Yang-Biao Xue, Hai-Tao Jiang, Peng Luo, Hai-Juan Liu, Yu-Hang Yang, Qian-Kun Xue, Bin Wu, Guo-Liang Zhang, Mi Zheng, Min Zheng, Zuo-Shan Wang, Ming-Peng Zhuo
Flexible self-powered sensors with the significant ability to the information perception, decoding, and conveying processes have attracted tremendous attention in healthcare monitoring, motion detection, and intelligent interaction. Also, the solar thermoelectric technology holding the effective solar energy/heat harvesting capacity for sustainable electricity generation shows attractive prospects in self-powered wearable sensing but is terribly limited by its poor flexibility and complex construction. Herein, a solar thermoelectric system, prepared via facilely sandwiching the self-assemble MoS2/Carbon hollow nanoflower-based fabrics with [Fe(CN)6]3-/4− thermoelectric gels, is successfully applied for the self-powered wearable sensing. Owing to the hollow-heterostructure for the strong light absorption, MoS2/Carbon hollow nanoflower-based fabrics demonstrated a photothermal conversion efficiency of 39.6%. The strong heat concentration can supply a considered temperature gradient of 42.7 K for thermoelectric gels with a Seebeck coefficient of 1.08 mV K−1 under a solar intensity of 1 sun, outputting a voltage density of 101.2 V m−2 with a response of 431 ms. Their promising application in self-powered wearable fields, such as noncontact motion monitoring and language interaction is foreseen.
{"title":"Wearable Solar Ionic Thermoelectric Detectors for Human Motion Monitoring and Language Recognition Conversion","authors":"Yang-Biao Xue, Hai-Tao Jiang, Peng Luo, Hai-Juan Liu, Yu-Hang Yang, Qian-Kun Xue, Bin Wu, Guo-Liang Zhang, Mi Zheng, Min Zheng, Zuo-Shan Wang, Ming-Peng Zhuo","doi":"10.1002/adfm.202422592","DOIUrl":"https://doi.org/10.1002/adfm.202422592","url":null,"abstract":"Flexible self-powered sensors with the significant ability to the information perception, decoding, and conveying processes have attracted tremendous attention in healthcare monitoring, motion detection, and intelligent interaction. Also, the solar thermoelectric technology holding the effective solar energy/heat harvesting capacity for sustainable electricity generation shows attractive prospects in self-powered wearable sensing but is terribly limited by its poor flexibility and complex construction. Herein, a solar thermoelectric system, prepared via facilely sandwiching the self-assemble MoS<sub>2</sub>/Carbon hollow nanoflower-based fabrics with [Fe(CN)<sub>6</sub>]<sup>3-/4−</sup> thermoelectric gels, is successfully applied for the self-powered wearable sensing. Owing to the hollow-heterostructure for the strong light absorption, MoS<sub>2</sub>/Carbon hollow nanoflower-based fabrics demonstrated a photothermal conversion efficiency of 39.6%. The strong heat concentration can supply a considered temperature gradient of 42.7 K for thermoelectric gels with a <i>Seebeck</i> coefficient of 1.08 mV K<sup>−1</sup> under a solar intensity of 1 sun, outputting a voltage density of 101.2 V m<sup>−2</sup> with a response of 431 ms. Their promising application in self-powered wearable fields, such as noncontact motion monitoring and language interaction is foreseen.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375602","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}
Zilu Lin, Yujia Li, Maloy Das, Caihong Liang, Xingchi Xiao, Zhihao Yen, Chandramouli Kulshreshtha, Luke Chia Wei Min, Aren Lim Junan, Kekeli N'konou, Tze Chien Sum, Nripan Mathews, Andrew C. Grimsdale, Leonard W. T. Ng
This study introduces a novel, biomass-derived, furan-based conjugated polymer, PBDF-DFC, enabling a simplified direct precursor integration fabrication method for hybrid perovskite solar cells (HPSCs). Unlike traditional thiophene-based polymers, PBDF-DFC exhibits high solubility in perovskite precursor solvents, allowing direct incorporation into the precursor solution. This direct precursor integration approach significantly streamlines the fabrication process, reducing steps and potentially lowering production costs. The PBDF-DFC-modified HPSCs achieves a power conversion efficiency (PCE) of 21.39%, a 7.8% improvement over the 19.84% PCE of control devices. Moreover, these devices demonstrates enhanced stability under various environmental stresses, retaining 90% of their initial efficiency after over 1100 h of storage compared to 52% for control devices. X-ray diffraction, scanning electron microscopy, and transmission electron microscopy analyses reveals that PBDF-DFC accumulates at grain boundaries, improving film crystallization and reducing defects. This dual innovation of a new polymer and simplified fabrication process presents a promising pathway for more efficient, stable, and potentially more sustainable HPSCs. The successful integration of PBDF-DFC and the direct precursor integration method opens new avenues for streamlined production of high-performance perovskite solar cells, addressing key challenges in scalability and environmental impact.
