Although bulk heterojunction (BHJ) structure ensures high power conversion efficiencies (PCEs) of organic solar cells (OSCs), the morphology of this donor:acceptor blend film is thermally unstable due to molecular diffusion of two components, especially small molecule acceptor (SMA). Herein, different from the widely applied oligomerization or polymerization of SMAs, we report a new and simple strategy of the substitution with adamantyl, the most rigid alkyl group, on a famous SMA of Y6-BO to improve thermal stability of OSCs. Through such molecular tailoring, two novel SMAs of BOAD and ADAD, which owns one and two adamantyl side chains, respectively, are synthesized. As expected, the glass transition temperatures of ADAD and BOAD are elevated from 78 oC of Y6-BO to 98 ℃ and 123 ℃, respectively. Thus, after thermal treatment at 80 ℃ for 375 hours, the BOAD-based OSC maintains 61.3% of its initial efficiency, outperforming the Y6-BO-based counterpart (44.9%). In addition, the BOAD-based device achieves a high PCE of 17.13%, which is comparable to the Y6-BO-based one (16.98%). Our work provides a valuable reference to design stable SMAs, advancing the commercialization of OSCs.
{"title":"Chemical modification of small molecule acceptor with adamantyl side chain for efficient and thermally stable organic solar cells","authors":"Yecheng Shen, Yiming Wang, Chenhe Wang, Yimei Zhang, Shanghui Su, Yibo Hu, Yuxuan Zhu, Caiwei Zhang, Mengting Wang, Xiukun Ye, Guang-Peng Wu, Zaifei Ma, Haiming Zhu, Minmin Shi, Hongzheng Chen","doi":"10.1039/d5ta00483g","DOIUrl":"https://doi.org/10.1039/d5ta00483g","url":null,"abstract":"Although bulk heterojunction (BHJ) structure ensures high power conversion efficiencies (PCEs) of organic solar cells (OSCs), the morphology of this donor:acceptor blend film is thermally unstable due to molecular diffusion of two components, especially small molecule acceptor (SMA). Herein, different from the widely applied oligomerization or polymerization of SMAs, we report a new and simple strategy of the substitution with adamantyl, the most rigid alkyl group, on a famous SMA of Y6-BO to improve thermal stability of OSCs. Through such molecular tailoring, two novel SMAs of BOAD and ADAD, which owns one and two adamantyl side chains, respectively, are synthesized. As expected, the glass transition temperatures of ADAD and BOAD are elevated from 78 oC of Y6-BO to 98 ℃ and 123 ℃, respectively. Thus, after thermal treatment at 80 ℃ for 375 hours, the BOAD-based OSC maintains 61.3% of its initial efficiency, outperforming the Y6-BO-based counterpart (44.9%). In addition, the BOAD-based device achieves a high PCE of 17.13%, which is comparable to the Y6-BO-based one (16.98%). Our work provides a valuable reference to design stable SMAs, advancing the commercialization of OSCs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"183 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813792","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tian-Zhen Ren, Lu-Kang Zhao, Xiao Zhang, Xuanwen Gao, Hong Chen, Zhaomeng Liu, Dong-Run Yang, Wenbin Luo
Perovskite oxides, with their flexible electronic structure and low cost, are highly attractive alternatives to noble metal catalysts for oxygen redox reactions (ORR). Herein, we report LaNiO3 perovskite as an efficient ORR catalyst, where oxygen vacancies and oxygen-containing functional groups work synergistically. LaNiO3 was subjected to thermal shock in different media to introduce defects on the structural surface. Experimental results indicate that thermal shock in air creates oxygen vacancies on the catalyst surface, while thermal shock in aqueous solution increases the content of oxygen-containing functional groups (-OH) on the surface. The thermally shocked samples exhibit superior ORR catalytic performance, with the limiting current density increasing from 4.2 mA cm-2 to 5.4 mA cm-2. This work provides a convenient and straightforward approach for constructing a series of materials enriched with surface defects.
