Pub Date : 2024-10-28DOI: 10.1016/j.jmat.2024.100945
Mingxin Lu, Yan Fang, Xiaoyu Xu, Xiaoying Feng, Haoqi Xu, Liyang Zhou, Hui Wang, Bin Yan, Chao Chen, Hui Mei, Jie Xu, Feng Gao
Aurivillius phase ceramics exhibit significant potential in high-temperature piezoelectric devices due to their high Curie temperature. However, the rapid decrease in electrical resistivity at high temperatures limits their application. In this work, a series of non-equimolar high-entropy piezoelectric ceramics [CaxSr(1–x)/3Ba(1–x)/3Pb(1–x)/3]Bi4Ti4O15 were designed and prepared via a conventional solid-state method, and the influence of configurational entropy on the microstructure and electrical properties was investigated. The results show that the pure Aurivillius phase was obtained for all compositions. Due to the hysteretic diffusion effect caused by high entropy design, the grain boundary density is effectively increased, leading to a degradation of electrical transport properties. The results of Raman and TEM indicate that disordered structure and various lattice distortions such as edge dislocations, twists, and tilts of oxygen octahedra coexist in high-entropy ceramics, which synergistically contribute to the increase in ceramic electrical resistivity. Consequently, the electrical resistivity at 500 °C increased by 1–2 orders of magnitude, the sample with x = 0.4 exhibits high electrical resistivity (1.18×108 Ω·cm), and also boasts a high piezoelectric coefficient (14 pC/N) and an optimal operating temperature (>550 °C). This work highlights a way to obtain high-performance piezoelectric ceramics with high Curie temperature through the non-equimolar high-entropy composition design.
{"title":"Non-equimolar bismuth-layered [CaxSr(1–x)/3Ba(1–x)/3Pb(1–x)/3]Bi4Ti4O15 high-entropy ceramics with high curie temperature","authors":"Mingxin Lu, Yan Fang, Xiaoyu Xu, Xiaoying Feng, Haoqi Xu, Liyang Zhou, Hui Wang, Bin Yan, Chao Chen, Hui Mei, Jie Xu, Feng Gao","doi":"10.1016/j.jmat.2024.100945","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100945","url":null,"abstract":"Aurivillius phase ceramics exhibit significant potential in high-temperature piezoelectric devices due to their high Curie temperature. However, the rapid decrease in electrical resistivity at high temperatures limits their application. In this work, a series of non-equimolar high-entropy piezoelectric ceramics [Ca<sub><em>x</em></sub>Sr<sub>(1–<em>x</em>)/3</sub>Ba<sub>(1–<em>x</em>)/3</sub>Pb<sub>(1–<em>x</em>)/3</sub>]Bi<sub>4</sub>Ti<sub>4</sub>O<sub>15</sub> were designed and prepared via a conventional solid-state method, and the influence of configurational entropy on the microstructure and electrical properties was investigated. The results show that the pure Aurivillius phase was obtained for all compositions. Due to the hysteretic diffusion effect caused by high entropy design, the grain boundary density is effectively increased, leading to a degradation of electrical transport properties. The results of Raman and TEM indicate that disordered structure and various lattice distortions such as edge dislocations, twists, and tilts of oxygen octahedra coexist in high-entropy ceramics, which synergistically contribute to the increase in ceramic electrical resistivity. Consequently, the electrical resistivity at 500 °C increased by 1–2 orders of magnitude, the sample with <em>x</em> = 0.4 exhibits high electrical resistivity (1.18×10<sup>8</sup> Ω·cm), and also boasts a high piezoelectric coefficient (14 pC/N) and an optimal operating temperature (>550 °C). This work highlights a way to obtain high-performance piezoelectric ceramics with high Curie temperature through the non-equimolar high-entropy composition design.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"118 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520129","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 : 2024-10-28DOI: 10.1016/j.jmat.2024.100943
Da Huo, Biao Wang, Jinhui Fan, Kai Li, Yang Liu, Xudong Qi, Limei Zheng
(K,Na)NbO3 (KNN)-based piezoelectric materials are candidates for replacing Pb-based materials. However, the piezoelectric properties of existing KNN-based single crystals are still inferior to those of Pb-based relaxor ferroelectric single crystals. Moreover, the piezoelectric response mechanism of KNN-based single crystals remains unclear. In this study, (Li,K,Na)(Nb,Sb,Ta)O3:Mn (KNNLST:Mn) single crystals with an excellent piezoelectric coefficient d33 of approximately 778 pC/N were prepared. Systematically studies of intrinsic and extrinsic piezoelectric responses have revealed that the high d33 of KNNLST:Mn single crystals is related to the shear piezoelectric response of a single-domain state and irreversible domain wall motion of the engineering domains. Furthermore, the effect of the orthorhombic (O)-tetragonal (T) phase boundary on intrinsic and extrinsic piezoelectric response is systematically studied, and the impact mechanism is elucidated. The results indicate that a lower dielectric response and elastic constant limit the intrinsic shear piezoelectric response of KNNLST:Mn single crystals, and approaching the O–T phase boundary can enhance both intrinsic and extrinsic piezoelectric responses. This study improves our understanding of the structure-performance relationship in KNN-based single crystals and offers insights for optimizing piezoelectric properties in KNN-based materials.
