Dmitrii Iudin, Mies J. van Steenbergen, Rosalinde Masereeuw, Bas G. P. van Ravensteijn, Tina Vermonden
The availability of realistic in vitro models is crucial for tissue engineering, disease modeling, and drug screening assays. However, reproducing the complex shapes and intricate structures of naturally occurring tissues or organs in the presence of functional cells remains a challenge. For example, it is still not trivial to obtain cell-laden tubular structures on a micrometer scale present in the nephrons of the human kidney. Here, a unique hydrogel-based shrinking approach making use of host–guest interactions to decrease the diameters of the preformed hydrogel tubules seeded with cells is proposed as a tool to overcome the abovementioned challenge. The hydrogels are composed of covalently crosslinked methacrylated hyaluronic acid and methacrylated dextran modified with either cyclodextrin or adamantane groups that can form dynamic bonds. The hydrogels are initially formed in the presence of small-molecule competitors that block any interpolymer host–guest interactions, and the shrinking process is triggered by the release of these competitor molecules. The high shrinking efficiency with a shrinking factor up to eight times in volume and robust cytocompatibility make the host-guest-based shrinking approach an appealing tool to obtain hydrogel tubular in vitro models with the desired dimensions on demand.
{"title":"Shrinkable Hydrogels through Host–Guest Interactions: A Robust Approach to Obtain Tubular Cell-Laden Scaffolds with Small Diameters","authors":"Dmitrii Iudin, Mies J. van Steenbergen, Rosalinde Masereeuw, Bas G. P. van Ravensteijn, Tina Vermonden","doi":"10.1002/adfm.202416522","DOIUrl":"https://doi.org/10.1002/adfm.202416522","url":null,"abstract":"The availability of realistic in vitro models is crucial for tissue engineering, disease modeling, and drug screening assays. However, reproducing the complex shapes and intricate structures of naturally occurring tissues or organs in the presence of functional cells remains a challenge. For example, it is still not trivial to obtain cell-laden tubular structures on a micrometer scale present in the nephrons of the human kidney. Here, a unique hydrogel-based shrinking approach making use of host–guest interactions to decrease the diameters of the preformed hydrogel tubules seeded with cells is proposed as a tool to overcome the abovementioned challenge. The hydrogels are composed of covalently crosslinked methacrylated hyaluronic acid and methacrylated dextran modified with either cyclodextrin or adamantane groups that can form dynamic bonds. The hydrogels are initially formed in the presence of small-molecule competitors that block any interpolymer host–guest interactions, and the shrinking process is triggered by the release of these competitor molecules. The high shrinking efficiency with a shrinking factor up to eight times in volume and robust cytocompatibility make the host-guest-based shrinking approach an appealing tool to obtain hydrogel tubular in vitro models with the desired dimensions on demand.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"75 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637079","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}
Sampath Gayathri, Paulraj Arunkumar, Dipankar Saha, Dolan Acharya, Jeyakumar Karthikeyan, Jong Hun Han
Engineering metal-oxygen (M‒O) interactions for catalyzing oxygen evolution reaction (OER) by tuning the coordination geometry of metal sites is crucial for improving catalytic performance, which remains unexplored, especially in structurally diverse phosphate-based catalysts. Herein, two NaCoPO4 (NCP) polymorphs with distinct metal coordinations: orthorhombic-Pnma (CoO6) and hexagonal-P65 (CoO4) denoted as O-NCP and H-NCP, respectively are synthesized through unique quenching-based synthesis, to investigate the impact of coordination geometry on M‒O covalency and OER performance. The CoO4 (H-NCP) polymorph delivered superior OER activity with low overpotential at 10 mA cm−2 (η10 = 303 mV) and long-term stability than CoO6-based O-NCP. Spectroscopic and computational studies linked the superior activity of CoO4 to higher Co‒O covalency, enhanced metal electronic states near the Fermi level, and improved electrochemical reconstruction. Further, M‒O covalency regulated OER mechanism, where high-covalent CoO4 follows conventional concerted proton-electron transfer pathway, while CoO6 entails a non-concerted pathway, where the lattice oxygen participation remains unfavorable due to downshifted O 2p band center. Further, OER-active tetrahedral metal is demonstrated in a high-entropy catalyst requiring lower η10 of ≈284 mV. This study unlocks a unique strategy for designing next-generation OER catalysts with superior activity and durability, harnessing the interplay between metal coordination and metal-oxygen covalency.