{"title":"Optimizing LaNiO3 Surface Structure as an Efficient Oxygen Reduction Reaction","authors":"Tian-Zhen Ren, Lu-Kang Zhao, Xiao Zhang, Xuanwen Gao, Hong Chen, Zhaomeng Liu, Dong-Run Yang, Wenbin Luo","doi":"10.1039/d5ta01346a","DOIUrl":"https://doi.org/10.1039/d5ta01346a","url":null,"abstract":"Perovskite oxides, with their flexible electronic structure and low cost, are highly attractive alternatives to noble metal catalysts for oxygen redox reactions (ORR). Herein, we report LaNiO3 perovskite as an efficient ORR catalyst, where oxygen vacancies and oxygen-containing functional groups work synergistically. LaNiO3 was subjected to thermal shock in different media to introduce defects on the structural surface. Experimental results indicate that thermal shock in air creates oxygen vacancies on the catalyst surface, while thermal shock in aqueous solution increases the content of oxygen-containing functional groups (-OH) on the surface. The thermally shocked samples exhibit superior ORR catalytic performance, with the limiting current density increasing from 4.2 mA cm-2 to 5.4 mA cm-2. This work provides a convenient and straightforward approach for constructing a series of materials enriched with surface defects.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"28 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813683","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The cathode-electrolyte interface plays a crucial role in determining the structural stability, electrochemical behavior and cycling performance of Li-ion batteries (LIBs). However, the dynamic structural evolution and microscopic reaction mechanisms at the interface remain poorly understood. Here, we provide a microscopic picture for the dynamic structure and the initial ring-opening reaction dynamics of ethylene carbonate (EC) ring-opening at the EC-LiCoO2 interface, one of the most commonly used battery systems, identifying two distinct mechanisms for the initial EC decomposition reactions, based on the on-the-fly machine learning accelerated molecular dynamics simulations. Explicit solvent modeling reveals various binding configurations of EC, with multiple binding sites and various orientations, which tend to influence its reactivity at the interface. Notably, the interaction between the carbonyl carbon of EC and the oxygen sites on the LiCoO2 (104) facet is strongly correlated with ring-opening of the bound EC. At 300 K, the C–O (ether O) bond of the EC molecules can be cleaved by a nucleophilic attack from the surface oxygen of LiCoO₂, leading to ring opening. In the absence of additional chemical species, spontaneous ring closure was usually observed on the stoichiometric LiCoO2 surface, presenting a dynamic equilibrium between transient ring-opening and self-healing for the adsorbed EC molecules at the interface. Furthermore, a longer ring-opened state of EC was observed, facilitated by an Li+ ion extraction from the stoichiometric LiCoO2, with an intermediate process of Co3+ oxidation to Co4+. A greater Li⁺ deficiency in the substrate was found to further promote EC ring opening. These findings not only provide fundamental insights into electrode-electrolyte interfacial reactions but also offer guidance for the efficient design of LIBs with enhanced stability and electrochemical/cycling performance.
