Cooperative coupling of hydrogen peroxide (H2O2) photosynthesis with organic pollutant degradation is promising strategy applied in chemical synthesis and environmental protection. Nonetheless, the photocatalytic performance is limited by sluggish photogenerated carrier separation and limited redox potentials. Herein, an S-scheme heterojunction was constructed by assembling the TiO2 nanoparticles and a Schiff-base COF together. The formed S-scheme TiO2/COF heterojunction can efficiently produce H2O2 and degrade Rhodamine B (RhB) synchronously. The S-scheme charge transfer mechanism in TiO2/COF composite is well unveiled by in situ irradiated X-ray photoelectron spectroscopy and DFT calculation. The femtosecond transient absorption spectra reveal the superior charge migration at interface between TiO2 and COF. The designed TiO2/COF composite shows drastically enhanced H2O2 yield of 1326 μmol·g–1·h–1 in RhB solution, and the AQY value of 4.11% under 420 nm monochromatic light irradiation is achieved. Meanwhile, 100% of RhB degraded under light irradiation for 40 min with TiO2/TD COF as photocatalyst. This work exemplifies a promising approach to design COF-based S-scheme heterojunction with ameliorative photocatalytic performance for simultaneous organic pollutants degradation and H2O2 production.
过氧化氢（H2O2）光合作用与有机污染物降解的合作耦合是一种应用于化学合成和环境保护的前景广阔的策略。然而，光生载流子分离缓慢和有限的氧化还原电位限制了光催化性能。本文通过将二氧化钛纳米颗粒和希夫碱 COF 组装在一起，构建了一种 S 型异质结。所形成的 S 型 TiO2/COF 异质结能高效地同步产生 H2O2 和降解罗丹明 B（RhB）。原位辐照 X 射线光电子能谱和 DFT 计算很好地揭示了 TiO2/COF 复合材料中的 S 型电荷转移机制。飞秒瞬态吸收光谱揭示了 TiO2 和 COF 界面上的电荷迁移。设计的 TiO2/COF 复合材料在 RhB 溶液中的 H2O2 产率大幅提高，达到 1326 μmol-g-1-h-1，在 420 纳米单色光照射下的 AQY 值为 4.11%。同时，以 TiO2/TD COF 为光催化剂，在光照射 40 分钟后，100% 的 RhB 降解。这项工作为设计基于 COF 的 S 型异质结提供了一种具有良好光催化性能的方法，可同时降解有机污染物和产生 H2O2。
{"title":"Rapid charge transfer in TiO2/COF S-scheme heterojunction for boosting H2O2 photosynthesis and Rhodamine B degradation","authors":"Yanyan Zhao, Yong Zhang, Haiyan Tan, Chenbin Ai, Jianjun Zhang","doi":"10.1016/j.jmat.2024.100970","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100970","url":null,"abstract":"Cooperative coupling of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) photosynthesis with organic pollutant degradation is promising strategy applied in chemical synthesis and environmental protection. Nonetheless, the photocatalytic performance is limited by sluggish photogenerated carrier separation and limited redox potentials. Herein, an S-scheme heterojunction was constructed by assembling the TiO<sub>2</sub> nanoparticles and a Schiff-base COF together. The formed S-scheme TiO<sub>2</sub>/COF heterojunction can efficiently produce H<sub>2</sub>O<sub>2</sub> and degrade Rhodamine B (RhB) synchronously. The S-scheme charge transfer mechanism in TiO<sub>2</sub>/COF composite is well unveiled by <em>in situ</em> irradiated X-ray photoelectron spectroscopy and DFT calculation. The femtosecond transient absorption spectra reveal the superior charge migration at interface between TiO<sub>2</sub> and COF. The designed TiO<sub>2</sub>/COF composite shows drastically enhanced H<sub>2</sub>O<sub>2</sub> yield of 1326 μmol·g<sup>–1</sup>·h<sup>–1</sup> in RhB solution, and the AQY value of 4.11% under 420 nm monochromatic light irradiation is achieved. Meanwhile, 100% of RhB degraded under light irradiation for 40 min with TiO<sub>2</sub>/TD COF as photocatalyst. This work exemplifies a promising approach to design COF-based S-scheme heterojunction with ameliorative photocatalytic performance for simultaneous organic pollutants degradation and H<sub>2</sub>O<sub>2</sub> production.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"8 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642744","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}
Pub Date : 2024-11-15DOI: 10.1016/j.jmat.2024.100968
Shaoan Yan, Pei Xu, Gang Li, Yingfang Zhu, Yujie Wu, Qilai Chen, Sen Liu, Qingjiang Li, Minghua Tang
