Grant M Musgrave, Eden Y Yau, Huang Sijia, Caleb Reese, Chen Wang
Bio-based carboxylic acids are some of the most available renewable chemicals, but since they are solids with high melting temperatures, they cannot be directly used as liquid resins. To this end, we report the formation of supramolecular complexes between an amino methacrylate and various solid carboxylic acids. The ionically bonded methacrylates exhibit low viscosities and rapid reaction kinetics for free-radical mediated polymerization, showing quantitative methacrylate conversions within one minute of irradiation at 5 mW/cm2 405nm light. We demonstrate the implementation of these acid-base complexes as a neat resin system that comprises orthogonal polymerization reactions (free-radical methacrylate polymerization and epoxy-acid polymerization reactions), which yields high-strength network polymer materials.
{"title":"Solventless, Rapid-polymerizable Liquid Resins from Solid Carboxylic Acids through Low-viscosity Acid/Base Complexes","authors":"Grant M Musgrave, Eden Y Yau, Huang Sijia, Caleb Reese, Chen Wang","doi":"10.1039/d4ta05417b","DOIUrl":"https://doi.org/10.1039/d4ta05417b","url":null,"abstract":"Bio-based carboxylic acids are some of the most available renewable chemicals, but since they are solids with high melting temperatures, they cannot be directly used as liquid resins. To this end, we report the formation of supramolecular complexes between an amino methacrylate and various solid carboxylic acids. The ionically bonded methacrylates exhibit low viscosities and rapid reaction kinetics for free-radical mediated polymerization, showing quantitative methacrylate conversions within one minute of irradiation at 5 mW/cm2 405nm light. We demonstrate the implementation of these acid-base complexes as a neat resin system that comprises orthogonal polymerization reactions (free-radical methacrylate polymerization and epoxy-acid polymerization reactions), which yields high-strength network polymer materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"18 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685078","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}
Jitesh Pani, Priyanka Chaudhary, Hitesh Borkar, Meng-Fang Lin
Flexible supercapacitors are emerging as efficient, fast storage devices for new generation electronics. Two-dimensional (2D) transition metal carbides (MXene) have garnered attention as supercapacitor electrodes owing to their conductive layered sheets and the tunability of surface functional groups. In the present work, the Ti C3 2Tx MXene surface was sulphonated using dimethyl sulfoxide (DMSO) and intercalated with AB2O4(A= Co and Ni, B= Fe) perovskite nanoparticle (NPs). The sulphonated MXene (TMS) was processed using a sonication method in DMSO solventelectrolyte (0.1M H2SO4) interaction. to enhance the surface area and redox active sites forThe redox dominated enhanced specific capacitance was observed in 3 wt% CoFe2O4 (CFO) interacted TMS (3CTMS) and 3 wt% NiFe2O4 (NFO) interacted TMS (3NTMS), confirmed by Electrochemical Impedance Spectroscopy (EIS) and the Dunn’s method analysis. The specific capacitance of 3CTMS was found to be 593.81 F/g at 5 mV/sec, with an excellent cyclic stability of 81.75% after 10,000 cycles. A flexible symmetric supercapacitor fabricated with 3CTMS showed energy and power density of 4.177 Wh/kg and 512.17 W/kg, respectively. The flexible supercapacitor has been utilized in real time applications by charging and discharge to power 5 Light-Emitting Diodes (LEDs) with different forward voltages.