{"title":"Microscopic Insights into Ring-Opening Reaction of Ethylene Carbonate on LiCoO2 by On-the-Fly Machine Learning Molecular Dynamics","authors":"Fanghui Mi, Ying Ou, Rui Luo, Shixian Wang, Zhijun Zhang, Chunwen Sun, Zhaoxiang Wang, Yurui Gao","doi":"10.1039/d5ta01193k","DOIUrl":"https://doi.org/10.1039/d5ta01193k","url":null,"abstract":"The cathode-electrolyte interface plays a crucial role in determining the structural stability, electrochemical behavior and cycling performance of Li-ion batteries (LIBs). However, the dynamic structural evolution and microscopic reaction mechanisms at the interface remain poorly understood. Here, we provide a microscopic picture for the dynamic structure and the initial ring-opening reaction dynamics of ethylene carbonate (EC) ring-opening at the EC-LiCoO2 interface, one of the most commonly used battery systems, identifying two distinct mechanisms for the initial EC decomposition reactions, based on the on-the-fly machine learning accelerated molecular dynamics simulations. Explicit solvent modeling reveals various binding configurations of EC, with multiple binding sites and various orientations, which tend to influence its reactivity at the interface. Notably, the interaction between the carbonyl carbon of EC and the oxygen sites on the LiCoO2 (104) facet is strongly correlated with ring-opening of the bound EC. At 300 K, the C–O (ether O) bond of the EC molecules can be cleaved by a nucleophilic attack from the surface oxygen of LiCoO₂, leading to ring opening. In the absence of additional chemical species, spontaneous ring closure was usually observed on the stoichiometric LiCoO2 surface, presenting a dynamic equilibrium between transient ring-opening and self-healing for the adsorbed EC molecules at the interface. Furthermore, a longer ring-opened state of EC was observed, facilitated by an Li+ ion extraction from the stoichiometric LiCoO2, with an intermediate process of Co3+ oxidation to Co4+. A greater Li⁺ deficiency in the substrate was found to further promote EC ring opening. These findings not only provide fundamental insights into electrode-electrolyte interfacial reactions but also offer guidance for the efficient design of LIBs with enhanced stability and electrochemical/cycling performance.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"96 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813784","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jinbo Wang, Xilin Li, Huihe Chen, Jingjing Jiang, Jieyu Huang, Jiaxiang Lu, Liang Su, Shuaikai Xu, Sen Lin
The synergistic optimization of mechanical strength, skin-like elastic modulus, electrode-skin impedance, permeability, and biocompatibility remains a critical challenge in the deployment of flexible electrodes as a central component of noninvasive electrophysiological signal recording. Here, we propose a fiber-reinforced hybrid hydrogel (FRHH) electrode that integrates the conductivity of poly (3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and titanium carbide (Ti3C2Tx) with the mechanical resilience of styrene-ethylene-butylene-styrene (SEBS) fibers within a PVA hydrogel matrix. The FRHH electrode demonstrates remarkable stretchability, with a tensile strain reaching up to 1485%, coupled with moderate tackiness. It also shows low impedance at a frequency of 1,000 Hz at the electrode-skin interface (2829.3 Ω), which is significantly lower than the impedance of commercial wet electrodes (6654.5 Ω) and dry electrodes (17611.2 Ω). Furthermore, the FRHH electrode showed excellent biocompatibility in preliminary in vivo tests, allowing for continuous on-skin application for up to 12 hours without causing inflammation or allergic reaction. The electrode maintains conductivity and signal integrity under significant deformation, making it suitable for continuous and stable recording of electrocardiogram (ECG) and electromyogram (EMG) signals, even during physical activity. Additionally, the FRHH electrode shows promise in EMG-based gesture recognition and can recognize precise muscle activation patterns. The FRHH electrode holds promise for a wide range of applications, including continuous health monitoring, athletic performance tracking, and medical diagnostics, and could significantly contribute to advances in noninvasive and wearable healthcare technologies.
