Advanced Functional Materials最新文献_第8页

Laser Derived Co1Ni1@MOF with Efficient Charge Exchanges Boosting Selective Catalytic Hydrogenation

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-30 DOI: 10.1002/adfm.202421357

Jiulong Wang, Lanxing Ren, Yan Kong, Yazhou Shuang, Qian Ye, Chunxia Hong, Shiyuan Wang, Zelin Ma, Fang Wang, Jie Jian, XiaoLi Fan, Lijuan Song, Tengfei Cao, Hongqiang Wang

{"title":"Laser Derived Co1Ni1@MOF with Efficient Charge Exchanges Boosting Selective Catalytic Hydrogenation","authors":"Jiulong Wang, Lanxing Ren, Yan Kong, Yazhou Shuang, Qian Ye, Chunxia Hong, Shiyuan Wang, Zelin Ma, Fang Wang, Jie Jian, XiaoLi Fan, Lijuan Song, Tengfei Cao, Hongqiang Wang","doi":"10.1002/adfm.202421357","DOIUrl":"https://doi.org/10.1002/adfm.202421357","url":null,"abstract":"Metal–organic framework (MOF) catalysts promise selective hydrogenation of C═O bonds, a process that is thermodynamically unfavorable because of the presence of C─O, C═C, and C─C bonds within furan rings. However, the reactivity and stability of MOF are often impeded in catalytic reactions by structural collapse or phase transition stemming from commonly employed strategies such as defect engineering. The present work investigates a novel strategy for designing highly active Co₁Ni₁@UiO-66-NH₂ catalysts by embedding Co₁Ni₁ within the UiO-66-NH₂ framework. This approach facilitates efficient charge transfer between the reactants and the catalysts, thereby preserving both reactivity and structural integrity. The turnover frequency of Co1Ni1@UiO-66-NH2 is 430 h⁻¹, in contrast to 18 h⁻¹ of UiO-66-NH2, demonstrating that the transfer hydrogenation activity of Co1Ni1@UiO-66-NH2 is 24 times greater than that of UiO-66-NH2. More importantly, the reaction rate achieves 7.27 mol g⁻¹ h⁻¹, with a furfuryl alcohol (FOL) yield of 100%, and the Co₁Ni₁@UiO-66-NH₂ catalyst retains its excellent catalytic activity even after eight cycles of applications. Density functional theory calculations indicate that, in comparison to UiO-66-NH₂, Co- and Ni@UiO-66-NH₂, Co₁Ni₁@UiO-66-NH₂ exhibits relatively strong interactions and significant charge exchanges between reactants and catalysts. These interactions not only facilitate the dehydrogenation of isopropanol but also enhance the hydrogenation of furfural. Furthermore, the density of states reveals a greater number of states near the Fermi level in Co1Ni1@UiO-66-NH2 compared to Co- and Ni@UiO-66-NH2, and thereby facilitates the substantial charge exchanges and efficient catalytic performance of Co1Ni1@UiO-66-NH2.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"7 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901749","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Humidity-Resistant Wearable Triboelectric Nanogenerator Utilizing a Bound-Water-Rich Zwitterionic Hydrogel With Microphase-Separated Domains

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202421164

Yutong Ding, Hongxin Guo, Mi Ouyang, Ge Meng, Feng Chen, Tairong Kuang

{"title":"Humidity-Resistant Wearable Triboelectric Nanogenerator Utilizing a Bound-Water-Rich Zwitterionic Hydrogel With Microphase-Separated Domains","authors":"Yutong Ding, Hongxin Guo, Mi Ouyang, Ge Meng, Feng Chen, Tairong Kuang","doi":"10.1002/adfm.202421164","DOIUrl":"https://doi.org/10.1002/adfm.202421164","url":null,"abstract":"Triboelectric nanogenerators (TENGs) represent an effective approach for transforming mechanical energy into electrical power, making them suitable for wearable electronic applications. Hydrogels as TENGs electrodes are common, but their use as direct triboelectric layers remains insufficiently explored. Here, a novel zwitterionic monomer 3-{1-[6-(hydroxymethyl)-2-methyl-3,8-dioxo-9-aza-4,7-dioxadodec-1-en-12-yl]imidazol-3-ium-3-yl}propane-1-sulfonate (VNIPS) is synthesized in combination with acrylic acid (AA) and zwitterionic sulfobetaine methacrylate (SBMA) to create a double-network zwitterionic hydrogel. The hydrogel is developed using a solvent-exchange process that facilitated the creation of microphase-separated domains, notablely increasing its mechanical strength (211.9 kPa, 472.3%), conductivity (0.6 mS cm−1), and anti-freezing capability (−18.3 °C). In addition, the hydrogel's hydrophilic groups interacted with water molecules, reducing charge loss in humid conditions. When employed as the triboelectric positive layer, the hydrogel-based TENGs achieved a substantial charge density of 456 µC m−2 and an output power density of 464 mW m−2, while maintaining a steady open-circuit voltage (Voc) of 97 V, with 92% retention under 80% relative humidity. Moreover, the hydrogel's strong adhesion and biocompatibility make it suitable for wearable applications, such as motion sensing and Morse code communication. This work demonstrates the feasibility of zwitterionic hydrogels as triboelectric materials, providing a new strategy for creating efficient, humidity-resistant energy harvesters.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"33 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901793","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Off-Photosensitizing Derived Immuno-Photodynamic Therapy toward Postoperative Care