{"title":"Strategic intercalation of AB2O4 perovskite oxides for synergistic enhanced redox activity in sulphonated Ti3C2Tx MXene for energy storage applications","authors":"Jitesh Pani, Priyanka Chaudhary, Hitesh Borkar, Meng-Fang Lin","doi":"10.1039/d4ta05816j","DOIUrl":"https://doi.org/10.1039/d4ta05816j","url":null,"abstract":"Flexible supercapacitors are emerging as efficient, fast storage devices for new generation electronics. Two-dimensional (2D) transition metal carbides (MXene) have garnered attention as supercapacitor electrodes owing to their conductive layered sheets and the tunability of surface functional groups. In the present work, the Ti C3 2Tx MXene surface was sulphonated using dimethyl sulfoxide (DMSO) and intercalated with AB2O4(A= Co and Ni, B= Fe) perovskite nanoparticle (NPs). The sulphonated MXene (TMS) was processed using a sonication method in DMSO solventelectrolyte (0.1M H2SO4) interaction. to enhance the surface area and redox active sites forThe redox dominated enhanced specific capacitance was observed in 3 wt% CoFe2O4 (CFO) interacted TMS (3CTMS) and 3 wt% NiFe2O4 (NFO) interacted TMS (3NTMS), confirmed by Electrochemical Impedance Spectroscopy (EIS) and the Dunn’s method analysis. The specific capacitance of 3CTMS was found to be 593.81 F/g at 5 mV/sec, with an excellent cyclic stability of 81.75% after 10,000 cycles. A flexible symmetric supercapacitor fabricated with 3CTMS showed energy and power density of 4.177 Wh/kg and 512.17 W/kg, respectively. The flexible supercapacitor has been utilized in real time applications by charging and discharge to power 5 Light-Emitting Diodes (LEDs) with different forward voltages.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"71 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679003","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}
Yulin Jiang, Xia Wen, Yinuo Li, Yuhang Li, Yanan Peng, Wang Feng, Xiaohui Li, Junbo Yang, Luying Song, Ling Huang, Hang Sun, Jianping Shi
Aqueous zinc-ion batteries (AZIBs) have received increasing attention in large-scale energy storage systems because of their appealing features with respect to safety, cost, and scalability. Although vanadium oxides with different compositions demonstrate promising potential as the cathodes of AZIBs, the narrow interlayer spacing, inferior electronic conductivity, and high dissolution in electrolyte seriously restrict their practical applications. Here we design an ingenious bimetallic-ions (Mg2+ and Al3+) co-intercalation strategy to boost the AZIBs performances of V6O131.31H2O (VOH). The bimetallic-ions intercalation expands the interlayer spacing, increases the electronic conductivity, and more importantly stabilizes the vanadium-oxygen bond in VOH, which promotes the ion/electron transport kinetics and restrains the vanadium oxides dissolution. As expected, MgAl-VOH cathodes deliver ultrahigh specific capacities of 524.9 and 275.6 mAh g−1 at the current densities of 0.1 and 5 A g−1, respectively, comparable to the highest value in vanadium oxides. The underlying zinc-ion storage mechanism is unambiguously clarified with the aid of density function theory calculations and in-situ structure characterizations. This work opens up a new avenue for boosting AZIBs performances by designing bimetallic-ions co-intercalated cathodes.
{"title":"Bimetallic-ions co-intercalation to stabilize vanadium-oxygen bond towards high-performance aqueous zinc-ion storage","authors":"Yulin Jiang, Xia Wen, Yinuo Li, Yuhang Li, Yanan Peng, Wang Feng, Xiaohui Li, Junbo Yang, Luying Song, Ling Huang, Hang Sun, Jianping Shi","doi":"10.1039/d4ta05938g","DOIUrl":"https://doi.org/10.1039/d4ta05938g","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) have received increasing attention in large-scale energy storage systems because of their appealing features with respect to safety, cost, and scalability. Although vanadium oxides with different compositions demonstrate promising potential as the cathodes of AZIBs, the narrow interlayer spacing, inferior electronic conductivity, and high dissolution in electrolyte seriously restrict their practical applications. Here we design an ingenious bimetallic-ions (Mg2+ and Al3+) co-intercalation strategy to boost the AZIBs performances of V6O131.31H2O (VOH). The bimetallic-ions intercalation expands the interlayer spacing, increases the electronic conductivity, and more importantly stabilizes the vanadium-oxygen bond in VOH, which promotes the ion/electron transport kinetics and restrains the vanadium oxides dissolution. As expected, MgAl-VOH cathodes deliver ultrahigh specific capacities of 524.9 and 275.6 mAh g−1 at the current densities of 0.1 and 5 A g−1, respectively, comparable to the highest value in vanadium oxides. The underlying zinc-ion storage mechanism is unambiguously clarified with the aid of density function theory calculations and in-situ structure characterizations. This work opens up a new avenue for boosting AZIBs performances by designing bimetallic-ions co-intercalated cathodes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678458","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 role of ammonia concentration in determining the particle shape and size of Ni-rich cathode materials during co-precipitation, though recognized as important, remains insufficiently understood in terms of its underlying mechanisms. In this study, we explore the effects of five distinct ammonia concentrations (0.2 mol/L, 0.3 mol/L, 0.4 mol/L, gradually increasing from 0 to 0.4 mol/L, and decreasing from 0.4 to 0.12 mol/L) on the microstructure of the Ni0.95Al0.05(OH)2.05 precursor throughout the precipitation process. The results reveal that ammonia concentration significantly influences both nucleation and crystal growth rates, with higher ammonia levels reducing nucleation rates and leading to more uniform agglomerates. Additionally, ammonia concentration affects the thickness-to-length ratio of the precursor's primary particles, which in turn influences the morphology of the LiNi0.95Al0.05O2 cathode materials during lithiation. Importantly, the study demonstrates that the electrochemical properties of LiNi0.95Al0.05O2 are more closely related to the shape of the primary particles than to the secondary particles, highlighting the critical importance of microstructural control in the design of next-generation Li-ion batteries. This study demonstrates the critical impact of ammonia concentration on particle characteristics. The results offer valuable insights for improving battery performance.