{"title":"Direct Integration of Biomass-Derived Furan Polymers for Enhanced Stability and Efficiency in Hybrid Perovskite Solar Cells","authors":"Zilu Lin, Yujia Li, Maloy Das, Caihong Liang, Xingchi Xiao, Zhihao Yen, Chandramouli Kulshreshtha, Luke Chia Wei Min, Aren Lim Junan, Kekeli N'konou, Tze Chien Sum, Nripan Mathews, Andrew C. Grimsdale, Leonard W. T. Ng","doi":"10.1002/adfm.202423635","DOIUrl":"https://doi.org/10.1002/adfm.202423635","url":null,"abstract":"This study introduces a novel, biomass-derived, furan-based conjugated polymer, PBDF-DFC, enabling a simplified direct precursor integration fabrication method for hybrid perovskite solar cells (HPSCs). Unlike traditional thiophene-based polymers, PBDF-DFC exhibits high solubility in perovskite precursor solvents, allowing direct incorporation into the precursor solution. This direct precursor integration approach significantly streamlines the fabrication process, reducing steps and potentially lowering production costs. The PBDF-DFC-modified HPSCs achieves a power conversion efficiency (PCE) of 21.39%, a 7.8% improvement over the 19.84% PCE of control devices. Moreover, these devices demonstrates enhanced stability under various environmental stresses, retaining 90% of their initial efficiency after over 1100 h of storage compared to 52% for control devices. X-ray diffraction, scanning electron microscopy, and transmission electron microscopy analyses reveals that PBDF-DFC accumulates at grain boundaries, improving film crystallization and reducing defects. This dual innovation of a new polymer and simplified fabrication process presents a promising pathway for more efficient, stable, and potentially more sustainable HPSCs. The successful integration of PBDF-DFC and the direct precursor integration method opens new avenues for streamlined production of high-performance perovskite solar cells, addressing key challenges in scalability and environmental impact.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"41 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375559","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}
Marine creatures achieve effective survival in unstructured ocean environments via fast swimming or transparent camouflage. Aqueous soft robots, capable of reproducing soft features of marine creatures, have the advantages of safe biological interaction, high environmental adaptation, and noise-free when compared with traditional rigid robots. Yet, there exists a persistent challenge to develop both fast and energy-efficient aqueous soft robots that can achieve better underwater operation or exploration. Enlightened by the morphology and swimming strategy of Ocyropsis — a jellyfish-like creature, Ocyropsis-inspired robots (i.e., Ocyrobots) that merge electro-hydraulic actuation and Ocyropsis-type rowing mechanisms to achieve high-performance underwater locomotion are developed. Ocyrobots demonstrate a record-high speed of 1.1 body length/s, which is approximately three times of previously reported fastest jellyfish-like robots while maintaining a low power consumption of 37 mW. Ocyrobots also exhibit an impressive turning speed of 34° s−1, enabling dexterous locomotion and effective obstacle avoidance in confined underwater scenarios. Attributed to the self-developed highly reliable polymer-based ionic gel, Ocyrobots possess remarkable advantages of full transparency and high durability, which improves their lifetime and reduces potential disturbances to underwater ecosystems. The unprecedented biomimetic idea in this study is essential in enlightening the prototyping of future aqueous soft robotics.