Constrained by the inefficiency of traditional trial-and-error methods, especially when dealing with thousands of candidate materials, the swift discovery of materials with specific properties remains a central challenge in contemporary materials research. This study employed an artificial intelligence-driven materials design framework for identifying dopants that impart antiferroelectric properties to HfO2 materials. This strategy integrates density functional theory (DFT) with machine learning (ML) techniques to swiftly screen HfO2 materials exhibiting stable antiferroelectric properties based on the critical electric field. This approach aims to overcome the high cost and lengthy cycles associated with traditional trial-and-error and experimental methods. Among 30 undeveloped dopants, four candidate dopants demonstrating stable antiferroelectric properties were identified. Subsequent DFT analysis highlighted the Ga dopant, which displayed favorable characteristics such as a small volume change, minimal lattice deformation, and a low critical electric field after incorporation into hafnium oxide. These findings suggest the potential for stable antiferroelectric performance. Essentially, we established a correlation between the physical characteristics of hafnium oxide dopants and their antiferroelectric performance. The approach facilitates large-scale ML predictions, rendering it applicable to a broad spectrum of functional material designs.
{"title":"Phase transition mechanism and property prediction of hafnium oxide-based antiferroelectric materials revealed by artificial intelligence","authors":"Shaoan Yan, Pei Xu, Gang Li, Yingfang Zhu, Yujie Wu, Qilai Chen, Sen Liu, Qingjiang Li, Minghua Tang","doi":"10.1016/j.jmat.2024.100968","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100968","url":null,"abstract":"Constrained by the inefficiency of traditional trial-and-error methods, especially when dealing with thousands of candidate materials, the swift discovery of materials with specific properties remains a central challenge in contemporary materials research. This study employed an artificial intelligence-driven materials design framework for identifying dopants that impart antiferroelectric properties to HfO<sub>2</sub> materials. This strategy integrates density functional theory (DFT) with machine learning (ML) techniques to swiftly screen HfO<sub>2</sub> materials exhibiting stable antiferroelectric properties based on the critical electric field. This approach aims to overcome the high cost and lengthy cycles associated with traditional trial-and-error and experimental methods. Among 30 undeveloped dopants, four candidate dopants demonstrating stable antiferroelectric properties were identified. Subsequent DFT analysis highlighted the Ga dopant, which displayed favorable characteristics such as a small volume change, minimal lattice deformation, and a low critical electric field after incorporation into hafnium oxide. These findings suggest the potential for stable antiferroelectric performance. Essentially, we established a correlation between the physical characteristics of hafnium oxide dopants and their antiferroelectric performance. The approach facilitates large-scale ML predictions, rendering it applicable to a broad spectrum of functional material designs.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"6 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637787","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}
Pub Date : 2024-11-14DOI: 10.1016/j.jmat.2024.100964
Lane E. Schultz, Benjamin Afflerbach, Paul M. Voyles, Dane Morgan
We have developed a machine learning model for critical cooling rates for metallic glasses based on computational properties, supporting in-silico screening for desired Rc values and significantly reducing reliance on time-consuming laboratory work. We compare results for features derived from easy-to-compute functions of elemental properties to more complex physically motivated properties using ab initio, machine-learning potentials, and empirical potential molecular dynamics methods. The established approach enables property acquisition across a diverse range of alloys. Analysis of various features for 34 alloys from 20 chemical systems shows that the best model for critical cooling rates was learned from one elemental property-based feature and three simulated features. The elemental property based feature is an ideal entropy value based on alloy stoichiometry. The simulated features were acquired from estimates of energies above the convex hull, changes in heat capacity, and the fraction of icosahedra-like Voronoi polyhedra. Models were assessed through a demanding cross validation test based on repeatedly leaving out full chemical systems as test sets and had an R2 of 0.78 and a mean average error of 0.76 in units of log10(K/s). We demonstrate with Shapley additive explanation analysis that the most impactful features have physically reasonable influence on model predictions. The established methodology can be applied to other high-throughput studies of material properties of diverse compositions.