通过调整金属位点的配位几何来设计催化氧进化反应（OER）的金属-氧（M-O）相互作用对于提高催化性能至关重要，但这一问题仍有待探索，尤其是在结构多样化的磷酸盐基催化剂中。本文通过独特的淬火合成法合成了两种具有不同金属配位的 NaCoPO4（NCP）多晶体：正交-Pnma（CoOO6）和六方-P65（CoO4），分别称为 O-NCP 和 H-NCP，以研究配位几何对 M-O 共价性和 OER 性能的影响。与基于 CoO6 的 O-NCP 相比，CoO4（H-NCP）多晶体在 10 mA cm-2 时具有较低的过电位（η10 = 303 mV）和长期稳定性，具有更高的 OER 活性。光谱和计算研究表明，CoO4 的卓越活性与 Co-O 共价性更高，费米级附近的金属电子态增强以及电化学重构改善有关。此外，M-O 共价调节了 OER 机制，其中高共价 CoO4 遵循传统的协同质子-电子转移途径，而 CoO6 则采用非协同途径，由于 O 2p 带中心下移，晶格氧的参与仍然不利。此外，OER 活性四面体金属在高熵催化剂中得到了证实，需要较低的η10 ≈284 mV。这项研究利用金属配位和金属氧共价之间的相互作用，为设计具有卓越活性和耐久性的下一代 OER 催化剂提供了一种独特的策略。
{"title":"Modulating Coordination-Driven Metal-Oxygen Interaction Triggers Oxygen Evolution in Polymorphic and High-Entropy Phosphate Electrocatalyst","authors":"Sampath Gayathri, Paulraj Arunkumar, Dipankar Saha, Dolan Acharya, Jeyakumar Karthikeyan, Jong Hun Han","doi":"10.1002/adfm.202416834","DOIUrl":"https://doi.org/10.1002/adfm.202416834","url":null,"abstract":"Engineering metal-oxygen (M‒O) interactions for catalyzing oxygen evolution reaction (OER) by tuning the coordination geometry of metal sites is crucial for improving catalytic performance, which remains unexplored, especially in structurally diverse phosphate-based catalysts. Herein, two NaCoPO<sub>4</sub> (NCP) polymorphs with distinct metal coordinations: orthorhombic-<i>Pnma</i> (CoO<sub>6</sub>) and hexagonal-P<i>6<sub>5</sub></i> (CoO<sub>4</sub>) denoted as O-NCP and H-NCP, respectively are synthesized through unique quenching-based synthesis, to investigate the impact of coordination geometry on M‒O covalency and OER performance. The CoO<sub>4</sub> (H-NCP) polymorph delivered superior OER activity with low overpotential at 10 mA cm<sup>−2</sup> (η<sub>10</sub> = 303 mV) and long-term stability than CoO<sub>6</sub>-based O-NCP. Spectroscopic and computational studies linked the superior activity of CoO<sub>4</sub> to higher Co‒O covalency, enhanced metal electronic states near the Fermi level, and improved electrochemical reconstruction. Further, M‒O covalency regulated OER mechanism, where high-covalent CoO<sub>4</sub> follows conventional concerted proton-electron transfer pathway, while CoO<sub>6</sub> entails a non-concerted pathway, where the lattice oxygen participation remains unfavorable due to downshifted O 2p band center. Further, OER-active tetrahedral metal is demonstrated in a high-entropy catalyst requiring lower η<sub>10</sub> of ≈284 mV. This study unlocks a unique strategy for designing next-generation OER catalysts with superior activity and durability, harnessing the interplay between metal coordination and metal-oxygen covalency.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"98 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637081","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}
Chan Guo, Lige Wang, Yunxiang Tang, Zhengyi Yang, Yufei Zhao, Yanyan Jiang, Xiaodong Wen, Fenglong Wang
Developing solid‐solution nano‐alloys from immiscible metals has garnered significant interest; however, the high formation entropy poses substantial challenges in synthesis, hindering a comprehensive understanding of the catalytic mechanisms under alloying effects. Herein, the synthesis of small‐sized (≈2.5 nm) RuxNi1‐x solid‐solution alloy nanoparticles with precisely controlled Ru/Ni ratios across a broad compositional range is reported for the first time, despite their bulk immiscibility. The Ru0.76Ni0.24/TiO2 catalyst, with an optimized Ru/Ni ratio, delivers superior photo‐thermal catalytic activity for CO2 methanation, achieving a CH4 production rate of 3.58 mol gmetal−1 h−1 with 94% selectivity at 250 °C under light irradiation, representing a 2.82‐fold enhancement over monometallic Ru/TiO2. Comprehensive investigations reveal that the reconstruction of electronic structure at Ru–Ni active sites enhances the adsorption/activation of reactants, promotes the transformation of intermediate HCO3* to HCOO*, and facilitates the separation of the photo‐generated charge carriers witnessed by the femtosecond time‐resolved transient absorption (fs‐TA) spectroscopy. These combined effects collectively result in significantly enhanced CH4 formation performance. This work highlights the potential of regulating catalytic sites in immiscible metal combinations for photo‐thermal catalytic CO2 conversion, underscoring the promise of these cost‐effective alloys in heterogeneous catalysis.
