The exceptional photoelectric performance and high compatibility of perovskite materials render perovskite solar cells highly promising for extensive development, thus garnering significant attention. In perovskite solar cells, the hole transport layer plays a crucial role. For the commonly employed organic small molecule hole transport material Spiro-OMeTAD, a certain period of oxidation treatment is required to achieve complete transport performance. However, this posttreatment oxidation processes typically rely on ambient oxidation, which poses challenges in terms of precise control and leads to degradation of the perovskite light absorption layer. This approach fails to meet the demands for high efficiency and stability in practical application. Herein, the mechanism of ultrafast laser on Spiro-OMeTAD and the reaction process for laser-induced oxidation of it are investigated. PbI2 at Perovskite/Spiro-OMeTAD interface breaks down to produce I2 upon ultrafast laser irradiation and I2 promote the oxidation process. Through the laser irradiation oxidation processing, a higher stability of perovskite solar cells is achieved. This work establishes a new approach toward oxidation treatment of Spiro-OMeTAD.
{"title":"Ultrafast Laser Irradiation Induced Oxidation of Dopant-Free Spiro-OMeTAD for Improving the Perovskite Solar Cells Performance","authors":"Jiaqi Meng, Xiangyu Chen, Weihan Li, Nianyao Chai, Zhongle Zeng, Yunfan Yue, Fengyi Zhao, Xuewen Wang","doi":"10.1002/eem2.12818","DOIUrl":"https://doi.org/10.1002/eem2.12818","url":null,"abstract":"The exceptional photoelectric performance and high compatibility of perovskite materials render perovskite solar cells highly promising for extensive development, thus garnering significant attention. In perovskite solar cells, the hole transport layer plays a crucial role. For the commonly employed organic small molecule hole transport material Spiro-OMeTAD, a certain period of oxidation treatment is required to achieve complete transport performance. However, this posttreatment oxidation processes typically rely on ambient oxidation, which poses challenges in terms of precise control and leads to degradation of the perovskite light absorption layer. This approach fails to meet the demands for high efficiency and stability in practical application. Herein, the mechanism of ultrafast laser on Spiro-OMeTAD and the reaction process for laser-induced oxidation of it are investigated. PbI<sub>2</sub> at Perovskite/Spiro-OMeTAD interface breaks down to produce I<sub>2</sub> upon ultrafast laser irradiation and I<sub>2</sub> promote the oxidation process. Through the laser irradiation oxidation processing, a higher stability of perovskite solar cells is achieved. This work establishes a new approach toward oxidation treatment of Spiro-OMeTAD.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142182240","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}
Kubra Aydin, Mansu Kim, Hyunho Seok, Chulwoo Bae, Jinhyoung Lee, Muyoung Kim, Jonghwan Park, Joseph T. Hupp, Dongmok Whang, Hyeong-U Kim, Taesung Kim
The exploration of heterostructures composed of two-dimensional (2D) transition metal dichalcogenide (TMDc) materials has garnered significant research attention due to the distinctive properties of each individual component and their phase-dependent unique properties. Using the plasma-enhanced chemical vapor deposition (PECVD) method, we analyze the fabrication of heterostructures consisting of two phases of molybdenum disulfide (MoS2) in four different cases. The initial hydrogen evolution reaction (HER) polarization curve indicates that the activity of the heterostructure MoS2 is consistent with that of the underlying MoS2, rather than the surface activity of the upper MoS2. This behavior can be attributed to the presence of Schottky barriers, which include contact resistance, which significantly hampers the efficient charge transfer at junctions between the two different phases of MoS2 layers and is mediated by van der Waals bonds. Remarkably, the energy barrier at the junction dissipates upon reaching a certain electrochemical potential, indicating surface activation from the top phase of MoS2 in the heterostructure. Notably, the 1T/2H MoS2 heterostructure demonstrates enhanced electrochemical stability compared to its metastable 1T-MoS2. This fundamental understanding paves the way for the creation of phase-controllable heterostructures through an experimentally viable PECVD, offering significant promise for a wide range of applications.