{"title":"A Stretchable, Permeable, and Biocompatible Fiber-Reinforced Hybrid Hydrogel Electrode for Highly Stable Electrophysiological Signal Recording","authors":"Jinbo Wang, Xilin Li, Huihe Chen, Jingjing Jiang, Jieyu Huang, Jiaxiang Lu, Liang Su, Shuaikai Xu, Sen Lin","doi":"10.1039/d4ta08229j","DOIUrl":"https://doi.org/10.1039/d4ta08229j","url":null,"abstract":"The synergistic optimization of mechanical strength, skin-like elastic modulus, electrode-skin impedance, permeability, and biocompatibility remains a critical challenge in the deployment of flexible electrodes as a central component of noninvasive electrophysiological signal recording. Here, we propose a fiber-reinforced hybrid hydrogel (FRHH) electrode that integrates the conductivity of poly (3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and titanium carbide (Ti3C2Tx) with the mechanical resilience of styrene-ethylene-butylene-styrene (SEBS) fibers within a PVA hydrogel matrix. The FRHH electrode demonstrates remarkable stretchability, with a tensile strain reaching up to 1485%, coupled with moderate tackiness. It also shows low impedance at a frequency of 1,000 Hz at the electrode-skin interface (2829.3 Ω), which is significantly lower than the impedance of commercial wet electrodes (6654.5 Ω) and dry electrodes (17611.2 Ω). Furthermore, the FRHH electrode showed excellent biocompatibility in preliminary in vivo tests, allowing for continuous on-skin application for up to 12 hours without causing inflammation or allergic reaction. The electrode maintains conductivity and signal integrity under significant deformation, making it suitable for continuous and stable recording of electrocardiogram (ECG) and electromyogram (EMG) signals, even during physical activity. Additionally, the FRHH electrode shows promise in EMG-based gesture recognition and can recognize precise muscle activation patterns. The FRHH electrode holds promise for a wide range of applications, including continuous health monitoring, athletic performance tracking, and medical diagnostics, and could significantly contribute to advances in noninvasive and wearable healthcare technologies.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"74 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hualing Tian, Jiajia Li, Yanjun Cai, Xiang Yao, Zhi Su
Low ionic conductivity and poor interfacial stability restrict the practical application of all-solid-state sodium-ion batteries (SIBs). To solve these issues, a facile strategy involving the use of an inorganic-organic composite solid electrolyte (SE) composed of Na2ZrCl6 and polyacrylonitrile (PAN) is proposed. The introduction of Na2ZrCl6 results in a reduction in the crystallinity of PAN, which creates numerous pathways for Na+ migration and significantly enhances the ionic conductivity of SE. When utilized in a Na||Na symmetric half-cell, the Na2ZrCl6-PAN composite SE exhibited good interface stability, with no Na dendrite formation even after 4000 h of Na electroplating and Na stripping. In addition, non-in situ X-ray diffraction, X-ray photoelectron spectroscopy, and in situ AC impedance tests confirmed the favorable interfacial stability of the Na2ZrCl6-PAN SE in contact with Na metal and Na3V2(PO4)3 (NVP). Furthermore, Na|Na2ZrCl6-PAN|NVP exhibits outstanding electrochemical performance. The battery achieves an initial discharge capacity of 80.7 mA h g–1 at 1 C, which remains at 69.2 mA h g–1 after 500 cycles. Additionally, all-solid-state SIBs with a hard carbon (HC)|Na2ZrCl6-PAN|NVP configuration demonstrate excellent electrochemical cycling stability.
{"title":"Dendrite-free, interfacially compatible Na2ZrCl6 composite halide solid-state electrolyte for solid state sodium-ion batteries","authors":"Hualing Tian, Jiajia Li, Yanjun Cai, Xiang Yao, Zhi Su","doi":"10.1039/d4ta07957d","DOIUrl":"https://doi.org/10.1039/d4ta07957d","url":null,"abstract":"Low ionic conductivity and poor interfacial stability restrict the practical application of all-solid-state sodium-ion batteries (SIBs). To solve these issues, a facile strategy involving the use of an inorganic-organic composite solid electrolyte (SE) composed of Na2ZrCl6 and polyacrylonitrile (PAN) is proposed. The introduction of Na2ZrCl6 results in a reduction in the crystallinity of PAN, which creates numerous pathways for Na+ migration and significantly enhances the ionic conductivity of SE. When utilized in a Na||Na symmetric half-cell, the Na2ZrCl6-PAN composite SE exhibited good interface stability, with no Na dendrite formation even after 4000 h of Na electroplating and Na stripping. In addition, non-in situ X-ray diffraction, X-ray photoelectron spectroscopy, and in situ AC impedance tests confirmed the favorable interfacial stability of the Na2ZrCl6-PAN SE in contact with Na metal and Na3V2(PO4)3 (NVP). Furthermore, Na|Na2ZrCl6-PAN|NVP exhibits outstanding electrochemical performance. The battery achieves an initial discharge capacity of 80.7 mA h g–1 at 1 C, which remains at 69.2 mA h g–1 after 500 cycles. Additionally, all-solid-state SIBs with a hard carbon (HC)|Na2ZrCl6-PAN|NVP configuration demonstrate excellent electrochemical cycling stability.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"11 4 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813681","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