{"title":"Exploring the mechanisms of enhanced piezoelectric properties in (K,Na)NbO3 single crystals","authors":"Da Huo, Biao Wang, Jinhui Fan, Kai Li, Yang Liu, Xudong Qi, Limei Zheng","doi":"10.1016/j.jmat.2024.100943","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100943","url":null,"abstract":"(K,Na)NbO<sub>3</sub> (KNN)-based piezoelectric materials are candidates for replacing Pb-based materials. However, the piezoelectric properties of existing KNN-based single crystals are still inferior to those of Pb-based relaxor ferroelectric single crystals. Moreover, the piezoelectric response mechanism of KNN-based single crystals remains unclear. In this study, (Li,K,Na)(Nb,Sb,Ta)O<sub>3</sub>:Mn (KNNLST:Mn) single crystals with an excellent piezoelectric coefficient <em>d</em><sub>33</sub> of approximately 778 pC/N were prepared. Systematically studies of intrinsic and extrinsic piezoelectric responses have revealed that the high <em>d</em><sub>33</sub> of KNNLST:Mn single crystals is related to the shear piezoelectric response of a single-domain state and irreversible domain wall motion of the engineering domains. Furthermore, the effect of the orthorhombic (O)-tetragonal (T) phase boundary on intrinsic and extrinsic piezoelectric response is systematically studied, and the impact mechanism is elucidated. The results indicate that a lower dielectric response and elastic constant limit the intrinsic shear piezoelectric response of KNNLST:Mn single crystals, and approaching the O–T phase boundary can enhance both intrinsic and extrinsic piezoelectric responses. This study improves our understanding of the structure-performance relationship in KNN-based single crystals and offers insights for optimizing piezoelectric properties in KNN-based materials.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"101 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519710","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 : 2024-10-15DOI: 10.1016/j.jmat.2024.100944
Xinyu Song, Sen Yan, Yong Wang, Haojie Zhang, Jiacheng Xue, Tengfei Liu, Xiaoyong Tian, Lingling Wu, Hanqing Jiang, Dichen Li
Mechanical vibration isolation with adaptable payloads has always been one of the most challenging topics in mechanical engineering. In this study, we address this problem by introducing machine learning method to search for quasi-zero stiffness metamaterials with arbitrarily predetermined payloads and by employing multi-material 3D printing technology to fabricate them as an integrated part. Dynamic tests demonstrate that both the single- and multi-payload metamaterials can effectively isolate mechanical vibration in low frequency domain. Importantly, the payload of the metamaterial could be arbitrarily designed according to the application scenario and could function at multiple payloads. This design strategy opens new avenues for mechanical energy shielding under various scenarios and under variable loading conditions.
{"title":"Genetic algorithm-enabled mechanical metamaterials for vibration isolation with different payloads","authors":"Xinyu Song, Sen Yan, Yong Wang, Haojie Zhang, Jiacheng Xue, Tengfei Liu, Xiaoyong Tian, Lingling Wu, Hanqing Jiang, Dichen Li","doi":"10.1016/j.jmat.2024.100944","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100944","url":null,"abstract":"Mechanical vibration isolation with adaptable payloads has always been one of the most challenging topics in mechanical engineering. In this study, we address this problem by introducing machine learning method to search for quasi-zero stiffness metamaterials with arbitrarily predetermined payloads and by employing multi-material 3D printing technology to fabricate them as an integrated part. Dynamic tests demonstrate that both the single- and multi-payload metamaterials can effectively isolate mechanical vibration in low frequency domain. Importantly, the payload of the metamaterial could be arbitrarily designed according to the application scenario and could function at multiple payloads. This design strategy opens new avenues for mechanical energy shielding under various scenarios and under variable loading conditions.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439311","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}
There is an urgent need for piezoelectric materials possessing both high piezoelectric properties and good thermal stability to facilitate the advancement of high temperature piezoelectric devices. However, conventional strategy for enhancing piezoelectricity via chemical modifications often comes at the cost of thermal stability due to a drop in Curie temperatures. In this study, we achieved remarkable results in <001>-oriented 0.75BiFeO3–0.25BaTiO3 (0.75BF–0.25BT) lead-free textured ceramics. These textured ceramics exhibit a high Curie temperatures Tc of 552 °C, large piezoelectric coefficients d33 of 265 pC/N, and exceptional piezoelectric thermal stability, with minimal variation of 8% across temperature from 25 °C to 300 °C. Compared to randomly oriented ceramics, the piezoelectric coefficient is about 2.5 times higher, marking it as one of the highest reported value for ceramics with Tc near 550 °C. The enhanced piezoelectric properties can be ascribed to improvements in both intrinsic lattice distortions and extrinsic non-180o domain motions, while the excellent piezoelectric thermal stability is attributed to the stable domain texture. These superior properties of the studied textured 0.75BF–0.25BT ceramics position them as competitive lead-free candidates for high-temperature piezoelectric applications.