{"title":"What impact does ammonia have on the microstructure of the precursor and the electrochemical performance of Ni-rich layered oxides?","authors":"Jilu Zhang, Xinyue Zhai, Tian Zhao, Xiaoxia Yang, Qin Wang, Zhongjun Chen, Meng-Cheng Chen, Jian-Jie Ma, Ying-Rui Lu, Sung-Fu Hung, Weibo Hua","doi":"10.1039/d4ta06142j","DOIUrl":"https://doi.org/10.1039/d4ta06142j","url":null,"abstract":"The role of ammonia concentration in determining the particle shape and size of Ni-rich cathode materials during co-precipitation, though recognized as important, remains insufficiently understood in terms of its underlying mechanisms. In this study, we explore the effects of five distinct ammonia concentrations (0.2 mol/L, 0.3 mol/L, 0.4 mol/L, gradually increasing from 0 to 0.4 mol/L, and decreasing from 0.4 to 0.12 mol/L) on the microstructure of the Ni0.95Al0.05(OH)2.05 precursor throughout the precipitation process. The results reveal that ammonia concentration significantly influences both nucleation and crystal growth rates, with higher ammonia levels reducing nucleation rates and leading to more uniform agglomerates. Additionally, ammonia concentration affects the thickness-to-length ratio of the precursor's primary particles, which in turn influences the morphology of the LiNi0.95Al0.05O2 cathode materials during lithiation. Importantly, the study demonstrates that the electrochemical properties of LiNi0.95Al0.05O2 are more closely related to the shape of the primary particles than to the secondary particles, highlighting the critical importance of microstructural control in the design of next-generation Li-ion batteries. This study demonstrates the critical impact of ammonia concentration on particle characteristics. The results offer valuable insights for improving battery performance.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678459","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}
Junye Pan, Jiahui Chen, Bingxin Duan, Yuxi Zhang, Peiran Hou, Yanqing Zhu, Min Hu, Wangnan Li, Yi-Bing Cheng, Jianfeng Lu
Semi-transparent perovskite solar cells (ST-PSCs) have tremendous potential as smart windows owing to their higher efficiency and visible transmittance. However, most of previous ST-PSCs were fabricated by spin-coating methods with vulnerable materials, which are not stable at higher temperature (> 60 °C) and the processes are not scalable. Herein, thermal stable ST-PSCs have been fabricated by using vacuum deposited CsPbBr3 perovskite and electron-beam evaporation deposited NiOX. Furthermore, we further introduced an ultrathin P3HT buffer layer before depositing NiOX to avoid the damage of perovskite morphology by electron-beam. We found that this P3HT buffer layer not only protects the perovskite film from the damage of electron beam, but also facilitates the hole transfer from perovskite to NiOX. As a result, we achieved champion efficiencies of 7.1% for small area (active area = 0.16 cm2) solar cells and 5.5% for 5 cm × 5 cm mini-modules (active area = 10.0 cm2) with an AVT of 49.1%. Moreover, the non-encapsulated devices retained 93% of their initial performance after aging at 65 °C and a relative humidity (RH) of 55 ± 10% for 30 days.