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202419598

Jing Li, E Pang, Jusung An, Zhao Xiong, Eunji Kim, Minhuan Lan, Qian-Yong Cao, Jong Seung Kim

{"title":"Off-Photosensitizing Derived Immuno-Photodynamic Therapy toward Postoperative Care","authors":"Jing Li, E Pang, Jusung An, Zhao Xiong, Eunji Kim, Minhuan Lan, Qian-Yong Cao, Jong Seung Kim","doi":"10.1002/adfm.202419598","DOIUrl":"https://doi.org/10.1002/adfm.202419598","url":null,"abstract":"Immuno-photodynamic therapy (IPDT) has emerged as a promising cancer treatment strategy. However, conventional IPDT faces challenges related to post-treatment safety, owing to the use of residual photosensitizers (PSs). In this study, on a novel H2O2-responsive aggregation-induced emission PS is reported, TBZPYBE, designed to selectively target cancer cells and enhance the therapeutic efficacy and postoperative safety of IPDT. Although TBZPYBE exhibits weak fluorescence, strong reactive oxygen species (ROS) are produced under light irradiation, demonstrating its high photodynamic therapy (PDT) efficacy in vitro and in vivo. Following PDT, TBZPYBE underwent self-quenching in the presence of H2O2, converting it to TBZPY, which exhibits strong fluorescence but reduced ROS generation. Simultaneously, quinone methide, a glutathione scavenger that amplifies PDT efficiency, is released. Furthermore, TBZPYBE activated the immune response by promoting dendritic cell maturation and polarizing M2 to M1 macrophages. The observed IPDT effects of TBZPYBE can be attributed to tumor selectivity, self-quenching mechanisms, and the ability to trigger immune responses, offering a balanced cancer treatment approach with improved post-treatment safety.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"70 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901871","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dislocation-Induced Local and Global Photoconductivity Enhancement and Mechanisms in Iron-Doped SrTiO3

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202417952

Mehrzad Soleimany, Till Frömling, Jürgen Rödel, Marin Alexe

引用次数: 0

Thickness-Dependent Heat Dissipation in CrOCl Heat-Escaping Channel

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202412469

Yu Yang, Yan Zhou, Gang Zhang, Fanyu Liu, Bo Li, Yunshan Zhao, Lifa Zhang

引用次数: 0

Defect Engineering of Bi2SeO2 Thermoelectrics

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202416509

Andrei Novitskii, Michael Y. Toriyama, Illia Serhiienko, Takao Mori, G. Jeffrey Snyder, Prashun Gorai

{"title":"Defect Engineering of Bi2SeO2 Thermoelectrics","authors":"Andrei Novitskii, Michael Y. Toriyama, Illia Serhiienko, Takao Mori, G. Jeffrey Snyder, Prashun Gorai","doi":"10.1002/adfm.202416509","DOIUrl":"https://doi.org/10.1002/adfm.202416509","url":null,"abstract":"Bi2SeO2 is a promising n-type semiconductor to pair with p-type BiCuSeO in a thermoelectric (TE) device. The TE figure of merit zT and, therefore, the device efficiency must be optimized by tuning the carrier concentration. However, electron concentrations in self-doped n-type Bi2SeO2 span several orders of magnitude, even in samples with the same nominal compositions. Such unsystematic variations in the electron concentration have a thermodynamic origin related to the variations in native defect concentrations. In this study, first-principles calculations are used to show that the selenium vacancy, which is the source of n-type conductivity in Bi2SeO2, varies by 1–2 orders of magnitude depending on the thermodynamic conditions. It is predicted that the electron concentration can be enhanced by synthesizing under more Se-poor conditions and/or at higher solid-state reaction temperatures (TSSR), which promote the formation of selenium vacancies without introducing extrinsic dopants. The computational predictions are validated through solid-state synthesis of Bi2SeO2. More than two orders of magnitude increase are observed in the electron concentration simply by adjusting the synthesis conditions. Additionally, a significant effect of grain boundary scattering on the electron mobility in Bi2SeO2 is revealed, which can also be controlled by adjusting TSSR. By simultaneously optimizing the electron concentration and mobility, a zT of ≈0.2 is achieved at 773 K for self-doped n-type Bi2SeO2. The study highlights the need for careful control of thermodynamic growth conditions and demonstrates TE performance improvement by varying synthesis parameters according to thermodynamic guidelines.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"41 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901864","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Nickel-Based Hollow Spheres with Optimized Interfacial Electronic Structures by Highly Dispersed MoN for Efficient Urea Electrolysis