All-solid-state batteries based on abundant elements may pave the way for safer and cheaper energy storage. Magnesium borohydride derivatives with neutral ligands are a new emerging class of solid-state Mg2+ ionic conductors, and here we report the discovery of two new pyridine derivatives, Mg(BH4)2∙xN(CH)5 (x = 2 or 3). Magnesium tetrahydridoborate tripyridine, Mg(BH4)2∙3N(CH)5, crystallizes in the monoclinic space group C2/c and is built from molecular units consisting of trigonal bipyramidal [Mg(N(CH)5)3(BH4)2] complexes, where the pyridine molecules are packed efficiently as a result of π−π stacking. Magnesium tetrahydridoborate dipyridine, Mg(BH4)2∙2N(CH)5, crystallizes in the monoclinic space group Cc and is built from tetrahedral [Mg(N(CH)5)2(BH4)2] complexes. The highest ionic conductivity is observed for Mg(BH4)2∙3N(CH)5 with σ(Mg2+) = 7.2∙10-5 S∙cm-1 at 24 °C, increasing to (Mg2+) = 1.4∙10-4 S∙cm-1 at 49 °C. The low activation energy of 0.25 eV shows promise for low temperature conductivity. A low electronic conductivity of σe = 2.5∙10-10 S cm-1 was determined for Mg(BH4)2∙3N(CH)5 at 24 °C, providing a high ionic transport number of tion = 0.999997.
{"title":"Magnesium Borohydride Pyridine Derivatives as Solid Electrolytes for All-Solid-State Batteries","authors":"Jakob B. Grinderslev, Torben Rene Jensen","doi":"10.1039/d5ta00239g","DOIUrl":"https://doi.org/10.1039/d5ta00239g","url":null,"abstract":"All-solid-state batteries based on abundant elements may pave the way for safer and cheaper energy storage. Magnesium borohydride derivatives with neutral ligands are a new emerging class of solid-state Mg2+ ionic conductors, and here we report the discovery of two new pyridine derivatives, Mg(BH4)2∙xN(CH)5 (x = 2 or 3). Magnesium tetrahydridoborate tripyridine, Mg(BH4)2∙3N(CH)5, crystallizes in the monoclinic space group C2/c and is built from molecular units consisting of trigonal bipyramidal [Mg(N(CH)5)3(BH4)2] complexes, where the pyridine molecules are packed efficiently as a result of π−π stacking. Magnesium tetrahydridoborate dipyridine, Mg(BH4)2∙2N(CH)5, crystallizes in the monoclinic space group Cc and is built from tetrahedral [Mg(N(CH)5)2(BH4)2] complexes. The highest ionic conductivity is observed for Mg(BH4)2∙3N(CH)5 with σ(Mg2+) = 7.2∙10-5 S∙cm-1 at 24 °C, increasing to (Mg2+) = 1.4∙10-4 S∙cm-1 at 49 °C. The low activation energy of 0.25 eV shows promise for low temperature conductivity. A low electronic conductivity of σe = 2.5∙10-10 S cm-1 was determined for Mg(BH4)2∙3N(CH)5 at 24 °C, providing a high ionic transport number of tion = 0.999997.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"37 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819125","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Liu Dan Yu, Pan Xue, Zhang Jingli, Tong Yinjia, Zhang Yixuan, Yu Yanjing, Zhang Qingda, Huang Mengfei, Yiheng Gao, Jie Li, Qufu Wei, Pengfei Lv
The rapid development of intelligent wearable devices and health monitoring equipment demands bio-based materials that integrate multiple functions with enhanced durability. Herein, this work is an first attempt to develop flexible electromagnetic shielding and stress-strain sensing based on a composite of polydopamine (PDA) modified-MXene (p-MXene) film with waterborne polyurethane (WPU)/bacterial cellulose (BC) film. The durable p-MXene@WPU/BC composite films are found to demonstrate excellent mechanical properties (370 MPa) and stable interfacial adhesion, attributing to the interlocking network structure between WPU and WBC and the strong hydrogen bonding between p-MXene layer and WPU/BC layer. The resultant composite film displays remarkable mechanosensing performance, facilitating the accurate and reliable detection of human physiological signals. Importantly, the prepared composite film could effectively reflect and absorb electromagnetic waves through the high conductivity of p-MXene layer and the staggered nanonetwork structure of WPU/BC layer, thus achieving a shielding effect of up to 72 dB. As proof-of-concept illustrations, it is noteworthy that the electromagnetic shielding efficacy displays a dynamic interaction with the strain sensing performance during the stretching process, which is primarily attributed to the moderating effect of the efficient attachment and parallel-aligned structure of p-MXene nanosheets. The research herein can offer new perspectives on the development of advanced bio-based multiple functions materials and dynamic perceptual interaction and smart wearables.