为促进高温压电器件的发展，迫切需要同时具有高压电特性和良好热稳定性的压电材料。然而，通过化学修饰增强压电性的传统策略往往以居里温度下降导致热稳定性降低为代价。在这项研究中，我们在取向 0.75BiFeO3-0.25BaTiO3 （0.75BF-0.25BT）无铅纹理陶瓷中取得了令人瞩目的成果。这些纹理陶瓷的居里温度 Tc 高达 552 °C，压电系数 d33 高达 265 pC/N，并且具有优异的压电热稳定性，在 25 °C 至 300 °C 的温度范围内变化极小，仅为 8%。与随机取向陶瓷相比，其压电系数高出约 2.5 倍，是所报道的 Tc 接近 550 °C 的陶瓷中最高值之一。压电特性的增强可归因于内在晶格畸变和外在非 180o 畴运动的改善，而优异的压电热稳定性则归因于稳定的畴纹理。所研究的纹理 0.75BF-0.25BT 陶瓷的这些优异特性使其成为高温压电应用中具有竞争力的无铅候选材料。
{"title":"Advancing piezoelectricity and excellent thermal stability: <001>-textured 0.75BF–0.25BT lead-free ceramics for high temperature applications","authors":"Zhangpan Shen, Jian Guo, Xiaoyi Gao, Weidong Xuan, Jiye Zhang, Dawei Wang, Jinrong Cheng, Shujun Zhang, Jianguo Chen","doi":"10.1016/j.jmat.2024.100946","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100946","url":null,"abstract":"There is an urgent need for piezoelectric materials possessing both high piezoelectric properties and good thermal stability to facilitate the advancement of high temperature piezoelectric devices. However, conventional strategy for enhancing piezoelectricity via chemical modifications often comes at the cost of thermal stability due to a drop in Curie temperatures. In this study, we achieved remarkable results in <001>-oriented 0.75BiFeO<sub>3</sub>–0.25BaTiO<sub>3</sub> (0.75BF–0.25BT) lead-free textured ceramics. These textured ceramics exhibit a high Curie temperatures <em>T</em><sub>c</sub> of 552 °C, large piezoelectric coefficients <em>d</em><sub>33</sub> of 265 pC/N, and exceptional piezoelectric thermal stability, with minimal variation of 8% across temperature from 25 °C to 300 °C. Compared to randomly oriented ceramics, the piezoelectric coefficient is about 2.5 times higher, marking it as one of the highest reported value for ceramics with <em>T</em><sub>c</sub> near 550 °C. The enhanced piezoelectric properties can be ascribed to improvements in both intrinsic lattice distortions and extrinsic non-180<sup>o</sup> domain motions, while the excellent piezoelectric thermal stability is attributed to the stable domain texture. These superior properties of the studied textured 0.75BF–0.25BT ceramics position them as competitive lead-free candidates for high-temperature piezoelectric applications.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"67 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142430442","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 : 2024-10-03DOI: 10.1016/j.jmat.2024.100942
Chunxu Zhao, Huiping Wang, Xinyu Gu, Wei Zhang, Yubao Li
Here we report substantial effects of inserting PVD-prepared highly-conductive ultrathin WOx as interfacial layer in TiN/Hf0.5Zr0.5O2(HZO)/TiN structure on the ferroelectricity of HZO thin films. The prepared TiN/WOx/HZO/WOx/TiN capacitor, exhibiting a remnant polarization (Pr) of 18.8 μC/cm2 at 2 MV/cm and outstanding endurance of over 3.2×109 cycles under 105 Hz bipolar square field cycling. Furthermore, a scalable transfer technique, in which CVD-grown few-layered graphene thin film is used as a sacrificial layer, is developed for transferring HZO-based ferroelectric stack pre-fabricated on SiO2/Si substrate onto a flexible polyimide (PI) membrane, with marginal loss in the ferroelectric properties of HZO. Importantly, mechanical bending testing demonstrates excellent flexibility of TiN/WOx/HZO/WOx/TiN stack, with robust polarization and superb endurance properties being well-maintained even after 104 cycles at a small bending radius of 2 mm. Both implementing ultrathin WOx as interfacial layers and utilizing two-dimensional materials assisted transfer technique would be of great value in the development of HfO2-based flexible ferroelectric memory.