{"title":"Machine learning metallic glass critical cooling rates through elemental and molecular simulation based featurization","authors":"Lane E. Schultz, Benjamin Afflerbach, Paul M. Voyles, Dane Morgan","doi":"10.1016/j.jmat.2024.100964","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100964","url":null,"abstract":"We have developed a machine learning model for critical cooling rates for metallic glasses based on computational properties, supporting in-silico screening for desired <em>R</em><sub>c</sub> values and significantly reducing reliance on time-consuming laboratory work. We compare results for features derived from easy-to-compute functions of elemental properties to more complex physically motivated properties using ab initio, machine-learning potentials, and empirical potential molecular dynamics methods. The established approach enables property acquisition across a diverse range of alloys. Analysis of various features for 34 alloys from 20 chemical systems shows that the best model for critical cooling rates was learned from one elemental property-based feature and three simulated features. The elemental property based feature is an ideal entropy value based on alloy stoichiometry. The simulated features were acquired from estimates of energies above the convex hull, changes in heat capacity, and the fraction of icosahedra-like Voronoi polyhedra. Models were assessed through a demanding cross validation test based on repeatedly leaving out full chemical systems as test sets and had an <em>R</em><sup>2</sup> of 0.78 and a mean average error of 0.76 in units of log<sub>10</sub>(K/s). We demonstrate with Shapley additive explanation analysis that the most impactful features have physically reasonable influence on model predictions. The established methodology can be applied to other high-throughput studies of material properties of diverse compositions.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"72 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609975","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}
Pub Date : 2024-11-13DOI: 10.1016/j.jmat.2024.100965
Yu Xin, Zerui Liu, Chunyan Wang, Likai Wang, Zhen Zhou, Lu Yang, Hongguo Hao, Lin Jiang, Daopeng Zhang, Jianzhuang Jiang
As a desirable alternative for oxygen evolution reaction (OER), urea oxidation reaction (UOR) with the effectively reduced overpotential has attracted considerable attention in pollutant degradation and rechargeable Zn-air battery (ZAB). Herein, a bifunctional electrocatalyst with CoNi alloy and Co–N dual active sites encapsulated by nitrogen-doped carbon nanotubes have been rationally designed and successfully prepared. The as-obtained catalyst CoNi/Co–NCNT displays excellent catalytic activity for oxygen reduction (ORR) and UOR with a narrow potential difference of 0.56 V. The urea-assisted rechargeable ZABs based on CoNi/Co–NCNT provide higher energy conversion efficiency (61%), 15% higher than that of conventional ZABs. In addition to verify the UOR pathway on the CoNi/Co–NCNT, DFT calculations reveal that CoNi alloy and Co–N in CoNi/Co–NCNT synergistically function as the main active sites for ORR and UOR. The excellent ORR catalytic performance and the superior energy conversion efficiency of CoNi/Co–NCNT based urea-assisted rechargeable ZAB is expected to accelerate the practical application of ZAB technology. This work paved a new way for the development of bifunctional catalysts for higher efficiency ZABs, and also provides a potential scheme for disposing urea rich wastewater.
{"title":"Co–doped nitrogenated carbon nanotubes encapsulating CoNi alloys as bifunctional catalysts for urea-assisted rechargeable Zn-air battery","authors":"Yu Xin, Zerui Liu, Chunyan Wang, Likai Wang, Zhen Zhou, Lu Yang, Hongguo Hao, Lin Jiang, Daopeng Zhang, Jianzhuang Jiang","doi":"10.1016/j.jmat.2024.100965","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100965","url":null,"abstract":"As a desirable alternative for oxygen evolution reaction (OER), urea oxidation reaction (UOR) with the effectively reduced overpotential has attracted considerable attention in pollutant degradation and rechargeable Zn-air battery (ZAB). Herein, a bifunctional electrocatalyst with CoNi alloy and Co–N dual active sites encapsulated by nitrogen-doped carbon nanotubes have been rationally designed and successfully prepared. The as-obtained catalyst CoNi/Co–NCNT displays excellent catalytic activity for oxygen reduction (ORR) and UOR with a narrow potential difference of 0.56 V. The urea-assisted rechargeable ZABs based on CoNi/Co–NCNT provide higher energy conversion efficiency (61%), 15% higher than that of conventional ZABs. In addition to verify the UOR pathway on the CoNi/Co–NCNT, DFT calculations reveal that CoNi alloy and Co–N in CoNi/Co–NCNT synergistically function as the main active sites for ORR and UOR. The excellent ORR catalytic performance and the superior energy conversion efficiency of CoNi/Co–NCNT based urea-assisted rechargeable ZAB is expected to accelerate the practical application of ZAB technology. This work paved a new way for the development of bifunctional catalysts for higher efficiency ZABs, and also provides a potential scheme for disposing urea rich wastewater.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"127 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601173","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}