{"title":"Ocyropsis-Inspired Fast-Swimming Transparent Soft Robots","authors":"Zhiqiu Ye, Geng Yang, Huaixuan Dai, Yinliang Gan, Yihui Jian, Kaichen Xu, M. Jamal Deen, Jiaxu Xia, Nichen Tian, Yihong Yang, Huayong Yang, Chao Zhang","doi":"10.1002/adfm.202421522","DOIUrl":"https://doi.org/10.1002/adfm.202421522","url":null,"abstract":"Marine creatures achieve effective survival in unstructured ocean environments via fast swimming or transparent camouflage. Aqueous soft robots, capable of reproducing soft features of marine creatures, have the advantages of safe biological interaction, high environmental adaptation, and noise-free when compared with traditional rigid robots. Yet, there exists a persistent challenge to develop both fast and energy-efficient aqueous soft robots that can achieve better underwater operation or exploration. Enlightened by the morphology and swimming strategy of <i>Ocyropsis</i> — a jellyfish-like creature, <i>Ocyropsis</i>-inspired robots (i.e., Ocyrobots) that merge electro-hydraulic actuation and <i>Ocyropsis</i>-type rowing mechanisms to achieve high-performance underwater locomotion are developed. Ocyrobots demonstrate a record-high speed of 1.1 body length/s, which is approximately three times of previously reported fastest jellyfish-like robots while maintaining a low power consumption of 37 mW. Ocyrobots also exhibit an impressive turning speed of 34° s<sup>−1</sup>, enabling dexterous locomotion and effective obstacle avoidance in confined underwater scenarios. Attributed to the self-developed highly reliable polymer-based ionic gel, Ocyrobots possess remarkable advantages of full transparency and high durability, which improves their lifetime and reduces potential disturbances to underwater ecosystems. The unprecedented biomimetic idea in this study is essential in enlightening the prototyping of future aqueous soft robotics.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"51 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375560","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}
Ximing Li, Qibing Dong, Junjun Wang, Xinxin Liang, Peter K. J. Robertson, Fei Li, Ming Guo, Wonyong Choi, Chuanyi Wang
Precisely modulating the chemical microenvironment of catalytic centers at the molecular level to achieve efficient photocatalytic nitrogen fixation remains a grand challenge. Herein, a polyoxometalates (POMs) metalloporphyrin organic framework Fe-PMOF {POM-TCPP(Fe)} is constructed by integrating the oxygen-rich unit POMs {ε-PMo8VMo4VIO40Zn4} and the photosensitive metalloporphyrin (Fe-TCPP) as a model to precisely regulate intermolecular electron transfer. Benefiting from electronic interactions, the optimized POM-TCPP(Fe) exhibits a favorable activity toward NH3 production with a rate of 110.06 µmol g−1 h−1. The improved performance can be attributed to the effective regulation of the chemical microenvironment surrounding the active centers, enabling the synergistic interaction of multiple active sites (Fe and Mo) to facilitate the adsorption and activation of nitrogen. More specifically, oxygen-rich unit POMs exhibit strong electronegativity, which can attract electrons from Fe atoms, thereby decreasing the 3d orbitals’ electron density of Fe sites and elevating its unoccupied d-orbitals to facilitate N2 adsorption. Moreover, the porphyrin units with high photosensitivity efficiently generate electrons under photoexcitation, which can rapidly migrate and inject them to the active Fe-N-N* sites to facilitate N2 activation. Ultimately, the mimic nitrogenase active site intelligently integrates multiple active sites of transition metals Fe and Mo, thus improving the nitrogen fixation efficiency.