{"title":"Enhanced Photo‐Thermal CO2 Methanation with Tunable RuxNi1‐x Catalytic Sites: Alloying Beyond Pure Ru","authors":"Chan Guo, Lige Wang, Yunxiang Tang, Zhengyi Yang, Yufei Zhao, Yanyan Jiang, Xiaodong Wen, Fenglong Wang","doi":"10.1002/adfm.202414931","DOIUrl":"https://doi.org/10.1002/adfm.202414931","url":null,"abstract":"Developing solid‐solution nano‐alloys from immiscible metals has garnered significant interest; however, the high formation entropy poses substantial challenges in synthesis, hindering a comprehensive understanding of the catalytic mechanisms under alloying effects. Herein, the synthesis of small‐sized (≈2.5 nm) Ru<jats:sub>x</jats:sub>Ni<jats:sub>1‐x</jats:sub> solid‐solution alloy nanoparticles with precisely controlled Ru/Ni ratios across a broad compositional range is reported for the first time, despite their bulk immiscibility. The Ru<jats:sub>0.76</jats:sub>Ni<jats:sub>0.24</jats:sub>/TiO<jats:sub>2</jats:sub> catalyst, with an optimized Ru/Ni ratio, delivers superior photo‐thermal catalytic activity for CO<jats:sub>2</jats:sub> methanation, achieving a CH<jats:sub>4</jats:sub> production rate of 3.58 mol g<jats:sub>metal</jats:sub><jats:sup>−1</jats:sup> h<jats:sup>−1</jats:sup> with 94% selectivity at 250 °C under light irradiation, representing a 2.82‐fold enhancement over monometallic Ru/TiO<jats:sub>2</jats:sub>. Comprehensive investigations reveal that the reconstruction of electronic structure at Ru–Ni active sites enhances the adsorption/activation of reactants, promotes the transformation of intermediate HCO<jats:sub>3</jats:sub><jats:sup>*</jats:sup> to HCOO<jats:sup>*</jats:sup>, and facilitates the separation of the photo‐generated charge carriers witnessed by the femtosecond time‐resolved transient absorption (fs‐TA) spectroscopy. These combined effects collectively result in significantly enhanced CH<jats:sub>4</jats:sub> formation performance. This work highlights the potential of regulating catalytic sites in immiscible metal combinations for photo‐thermal catalytic CO<jats:sub>2</jats:sub> conversion, underscoring the promise of these cost‐effective alloys in heterogeneous catalysis.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"69 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637083","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}
When nanoporous aerogels with excellent thermal insulation performance are processed into 1D fibers, they have great potential for application in the field of personal thermal management. However, coping with the impact of external forces, especially radial extrusion, and maintaining the macro morphology and microstructure of aerogels during use are remaining issues. To address these challenges, this study proposes a method that uses ultrafine and ultra-highly entangled bacterial cellulose nanofibers as the basis to achieve high radial elasticity by forming an isomorphic coating of rigid silica on the soft gel skeleton of aerogel fibers. The obtained aerogel fibers can achieve an elastic recovery of 88% over 50 compression cycles under 90% strain, and they can be knotted, woven into textiles, and are washable. This strategy improves the radial compression resistance of aerogel fibers, providing rich possibilities for the development of aerogel fibers with excellent mechanical properties.