{"title":"Robust integration of p-MXene ink with bacterial cellulose-reinforced polymer enables dynamic interaction of superior electromagnetic shielding and sensing","authors":"Liu Dan Yu, Pan Xue, Zhang Jingli, Tong Yinjia, Zhang Yixuan, Yu Yanjing, Zhang Qingda, Huang Mengfei, Yiheng Gao, Jie Li, Qufu Wei, Pengfei Lv","doi":"10.1039/d5ta01796c","DOIUrl":"https://doi.org/10.1039/d5ta01796c","url":null,"abstract":"The rapid development of intelligent wearable devices and health monitoring equipment demands bio-based materials that integrate multiple functions with enhanced durability. Herein, this work is an first attempt to develop flexible electromagnetic shielding and stress-strain sensing based on a composite of polydopamine (PDA) modified-MXene (p-MXene) film with waterborne polyurethane (WPU)/bacterial cellulose (BC) film. The durable p-MXene@WPU/BC composite films are found to demonstrate excellent mechanical properties (370 MPa) and stable interfacial adhesion, attributing to the interlocking network structure between WPU and WBC and the strong hydrogen bonding between p-MXene layer and WPU/BC layer. The resultant composite film displays remarkable mechanosensing performance, facilitating the accurate and reliable detection of human physiological signals. Importantly, the prepared composite film could effectively reflect and absorb electromagnetic waves through the high conductivity of p-MXene layer and the staggered nanonetwork structure of WPU/BC layer, thus achieving a shielding effect of up to 72 dB. As proof-of-concept illustrations, it is noteworthy that the electromagnetic shielding efficacy displays a dynamic interaction with the strain sensing performance during the stretching process, which is primarily attributed to the moderating effect of the efficient attachment and parallel-aligned structure of p-MXene nanosheets. The research herein can offer new perspectives on the development of advanced bio-based multiple functions materials and dynamic perceptual interaction and smart wearables.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"75 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813699","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
With the development of aerospace technology, the thermal insulation layer between the engine casing and the propellant needs to have excellent mechanical and ablative resistance properties to meet higher environmental requirements. Herein, two novel reactive phosphonitrile derivatives containing P and N heteroatoms, namely, hexa(2-allylphenoxy) cyclotriphosphonitrile (HAPPCP) and hexa(3-ethynylphenylamino) cyclotriphosphonitrile (HEACP), were designed and synthesized to crosslink with EPDM for modulating its chain structure on a molecular scale, forming P- and N-atom hybridized EPDM dense crosslinked networks, which collectively improve the mechanical and ablative resistance. Results showed that HEACP was more effective for boosting the overall performance, accompanied by improvements of 64.6% and 89.2% in tensile strength and breaking elongation, respectively, and reductions of 52.6% and 33.1% in the linear ablation rate and mass ablation rate, respectively. The ablation-condensed phase, microscopic carbon crystal structure, and the gas-phase thermal barrier mechanism were investigated to elucidate the ablative resistance mechanism.