{"title":"Ultrathin WOx interfacial layer improving the ferroelectricity and endurance of Hf0.5Zr0.5O2 thin films on polyimide","authors":"Chunxu Zhao, Huiping Wang, Xinyu Gu, Wei Zhang, Yubao Li","doi":"10.1016/j.jmat.2024.100942","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100942","url":null,"abstract":"Here we report substantial effects of inserting PVD-prepared highly-conductive ultrathin WO<sub>x</sub> as interfacial layer in TiN/Hf<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub>(HZO)/TiN structure on the ferroelectricity of HZO thin films. The prepared TiN/WO<sub><em>x</em></sub>/HZO/WO<sub>x</sub>/TiN capacitor, exhibiting a remnant polarization (<em>P</em><sub>r</sub>) of 18.8 μC/cm<sup>2</sup> at 2 MV/cm and outstanding endurance of over 3.2×10<sup>9</sup> cycles under 10<sup>5</sup> Hz bipolar square field cycling. Furthermore, a scalable transfer technique, in which CVD-grown few-layered graphene thin film is used as a sacrificial layer, is developed for transferring HZO-based ferroelectric stack pre-fabricated on SiO<sub>2</sub>/Si substrate onto a flexible polyimide (PI) membrane, with marginal loss in the ferroelectric properties of HZO. Importantly, mechanical bending testing demonstrates excellent flexibility of TiN/WO<sub><em>x</em></sub>/HZO/WO<sub><em>x</em></sub>/TiN stack, with robust polarization and superb endurance properties being well-maintained even after 10<sup>4</sup> cycles at a small bending radius of 2 mm. Both implementing ultrathin WO<sub><em>x</em></sub> as interfacial layers and utilizing two-dimensional materials assisted transfer technique would be of great value in the development of HfO<sub>2</sub>-based flexible ferroelectric memory.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"223 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142374061","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}
With increasing application demands of electronics and electric vehicles, the energy density of lithium-ion batteries (LIBs) is expected to be higher and higher. The silicon-based anode materials have triggered global research interest due to low operating voltage and high specific capacity. However, for the Si-based anode, the large volume change during cycling causes cracking and pulverization of Si particles, leading to the sluggish kinetics and poor cycle life. In this work, fluoroethylene carbonate (FEC) and lithium bis(fluorosulfonyl)imide (LiFSI) are used as synergistic functional additives to enhance the performance of silicon–carbon (Si–C) composite anode in pouch cell. The properties of solid electrolyte interphase (SEI) formed on the surface of Si–C composite anode have been systematically investigated. The images of different electrolytes infiltration and gas production after formation are analyzed with ultrasonic transmission scanning technique. DFT calculations are used to illustrate the mechanism. All date collection is at pouch cell level, which is more persuasive.