{"title":"Ultra-High Radial Elastic Aerogel Fibers for Thermal Insulation Textile","authors":"Jiahui Wang, Lipeng Liu, Wenlian Dong, Junhui Tao, Rui Fu, Yinghui Liu, Xin Yang, Hanqing Yu, Huazheng Sai","doi":"10.1002/adfm.202417873","DOIUrl":"https://doi.org/10.1002/adfm.202417873","url":null,"abstract":"When nanoporous aerogels with excellent thermal insulation performance are processed into 1D fibers, they have great potential for application in the field of personal thermal management. However, coping with the impact of external forces, especially radial extrusion, and maintaining the macro morphology and microstructure of aerogels during use are remaining issues. To address these challenges, this study proposes a method that uses ultrafine and ultra-highly entangled bacterial cellulose nanofibers as the basis to achieve high radial elasticity by forming an isomorphic coating of rigid silica on the soft gel skeleton of aerogel fibers. The obtained aerogel fibers can achieve an elastic recovery of 88% over 50 compression cycles under 90% strain, and they can be knotted, woven into textiles, and are washable. This strategy improves the radial compression resistance of aerogel fibers, providing rich possibilities for the development of aerogel fibers with excellent mechanical properties.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"44 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637085","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}
Bishnu P. Thapaliya, Babafemi Adigun, Tao Wang, Md Dipu Ahmed, Harry M. Meyer, Ivan Popov, Sheng Dai
Ionogels are emerging as high-potential pseudosolid electrolytes for lithium-metal batteries (LMBs), leveraging their intrinsic high ionic conductivity from entrapped ionic liquid (IL) electrolytes. However, their practical application is hindered by poor mechanical strength stemming from the confinement of ILs within a polymer matrix. To address this challenge, the formation of conformal polyion coatings with functional groups is reported to be relevant to LMBs’ application on ionogels, utilizing a layer-by-layer (LbL) assembly strategy. This approach significantly enhances the mechanical strength (Young's modulus and tensile strength) and electrochemical performance of ionogels, owing to the tailored interface modifications introduced by functional groups’ specific conformal polyion coatings. The core of this methodology leverages the inherent ionic structure of ionogels to enable facile interface modification through Coulombic interactions between polyanions and polycations. These conformally coated interface functionalized membranes show improved electrochemical performance when integrated with cathode materials such as LiFePO4 (LFP) and LiNi0.8Mn0.1Co0.1O2 (NMC811) in an LMB configuration, underscoring their potential for robust, high-conductivity, pseudosolid membranes for LMB applications. These innovative pseudosolid membranes offer improved mechanical and electrochemical properties, leading to higher battery efficiency and safety, making them promising candidates for next-generation LMB technology.
{"title":"Mechanically Reinforced Pseudosolid Polyelectrolyte Membranes via Layer-by-Layer Assembly for High-Performing Lithium-Metal Batteries","authors":"Bishnu P. Thapaliya, Babafemi Adigun, Tao Wang, Md Dipu Ahmed, Harry M. Meyer, Ivan Popov, Sheng Dai","doi":"10.1002/adfm.202413966","DOIUrl":"https://doi.org/10.1002/adfm.202413966","url":null,"abstract":"Ionogels are emerging as high-potential pseudosolid electrolytes for lithium-metal batteries (LMBs), leveraging their intrinsic high ionic conductivity from entrapped ionic liquid (IL) electrolytes. However, their practical application is hindered by poor mechanical strength stemming from the confinement of ILs within a polymer matrix. To address this challenge, the formation of conformal polyion coatings with functional groups is reported to be relevant to LMBs’ application on ionogels, utilizing a layer-by-layer (LbL) assembly strategy. This approach significantly enhances the mechanical strength (Young's modulus and tensile strength) and electrochemical performance of ionogels, owing to the tailored interface modifications introduced by functional groups’ specific conformal polyion coatings. The core of this methodology leverages the inherent ionic structure of ionogels to enable facile interface modification through Coulombic interactions between polyanions and polycations. These conformally coated interface functionalized membranes show improved electrochemical performance when integrated with cathode materials such as LiFePO<sub>4</sub> (LFP) and LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) in an LMB configuration, underscoring their potential for robust, high-conductivity, pseudosolid membranes for LMB applications. These innovative pseudosolid membranes offer improved mechanical and electrochemical properties, leading to higher battery efficiency and safety, making them promising candidates for next-generation LMB technology.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"154 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637078","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}
Peng Wu, Yi Li, Yan Luo, Yongxu Yan, Ran Zhuo, Dibo Wang, Ju Tang, Hongye Yuan, Xiaoxing Zhang, Song Xiao
The detection of trace impurity gases in fluorinated gas (F-gas) that are widely used in the industry offers a significant avenue for equipment status monitoring and mitigating unnecessary emissions. However, the formidable electron affinity (EA) and adsorption propensity of F-gas molecules render the identification of trace impurities within a high-concentration F-gas atmosphere exceptionally challenging. Herein, the filtration-sensing strategy is proposed to realize highly sensitive and selective Room Temperature (RT) sensing of trace gases in the F-gas environment. Through the innovative construction of a bilayer structure, comprising Co3(HITP)2 as the overlayer and SnO2 nanofibers (NFs) as the sensing layer, remarkably sensitive detection of trace impurity gases under intense F-gas interference conditions is achieved. The efficacy of the Co3(HITP)2 overlayer is further corroborated through the incorporation of Pd-SnO2 and MoS2-SnO2 sensors, concurrently facilitating targeted quantitative identification within a complex gas mixture environment. The underlying sensing mechanism is predominantly attributed to interatomic adsorption interactions and the modulation of gas diffusion by microporous structures. This work provides pioneering insights into trace impurity detection within high-concentration F-gas atmosphere while presenting a potentially viable solution for the operational maintenance of F-gas-based industrial equipment (F-equipment) in industrial applications.