Pub Date : 2024-11-13DOI: 10.1016/j.jmat.2024.100962
Laura Cangini, Haofeng Huang, Changhao Zhao, Jurij Koruza, Ke Wang, Jürgen Rödel, Lovro Fulanović
This study investigates the relationship between the electro-mechanical properties of Cu-doped potassium sodium niobate (KNN) piezoceramics driven at high vibration velocities and their structural origins. Intrinsic and extrinsic contributions to the dynamic strain were quantified at high-power resonance conditions by in-situ high-energy X-ray diffraction. These contributions were correlated to the observed sub-coercive dielectric and piezoelectric responses. Cu doping impairs extrinsic contributions of KNN due to the movement of non-180° domains, akin to acceptor-doped hard PZT, reducing the fraction of transverse strain originating from non-180° domain wall motion over the total strain of 5% at 0.8 m/s. Therefore, the performance of Cu-doped KNN and PZT were found to be comparable. Both systems exhibit a high mechanical quality factor at low vibration velocity, which decreases at high displacement rates.Additionally, the temperature dependence of electromechanical properties for different Cu doping amounts was investigated. In particular, the mechanical quality factor at the vibration velocity of 1 m/s in a temperature range of –40 °C to 140 °C was studied. According to the findings, the composition doped with 0.5% Cu exhibited a stable vibration at 1 m/s, with only 10% variation in the mechanical quality factor between 20 °C and 140 °C.
{"title":"Hardening of K0.5Na0.5NbO3 piezoceramics with Cu and the temperature dependence in high-power drive","authors":"Laura Cangini, Haofeng Huang, Changhao Zhao, Jurij Koruza, Ke Wang, Jürgen Rödel, Lovro Fulanović","doi":"10.1016/j.jmat.2024.100962","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100962","url":null,"abstract":"This study investigates the relationship between the electro-mechanical properties of Cu-doped potassium sodium niobate (KNN) piezoceramics driven at high vibration velocities and their structural origins. Intrinsic and extrinsic contributions to the dynamic strain were quantified at high-power resonance conditions by <em>in-situ</em> high-energy X-ray diffraction. These contributions were correlated to the observed sub-coercive dielectric and piezoelectric responses. Cu doping impairs extrinsic contributions of KNN due to the movement of non-180° domains, akin to acceptor-doped hard PZT, reducing the fraction of transverse strain originating from non-180° domain wall motion over the total strain of 5% at 0.8 m/s. Therefore, the performance of Cu-doped KNN and PZT were found to be comparable. Both systems exhibit a high mechanical quality factor at low vibration velocity, which decreases at high displacement rates.Additionally, the temperature dependence of electromechanical properties for different Cu doping amounts was investigated. In particular, the mechanical quality factor at the vibration velocity of 1 m/s in a temperature range of –40 °C to 140 °C was studied. According to the findings, the composition doped with 0.5% Cu exhibited a stable vibration at 1 m/s, with only 10% variation in the mechanical quality factor between 20 °C and 140 °C.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"216 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601170","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}
Traditional ferroelectric materials, such as lead zirconate titanate (PZT) ceramics, exhibit positive strain when subjected to an electric field along the polarization direction. In contrast, the piezoelectric polymer polyvinylidene fluoride (PVDF) and its copolymer P(VDF-TrFE) display unique negative strain properties. While extensive research has focused on understanding the origin and mechanisms of this negative strain, limited efforts have been directed toward regulating these properties. This study optimizes the electro-strain and ferroelectric properties of P(VDF-TrFE) piezoelectric films through the synergistic effect of PbTiO3 nanosheets and an in-situ electrostatic field. Our results demonstrate that while the incorporation of PbTiO3 nanosheets does not notably enhance ferroelectricity, it significantly improves electro-strain properties, particularly negative strain, which increases from –0.097% to –0.185%, an enhancement of 91%. Moreover, the ferroelectric polarization and positive strain of P(VDF-TrFE) are further enhanced under the combined influence of PbTiO3 nanosheets and in-situ electrostatic field, increasing maximum polarization from 10.79 μC/cm2 to 13.16 μC/cm2, a 22% improvement, and positive strain from 0.213% to 0.267%, a 25% enhancement. We propose a possible mechanism for these improvements, attributed to the enhanced flexibility of the amorphous phase and increased content of polar β-phase in P(VDF-TrFE) films under this synergistic effect. This work highlights novel strategies for controlling the electro-strain and ferroelectric properties of P(VDF-TrFE) piezoelectric films.