{"title":"Molecular Engineering of Active Fe Center in Metalloporphyrin Coupled with Polyoxometalates for Efficient Photochemical Nitrogen Fixation: Synergistic Effect of Multiactive Sites Strengthening Metal-N-N* Interactions","authors":"Ximing Li, Qibing Dong, Junjun Wang, Xinxin Liang, Peter K. J. Robertson, Fei Li, Ming Guo, Wonyong Choi, Chuanyi Wang","doi":"10.1002/adfm.202424128","DOIUrl":"https://doi.org/10.1002/adfm.202424128","url":null,"abstract":"Precisely modulating the chemical microenvironment of catalytic centers at the molecular level to achieve efficient photocatalytic nitrogen fixation remains a grand challenge. Herein, a polyoxometalates (POMs) metalloporphyrin organic framework Fe-PMOF {POM-TCPP(Fe)} is constructed by integrating the oxygen-rich unit POMs {ε-PMo<sub>8</sub><sup>V</sup>Mo<sub>4</sub><sup>VI</sup>O<sub>40</sub>Zn<sub>4</sub>} and the photosensitive metalloporphyrin (Fe-TCPP) as a model to precisely regulate intermolecular electron transfer. Benefiting from electronic interactions, the optimized POM-TCPP(Fe) exhibits a favorable activity toward NH<sub>3</sub> production with a rate of 110.06 µmol g<sup>−1</sup> h<sup>−1</sup>. The improved performance can be attributed to the effective regulation of the chemical microenvironment surrounding the active centers, enabling the synergistic interaction of multiple active sites (Fe and Mo) to facilitate the adsorption and activation of nitrogen. More specifically, oxygen-rich unit POMs exhibit strong electronegativity, which can attract electrons from Fe atoms, thereby decreasing the 3d orbitals’ electron density of Fe sites and elevating its unoccupied d-orbitals to facilitate N<sub>2</sub> adsorption. Moreover, the porphyrin units with high photosensitivity efficiently generate electrons under photoexcitation, which can rapidly migrate and inject them to the active Fe-N-N* sites to facilitate N<sub>2</sub> activation. Ultimately, the mimic nitrogenase active site intelligently integrates multiple active sites of transition metals Fe and Mo, thus improving the nitrogen fixation efficiency.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"84 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375569","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 construction of a 3D conductive structure with cavities is an effective strategy to suppress volume change and shuttle effect of tin sulfide materials during lithium storage, while the influence of cavity size on its electrochemical properties is yet to be clarified due to the lack of controllable methods. Herein, a 3D network-structured hybrid material is reported by a template-induced self-assembly strategy, featuring adjustable spherical cavities with uniformly anchored ultrafine SnS2 nanosheets inside (3D-SnS2@rGO), which allows for an ideal cavity volume occupancy rate of 98%. Moreover, the integrated and interconnected 3D cavity structure raises lithium-ion diffusion kinetics and provides transport pathways for electrons. The optimal 3D-SnS2@rGO material demonstrates superior initial coulombic efficiency (ICE) of 88% and a notable reversible capacity of 1274 mAh g−1 at 0.5 A g−1 along with an excellent capacity retention rate of 102% over 340 cycles. Even after 1000 and 2500 cycles at the current densities of 1 and 5 A g−1, it maintains capacities of 910 and 410 mAh g−1, indicating outstanding volume adaptability and space utilization. Additionally, this facile method can be applied to synthesize other high-performance anode materials (such as MoS2) with similar integrated 3D structure and high ICE, indicating its good scalability.