{"title":"Electron-Beam-Evaporated NiOX for Efficient and Stable Semi-Transparent Perovskite Solar Cells and Modules","authors":"Junye Pan, Jiahui Chen, Bingxin Duan, Yuxi Zhang, Peiran Hou, Yanqing Zhu, Min Hu, Wangnan Li, Yi-Bing Cheng, Jianfeng Lu","doi":"10.1039/d4ta07138g","DOIUrl":"https://doi.org/10.1039/d4ta07138g","url":null,"abstract":"Semi-transparent perovskite solar cells (ST-PSCs) have tremendous potential as smart windows owing to their higher efficiency and visible transmittance. However, most of previous ST-PSCs were fabricated by spin-coating methods with vulnerable materials, which are not stable at higher temperature (> 60 °C) and the processes are not scalable. Herein, thermal stable ST-PSCs have been fabricated by using vacuum deposited CsPbBr3 perovskite and electron-beam evaporation deposited NiOX. Furthermore, we further introduced an ultrathin P3HT buffer layer before depositing NiOX to avoid the damage of perovskite morphology by electron-beam. We found that this P3HT buffer layer not only protects the perovskite film from the damage of electron beam, but also facilitates the hole transfer from perovskite to NiOX. As a result, we achieved champion efficiencies of 7.1% for small area (active area = 0.16 cm2) solar cells and 5.5% for 5 cm × 5 cm mini-modules (active area = 10.0 cm2) with an AVT of 49.1%. Moreover, the non-encapsulated devices retained 93% of their initial performance after aging at 65 °C and a relative humidity (RH) of 55 ± 10% for 30 days.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"35 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678453","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}
Hongjiang Li, Ning Chen, Jie Xing, Wenbin Liu, Wei Shi, Hao Chen, Zhi Tan, Manjing Tang, Mingyue Mo, Jianguo Zhu
Both low mechanical losses and large piezoelectric coefficient (d33) are essential in high-power piezoelectric applications. However, achieving both a large d33 and a high mechanical quality factor (Qm) is generally considered challenging due to the inherent trade-off between these properties. This challenge is particularly pronounced in the development of lead-free piezoelectric materials. In this work, we present a novel approach that integrates heterogeneous diffusion with remnant hardening in potassium sodium niobate (KNN)-based composites. This method results in a more than threefold increase in the Qm, jumping from 56 to 205 while a high d33 value (d33 = 370 pC/N) is maintained, significantly outperforming previous reports. Structural characterization and phase-field simulations revealed that the synergistic effects of local structural heterogeneity and local stress fields achieve excellent electromechanical compatibility. This dual modulation effectively overcomes the longstanding conflict between piezoelectric properties and mechanical losses. These findings present a promising pathway to enhance the commercial viability of lead-free KNN-based piezoelectric ceramics, making a significant advancement in the development of high-performance, environmentally friendly piezoelectric materials.
{"title":"Heterogeneous diffusion and remnant hardening with excellent electromechanical compatibility in alkaline niobate composites","authors":"Hongjiang Li, Ning Chen, Jie Xing, Wenbin Liu, Wei Shi, Hao Chen, Zhi Tan, Manjing Tang, Mingyue Mo, Jianguo Zhu","doi":"10.1039/d4ta07326f","DOIUrl":"https://doi.org/10.1039/d4ta07326f","url":null,"abstract":"Both low mechanical losses and large piezoelectric coefficient (<em>d</em><small><sub>33</sub></small>) are essential in high-power piezoelectric applications. However, achieving both a large <em>d</em><small><sub>33</sub></small> and a high mechanical quality factor (<em>Q</em><small><sub>m</sub></small>) is generally considered challenging due to the inherent trade-off between these properties. This challenge is particularly pronounced in the development of lead-free piezoelectric materials. In this work, we present a novel approach that integrates heterogeneous diffusion with remnant hardening in potassium sodium niobate (KNN)-based composites. This method results in a more than threefold increase in the <em>Q</em><small><sub>m</sub></small>, jumping from 56 to 205 while a high <em>d</em><small><sub>33</sub></small> value (<em>d</em><small><sub>33</sub></small> = 370 pC/N) is maintained, significantly outperforming previous reports. Structural characterization and phase-field simulations revealed that the synergistic effects of local structural heterogeneity and local stress fields achieve excellent electromechanical compatibility. This dual modulation effectively overcomes the longstanding conflict between piezoelectric properties and mechanical losses. These findings present a promising pathway to enhance the commercial viability of lead-free KNN-based piezoelectric ceramics, making a significant advancement in the development of high-performance, environmentally friendly piezoelectric materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"108 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678455","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}
High-quality perovskite films are crucial for achieving efficient carbon-based printable mesoscopic perovskite solar cells (MPSCs). However, rapid crystallization leads to poor film quality and the formation of defects, resulting in severe non-radiative recombination that hinders the improvement of device performance. In this work, an organic small molecule, dicyandiamide (DCDA), with multifunctional groups was incorporated into the perovskite precursor solution to concurrently regulate crystallization and manage defects in the perovskite in the mesoporous scaffold, and high performance MPSCs were obtained. Due to the robust interactions of the –CN and –CN groups in DCDA with un-coordinated Pb2+, and/or FA+/MA+via hydrogen bonding, coupled with the –NH2 groups of DCDA forming hydrogen bonding or electrostatic interactions with halide anions to inhibit ion migration, the defects were passivated. The introduction of DCDA effectively retarded nucleation and grain growth, and significantly reduced the film formation rate. Thus, perovskite films with larger grain sizes, preferred orientation, and lower trap state density were obtained, thereby greatly suppressing non-radiative recombination. As a result, the average power conversion efficiency (PCE) of MPSCs treated with DCDA was improved from 17.15 ± 0.48% to 18.75 ± 0.42%, and a champion PCE of 19.12% was obtained. Meanwhile, the PCE of unpackaged MPSC devices still remained at 94.00% of the initial efficiency when stored in an air environment after 103 days, demonstrating excellent stability. The strategy facilitates a deeper understanding of perovskite crystallization in printable MPSCs.