{"title":"2D MOF-Based Filtration-Sensing Strategy for Trace Gas Sensing Under Intense F-Gas Interference at Room Temperature","authors":"Peng Wu, Yi Li, Yan Luo, Yongxu Yan, Ran Zhuo, Dibo Wang, Ju Tang, Hongye Yuan, Xiaoxing Zhang, Song Xiao","doi":"10.1002/adfm.202415517","DOIUrl":"https://doi.org/10.1002/adfm.202415517","url":null,"abstract":"The detection of trace impurity gases in fluorinated gas (F-gas) that are widely used in the industry offers a significant avenue for equipment status monitoring and mitigating unnecessary emissions. However, the formidable electron affinity (EA) and adsorption propensity of F-gas molecules render the identification of trace impurities within a high-concentration F-gas atmosphere exceptionally challenging. Herein, the filtration-sensing strategy is proposed to realize highly sensitive and selective Room Temperature (RT) sensing of trace gases in the F-gas environment. Through the innovative construction of a bilayer structure, comprising Co<sub>3</sub>(HITP)<sub>2</sub> as the overlayer and SnO<sub>2</sub> nanofibers (NFs) as the sensing layer, remarkably sensitive detection of trace impurity gases under intense F-gas interference conditions is achieved. The efficacy of the Co<sub>3</sub>(HITP)<sub>2</sub> overlayer is further corroborated through the incorporation of Pd-SnO<sub>2</sub> and MoS<sub>2</sub>-SnO<sub>2</sub> sensors, concurrently facilitating targeted quantitative identification within a complex gas mixture environment. The underlying sensing mechanism is predominantly attributed to interatomic adsorption interactions and the modulation of gas diffusion by microporous structures. This work provides pioneering insights into trace impurity detection within high-concentration F-gas atmosphere while presenting a potentially viable solution for the operational maintenance of F-gas-based industrial equipment (F-equipment) in industrial applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"46 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637082","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}
Tao Liu, Xue Cui, Ziyi Ye, Xuedi Li, Yanhua Liu, Bin Luo, Song Zhang, Mingchao Chi, Jinlong Wang, Chenchen Cai, Yayu Bai, Shuangfei Wang, Shuangxi Nie
Harnessing energy from underwater bubbles has garnered significant attention, particularly for powering off-grid circuitry. However, the efficiency of bubble-driven liquid-solid interface charge transfer remains low. This research unveils a phenomenon: accelerated bubble slippage enhances liquid-solid interfacial charge transfer. Building upon this discovery, a pulse bubble-based power generation technique is proposed, achieving an energy density of 24.2 mJ L−1 generated by pulsed bubbles. The crux of pulse bubble power generation lies in the precise control of impact velocity. By meticulously regulating the impact kinetic energy of bubbles, the accumulated potential energy of multiple small bubbles is converted into instantaneous pulse kinetic energy. A typical pulse bubble is controlled within a 72 ms timeframe, unleashing a surge of energy that can directly illuminate 400 light-emitting diodes. This approach represents a groundbreaking advancement in underwater energy harvesting technology, dramatically expanding its potential applications.
{"title":"A Pulsed Bubble-Driven Efficient Liquid-Solid Triboelectric Nanogenerator","authors":"Tao Liu, Xue Cui, Ziyi Ye, Xuedi Li, Yanhua Liu, Bin Luo, Song Zhang, Mingchao Chi, Jinlong Wang, Chenchen Cai, Yayu Bai, Shuangfei Wang, Shuangxi Nie","doi":"10.1002/adfm.202415483","DOIUrl":"https://doi.org/10.1002/adfm.202415483","url":null,"abstract":"Harnessing energy from underwater bubbles has garnered significant attention, particularly for powering off-grid circuitry. However, the efficiency of bubble-driven liquid-solid interface charge transfer remains low. This research unveils a phenomenon: accelerated bubble slippage enhances liquid-solid interfacial charge transfer. Building upon this discovery, a pulse bubble-based power generation technique is proposed, achieving an energy density of 24.2 mJ L<sup>−1</sup> generated by pulsed bubbles. The crux of pulse bubble power generation lies in the precise control of impact velocity. By meticulously regulating the impact kinetic energy of bubbles, the accumulated potential energy of multiple small bubbles is converted into instantaneous pulse kinetic energy. A typical pulse bubble is controlled within a 72 ms timeframe, unleashing a surge of energy that can directly illuminate 400 light-emitting diodes. This approach represents a groundbreaking advancement in underwater energy harvesting technology, dramatically expanding its potential applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"246 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637084","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}
Yan Li, Haoxiang Zhang, Yiwen Su, Yuhan Zou, Wenyi Guo, Changpeng Qiao, Guangping Zheng, Qilu Li, Lai Xu, Jingyu Sun
Electrolyte additive engineering is a feasible protocol in improving Zn anode stability. Typical additive designs center on the regulation of Zn deposition; nevertheless, versatile additives are urgently requested to comprehensively manage the surface landscape, interface physicochemistry, and by-product elimination. Here, a straightforward strategy is presented to meet such needs employing an environmentally-friendly chelator, hydroxyethyl-ethylenediaminetriacetate acid (HEDTA), as an additive for ZnSO4 electrolyte. Throughout theoretical computations and experimental investigations, it is demonstrated that protons released from the gradual ionization of HEDTA during rest periods aid in the mild engraving of the Zn surface. Both the amino and carboxyl groups of HEDTA⁻ can be protonated, which effectively buffers the interfacial pH value in the entire battery lifespan and eliminates the formation of by-products. The HEDTA− anions can also adsorb onto the Zn surface, helping facilitate Zn2⁺ mass transfer and accelerate the desolvation process. Benefiting from the synchronous modulation of surface topography and interfacial physicochemistry, the assembled half cells affording HEDTA additive maintain a durable operation of up to 8821 cycles at 5.0 mA cm−2/1.0 mAh cm−2. Additionally, symmetric cells manifest stable cycling for over 4600 h at 0.5 mA cm−2/0.25 mAh cm−2.