{"title":"Enabling High Initial Coulombic Efficiency for Li-ion Storage via 3D SnS2@rGO Anode With Tailorable Cavity Size","authors":"Jinyang Zhao, Chengyu Zhu, Jianjiang Mao, Fei Cheng","doi":"10.1002/adfm.202424339","DOIUrl":"https://doi.org/10.1002/adfm.202424339","url":null,"abstract":"The construction of a 3D conductive structure with cavities is an effective strategy to suppress volume change and shuttle effect of tin sulfide materials during lithium storage, while the influence of cavity size on its electrochemical properties is yet to be clarified due to the lack of controllable methods. Herein, a 3D network-structured hybrid material is reported by a template-induced self-assembly strategy, featuring adjustable spherical cavities with uniformly anchored ultrafine SnS<sub>2</sub> nanosheets inside (3D-SnS<sub>2</sub>@rGO), which allows for an ideal cavity volume occupancy rate of 98%. Moreover, the integrated and interconnected 3D cavity structure raises lithium-ion diffusion kinetics and provides transport pathways for electrons. The optimal 3D-SnS<sub>2</sub>@rGO material demonstrates superior initial coulombic efficiency (ICE) of 88% and a notable reversible capacity of 1274 mAh g<sup>−1</sup> at 0.5 A g<sup>−1</sup> along with an excellent capacity retention rate of 102% over 340 cycles. Even after 1000 and 2500 cycles at the current densities of 1 and 5 A g<sup>−1</sup>, it maintains capacities of 910 and 410 mAh g<sup>−1</sup>, indicating outstanding volume adaptability and space utilization. Additionally, this facile method can be applied to synthesize other high-performance anode materials (such as MoS<sub>2</sub>) with similar integrated 3D structure and high ICE, indicating its good scalability.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"129 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375603","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}
2D transition metal dichalcogenides (TMDs) materials with inherent flexibility, transparency, and sizable bandgap have gained significant attention as promising candidates for future semiconductor nanodevices. However, complementary doping in these 2D semiconductors remains a challenge because conventional ion implantation can lead to permanent damage to the atomically thin 2D channels. Here, programmable WSe2 2D lateral p-n homojunction controlled by dual floating gates on a SiO2/Si substrate, achieving a rectification ratio of ≈105 and three dynamically switchable current levels is demonstrated. By injecting charges into two floating gates by applying voltage pulses with different polarities, lateral p-n, n-p, n-n, p-p homojunction can be formed. The ideality factors for the p-n and n-p junctions are extracted as ≈1.56 and ≈1.57, respectively. The WSe2 p-n homojunction shows a maximum photovoltage responsivity of 6.67 × 109 V W−1 under a weak light power of 0.09 nW. These results demonstrate outstanding electrical and optoelectronic properties in the programmable 2D lateral p-n junctions, establishing a solid foundation for the development of future non-volatile reconfigurable devices.
{"title":"Programmable WSe2 2D Lateral p-n Junctions Controlled by Dual Floating Gates","authors":"Nuertai Jiazila, Peng Song, Chijun Wei, Xuanye Liu, Hui Gao, Jiequn Sun, Chengze Du, Hui Guo, Haitao Yang, Lihong Bao, Hong-Jun Gao","doi":"10.1002/adfm.202423196","DOIUrl":"https://doi.org/10.1002/adfm.202423196","url":null,"abstract":"2D transition metal dichalcogenides (TMDs) materials with inherent flexibility, transparency, and sizable bandgap have gained significant attention as promising candidates for future semiconductor nanodevices. However, complementary doping in these 2D semiconductors remains a challenge because conventional ion implantation can lead to permanent damage to the atomically thin 2D channels. Here, programmable WSe<sub>2</sub> 2D lateral p-n homojunction controlled by dual floating gates on a SiO<sub>2</sub>/Si substrate, achieving a rectification ratio of ≈10<sup>5</sup> and three dynamically switchable current levels is demonstrated. By injecting charges into two floating gates by applying voltage pulses with different polarities, lateral p-n, n-p, n-n, p-p homojunction can be formed. The ideality factors for the p-n and n-p junctions are extracted as ≈1.56 and ≈1.57, respectively. The WSe<sub>2</sub> p-n homojunction shows a maximum photovoltage responsivity of 6.67 × 10<sup>9</sup> V W<sup>−1</sup> under a weak light power of 0.09 nW. These results demonstrate outstanding electrical and optoelectronic properties in the programmable 2D lateral p-n junctions, establishing a solid foundation for the development of future non-volatile reconfigurable devices.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375604","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}
HCOOH can be used as a hydrogen donor in catalytic transfer hydrogenation (CTH) or a hydrogen storage molecule. The desorption-combination of H* species from H-binding sites after dissociation of HCOOH is necessary for hydrogen evolution reaction (HER) but undesired for CTH. In this work, it is found that the process of high-temperature calcination can cause defects in the nitrogen-doped carbon anchored single atom Co catalyst (Co1-N-C) and adjust the electronic state of Co, thereby affecting the H-binding energy on single atom Co sites. The three-coordinated single atom Co with the most abundant defects (def-CoN3) has best catalytic activity in CTH of nitrobenzene using FA as hydrogen donor in reductive formylation reaction. While the single atom Co with minimal defects (CoN3) shows optimal HER efficiency of HCOOH than def-CoN3 and four-coordinated single atom Co. Through density functional theory calculation, the defective sites promoted the dissociation of HCOOH and H* absorption but inhibited the H* desorption, which is conducive to CTH. The H* is moderately absorbed on defect-free CoN3 and easily desorbed to generate H2 molecule. The regulation on defect structures of single atom Co will provide new avenue for designing catalysts in catalytic processes involving H-atom transfer.