{"title":"Optimization of electro-strain and ferroelectric properties of P(VDF-TrFE) films under the synergistic effect of PTO nanosheets and in-situ electrostatic field","authors":"Kaiqi Zhu, Fu Lv, Jiamin Lin, Zijian Hong, Yongjun Wu, Yuhui Huang","doi":"10.1016/j.jmat.2024.100963","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100963","url":null,"abstract":"Traditional ferroelectric materials, such as lead zirconate titanate (PZT) ceramics, exhibit positive strain when subjected to an electric field along the polarization direction. In contrast, the piezoelectric polymer polyvinylidene fluoride (PVDF) and its copolymer P(VDF-TrFE) display unique negative strain properties. While extensive research has focused on understanding the origin and mechanisms of this negative strain, limited efforts have been directed toward regulating these properties. This study optimizes the electro-strain and ferroelectric properties of P(VDF-TrFE) piezoelectric films through the synergistic effect of PbTiO<sub>3</sub> nanosheets and an <em>in-situ</em> electrostatic field. Our results demonstrate that while the incorporation of PbTiO<sub>3</sub> nanosheets does not notably enhance ferroelectricity, it significantly improves electro-strain properties, particularly negative strain, which increases from –0.097% to –0.185%, an enhancement of 91%. Moreover, the ferroelectric polarization and positive strain of P(VDF-TrFE) are further enhanced under the combined influence of PbTiO<sub>3</sub> nanosheets and <em>in-situ</em> electrostatic field, increasing maximum polarization from 10.79 μC/cm<sup>2</sup> to 13.16 μC/cm<sup>2</sup>, a 22% improvement, and positive strain from 0.213% to 0.267%, a 25% enhancement. We propose a possible mechanism for these improvements, attributed to the enhanced flexibility of the amorphous phase and increased content of polar β-phase in P(VDF-TrFE) films under this synergistic effect. This work highlights novel strategies for controlling the electro-strain and ferroelectric properties of P(VDF-TrFE) piezoelectric films.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"95 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601172","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}
Pub Date : 2024-11-06DOI: 10.1016/j.jmat.2024.100960
Xiang Yu, Chenyi Li, Li Li, Minghai Yao, Hanxiao Gao, Yuquan Liu, Ze Yuan, Shengfei Tang, Quan Luo, Haibo Zhang, Yang Liu, Huamin Zhou
Biomass dielectric polymers hold promise in developing renewable and biodegradable capacitive energy storage devices. However, their typical discharged energy density remains relatively low (<20 J/cm3) compared to other existing synthetic polymers derived from petroleum sources. Here a greatly enhanced discharged energy density is reported in diluted cyanoethyl cellulose (CEC) nanocomposites with inclusion of ultralow loadings (0.3%, in volume) of 30-nm-sized TiO2 nanoparticles. Owing to the interfacial polarization introduced by interface, the composite of 0.3% exhibits a large dielectric constant of 29.2 at 1 kHz, which can be described by interphase dielectric model. Meanwhile, the introduction of nanofillers facilitate the formation of deeper traps impeding electrical conduction in CEC, which results in an ultrahigh breakdown strength of 732 MV/m. As a result, a remarkable discharged energy density of 12.7 J/cm3 with a charge-discharge efficiency above 90% is achieved, exceeding current ferroelectric-based and biomass-based nanocomposites. Our work opens a novel route for scalable biomass-based dielectrics with high energy storage properties.