电解质添加剂工程是提高锌阳极稳定性的可行方案。典型的添加剂设计以调节锌沉积为中心；然而，迫切需要多功能添加剂来全面管理表面景观、界面物理化学和副产品消除。本文介绍了一种简单直接的策略，即采用一种环境友好型螯合剂羟乙基乙二胺三乙酸酯（HEDTA）作为 ZnSO4 电解质的添加剂，以满足上述需求。通过理论计算和实验研究证明，HEDTA 在静止期间逐渐电离释放出的质子有助于锌表面的温和雕刻。HEDTA- 的氨基和羧基都能被质子化，从而在整个电池寿命期间有效地缓冲了界面 pH 值，并消除了副产品的形成。HEDTA- 阴离子还能吸附在锌表面，有助于促进 Zn2⁺的传质并加速脱溶过程。得益于表面形貌和界面物理化学的同步调节，添加了 HEDTA 添加剂的组装半电池在 5.0 mA cm-2/1.0 mAh cm-2 的条件下可保持长达 8821 个循环的持久运行。此外，对称电池在 0.5 mA cm-2/0.25 mAh cm-2 的条件下可稳定循环超过 4600 小时。
{"title":"Concurrent Regulation of Surface Topography and Interfacial Physicochemistry via Trace Chelation Acid Additives toward Durable Zn Anodes","authors":"Yan Li, Haoxiang Zhang, Yiwen Su, Yuhan Zou, Wenyi Guo, Changpeng Qiao, Guangping Zheng, Qilu Li, Lai Xu, Jingyu Sun","doi":"10.1002/adfm.202417462","DOIUrl":"https://doi.org/10.1002/adfm.202417462","url":null,"abstract":"Electrolyte additive engineering is a feasible protocol in improving Zn anode stability. Typical additive designs center on the regulation of Zn deposition; nevertheless, versatile additives are urgently requested to comprehensively manage the surface landscape, interface physicochemistry, and by-product elimination. Here, a straightforward strategy is presented to meet such needs employing an environmentally-friendly chelator, hydroxyethyl-ethylenediaminetriacetate acid (HEDTA), as an additive for ZnSO<sub>4</sub> electrolyte. Throughout theoretical computations and experimental investigations, it is demonstrated that protons released from the gradual ionization of HEDTA during rest periods aid in the mild engraving of the Zn surface. Both the amino and carboxyl groups of HEDTA⁻ can be protonated, which effectively buffers the interfacial pH value in the entire battery lifespan and eliminates the formation of by-products. The HEDTA<sup>−</sup> anions can also adsorb onto the Zn surface, helping facilitate Zn<sup>2</sup>⁺ mass transfer and accelerate the desolvation process. Benefiting from the synchronous modulation of surface topography and interfacial physicochemistry, the assembled half cells affording HEDTA additive maintain a durable operation of up to 8821 cycles at 5.0 mA cm<sup>−2</sup>/1.0 mAh cm<sup>−2</sup>. Additionally, symmetric cells manifest stable cycling for over 4600 h at 0.5 mA cm<sup>−2</sup>/0.25 mAh cm<sup>−2</sup>.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"75 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637091","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}
Qi Zheng, Jing-Qi Wang, Wen-Qiang Cao, Hua-Zhang Zhai, Mao-Sheng Cao
Human spaceflight, lunar exploration projects, and interstellar travel are the grand visions of human exploration of the universe. However, the energy sustainability of these projects is a concern. Electromagnetic functional materials and devices are expected to fulfill their potential in electronic communication and energy utilization. Herein, hetero-dimensional micro-nano architectures composed of Cu3Se2 microspheres and reduced graphene oxide (rGO) sheets are fabricated for the first time by the sacrificial template method, anion substitution engineering, electrostatic adsorption, and reduction-oxidation reaction. Based on the excellent electromagnetic response of the composites, they exhibit strong and ultra-wide microwave absorption ability with the effective absorption bandwidth (EAB) reaching 8.24 GHz at a thickness of 2.2 mm. In addition, an electromagnetic metamaterial with an EAB to ≈13.5 GHz is proposed, exhibiting significant properties. More significantly, the composites can be used to construct a range of electromagnetic devices: a spiral antenna with adjustable return loss and gain, with a maximum gain of up to 2.5 dBi; a microstrip power divider that can efficiently split the input signal into four equal parts and output it; a hybridized energy transport device can convert and store electromagnetic energy. This work provides new inspiration for electromagnetic protection, electronic communication, and energy development.