{"title":"The Defects of Single Atom Co1-N-C Regulate the H-Binding Energy to Achieve Divergent Hydrogen Evolution or Transfer Hydrogenation with HCOOH","authors":"Shanshan Lv, Yan Zhou, Wenjuan Yang, Manman Song, Feng Li, Mengmeng Feng, Chen Chen, Zheng Chen","doi":"10.1002/adfm.202423864","DOIUrl":"https://doi.org/10.1002/adfm.202423864","url":null,"abstract":"HCOOH can be used as a hydrogen donor in catalytic transfer hydrogenation (CTH) or a hydrogen storage molecule. The desorption-combination of H<sup>*</sup> species from H-binding sites after dissociation of HCOOH is necessary for hydrogen evolution reaction (HER) but undesired for CTH. In this work, it is found that the process of high-temperature calcination can cause defects in the nitrogen-doped carbon anchored single atom Co catalyst (Co<sub>1</sub>-N-C) and adjust the electronic state of Co, thereby affecting the H-binding energy on single atom Co sites. The three-coordinated single atom Co with the most abundant defects (def-CoN<sub>3</sub>) has best catalytic activity in CTH of nitrobenzene using FA as hydrogen donor in reductive formylation reaction. While the single atom Co with minimal defects (CoN<sub>3</sub>) shows optimal HER efficiency of HCOOH than def-CoN<sub>3</sub> and four-coordinated single atom Co. Through density functional theory calculation, the defective sites promoted the dissociation of HCOOH and H<sup>*</sup> absorption but inhibited the H<sup>*</sup> desorption, which is conducive to CTH. The H<sup>*</sup> is moderately absorbed on defect-free CoN<sub>3</sub> and easily desorbed to generate H<sub>2</sub> molecule. The regulation on defect structures of single atom Co will provide new avenue for designing catalysts in catalytic processes involving H-atom transfer.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375605","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}
Nonaromatic amino acids with intrinsic photoluminescence (PL) have drawn growing attention due to their crucial role in the luminescence of natural proteins. However, the weak luminescence significantly constrains the study of specific photophysical processes, emission mechanism of biomolecules, and their applications. Here, a serendipitous finding of synergistic PL enhancement by coupling nonaromatic amino acids and sugars via glycosidic bonds is reported. For example, the crystals of glucose, L-serine, alongside their corresponding disaccharide and dipeptide are weakly emissive, while glycosylation drastically boosts the quantum yields of L-serine crystals from 0.3% to as high as 9.2%, accompanied by the emergence of pronounced persistent room temperature phosphorescence (p-RTP). This synergistic PL enhancement arises from the ingenious integration of the electron-rich oxygen clusters present in sugar with the charge separation characteristics of amino acids. Furthermore, the ultrafast femtosecond to nanosecond transient absorption spectroscopy and theoretical calculations further reveal the importance of hybridization of locally excited and charge transfer states for PL enhancement and p-RTP features. These results not only provide a universal strategy for constructing efficient nonconventional luminophores but also shed new light on the underlying mechanism of biological autofluorescence.