{"title":"Unlocking of Schottky Barrier Near the Junction of MoS2 Heterostructure Under Electrochemical Potential","authors":"Kubra Aydin, Mansu Kim, Hyunho Seok, Chulwoo Bae, Jinhyoung Lee, Muyoung Kim, Jonghwan Park, Joseph T. Hupp, Dongmok Whang, Hyeong-U Kim, Taesung Kim","doi":"10.1002/eem2.12800","DOIUrl":"https://doi.org/10.1002/eem2.12800","url":null,"abstract":"The exploration of heterostructures composed of two-dimensional (2D) transition metal dichalcogenide (TMDc) materials has garnered significant research attention due to the distinctive properties of each individual component and their phase-dependent unique properties. Using the plasma-enhanced chemical vapor deposition (PECVD) method, we analyze the fabrication of heterostructures consisting of two phases of molybdenum disulfide (MoS<sub>2</sub>) in four different cases. The initial hydrogen evolution reaction (HER) polarization curve indicates that the activity of the heterostructure MoS<sub>2</sub> is consistent with that of the underlying MoS<sub>2</sub>, rather than the surface activity of the upper MoS<sub>2</sub>. This behavior can be attributed to the presence of Schottky barriers, which include contact resistance, which significantly hampers the efficient charge transfer at junctions between the two different phases of MoS<sub>2</sub> layers and is mediated by van der Waals bonds. Remarkably, the energy barrier at the junction dissipates upon reaching a certain electrochemical potential, indicating surface activation from the top phase of MoS<sub>2</sub> in the heterostructure. Notably, the 1T/2H MoS<sub>2</sub> heterostructure demonstrates enhanced electrochemical stability compared to its metastable 1T-MoS<sub>2</sub>. This fundamental understanding paves the way for the creation of phase-controllable heterostructures through an experimentally viable PECVD, offering significant promise for a wide range of applications.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"40 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141934965","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}
Triboelectric nanogenerators (TENGs) are emerging as new technologies to harvest electrical power from mechanical energy. With the distinctive working mechanism of triboelectric nanogenerators, they attract particular interest in healthcare monitoring, wearable electronics, and deformable energy harvesting, which raises the requirement for highly conformable devices with substantial energy outputs. Here, a simple, low-cost strategy for fabricating stretchable triboelectric nanogenerators with ultra-high electrical output is developed. The TENG is prepared using PTFE micron particles (PP-TENG), contributing a different electrostatic induction process compared to TENG based on dielectric films, which was associated with the dynamics of particle motions in PP-TENG. The generator achieved an impressive voltage output of 1000 V with a current of 25 μA over a contact area of 40 × 20 mm2. Additionally, the TENG exhibits excellent durability with a stretching strain of 500%, and the electrical output performance does not show any significant degradation even after 3000 cycles at a strain of 400%. The unique design of the device provides high conformability and can be used as a self-powered sensor for human motion detection.
{"title":"A High-Performance Stretchable Triboelectric Nanogenerator Based on Polytetrafluoroethylene (PTFE) Particles","authors":"Jiawei Liu, Jinhui Wang, Yawen Wang, Zhilin Wu, Hongbiao Sun, Yan Yang, Lisheng Zhang, Xu Kou, Pengyuan Li, Wenbin Kang, Jiangxin Wang","doi":"10.1002/eem2.12814","DOIUrl":"https://doi.org/10.1002/eem2.12814","url":null,"abstract":"Triboelectric nanogenerators (TENGs) are emerging as new technologies to harvest electrical power from mechanical energy. With the distinctive working mechanism of triboelectric nanogenerators, they attract particular interest in healthcare monitoring, wearable electronics, and deformable energy harvesting, which raises the requirement for highly conformable devices with substantial energy outputs. Here, a simple, low-cost strategy for fabricating stretchable triboelectric nanogenerators with ultra-high electrical output is developed. The TENG is prepared using PTFE micron particles (PP-TENG), contributing a different electrostatic induction process compared to TENG based on dielectric films, which was associated with the dynamics of particle motions in PP-TENG. The generator achieved an impressive voltage output of 1000 V with a current of 25 μA over a contact area of 40 × 20 mm<sup>2</sup>. Additionally, the TENG exhibits excellent durability with a stretching strain of 500%, and the electrical output performance does not show any significant degradation even after 3000 cycles at a strain of 400%. The unique design of the device provides high conformability and can be used as a self-powered sensor for human motion detection.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"44 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141968801","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}