{"title":"Hetero-Dimensional Micro-Nano Architectures Toward Electromagnetic Devices and Hybrid Energy Transport","authors":"Qi Zheng, Jing-Qi Wang, Wen-Qiang Cao, Hua-Zhang Zhai, Mao-Sheng Cao","doi":"10.1002/adfm.202417972","DOIUrl":"https://doi.org/10.1002/adfm.202417972","url":null,"abstract":"Human spaceflight, lunar exploration projects, and interstellar travel are the grand visions of human exploration of the universe. However, the energy sustainability of these projects is a concern. Electromagnetic functional materials and devices are expected to fulfill their potential in electronic communication and energy utilization. Herein, hetero-dimensional micro-nano architectures composed of Cu<sub>3</sub>Se<sub>2</sub> microspheres and reduced graphene oxide (rGO) sheets are fabricated for the first time by the sacrificial template method, anion substitution engineering, electrostatic adsorption, and reduction-oxidation reaction. Based on the excellent electromagnetic response of the composites, they exhibit strong and ultra-wide microwave absorption ability with the effective absorption bandwidth (EAB) reaching 8.24 GHz at a thickness of 2.2 mm. In addition, an electromagnetic metamaterial with an EAB to ≈13.5 GHz is proposed, exhibiting significant properties. More significantly, the composites can be used to construct a range of electromagnetic devices: a spiral antenna with adjustable return loss and gain, with a maximum gain of up to 2.5 dBi; a microstrip power divider that can efficiently split the input signal into four equal parts and output it; a hybridized energy transport device can convert and store electromagnetic energy. This work provides new inspiration for electromagnetic protection, electronic communication, and energy development.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"24 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637092","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}
Shayan Angizi, Mahdis Nankali, Amir Foroozan, Jihyeon Park, Ecem Yelekli Kirici, Navid Noor, Michael Fefer, Yuichi Terazono, Drew Higgins
Partial electro-oxidation using renewable electricity offers a sustainable route for valorizing glycerol, a major by-product of biofuel production. This study introduces a bimetallic electrode with nanostructured platinum dendrites on nickel foam (Pt/NiF), achieving a peak geometric current density of 235 mA cm−2 and a Pt-mass normalized current density of 3.71 for glycerol electro-oxidation at 0.92 V versus a reversible hydrogen electrode (RHE) in 3 m KOH electrolyte containing 1 m glycerol, outperforming most previously reported Pt-containing catalysts. The Pt/NiF electrode demonstrates over 92% cumulative selectivity toward C3 products, with 64% selectivity for lactic acid at 0.65 V versus RHE over 5 h of testing. This research also highlights the role of chemical oxidation pathways (isomerization and rearrangements) in converting glycerol to lactic acid. After 5 h at 0.65 V versus RHE, the Pt/NiF electrode maintains 35% of its initial current density, plateauing at 12.2 mA cm−2 (0.15 ), with performance loss likely due to surface poisoning by carbon-based reaction intermediates/byproducts or passivating platinum (hydr)oxide species. These findings pave the way for developing low-platinum group metal catalysts with high glycerol oxidation affinity and highlight the importance of considering chemical transformations during catalyst evaluation and reactor design.