{"title":"Defect management and crystallization regulation for high-efficiency carbon-based printable mesoscopic perovskite solar cells via a single organic small molecule","authors":"Jinjiang Wang, Dongjie Wang, Dang Xu, Yang Zhang, Tianhuan Huang, Doudou Zhang, Zheling Zhang, Jian Xiong, Yu Huang, Jian Zhang","doi":"10.1039/d4ta06877g","DOIUrl":"https://doi.org/10.1039/d4ta06877g","url":null,"abstract":"High-quality perovskite films are crucial for achieving efficient carbon-based printable mesoscopic perovskite solar cells (MPSCs). However, rapid crystallization leads to poor film quality and the formation of defects, resulting in severe non-radiative recombination that hinders the improvement of device performance. In this work, an organic small molecule, dicyandiamide (DCDA), with multifunctional groups was incorporated into the perovskite precursor solution to concurrently regulate crystallization and manage defects in the perovskite in the mesoporous scaffold, and high performance MPSCs were obtained. Due to the robust interactions of the –C<img alt=\"[double bond, length as m-dash]\" border=\"0\" src=\"https://www.rsc.org/images/entities/char_e001.gif\"/>N and –CN groups in DCDA with un-coordinated Pb<small><sup>2+</sup></small>, and/or FA<small><sup>+</sup></small>/MA<small><sup>+</sup></small> <em>via</em> hydrogen bonding, coupled with the –NH<small><sub>2</sub></small> groups of DCDA forming hydrogen bonding or electrostatic interactions with halide anions to inhibit ion migration, the defects were passivated. The introduction of DCDA effectively retarded nucleation and grain growth, and significantly reduced the film formation rate. Thus, perovskite films with larger grain sizes, preferred orientation, and lower trap state density were obtained, thereby greatly suppressing non-radiative recombination. As a result, the average power conversion efficiency (PCE) of MPSCs treated with DCDA was improved from 17.15 ± 0.48% to 18.75 ± 0.42%, and a champion PCE of 19.12% was obtained. Meanwhile, the PCE of unpackaged MPSC devices still remained at 94.00% of the initial efficiency when stored in an air environment after 103 days, demonstrating excellent stability. The strategy facilitates a deeper understanding of perovskite crystallization in printable MPSCs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"11 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678862","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}
Yujia Shan, Shi Huang, Tianyu Jiang, Ye Cao, Jinxin Wang, Yuteng Cao, Wenquan Zhang
Designing and synthesizing high-energy, low-sensitivity energetic molecules has become an urgent challenge in the field of energetic materials. Here, the concept of chimerism was introduced into the development of energetic molecules, proposing a systematic and effective research model for the design, screening, and synthesis of high-energy, low-sensitivity energetic molecules. We selected the classical insensitive energetic molecule nitroguanidine as the parent molecule and merged it with three other classic energetic molecules through a one-step substitution reaction, efficiently obtaining three classes of new energetic molecules. Analysis and characterization of their properties show that the chimeric molecules 3 and 6 inherit the advantages of the parent energetic molecules, demonstrating high-energy and insensitivity (detonation velocity of 8113 m s-1, impact sensitivity of 35 J for 3; detonation velocity of 8539 m s-1, impact sensitivity of >60 J for 6). Remarkably, chimeric molecule 9 exhibits an acceptable sensitivity (7 J, similar to RDX) while surpassing the energy of the parent molecules significantly (>9000 m/s). The energy of energetic molecule 8 (8742 m/s) is comparable to that of RDX (8754 m/s), and its mechanical sensitivity (50 J) is less sensitive than that of RDX (5.6 J). This study demonstrates the potential of the chimeric energetic molecule strategy for efficiently designing and synthesizing new high-performance energetic molecules in a simple manner.