{"title":"Superb energy density in biomass-based nanocomposites with ultralow loadings of nanofillers","authors":"Xiang Yu, Chenyi Li, Li Li, Minghai Yao, Hanxiao Gao, Yuquan Liu, Ze Yuan, Shengfei Tang, Quan Luo, Haibo Zhang, Yang Liu, Huamin Zhou","doi":"10.1016/j.jmat.2024.100960","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100960","url":null,"abstract":"Biomass dielectric polymers hold promise in developing renewable and biodegradable capacitive energy storage devices. However, their typical discharged energy density remains relatively low (<20 J/cm<sup>3</sup>) compared to other existing synthetic polymers derived from petroleum sources. Here a greatly enhanced discharged energy density is reported in diluted cyanoethyl cellulose (CEC) nanocomposites with inclusion of ultralow loadings (0.3%, in volume) of 30-nm-sized TiO<sub>2</sub> nanoparticles. Owing to the interfacial polarization introduced by interface, the composite of 0.3% exhibits a large dielectric constant of 29.2 at 1 kHz, which can be described by interphase dielectric model. Meanwhile, the introduction of nanofillers facilitate the formation of deeper traps impeding electrical conduction in CEC, which results in an ultrahigh breakdown strength of 732 MV/m. As a result, a remarkable discharged energy density of 12.7 J/cm<sup>3</sup> with a charge-discharge efficiency above 90% is achieved, exceeding current ferroelectric-based and biomass-based nanocomposites. Our work opens a novel route for scalable biomass-based dielectrics with high energy storage properties.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"95 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594298","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}
Piezo-catalysis, which leverages mechanical energy to drive chemical reactions, is emerging as a promising method for sustainable energy production. While the enhancement of piezo-catalytic performance through metal-support interactions is well-documented, the critical influence of the synthesis atmosphere during metal-loaded piezo-catalyst preparation has been a notable gap in the field. To this end, we systematically investigate how different atmospheric conditions during the synthesis of catalysts—without gas flow or with Ar, N2 and O2—affect metal dispersion, oxidation states, piezo-carrier dynamics, and electronic structure, and subsequently shape the metal-support interactions and piezo-catalytic activity. ZnO/Au, with Au deposited on ZnO, is selected as the model system, and hydrogen evolution reaction is used as the probe reaction. Our results demonstrate that an oxygen-enriched atmosphere significantly enhances the metal-support interactions, achieving an ultrahigh net hydrogen yield of 16.5 mmol·g–1·h–1 on ZnO/Au, a 3.58-fold increase over pristine ZnO. Specifically, the performance improvements substantially surpass those synthesized under other atmospheric conditions. Conversely, exposure to CO2 transforms the ZnO support into ZnCO3, adversely affecting its catalytic activity. These findings reveal the crucial impact of synthesis conditions on piezo-catalyst performance and thereby open new avenues for optimizing catalyst systems for enhanced sustainability.
{"title":"Atmosphere-driven metal-support synergy in ZnO/Au catalysts for efficient piezo-catalytic hydrogen evolution","authors":"Di Wu, Yingxin He, Chi Lin, Bing Li, Jiangping Ma, Lujie Ruan, Yajie Feng, Chaogang Ban, Junjie Ding, Xiaoxing Wang, Danmei Yu, Li-Yong Gan, Xiaoyuan Zhou","doi":"10.1016/j.jmat.2024.100959","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100959","url":null,"abstract":"Piezo-catalysis, which leverages mechanical energy to drive chemical reactions, is emerging as a promising method for sustainable energy production. While the enhancement of piezo-catalytic performance through metal-support interactions is well-documented, the critical influence of the synthesis atmosphere during metal-loaded piezo-catalyst preparation has been a notable gap in the field. To this end, we systematically investigate how different atmospheric conditions during the synthesis of catalysts—without gas flow or with Ar, N<sub>2</sub> and O<sub>2</sub>—affect metal dispersion, oxidation states, piezo-carrier dynamics, and electronic structure, and subsequently shape the metal-support interactions and piezo-catalytic activity. ZnO/Au, with Au deposited on ZnO, is selected as the model system, and hydrogen evolution reaction is used as the probe reaction. Our results demonstrate that an oxygen-enriched atmosphere significantly enhances the metal-support interactions, achieving an ultrahigh net hydrogen yield of 16.5 mmol·g<sup>–1</sup>·h<sup>–1</sup> on ZnO/Au, a 3.58-fold increase over pristine ZnO. Specifically, the performance improvements substantially surpass those synthesized under other atmospheric conditions. Conversely, exposure to CO<sub>2</sub> transforms the ZnO support into ZnCO<sub>3</sub>, adversely affecting its catalytic activity. These findings reveal the crucial impact of synthesis conditions on piezo-catalyst performance and thereby open new avenues for optimizing catalyst systems for enhanced sustainability.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"87 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142579900","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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