problems with excessive dark current and low photoelectric conversion efficiency, resulting in the performance of PDs not meeting application requirements. Herein, the controllable growth of monocrystalline MoS<sub>2</sub>/polycrystalline ReS<sub>2</sub> lateral heterojunction via a two-step chemical vapor deposition (CVD) method has been proposed. According to the result of density functional theory (DFT) calculation and the characterization of multiple parallel experiments under different conditions, the controllable growth of lateral heterojunction, especially the competition mechanism between lateral epitaxy and vertical stacking is systematically analyzed from different perspectives. Based on the analysis above, a strategy for preparing monocrystalline MoS<sub>2</sub>/polycrystalline ReS<sub>2</sub> lateral heterojunction with a large-scale epitaxy layer and a high-quality lateral structure is provided. Finally, PDs based on the as-grown lateral heterojunction with responsivity and external quantum efficiency (EQE) up to 2.65 A W<sup>−1</sup> and 506% are successfully applied to the VLC demonstration. This work provides a potential approach for the design and fabrication of optoelectronic devices with the requirement of high responsivity and photoelectric conversion efficiency.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"87 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418396","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}
Bingkun Huang, Bin Wang, Feifei Zhao, Haizeng Li, William W. Yu
{"title":"A Dual-Mode Anode-Free Zinc-Prussian Blue Electrochromic Device","authors":"Bingkun Huang, Bin Wang, Feifei Zhao, Haizeng Li, William W. Yu","doi":"10.1002/adfm.202423532","DOIUrl":"https://doi.org/10.1002/adfm.202423532","url":null,"abstract":"Conventional Prussian blue (PB)-based electrochromic devices (ECDs) suffer from a narrow light modulation range due to their single absorption band. Herein, an anode-free Zn-PB electrochromic device is reported, utilizing a platinum (Pt) layer-modified ITO glass (denoted as Pt/ITO glass) counter electrode with a hybrid electrolyte containing propylene carbonate (PC). This device compensated for the charge released or consumed during the bleaching/coloring process of the PB electrode (i.e., ion-insertion/extraction) through a reversible Zn electrodeposition occurring on the surface of the Pt/ITO glass. The Pt layer ensured a uniformly distributed electric field across the electrode surface, leading to uniform Zn deposition. Concurrently, PC molecules modified the solvation structures of ions, engendering uniform Zn deposition and suppressing the “ion trapping” effect of PB. Meanwhile, PC suppressed water activity by changing the H-bonding network of electrolytes, thereby limiting the formation of by-products, the occurrence of side reactions, and the destruction of the PB structure. As a result, the optimized anode-free Zn-PB ECDs demonstrated high transmittance modulation ability (60.3% at 700 nm) and exceptional cycling durability (71.7% capacity retention and 69.1% of its initial <i>ΔT</i> after 1000 cycles). Finally, a dual-mode electrochromic device is developed with five color states to expand the light modulation range.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"30 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418011","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}
Xiaoyin Zhang, Bin Lian, Hujun Shen, Shaoan Cheng, Fujun Li
{"title":"Challenges and Strategies for Multi-Electron Reactions in High-Energy Phosphate-Based Cathodes for Sodium-Ion Batteries","authors":"Xiaoyin Zhang, Bin Lian, Hujun Shen, Shaoan Cheng, Fujun Li","doi":"10.1002/adfm.202420864","DOIUrl":"https://doi.org/10.1002/adfm.202420864","url":null,"abstract":"Sodium-ion batteries (SIBs) have been considered as promising candidates for large-scale energy storage systems and low-speed electric vehicles due to abundant sodium resources and low cost. Phosphate-based cathodes stand out for their high voltages, structural stability, superior safety, etc. However, their large molecular weight limits the overall capacity, compromising the energy density for practical applications. Recent advancements in multi-electron reactions based on transition metal (TM) ions provide a promising pathway to achieve both high energy density and stability. This review discusses the fundamental principles behind the multi-electron reactions of phosphate-based cathodes from the perspectives of electrochemistry and materials science. The key factors, such as the conservation of matter and charge, thermodynamic, and kinetic feasibility, are addressed for activating and regulating the multi-electron reactions, aiming for a high capacity exceeding 170 mAh g<sup>−1</sup>. The current progress in NASICON-type phosphate cathodes is summarized, and the challenges associated with pyrophosphate and mixed phosphate cathodes are analyzed for multi-electron reactions. Finally, the perspectives on the future development of high-energy phosphate-based cathodes are provided.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"1 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418350","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}