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202421222

Yuying Fan, Zhihui Li, Yue Liu, Jianan Liu, Dongxu Wang, Haijing Yan, Aleksandr I. Gubanov, Aiping Wu, Chungui Tian

{"title":"Nickel-Based Hollow Spheres with Optimized Interfacial Electronic Structures by Highly Dispersed MoN for Efficient Urea Electrolysis","authors":"Yuying Fan, Zhihui Li, Yue Liu, Jianan Liu, Dongxu Wang, Haijing Yan, Aleksandr I. Gubanov, Aiping Wu, Chungui Tian","doi":"10.1002/adfm.202421222","DOIUrl":"https://doi.org/10.1002/adfm.202421222","url":null,"abstract":"Ni-Mo-based catalysts that exhibit well-synergized and readily accessible catalytic sites are ideal catalysts for achieving efficient electrocatalysis. Herein, the synthesis of hollow Ni spheres with a hierarchical nanosheet surface modified by highly dispersed MoN for efficient urea electrolysis is reported. This synthesis is based on the design of hollow Mo-Ni precursors featuring a nanosheet array surface, achieved through the phosphomolybdic acid (PMo12)-mediated reconstruction of hollow Ni-BTC spheres. The optimized MoN-Ni catalyst can effectively drive both the urea oxidation reaction (UOR) and hydrogen evolution reaction at low potentials of 1.37 V and 191 mV, respectively, achieving a current density of 100 mA cm−2. The electrolytic cell utilizing these catalysts can sustain 100 mA cm−2 at a low voltage of 1.53 V and can operate continuously for over 220 h. The X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) analyses demonstrate the established built-in electric field facilitates electron transfer from MoN to Ni, optimizing the d-band center and consequently reducing the reaction barrier for the UOR. In situ electrochemical impedance spectroscopy (EIS) and in situ Fourier-transform infrared spectroscopy analyses indicate that MoN promotes the formation of high-valent Ni sites, which accelerates the UOR and facilitates the urea eletrolysis through a more environmentally friendly “carbonate” pathway.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"7 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901799","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhanced Transformation Kinetics of Polysulfides Enabled by Synergistic Catalysis of Functional Graphitic Carbon Nitride for High-Performance Li-S Batteries

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202420351

Peng Chen, Tianyu Huang, Tianyu Wei, Bing Ding, Hui Dou, Xiaogang Zhang

{"title":"Enhanced Transformation Kinetics of Polysulfides Enabled by Synergistic Catalysis of Functional Graphitic Carbon Nitride for High-Performance Li-S Batteries","authors":"Peng Chen, Tianyu Huang, Tianyu Wei, Bing Ding, Hui Dou, Xiaogang Zhang","doi":"10.1002/adfm.202420351","DOIUrl":"https://doi.org/10.1002/adfm.202420351","url":null,"abstract":"The introduction of an electrocatalyst to accelerate the kinetics of lithium polysulfides (LiPSs) reduction/oxidation is beneficial to enhance the capacity of sulfur cathode and inhibit the shuttling effect of LiPSs. However, current electrocatalysts mainly focus on the metal-based active sites to reduce the reaction barriers, and there remains a great challenge in developing light-weighted metal-free catalysts. In this work, 1D graphitic carbon nitride nanorods (g-C3N4-NRs) with carboxyl (─COOH) and acylamide (─CONH2) functional groups are designed as metal-free electrocatalysts for lithium-sulfur batteries to accelerate the transport of Li+ and the conversion of LiPSs. The density functional theory (DFT) calculations prove that the existence of ─COOH group realizes the adsorption of LiPSs and accelerates the transport of Li+, while the ─CONH2 groups reduce the reaction energy barrier of S8 to Li2S. In addition, in situ UV–vis and Li2S nucleation/dissociation experiments also verify that g-C3N4-NRs achieve rapid adsorption and transformation of LiPSs under the synergistic action of ─COOH and ─CONH2 functional groups. Consequently, the sulfur cathode based on the g-C3N4-NRs-PP separator remains at a specific capacity of 700.3 mAh g−1 after 70 cycles at 0.2 C, at 0 °C. This work provides a new strategy for breaking through the bottleneck of metal-free catalysts for high-performance lithium-sulfur batteries.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"202 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901806","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