{"title":"Synergistic functional additives on cycling performance of silicon-carbon composite anode in pouch cells","authors":"Jun Cheng, Zhenyu Huang, Anqi Lu, Aiqi He, Yuxuan Shao, Yuxin Fan, Yunhui Huang","doi":"10.1016/j.jmat.2024.100941","DOIUrl":"https://doi.org/10.1016/j.jmat.2024.100941","url":null,"abstract":"With increasing application demands of electronics and electric vehicles, the energy density of lithium-ion batteries (LIBs) is expected to be higher and higher. The silicon-based anode materials have triggered global research interest due to low operating voltage and high specific capacity. However, for the Si-based anode, the large volume change during cycling causes cracking and pulverization of Si particles, leading to the sluggish kinetics and poor cycle life. In this work, fluoroethylene carbonate (FEC) and lithium bis(fluorosulfonyl)imide (LiFSI) are used as synergistic functional additives to enhance the performance of silicon–carbon (Si–C) composite anode in pouch cell. The properties of solid electrolyte interphase (SEI) formed on the surface of Si–C composite anode have been systematically investigated. The images of different electrolytes infiltration and gas production after formation are analyzed with ultrasonic transmission scanning technique. DFT calculations are used to illustrate the mechanism. All date collection is at pouch cell level, which is more persuasive.","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"129 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142360660","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 : 2024-08-31DOI: 10.1016/j.jmat.2024.100935
Qi Geng , Zhen Liu , Yuzhou Liu , Zhe Wang , Zhongliang Gao , Xin Sun , Yingfeng Li , Lei Chen , Xiaojun Lv , Meicheng Li
Silicon (Si) hybrid solar cells have advantages of solution manufacturing process and the potential for achieving low-cost fabrication compared to crystalline Si solar cells. However, the functional layer prepared by solution method usually absorbs water molecules from the air, posing a challenge to the stability of the device. Here, a PEDOT derivative, PEDOT:A, was in situ prepared through the introduction of a fluoropolymer, yielding a strongly hydrophobic film that was assembled into a PEDOT:A/Si hybrid solar cell. The PEDOT:A/Si hybrid solar cells retained 90% of its initial performance after storage in the air for 300 h, while PEDOT:PSS only retained 60% with identical device structure. Meanwhile, first principles calculations indicate that the binding energy between fluoropolymer and water molecule was 3.48 kJ/mol, whereas the binding energy between PSS and water molecule was −5.76 kJ/mol. Benefiting from the weak interaction between fluoropolymer and water molecule, the contact angle of water on PEDOT:A film was 100.84°. After optimization, PEDOT:A/Si hybrid solar cells with ITO achieved a power conversion efficiency of 6.43%, retained 97% of its initial efficiency after testing under same conditions. The development of air-stable hybrid device technology is promising in opening up practical applications of low-cost Si based solar cells.
{"title":"Air-stable silicon hybrid solar cells constructed via hydrophobic polymer film","authors":"Qi Geng , Zhen Liu , Yuzhou Liu , Zhe Wang , Zhongliang Gao , Xin Sun , Yingfeng Li , Lei Chen , Xiaojun Lv , Meicheng Li","doi":"10.1016/j.jmat.2024.100935","DOIUrl":"10.1016/j.jmat.2024.100935","url":null,"abstract":"<div><div>Silicon (Si) hybrid solar cells have advantages of solution manufacturing process and the potential for achieving low-cost fabrication compared to crystalline Si solar cells. However, the functional layer prepared by solution method usually absorbs water molecules from the air, posing a challenge to the stability of the device. Here, a PEDOT derivative, PEDOT:A, was <em>in situ</em> prepared through the introduction of a fluoropolymer, yielding a strongly hydrophobic film that was assembled into a PEDOT:A/Si hybrid solar cell. The PEDOT:A/Si hybrid solar cells retained 90% of its initial performance after storage in the air for 300 h, while PEDOT:PSS only retained 60% with identical device structure. Meanwhile, first principles calculations indicate that the binding energy between fluoropolymer and water molecule was 3.48 kJ/mol, whereas the binding energy between PSS and water molecule was −5.76 kJ/mol. Benefiting from the weak interaction between fluoropolymer and water molecule, the contact angle of water on PEDOT:A film was 100.84°. After optimization, PEDOT:A/Si hybrid solar cells with ITO achieved a power conversion efficiency of 6.43%, retained 97% of its initial efficiency after testing under same conditions. The development of air-stable hybrid device technology is promising in opening up practical applications of low-cost Si based solar cells.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 3","pages":"Article 100935"},"PeriodicalIF":8.4,"publicationDate":"2024-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142535894","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.jmat.2024.100934
Jin Wang , Jiaming Li , Yuan Li, Gaoke Zhang
Achieving efficient photocatalytic activation of peroxymonosulfate (PMS) degradation of pollutants through the regulation strategy of surface microstructure in catalysts remains a challenge. Herein, CuBi2O4 nanorods (CBO NRs) and CuBi2O4 microspheres (CBO Ms) were synthesized by simply regulating the alkalinity of the reaction solvent. Under full–spectrum irradiation, CBO Ms exhibited remarkable photocatalytic performance, removing 92.48% of tetracycline (TC) within 12 min, with the reaction rate constant reaching 0.2135 min−1, which is approximately 2.7 times that of CBO NRs (0.0798 min−1). The exposure of oxygen vacancies on the surface of CBO Ms significantly promoted the generation and migration of photogenerated carriers internally, accelerated charge accumulation at the Cu active sites on the surface, and thereby enhanced the adsorption of CBO Ms on PMS. The charge density difference results confirmed the rapid transference of surface–enriched electrons to the PMS, facilitating further activation of PMS. Radical quenching experiment and EPR testing verified that both radical (SO4•−, •OH) and non–radical (1O2) pathways were involved in the reaction system. This study offers novel insights into the design of catalysts for the photocatalytic activation of PMS to efficiently degrade environmental pollutants.