{"title":"An Effective Strategy for Balancing Energy and Sensitivity: Design, Synthesis, and Properties of Chimeric Energetic Molecules","authors":"Yujia Shan, Shi Huang, Tianyu Jiang, Ye Cao, Jinxin Wang, Yuteng Cao, Wenquan Zhang","doi":"10.1039/d4ta06644h","DOIUrl":"https://doi.org/10.1039/d4ta06644h","url":null,"abstract":"Designing and synthesizing high-energy, low-sensitivity energetic molecules has become an urgent challenge in the field of energetic materials. Here, the concept of chimerism was introduced into the development of energetic molecules, proposing a systematic and effective research model for the design, screening, and synthesis of high-energy, low-sensitivity energetic molecules. We selected the classical insensitive energetic molecule nitroguanidine as the parent molecule and merged it with three other classic energetic molecules through a one-step substitution reaction, efficiently obtaining three classes of new energetic molecules. Analysis and characterization of their properties show that the chimeric molecules 3 and 6 inherit the advantages of the parent energetic molecules, demonstrating high-energy and insensitivity (detonation velocity of 8113 m s-1, impact sensitivity of 35 J for 3; detonation velocity of 8539 m s-1, impact sensitivity of >60 J for 6). Remarkably, chimeric molecule 9 exhibits an acceptable sensitivity (7 J, similar to RDX) while surpassing the energy of the parent molecules significantly (>9000 m/s). The energy of energetic molecule 8 (8742 m/s) is comparable to that of RDX (8754 m/s), and its mechanical sensitivity (50 J) is less sensitive than that of RDX (5.6 J). This study demonstrates the potential of the chimeric energetic molecule strategy for efficiently designing and synthesizing new high-performance energetic molecules in a simple manner.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"81 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678863","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}
Nian Cheng, Weiwei Li, Zhen-Yu Xiao, Han Pan, Dingshan Zheng, Wenxing Yang
Cu2ZnSnS4 (CZTS) and Cu2ZnGeS4 (CZGS) nanoparticles are important inorganic hole transport layers (HTLs) for carbon electrode-based perovskite solar cells (C-PSCs), however the performances of the corresponding C-PSCs are still not satisfactory, which mainly originates from the un-optimized photo-electronic properties of the pristine CZTS and CZGS nanoparticles. Herein, composition engineering via alloying CZTS and CZGS is used to optimize the photo-electronic properties of the resulting CZGxT1-xS HTLs (x = 0, 0.25, 0.50, 0.75, and 1.0), which plays a pivotal role on the performances of the C-PSCs. On one hand, the optimum CZG0.5T0.5S HTL exhibits suitable conduction band energy barrier at the perovskite/CZG0.5T0.5S interface, thus, charge carrier recombination at the perovskite/CZG0.5T0.5S interface could be effectively suppressed. On the other hand, CZG0.5T0.5S HTL exhibit much larger conductivity, which could efficiently transport the holes from perovskite to carbon electrode. Therefore, C-PSCs with the CZG0.5T0.5S HTL could demonstrate a champion power conversion efficiency of 19.76%.