In Situ Polymerized Fluorine-Free Ether Gel Polymer Electrolyte with Stable Interface for High-Voltage Lithium Metal Batteries

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202421965

Xuanfeng Chen, Fulu Chu, Daqing Li, Mingjiang Si, Mengting Liu, Feixiang Wu

{"title":"In Situ Polymerized Fluorine-Free Ether Gel Polymer Electrolyte with Stable Interface for High-Voltage Lithium Metal Batteries","authors":"Xuanfeng Chen, Fulu Chu, Daqing Li, Mingjiang Si, Mengting Liu, Feixiang Wu","doi":"10.1002/adfm.202421965","DOIUrl":"https://doi.org/10.1002/adfm.202421965","url":null,"abstract":"Lithium metal batteries offer increased energy density compared to traditional lithium-ion batteries. Commercial carbonate-based electrolytes are incompatible with lithium metal anodes, while ether-based electrolytes, though more suitable, tend to degrade under high potentials. Here, a fluorine-free ether-based gel polymer electrolyte (FEGPE) has been developed via incorporating lithium bis((trifluoromethyl)sulfonyl)azanide (LiTFSI) as lithium salt, 1,2-dimethoxyethane (DME) and 1,3-dioxolane (DOL) as solvents, and indium trifluoromethanesulphonate (In(OTF)3) as an initiator. DME is used to promote dissolution of the In(OTF)3 in DOL, along with enhanced ion transport of the FEGPE. Compared to traditional ether-based liquid electrolytes, the FEGPE demonstrates significantly improved antioxidant decomposition ability at high potentials, stemming from intermolecular hydrogen bond formation and decreased lone-pair electron activity of ether oxygen. Additionally, the FEGPE reduces the lithium deposition energy barrier and enables a stable electrolyte/electrode interface by forming Li-In alloys and LiF components in solid electrolyte interphases. In turn, Li|FEGPE|LiFePO4 cells exhibit a high initial capacity of 151 mAh g−1 at 0.5 C, with an outstanding capacity retention of 97% over 300 cycles. For high-voltage cathodes, Li|FEGPE|LiN0.8iCo0.1Mn0.1O2 cells deliver an initial capacity of 167 mAh g−1 at 1 C, achieving a capacity retention of 75% over 500 cycles.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"81 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901796","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Precursor Engineering for the Electrode of Vanadium Redox Flow Batteries

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2024-12-29 DOI: 10.1002/adfm.202418799

Shangkun Wang, Yingqiao Jiang, Zemin Feng, Yongguang Liu, Long Jiang, Lei Dai, Jing Zhu, Ling Wang, Zhangxing He

{"title":"Precursor Engineering for the Electrode of Vanadium Redox Flow Batteries","authors":"Shangkun Wang, Yingqiao Jiang, Zemin Feng, Yongguang Liu, Long Jiang, Lei Dai, Jing Zhu, Ling Wang, Zhangxing He","doi":"10.1002/adfm.202418799","DOIUrl":"https://doi.org/10.1002/adfm.202418799","url":null,"abstract":"As the demand for scalable electrochemical energy storage increases, vanadium redox flow batteries (VRFBs) offer multiple advantages due to their inherent safety, environmental friendliness, and power-to-capacity decoupling capability. However, the intrinsic structural limitations of the electrodes, coupled with deficiencies in their surface properties, significantly impede the practical implementation of VRFBs. The systematic optimization of electrodes through precursor engineering represents a forward-thinking approach with significant potential for advancing the field. In this paper, recent advances in VRFB electrodes are comprehensively reviewed from the perspective of precursor engineering. To begin with, the advantages based on different types of precursors and processing methods are elucidated. Next, the focus is on the additive modification and design of electrodes through various precursor engineering strategies to optimize their structural and surface properties. Lastly, this review also discusses the current dilemmas faced by the four types of precursor engineering and explores future directions. It is hoped that this review will contribute to the further innovation and production application of VRFB electrode materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"83 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901800","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0