Ashish Gaur, Enkhtuvshin Enkhbayar, Jatin Sharma, Sungwook Mhin, HyukSu Han
Seawater is the most abundant source of molecular hydrogen. Utilizing the hydrogen reserves present in the seawater may inaugurate innovative strategies aimed at advancing sustainable energy and environmental preservation endeavors in the future. Recently, there has been a surge in study in the field addressing the production of hydrogen through the electrochemical seawater splitting. However, the performance and durability of the electrode have limitations due to the fact that there are a few challenges that need to be addressed in order to make the technology suitable for the industrial purpose. The active site blockage caused by chloride ions that are prevalent in seawater and chloride corrosion is the most significant issue; it has a negative impact on both the activity and the durability of the anode component. Addressing this particular issue is of upmost importance in the seawater splitting area. This review concentrates on the newly developed materials and techniques for inhibiting chloride ions by blocking the active sites, simultaneously preventing the chloride corrosion. It is anticipated that the concept will be advantageous for a large audience and will inspire researchers to study on this particular area of concern.
{"title":"Chloride-Ion Blocking in Seawater Electrolysis: Narrating the Tale of Likes and Dislikes Between Anode and Ions","authors":"Ashish Gaur, Enkhtuvshin Enkhbayar, Jatin Sharma, Sungwook Mhin, HyukSu Han","doi":"10.1002/eem2.12817","DOIUrl":"https://doi.org/10.1002/eem2.12817","url":null,"abstract":"Seawater is the most abundant source of molecular hydrogen. Utilizing the hydrogen reserves present in the seawater may inaugurate innovative strategies aimed at advancing sustainable energy and environmental preservation endeavors in the future. Recently, there has been a surge in study in the field addressing the production of hydrogen through the electrochemical seawater splitting. However, the performance and durability of the electrode have limitations due to the fact that there are a few challenges that need to be addressed in order to make the technology suitable for the industrial purpose. The active site blockage caused by chloride ions that are prevalent in seawater and chloride corrosion is the most significant issue; it has a negative impact on both the activity and the durability of the anode component. Addressing this particular issue is of upmost importance in the seawater splitting area. This review concentrates on the newly developed materials and techniques for inhibiting chloride ions by blocking the active sites, simultaneously preventing the chloride corrosion. It is anticipated that the concept will be advantageous for a large audience and will inspire researchers to study on this particular area of concern.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"21 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141934964","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}
Yan Chen, Mingcong Yang, Wei Hu, Tao Chen, Jun Li, Shun Wang, Huile Jin, Jichang Wang
Organic cathode materials exhibit higher energy storage capacity, their poor cyclability due to dissolution in liquid organic electrolytes remains a challenge. However, recently, the electrochemical behavior of organopolysulfides incorporating N-heterocycles unveils promising cathode materials with stable cycling performance. Herein, the integration of organosulfides salt as cathodes with solid electrolytes, exemplified by sodium allyl(methyl)carbamodithioate and sodium diethylcarbamodithioate with a polymer solid electrolyte of polyethylene oxide and LiTFSI, addresses the poor electrochemical stability of organic electrodes. Comparative analysis highlights sodium allyl(methyl)carbamodithioate's superior electrochemical performance and stability compared with sodium diethylcarbamodithioate, emphasizing the efficacy of periphery aliphatic modification in enhancing electrode capacity, rate performance, and electrochemical stability for organosulfide materials within all-solid-state lithium organic batteries. We also explore the origin of periphery aliphatic modification in these enhancing electrochemical performances by kinetic analysis and thermodynamic analysis. Furthermore, employing density functional theory calculations and ex situ FTIR experiments elucidates the critical role of the N–C=S structure in the energy storage mechanism. This research advances organic cathode design within organosulfide materials, unlocking the potential of all-solid-state lithium organic batteries with enhanced cyclability, propelling the development of next-generation energy storage systems.