{"title":"Construction of phosphonitrile derivative-hybridized EPDM dense crosslinked networks for enhanced mechanics and ablation resistance","authors":"Shumeng Wang, Jian Wang, Xutao Ma, Zhaoqi Niu, Zongwu Zhang, Peibo Xu, Beixi Chen, Xiaoyan Ma, Shishan Yang, Xiao Hou","doi":"10.1039/d5ta00056d","DOIUrl":"https://doi.org/10.1039/d5ta00056d","url":null,"abstract":"With the development of aerospace technology, the thermal insulation layer between the engine casing and the propellant needs to have excellent mechanical and ablative resistance properties to meet higher environmental requirements. Herein, two novel reactive phosphonitrile derivatives containing P and N heteroatoms, namely, hexa(2-allylphenoxy) cyclotriphosphonitrile (HAPPCP) and hexa(3-ethynylphenylamino) cyclotriphosphonitrile (HEACP), were designed and synthesized to crosslink with EPDM for modulating its chain structure on a molecular scale, forming P- and N-atom hybridized EPDM dense crosslinked networks, which collectively improve the mechanical and ablative resistance. Results showed that HEACP was more effective for boosting the overall performance, accompanied by improvements of 64.6% and 89.2% in tensile strength and breaking elongation, respectively, and reductions of 52.6% and 33.1% in the linear ablation rate and mass ablation rate, respectively. The ablation-condensed phase, microscopic carbon crystal structure, and the gas-phase thermal barrier mechanism were investigated to elucidate the ablative resistance mechanism.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"37 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806259","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jieyu Yang, Chenyu Zhang, Ting Zhou, Yuanyuan Chen, Yanqiu Wang, Kuang Sheng, Luqiong Liu, Jie Li, Wenzhang Li, Yang Liu
As the most active catalyst material in acidic environment, the catalytic activity of RuO2 is higher than IrO2, but its poor stability limits its application. To this end, we propose a simple defect engineering strategy, namely the preparation of RuO2 nanoparticles (D-RuO2) with gradient distribution of oxygen vacancies as efficient acidic oxygen evolution reaction (OER) catalysts. Oxygen vacancies participate in lattice compression to form an unsaturated coordination environment, which increases the covalency of Ru-O bonds, effectively optimizes the adsorption of intermediates in OER process, and stabilizes the structure of the active site. Density functional theory (DFT) calculation showed that the oxygen defect shifted the d-band center of Ru down, balanced the adsorption and desorption behavior of oxygen-containing intermediates on the surface of RuO2, reduced the reaction barrier of OER process, and promoted the reaction. D-RuO2 exhibits a lower overpotential (η10 = 197 mV) and a lower Tafel slope (58.67 mV dec-1), with a stability of 60 h measured in 0.5 M H2SO4. This strategy provides a simple method to improve the activity and stability of RuO2 by regulating oxygen vacancies.