Abdulrahman Al-Shami, Haozheng Ma, Melissa Banks, Farbod Amirghasemi, Mona A Mohamed, Ali Soleimani, Sina Khazaee Nejad, Victor Ong, Alessandro Tasso, Alara Berkmen, Maral P. S. Mousavi
{"title":"Mom and Baby Wellness with a Smart Lactation Pad: A Wearable Sensor-Embedded Lactation Pad for on-Body Quantification of Glucose in Breast Milk","authors":"Abdulrahman Al-Shami, Haozheng Ma, Melissa Banks, Farbod Amirghasemi, Mona A Mohamed, Ali Soleimani, Sina Khazaee Nejad, Victor Ong, Alessandro Tasso, Alara Berkmen, Maral P. S. Mousavi","doi":"10.1002/adfm.202420973","DOIUrl":"https://doi.org/10.1002/adfm.202420973","url":null,"abstract":"Wearable sensors are transforming healthcare by facilitating rapid, non-invasive, on-body biochemical analysis in biofluids such as sweat, tears, saliva, and blood, providing real-time insights into health conditions. Despite extensive academic and industrial efforts in developing wearable devices, very few are tailored to meet women's health needs. None are specifically designed for measurements in human breast milk. Beyond being the optimal source of infant nutrition, milk serves as a rich biofluid containing potential biomarkers reflecting a mother's health as well. Analyzing the composition of milk offers valuable information for the health of the infant, and the mother. This work pioneers a wearable sensor embedded in a lactation pad for on-body sampling of breast milk and continuous analysis of glucose levels in breast milk. Lactation pads are worn by most lactating individuals to absorb milk leakage during the day, and keep the cloth dry. In this work, by integrating microfluidic channels and electrochemical sensors in the lactation pad, milk sampling and analysis becomes part of an existing daily routine for the mother, posing no additional burden for milk sampling and analysis. The electrochemical sensors are developed using laser-induced carbonization of polyimide thin films, allowing for development of flexible, low-cost, and high-surface area electrodes. Glucose sensing is done via an enzymatic membrane composed of glucose oxidase, glutaraldehyde, bovine serum albumin, and Nafion to achieve enhanced enzyme protection and extended biosensor shelf life and operation in milk. Notably, the wearable device demonstrates high accuracy (96.8 to 104.1%) in measurement of glucose in whole undiluted human milk, collected 1st, 6th, and 12th months postpartum. This innovative smart lactation pad empowers mothers to track their babies' glucose intake and potentially identify early signs of health concerns.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"16 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417955","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}
Wanqing Zhang, Xiaoman Ding, Jie Lv, Xiaokang Sun, Dingqin Hu, Guangye Zhang, Chuanlin Gao, Yizebang Xue, Yufei Zhong, Gang Li, Hanlin Hu
{"title":"Advancing Organic Photovoltaics: the Role of Dipole Distance and Acidity in Perylene-Diimide Electron Transport Layers","authors":"Wanqing Zhang, Xiaoman Ding, Jie Lv, Xiaokang Sun, Dingqin Hu, Guangye Zhang, Chuanlin Gao, Yizebang Xue, Yufei Zhong, Gang Li, Hanlin Hu","doi":"10.1002/adfm.202420588","DOIUrl":"https://doi.org/10.1002/adfm.202420588","url":null,"abstract":"The electronic transport layer (ETL) based on perylene-diimide (PDI) has been widely demonstrated for efficient organic solar cells (OSCs). However, the effect of ETL materials on interfacial traps and energy losses remains understudied. This study investigates the effects of dipole distance on PDINN interface defects using three specifically designed weak acidic materials with varying carboxyl and hydroxyl group amounts. Among these, 3,5-dihydroxybenzoic acid (2OH), with moderate pH and high dipole distance, enhanced intermolecular forces with PDINN. This interaction boosted π–π stacking, enhanced ohmic contact with the active layer and Ag electrode. The P-2OH film exhibited a higher and more uniform potential distribution, suppressing charge recombination at the interface, reducing the trap density to 2.12 × 10<sup>16</sup> cm<sup>3</sup>, and reducing the non-radiative loss ∆E<sub>3</sub> from 0.236 to 0.174 eV. Consequently, the energy loss decreased from 0.553 to 0.484 meV for the PM6: BTP-ec9/P-2OH device. Notably, a decent PCE of 19.1% is achieved for P-2OH (10 nm), and it impressively remains a power conversion efficiency (PCE) of 16.4% when thickness of P-2OH up to 50 nm. This work underscores the importance of hydroxyl and carboxyl groups in regulating the ETL to minimize energy loss and offers insights for developing thickness-insensitive interlayers for high-performance OSCs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"113 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417958","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}