利用可再生电力进行部分电氧化为生物燃料生产的主要副产品甘油的价值化提供了一条可持续的途径。本研究介绍了一种在泡沫镍（Pt/NiF）上具有纳米结构铂树枝状突起的双金属电极，其峰值几何电流密度为 235 mA cm-2，铂质量归一化电流密度为 3.71 AmgPt-1$ {{mathrm{Amg}}_{{mathrm{Pt}}^{ - {mathrm{1}}$ 在 0.92 V 的电压下与含有 1 m 甘油的 3 m KOH 电解液中的可逆氢电极 (RHE) 相比，甘油电氧化的电流密度达到了 3.71 AmgPt-1${{mathrm{A/mg}}_{{mathrm{Pt}}}^{ - {mathrm{1}}$ ，优于之前报道的大多数含铂催化剂。在 5 小时的测试中，Pt/NiF 电极对 C3 产物的累积选择性超过 92%，在 0.65 V 的电压下，乳酸对 RHE 的选择性为 64%。这项研究还强调了化学氧化途径（异构化和重排）在甘油转化为乳酸过程中的作用。在 0.65 V（相对于 RHE）电压下测试 5 小时后，Pt/NiF 电极的电流密度保持在初始值的 35%，稳定在 12.2 mA cm-2（0.15 AmgPt-1$ {{mathrm{Amg}}_{{mathrm{Pt}}^{ - {mathrm{1}}}$）。这些发现为开发具有高甘油氧化亲和力的低铂族金属催化剂铺平了道路，并强调了在催化剂评估和反应器设计过程中考虑化学转化的重要性。
{"title":"3D Bimetallic Platinum-Nickel Electrodes for Electro-Oxidation of Glycerol at Ambient Conditions","authors":"Shayan Angizi, Mahdis Nankali, Amir Foroozan, Jihyeon Park, Ecem Yelekli Kirici, Navid Noor, Michael Fefer, Yuichi Terazono, Drew Higgins","doi":"10.1002/adfm.202420622","DOIUrl":"https://doi.org/10.1002/adfm.202420622","url":null,"abstract":"Partial electro-oxidation using renewable electricity offers a sustainable route for valorizing glycerol, a major by-product of biofuel production. This study introduces a bimetallic electrode with nanostructured platinum dendrites on nickel foam (Pt/NiF), achieving a peak geometric current density of 235 mA cm<sup>−2</sup> and a Pt-mass normalized current density of 3.71 <span data-altimg=\"/cms/asset/86efbdb2-967f-4524-b6a5-f4818f1abb85/adfm202420622-math-0001.png\"></span><math altimg=\"urn:x-wiley:1616301X:media:adfm202420622:adfm202420622-math-0001\" display=\"inline\" location=\"graphic/adfm202420622-math-0001.png\">\u0000<semantics>\u0000<msubsup>\u0000<mrow>\u0000<mi mathvariant=\"normal\">A</mi>\u0000<mspace width=\"0.33em\"></mspace>\u0000<mi>mg</mi>\u0000</mrow>\u0000<mi>Pt</mi>\u0000<mrow>\u0000<mo>−</mo>\u0000<mn>1</mn>\u0000</mrow>\u0000</msubsup>\u0000${mathrm{A mg}}_{{mathrm{Pt}}}^{ - {mathrm{1}}}$</annotation>\u0000</semantics></math> for glycerol electro-oxidation at 0.92 V versus a reversible hydrogen electrode (RHE) in 3 <span>m</span> KOH electrolyte containing 1 <span>m</span> glycerol, outperforming most previously reported Pt-containing catalysts. The Pt/NiF electrode demonstrates over 92% cumulative selectivity toward C<sub>3</sub> products, with 64% selectivity for lactic acid at 0.65 V versus RHE over 5 h of testing. This research also highlights the role of chemical oxidation pathways (isomerization and rearrangements) in converting glycerol to lactic acid. After 5 h at 0.65 V versus RHE, the Pt/NiF electrode maintains 35% of its initial current density, plateauing at 12.2 mA cm<sup>−2</sup> (0.15 <span data-altimg=\"/cms/asset/3e123cb5-1879-44dd-8a25-a683723d8387/adfm202420622-math-0002.png\"></span><math altimg=\"urn:x-wiley:1616301X:media:adfm202420622:adfm202420622-math-0002\" display=\"inline\" location=\"graphic/adfm202420622-math-0002.png\">\u0000<semantics>\u0000<msubsup>\u0000<mrow>\u0000<mi mathvariant=\"normal\">A</mi>\u0000<mspace width=\"0.33em\"></mspace>\u0000<mi>mg</mi>\u0000</mrow>\u0000<mi>Pt</mi>\u0000<mrow>\u0000<mo>−</mo>\u0000<mn>1</mn>\u0000</mrow>\u0000</msubsup>\u0000${mathrm{A mg}}_{{mathrm{Pt}}}^{ - {mathrm{1}}}$</annotation>\u0000</semantics></math>), with performance loss likely due to surface poisoning by carbon-based reaction intermediates/byproducts or passivating platinum (hydr)oxide species. These findings pave the way for developing low-platinum group metal catalysts with high glycerol oxidation affinity and highlight the importance of considering chemical transformations during catalyst evaluation and reactor design.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"5 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637087","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}
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