{"title":"Gradient Oxygen Vacancy Engineering on RuO2-x for Efficient Acidic Water Oxidation","authors":"Jieyu Yang, Chenyu Zhang, Ting Zhou, Yuanyuan Chen, Yanqiu Wang, Kuang Sheng, Luqiong Liu, Jie Li, Wenzhang Li, Yang Liu","doi":"10.1039/d5ta01078k","DOIUrl":"https://doi.org/10.1039/d5ta01078k","url":null,"abstract":"As the most active catalyst material in acidic environment, the catalytic activity of RuO2 is higher than IrO2, but its poor stability limits its application. To this end, we propose a simple defect engineering strategy, namely the preparation of RuO2 nanoparticles (D-RuO2) with gradient distribution of oxygen vacancies as efficient acidic oxygen evolution reaction (OER) catalysts. Oxygen vacancies participate in lattice compression to form an unsaturated coordination environment, which increases the covalency of Ru-O bonds, effectively optimizes the adsorption of intermediates in OER process, and stabilizes the structure of the active site. Density functional theory (DFT) calculation showed that the oxygen defect shifted the d-band center of Ru down, balanced the adsorption and desorption behavior of oxygen-containing intermediates on the surface of RuO2, reduced the reaction barrier of OER process, and promoted the reaction. D-RuO2 exhibits a lower overpotential (η10 = 197 mV) and a lower Tafel slope (58.67 mV dec-1), with a stability of 60 h measured in 0.5 M H2SO4. This strategy provides a simple method to improve the activity and stability of RuO2 by regulating oxygen vacancies.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"4 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochemical nitrate reduction (NO3- RR) is a promising strategy to mitigate nitrate pollution, which has become a critical environmental concern due to its harmful effects on water resources and ecosystems. Metal-organic frameworks (MOFs), known for their highly tunable structures, large surface areas, and exceptional porosity, have emerged as potent materials for catalyzing NO3- RR reactions. However, the water stability of MOFs remains a major challenge in achieving efficient, durable NO3- RR under aqueous conditions. Recent advancements in water-stable MOFs (WS-MOFs) based materials offer promising solutions to this problem, enabling robust performance in electrochemical applications. This review explores the design, synthesis, and application of WS-MOFs for electrochemical NO₃-RR. Key strategies for enhancing water stability include the incorporation of hydrophobic ligands, post-synthetic modifications, and the development of MOF composites. The chapter examines the role of metal centers, such as transition metals (e.g., Fe, Cu, Co, and Ni), and their interaction with organic linkers in promoting selective NO3- RR to environmentally benign products including nitrogen gas (N₂) and ammonia (NH₃). The integration of MOFs with conductive materials to improve electrical conductivity and catalytic performance is also discussed. In addition to reviewing recent progress in water-stable MOF catalysts for NO3- RR, this review highlights challenges such as reaction selectivity, competitive side reactions, and long-term stability in electrochemical cells. Prospective directions for future research are outlined, including the development of more efficient catalysts, understanding reaction mechanisms at the molecular level, and scaling up MOF based NO₃⁻ RR systems for practical applications.
{"title":"Water-stable MOFs and Composites: Greener and Sustainable Approach for Enhanced Reactivity towards Electrochemical Nitrate Reduction Reactions","authors":"Muhammad Sheraz Ahmad, Tahir Rasheed","doi":"10.1039/d4ta09189b","DOIUrl":"https://doi.org/10.1039/d4ta09189b","url":null,"abstract":"Electrochemical nitrate reduction (NO3- RR) is a promising strategy to mitigate nitrate pollution, which has become a critical environmental concern due to its harmful effects on water resources and ecosystems. Metal-organic frameworks (MOFs), known for their highly tunable structures, large surface areas, and exceptional porosity, have emerged as potent materials for catalyzing NO3- RR reactions. However, the water stability of MOFs remains a major challenge in achieving efficient, durable NO3- RR under aqueous conditions. Recent advancements in water-stable MOFs (WS-MOFs) based materials offer promising solutions to this problem, enabling robust performance in electrochemical applications. This review explores the design, synthesis, and application of WS-MOFs for electrochemical NO₃-RR. Key strategies for enhancing water stability include the incorporation of hydrophobic ligands, post-synthetic modifications, and the development of MOF composites. The chapter examines the role of metal centers, such as transition metals (e.g., Fe, Cu, Co, and Ni), and their interaction with organic linkers in promoting selective NO3- RR to environmentally benign products including nitrogen gas (N₂) and ammonia (NH₃). The integration of MOFs with conductive materials to improve electrical conductivity and catalytic performance is also discussed. In addition to reviewing recent progress in water-stable MOF catalysts for NO3- RR, this review highlights challenges such as reaction selectivity, competitive side reactions, and long-term stability in electrochemical cells. Prospective directions for future research are outlined, including the development of more efficient catalysts, understanding reaction mechanisms at the molecular level, and scaling up MOF based NO₃⁻ RR systems for practical applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"75 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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