{"title":"Composition engineering of Cu2ZnGexSn1-xS4 nanoparticles hole transport layer for carbon electrode-based perovskite solar cells","authors":"Nian Cheng, Weiwei Li, Zhen-Yu Xiao, Han Pan, Dingshan Zheng, Wenxing Yang","doi":"10.1039/d4ta07106a","DOIUrl":"https://doi.org/10.1039/d4ta07106a","url":null,"abstract":"Cu2ZnSnS4 (CZTS) and Cu2ZnGeS4 (CZGS) nanoparticles are important inorganic hole transport layers (HTLs) for carbon electrode-based perovskite solar cells (C-PSCs), however the performances of the corresponding C-PSCs are still not satisfactory, which mainly originates from the un-optimized photo-electronic properties of the pristine CZTS and CZGS nanoparticles. Herein, composition engineering via alloying CZTS and CZGS is used to optimize the photo-electronic properties of the resulting CZGxT1-xS HTLs (x = 0, 0.25, 0.50, 0.75, and 1.0), which plays a pivotal role on the performances of the C-PSCs. On one hand, the optimum CZG0.5T0.5S HTL exhibits suitable conduction band energy barrier at the perovskite/CZG0.5T0.5S interface, thus, charge carrier recombination at the perovskite/CZG0.5T0.5S interface could be effectively suppressed. On the other hand, CZG0.5T0.5S HTL exhibit much larger conductivity, which could efficiently transport the holes from perovskite to carbon electrode. Therefore, C-PSCs with the CZG0.5T0.5S HTL could demonstrate a champion power conversion efficiency of 19.76%.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"42 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673754","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}
Gang-Ding Wang, Wenjie Shi, Yong-Zhi Li, Weigang Lu, Lei Hou, Dan Li
Separating acetylene (C2H2) from carbon dioxide (CO2) is of great industrial importance for achieving high-purity C2H2 (>99%). However, overcoming the trade-off effect between adsorption capacity and selectivity remains a daunting challenge owing to their similar physicochemical properties. Herein, we present a novel cage-like metal-organic framework termed Cu-TPHC for efficiently purifying C2H2 from C2H2/CO2 mixtures. Cu-TPHC exhibits a high C2H2 uptake (157.5 cm3 g-1), C2H2/CO2 selectivity (4.9), and a relatively low C2H2 adsorption enthalpy (29.6 kJ mol-1) at 298 K. The excellent separation potential was demonstrated by breakthrough experiments for an equimolar C2H2/CO2 mixture under various conditions, with good recyclability and a 99.4 % purity of the recovered C2H2. Grand canonical Monte Carlo simulations reveal that the uncoordinated carboxylate oxygen atoms, coordinated water molecules and free OH- anions provide multiple supramolecular binding sites that preferentially interact with C2H2 over CO2.
{"title":"Enabling High C2H2 Storage and Efficient C2H2/CO2 Separation in a Cage-like MOF with Multiple Supramolecular Binding Sites","authors":"Gang-Ding Wang, Wenjie Shi, Yong-Zhi Li, Weigang Lu, Lei Hou, Dan Li","doi":"10.1039/d4ta06472k","DOIUrl":"https://doi.org/10.1039/d4ta06472k","url":null,"abstract":"Separating acetylene (C2H2) from carbon dioxide (CO2) is of great industrial importance for achieving high-purity C2H2 (>99%). However, overcoming the trade-off effect between adsorption capacity and selectivity remains a daunting challenge owing to their similar physicochemical properties. Herein, we present a novel cage-like metal-organic framework termed Cu-TPHC for efficiently purifying C2H2 from C2H2/CO2 mixtures. Cu-TPHC exhibits a high C2H2 uptake (157.5 cm3 g-1), C2H2/CO2 selectivity (4.9), and a relatively low C2H2 adsorption enthalpy (29.6 kJ mol-1) at 298 K. The excellent separation potential was demonstrated by breakthrough experiments for an equimolar C2H2/CO2 mixture under various conditions, with good recyclability and a 99.4 % purity of the recovered C2H2. Grand canonical Monte Carlo simulations reveal that the uncoordinated carboxylate oxygen atoms, coordinated water molecules and free OH- anions provide multiple supramolecular binding sites that preferentially interact with C2H2 over CO2.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"18 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673762","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}
![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)
N and –CN groups in DCDA with un-coordinated Pb2+, and/or FA+/MA+ via hydrogen bonding, coupled with the –NH2 groups of DCDA forming hydrogen bonding or electrostatic interactions with halide anions to inhibit ion migration, the defects were passivated. The introduction of DCDA effectively retarded nucleation and grain growth, and significantly reduced the film formation rate. Thus, perovskite films with larger grain sizes, preferred orientation, and lower trap state density were obtained, thereby greatly suppressing non-radiative recombination. As a result, the average power conversion efficiency (PCE) of MPSCs treated with DCDA was improved from 17.15 ± 0.48% to 18.75 ± 0.42%, and a champion PCE of 19.12% was obtained. Meanwhile, the PCE of unpackaged MPSC devices still remained at 94.00% of the initial efficiency when stored in an air environment after 103 days, demonstrating excellent stability. The strategy facilitates a deeper understanding of perovskite crystallization in printable MPSCs.
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