通过调节催化剂的表面微结构来实现高效光催化激活过一硫酸盐（PMS）降解污染物仍然是一项挑战。本文通过简单调节反应溶剂的碱度，合成了 CuBi2O4 纳米棒（CBO NRs）和 CuBi2O4 微球（CBO Ms）。在全光谱辐照下，CBO Ms表现出显著的光催化性能，在12分钟内去除92.48%的四环素（TC），反应速率常数达到0.2135 min-1，约为CBO NRs（0.0798 min-1）的2.7倍。CBO Ms 表面氧空位的暴露极大地促进了光生载流子在内部的生成和迁移，加速了表面 Cu 活性位点的电荷积累，从而增强了 CBO Ms 在 PMS 上的吸附。电荷密度差结果证实了表面富集的电子迅速转移到 PMS 上，促进了 PMS 的进一步活化。自由基淬灭实验和 EPR 测试证实，反应体系中同时存在自由基（SO4--、-OH）和非自由基（1O2）途径。这项研究为设计光催化活化 PMS 以高效降解环境污染物的催化剂提供了新的见解。
{"title":"Unveiling the structure–activity relationships of tetracycline degradation by photocatalytic activation peroxymonosulfate of CuBi2O4 microspheres: DFT calculation and mechanism insight","authors":"Jin Wang , Jiaming Li , Yuan Li, Gaoke Zhang","doi":"10.1016/j.jmat.2024.100934","DOIUrl":"10.1016/j.jmat.2024.100934","url":null,"abstract":"<div><div>Achieving efficient photocatalytic activation of peroxymonosulfate (PMS) degradation of pollutants through the regulation strategy of surface microstructure in catalysts remains a challenge. Herein, CuBi<sub>2</sub>O<sub>4</sub> nanorods (CBO NRs) and CuBi<sub>2</sub>O<sub>4</sub> microspheres (CBO Ms) were synthesized by simply regulating the alkalinity of the reaction solvent. Under full–spectrum irradiation, CBO Ms exhibited remarkable photocatalytic performance, removing 92.48% of tetracycline (TC) within 12 min, with the reaction rate constant reaching 0.2135 min<sup>−1</sup>, which is approximately 2.7 times that of CBO NRs (0.0798 min<sup>−1</sup>). The exposure of oxygen vacancies on the surface of CBO Ms significantly promoted the generation and migration of photogenerated carriers internally, accelerated charge accumulation at the Cu active sites on the surface, and thereby enhanced the adsorption of CBO Ms on PMS. The charge density difference results confirmed the rapid transference of surface–enriched electrons to the PMS, facilitating further activation of PMS. Radical quenching experiment and EPR testing verified that both radical (SO<sub>4</sub><sup>•−</sup>, •OH) and non–radical (<sup>1</sup>O<sub>2</sub>) pathways were involved in the reaction system. This study offers novel insights into the design of catalysts for the photocatalytic activation of PMS to efficiently degrade environmental pollutants.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 3","pages":"Article 100934"},"PeriodicalIF":8.4,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142536060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-27DOI: 10.1016/j.jmat.2024.06.010
Aoyun Meng , Renqiang Yang , Wen Li , Zhen Li , Jinfeng Zhang
In addressing the severe energy crisis, adopting efficient and reliable strategies is crucial. Photocatalysis technology, utilizing solar energy to convert it into hydrogen, offers an effective pathway to alleviate energy issues. In this study, we have successfully developed the TiO2/CdSxSe1–x-Diethylenetriamine (abbreviated as DETA) nanocomposites with an S-scheme heterojunction structure. By precisely adjusting the value of x (x = 0, 0.25, 0.50, 0.75 or 1.00), we optimized the charge transfer process, achieving efficient photocatalytic hydrogen evolution reaction. Specifically, the sample containing 20% (in mass) TiO2, denoted as 20-TO, exhibited the best photocatalytic activity. In particular, the activity of 20% (in mass) TiO2/CdS0.25Se0.75-DETA (abbreviated as 20-TO/CS0.25E0.75) reached 32.7 mmol·g−1·h−1, maintaining high hydrogen evolution performance over ten consecutive cycles (totaling 40 h). We used electron paramagnetic resonance (EPR), ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS), femtosecond transient absorption spectroscopy (fs-TAS) and theoretical calculations to comprehensively confirm that the heterojunctions in all nanocomposites conform to the S-scheme mechanism. This mechanism provides an optimal path for charge transfer. Comparative analysis through theoretical calculations revealed that the charge transfer efficiency between TO and CS0.25E0.75 was the highest, which correlates well with the experimental results of photocatalytic hydrogen evolution. This innovative nanocomposites enhances new energy technologies with its efficient charge transfer.