{"title":"Synergistic Photoluminescence Enhancement in Nonaromatic Amino Acids and Sugars via Glycosylation","authors":"Qiang Zhang, Zihao Zhao, Guangxin Yang, Anze Li, Yijing Cui, Yusong Cai, Zhuojie Yin, Yuntian Tan, Chenyang Zhou, Qian Peng, Wang Zhang Yuan","doi":"10.1002/adfm.202423603","DOIUrl":"https://doi.org/10.1002/adfm.202423603","url":null,"abstract":"Nonaromatic amino acids with intrinsic photoluminescence (PL) have drawn growing attention due to their crucial role in the luminescence of natural proteins. However, the weak luminescence significantly constrains the study of specific photophysical processes, emission mechanism of biomolecules, and their applications. Here, a serendipitous finding of synergistic PL enhancement by coupling nonaromatic amino acids and sugars via glycosidic bonds is reported. For example, the crystals of glucose, L-serine, alongside their corresponding disaccharide and dipeptide are weakly emissive, while glycosylation drastically boosts the quantum yields of L-serine crystals from 0.3% to as high as 9.2%, accompanied by the emergence of pronounced persistent room temperature phosphorescence (p-RTP). This synergistic PL enhancement arises from the ingenious integration of the electron-rich oxygen clusters present in sugar with the charge separation characteristics of amino acids. Furthermore, the ultrafast femtosecond to nanosecond transient absorption spectroscopy and theoretical calculations further reveal the importance of hybridization of locally excited and charge transfer states for PL enhancement and p-RTP features. These results not only provide a universal strategy for constructing efficient nonconventional luminophores but also shed new light on the underlying mechanism of biological autofluorescence.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"55 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375645","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}
Circularly polarized luminescence (CPL) holds great potential for next-generation display techniques. However, dynamic, multicolor CPL with high luminescent quantum yield (PLQY) and tunable dissymmetry factor (glum) based on cost-effective, sustainable materials is scarcely attainable. Herein, a straightforward approach is proposed for engineering cellulose nanocrystal (CNC) chiral superstructures loaded with aggregation-induced emission luminogens (AIEgens) through the evaporation-induced self-assembly of renewable CNCs and tetra-(4-pyridylphenyl)ethylene molecules. The judicious design of two building blocks as chiral donor–acceptor pairs not only respectively achieves an 86-fold and 2.1-fold improvement in the PLQY of resulting systems in the suspension and aggregate states in comparison with bare AIEgens, but also endows AIEgen-loaded CNC chiral superstructures with pH-tunable, humidity-responsive, multicolor CPL with a maximal |glum| of 0.89. It is revealed that chiral induction and photonic bandgap effects—which are dominated by chiral donor–acceptor interactions and homogeneous or heterogeneous self-assembly processes—are involved in CPL mechanisms. Finally, humidity-responsive multiple changes (structural color, fluorescent color, CPL) are realized in both biobased inks and films, which is of paramount importance for potential applications in multicolor dynamic display and information encryption. This work offers the underlying insights for the construction of cost-effective, renewable superstructures with dynamically tunable CPL.
{"title":"Tunable and Responsive Circularly Polarized Luminescence of Self-Organized Cellulose Nanocrystal Chiral Superstructures Loaded with AIE Luminogen","authors":"Baohua Yuan, Jing Qin, Longxiang He, Zuowei Zhang, Yue Feng, Liezheng Lv, Xiao Wang, Cheng Zou, Meina Yu, Yuanwei Chen, Yanzi Gao, Huai Yang","doi":"10.1002/adfm.202424601","DOIUrl":"https://doi.org/10.1002/adfm.202424601","url":null,"abstract":"Circularly polarized luminescence (CPL) holds great potential for next-generation display techniques. However, dynamic, multicolor CPL with high luminescent quantum yield (PLQY) and tunable dissymmetry factor (<i>g</i><sub>lum</sub>) based on cost-effective, sustainable materials is scarcely attainable. Herein, a straightforward approach is proposed for engineering cellulose nanocrystal (CNC) chiral superstructures loaded with aggregation-induced emission luminogens (AIEgens) through the evaporation-induced self-assembly of renewable CNCs and tetra-(4-pyridylphenyl)ethylene molecules. The judicious design of two building blocks as chiral donor–acceptor pairs not only respectively achieves an 86-fold and 2.1-fold improvement in the PLQY of resulting systems in the suspension and aggregate states in comparison with bare AIEgens, but also endows AIEgen-loaded CNC chiral superstructures with pH-tunable, humidity-responsive, multicolor CPL with a maximal |<i>g</i><sub>lum</sub>| of 0.89. It is revealed that chiral induction and photonic bandgap effects—which are dominated by chiral donor–acceptor interactions and homogeneous or heterogeneous self-assembly processes—are involved in CPL mechanisms. Finally, humidity-responsive multiple changes (structural color, fluorescent color, CPL) are realized in both biobased inks and films, which is of paramount importance for potential applications in multicolor dynamic display and information encryption. This work offers the underlying insights for the construction of cost-effective, renewable superstructures with dynamically tunable CPL.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375568","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, Zhuo Zhao, Rongrong Liang, Huanjie He, Yanhua Liu, Kang Yu, Mingchao Chi, Bin Luo, Jinlong Wang, Song Zhang, Chenchen Cai, Shuangfei Wang, Shuangxi Nie
The synergistic integration of elastic porous material with self-powered sensing capabilities holds immense promise for smart wearable devices. However, the intrinsic contradiction between elasticity and strength has hindered the mechanical performance of elastic porous materials. This research reports a diffusion-driven layer-by-layer assembly strategy to enhance the mechanical strength of elastic porous materials. As a prerequisite, the anisotropic layered structure of natural materials is leveraged to endow the porous material with fundamental elasticity. Subsequently, vacuum and chemically-assisted enhanced solvent diffusion are sequentially employed to assemble conductive and elastic layers on cellulose from the inside out. This endows the triboelectric material (TM) with exceptional mechanical properties (elastic strain range of 0–80%, compressive strength reaching 4.55 MPa). Utilizing the TM as a sensing material, a self-powered sensor with a response time of 48 ms and a sensitivity of 0.57 kPa−1 is constructed. Moreover, the application of the sensor in a smart wearable helmet is demonstrated, enabling remote monitoring and traceability of head impact events. This research has overcome the incompatibility between the high strength and elasticity of porous materials and offers promising avenues for their utilization in smart wearable devices.
{"title":"Tough and Elastic Anisotropic Triboelectric Materials Enabled by Layer-by-Layer Assembly","authors":"Tao Liu, Zhuo Zhao, Rongrong Liang, Huanjie He, Yanhua Liu, Kang Yu, Mingchao Chi, Bin Luo, Jinlong Wang, Song Zhang, Chenchen Cai, Shuangfei Wang, Shuangxi Nie","doi":"10.1002/adfm.202500207","DOIUrl":"https://doi.org/10.1002/adfm.202500207","url":null,"abstract":"The synergistic integration of elastic porous material with self-powered sensing capabilities holds immense promise for smart wearable devices. However, the intrinsic contradiction between elasticity and strength has hindered the mechanical performance of elastic porous materials. This research reports a diffusion-driven layer-by-layer assembly strategy to enhance the mechanical strength of elastic porous materials. As a prerequisite, the anisotropic layered structure of natural materials is leveraged to endow the porous material with fundamental elasticity. Subsequently, vacuum and chemically-assisted enhanced solvent diffusion are sequentially employed to assemble conductive and elastic layers on cellulose from the inside out. This endows the triboelectric material (TM) with exceptional mechanical properties (elastic strain range of 0–80%, compressive strength reaching 4.55 MPa). Utilizing the TM as a sensing material, a self-powered sensor with a response time of 48 ms and a sensitivity of 0.57 kPa<sup>−1</sup> is constructed. Moreover, the application of the sensor in a smart wearable helmet is demonstrated, enabling remote monitoring and traceability of head impact events. This research has overcome the incompatibility between the high strength and elasticity of porous materials and offers promising avenues for their utilization in smart wearable devices.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"41 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375571","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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