要解决严重的能源危机，采取高效可靠的战略至关重要。利用太阳能将其转化为氢气的光催化技术为缓解能源问题提供了一条有效途径。在这项研究中，我们成功开发了具有 S 型异质结结构的 TiO2/CdSxSe1-x-Diethylenetriamine （简称 DETA）纳米复合材料。通过精确调节 x 值（x = 0、0.25、0.50、0.75 或 1.00），我们优化了电荷转移过程，实现了高效的光催化氢进化反应。具体而言，含有 20% （质量分数）TiO2 的样品（记为 20-TO）表现出最佳的光催化活性。其中，20%（质量分数）TiO2/CdS0.25Se0.75-DETA（简称 20-TO/CS0.25E0.75）的活性达到了 32.7 mmol-g-1-h-1，在连续十次循环（共 40 小时）中保持了较高的氢气进化性能。我们利用电子顺磁共振（EPR）、紫外可见光漫反射光谱（UV-Vis DRS）、飞秒瞬态吸收光谱（fs-TAS）和理论计算全面证实了所有纳米复合材料中的异质结都符合 S 型机制。这种机制为电荷转移提供了最佳路径。理论计算的对比分析表明，TO 和 CS0.25E0.75 之间的电荷转移效率最高，这与光催化氢进化的实验结果非常吻合。这种创新的纳米复合材料可通过高效的电荷转移增强新能源技术。
{"title":"Enhanced photocatalytic hydrogen production through tuning charge transfer in TiO2/CdSxSe1–x-DETA nanocomposites with S-scheme heterojunction structure","authors":"Aoyun Meng , Renqiang Yang , Wen Li , Zhen Li , Jinfeng Zhang","doi":"10.1016/j.jmat.2024.06.010","DOIUrl":"10.1016/j.jmat.2024.06.010","url":null,"abstract":"<div><div>In addressing the severe energy crisis, adopting efficient and reliable strategies is crucial. Photocatalysis technology, utilizing solar energy to convert it into hydrogen, offers an effective pathway to alleviate energy issues. In this study, we have successfully developed the TiO<sub>2</sub>/CdS<sub><em>x</em></sub>Se<sub>1–<em>x</em></sub>-Diethylenetriamine (abbreviated as DETA) nanocomposites with an S-scheme heterojunction structure. By precisely adjusting the value of <em>x</em> (<em>x</em> = 0, 0.25, 0.50, 0.75 or 1.00), we optimized the charge transfer process, achieving efficient photocatalytic hydrogen evolution reaction. Specifically, the sample containing 20% (in mass) TiO<sub>2</sub>, denoted as 20-TO, exhibited the best photocatalytic activity. In particular, the activity of 20% (in mass) TiO<sub>2</sub>/CdS<sub>0.25</sub>Se<sub>0.75</sub>-DETA (abbreviated as 20-TO/CS0.25E0.75) reached 32.7 mmol·g<sup>−1</sup>·h<sup>−1</sup>, maintaining high hydrogen evolution performance over ten consecutive cycles (totaling 40 h). We used electron paramagnetic resonance (EPR), ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS), femtosecond transient absorption spectroscopy (fs-TAS) and theoretical calculations to comprehensively confirm that the heterojunctions in all nanocomposites conform to the S-scheme mechanism. This mechanism provides an optimal path for charge transfer. Comparative analysis through theoretical calculations revealed that the charge transfer efficiency between TO and CS0.25E0.75 was the highest, which correlates well with the experimental results of photocatalytic hydrogen evolution. This innovative nanocomposites enhances new energy technologies with its efficient charge transfer.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 3","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141839896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-26DOI: 10.1016/j.jmat.2024.07.004
Huili Ran , Xue Liu , Jiajie Fan , Yun Yang , Lijie Zhang , Qin Guo , Bicheng Zhu , Quanlong Xu
The construction of heterojunction is an effective way to promote the photoinduced charge carrier separation in spatial, thus accelerating the photocatalytic reaction. However, the regulation of interface properties, as a crucial factor in affecting the charge carrier diffusion process, still remains a significant challenge. In this work, BiOBr/TpBD-COF heterojunction was successfully constructed via a novel phase transformation strategy. Specifically, perovskite Cs3Bi2Br9 was first synthesized and then in-situ transformed into BiOBr during the preparation of TpBD-COF procedure, thus obtaining BiOBr/TpBD-COF heterojunction with favorable interface. According to the in-situ X-ray photoelectron spectroscopy (XPS) characterization and electron paramagnetic resonance (EPR) analysis, the photogenerated electrons with weak reduction power transfer from BiOBr to TpBD-COF driven by the internal electric field under irradiation, conforming to S-scheme charge transfer mode. As a result, the photogenerated electrons and holes with strong redox abilities are spatially located on TpBD-COF and BiOBr surface, respectively, endowing the strong driving force toward the water splitting reaction. The optimized 10%BiOBr/TpBD-COF displayed remarkably enhanced photocatalytic hydrogen evolution rate (16.17 mmol⋅g−1⋅h−1) in comparison with TpBD-COF (5.18 mmol⋅g−1⋅h−1). This study will provide some novel inspirations for developing efficient COF-based S-scheme heterojunction photocatalysts.
构建异质结是促进空间光诱导电荷载流子分离，从而加速光催化反应的有效方法。然而，作为影响电荷载流子扩散过程的关键因素，界面性质的调控仍然是一个重大挑战。在这项工作中，通过一种新颖的相变策略，成功地构建了 BiOBr/TpBD-COF 异质结。具体来说，首先合成了包晶Cs3Bi2Br9，然后在制备TpBD-COF的过程中将其原位转化为BiOBr，从而获得了具有良好界面的BiOBr/TpBD-COF异质结。根据原位 X 射线光电子能谱（XPS）表征和电子顺磁共振（EPR）分析，在内部电场的驱动下，光生电子以微弱的还原力从 BiOBr 向 TpBD-COF 转移，符合 S 型电荷转移模式。因此，具有强氧化还原能力的光生电子和空穴分别位于 TpBD-COF 和 BiOBr 表面，为水分离反应提供了强大的驱动力。优化后的 10%BiOBr/TpBD-COF 与 TpBD-COF 相比（5.18 mmol⋅g-1⋅h-1），光催化氢进化率显著提高（16.17 mmol⋅g-1⋅h-1）。这项研究将为开发基于 COF 的高效 S 型异质结光催化剂提供一些新的启发。
{"title":"Engineering BiOBr/TpBD-COF S-scheme heterointerface via phase transformation strategy for boosted photocatalytic hydrogen generation","authors":"Huili Ran , Xue Liu , Jiajie Fan , Yun Yang , Lijie Zhang , Qin Guo , Bicheng Zhu , Quanlong Xu","doi":"10.1016/j.jmat.2024.07.004","DOIUrl":"10.1016/j.jmat.2024.07.004","url":null,"abstract":"<div><div>The construction of heterojunction is an effective way to promote the photoinduced charge carrier separation in spatial, thus accelerating the photocatalytic reaction. However, the regulation of interface properties, as a crucial factor in affecting the charge carrier diffusion process, still remains a significant challenge. In this work, BiOBr/TpBD-COF heterojunction was successfully constructed <em>via</em> a novel phase transformation strategy. Specifically, perovskite Cs<sub>3</sub>Bi<sub>2</sub>Br<sub>9</sub> was first synthesized and then <em>in-situ</em> transformed into BiOBr during the preparation of TpBD-COF procedure, thus obtaining BiOBr/TpBD-COF heterojunction with favorable interface. According to the <em>in-situ</em> X-ray photoelectron spectroscopy (XPS) characterization and electron paramagnetic resonance (EPR) analysis, the photogenerated electrons with weak reduction power transfer from BiOBr to TpBD-COF driven by the internal electric field under irradiation, conforming to S-scheme charge transfer mode. As a result, the photogenerated electrons and holes with strong redox abilities are spatially located on TpBD-COF and BiOBr surface, respectively, endowing the strong driving force toward the water splitting reaction. The optimized 10%BiOBr/TpBD-COF displayed remarkably enhanced photocatalytic hydrogen evolution rate (16.17 mmol⋅g<sup>−1</sup>⋅h<sup>−1</sup>) in comparison with TpBD-COF (5.18 mmol⋅g<sup>−1</sup>⋅h<sup>−1</sup>). This study will provide some novel inspirations for developing efficient COF-based S-scheme heterojunction photocatalysts.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 3","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141848492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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