{"title":"Tailoring the Periphery Aliphatic Group of Cathode Organosulfide for Rechargeable High-Performance All-Solid-State Lithium Battery","authors":"Yan Chen, Mingcong Yang, Wei Hu, Tao Chen, Jun Li, Shun Wang, Huile Jin, Jichang Wang","doi":"10.1002/eem2.12819","DOIUrl":"https://doi.org/10.1002/eem2.12819","url":null,"abstract":"Organic cathode materials exhibit higher energy storage capacity, their poor cyclability due to dissolution in liquid organic electrolytes remains a challenge. However, recently, the electrochemical behavior of organopolysulfides incorporating N-heterocycles unveils promising cathode materials with stable cycling performance. Herein, the integration of organosulfides salt as cathodes with solid electrolytes, exemplified by sodium allyl(methyl)carbamodithioate and sodium diethylcarbamodithioate with a polymer solid electrolyte of polyethylene oxide and LiTFSI, addresses the poor electrochemical stability of organic electrodes. Comparative analysis highlights sodium allyl(methyl)carbamodithioate's superior electrochemical performance and stability compared with sodium diethylcarbamodithioate, emphasizing the efficacy of periphery aliphatic modification in enhancing electrode capacity, rate performance, and electrochemical stability for organosulfide materials within all-solid-state lithium organic batteries. We also explore the origin of periphery aliphatic modification in these enhancing electrochemical performances by kinetic analysis and thermodynamic analysis. Furthermore, employing density functional theory calculations and ex situ FTIR experiments elucidates the critical role of the N–C=S structure in the energy storage mechanism. This research advances organic cathode design within organosulfide materials, unlocking the potential of all-solid-state lithium organic batteries with enhanced cyclability, propelling the development of next-generation energy storage systems.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"26 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141934969","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}
In this study, a framework for predicting the gas-sensitive properties of gas-sensitive materials by combining machine learning and density functional theory (DFT) has been proposed. The framework rapidly predicts the gas response of materials by establishing relationships between multisource physical parameters and gas-sensitive properties. In order to prove its effectiveness, the perovskite Cs3Cu2I5 has been selected as the representative material. The physical parameters before and after the adsorption of various gases have been calculated using DFT, and then a machine learning model has been trained based on these parameters. Previous studies have shown that a single physical parameter alone is not enough to accurately predict the gas sensitivity of materials. Therefore, a variety of physical parameters have been selected for machine learning, and the final machine learning model achieved 92% accuracy in predicting gas sensitivity. It is important to note that although there have been no previous reports on the response of Cs3Cu2I5 to hydrogen sulfide, the resulting model predicts the gas response of H2S; it is subsequently confirmed experimentally. This method not only enhances the understanding of the gas sensing mechanism, but also has a universal nature, making it suitable for the development of various new gas-sensitive materials.
{"title":"Rapid Discovery of Gas Response in Materials Via Density Functional Theory and Machine Learning","authors":"Shasha Gao, Yongchao Cheng, Lu Chen, Sheng Huang","doi":"10.1002/eem2.12816","DOIUrl":"https://doi.org/10.1002/eem2.12816","url":null,"abstract":"In this study, a framework for predicting the gas-sensitive properties of gas-sensitive materials by combining machine learning and density functional theory (DFT) has been proposed. The framework rapidly predicts the gas response of materials by establishing relationships between multisource physical parameters and gas-sensitive properties. In order to prove its effectiveness, the perovskite Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> has been selected as the representative material. The physical parameters before and after the adsorption of various gases have been calculated using DFT, and then a machine learning model has been trained based on these parameters. Previous studies have shown that a single physical parameter alone is not enough to accurately predict the gas sensitivity of materials. Therefore, a variety of physical parameters have been selected for machine learning, and the final machine learning model achieved 92% accuracy in predicting gas sensitivity. It is important to note that although there have been no previous reports on the response of Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> to hydrogen sulfide, the resulting model predicts the gas response of H<sub>2</sub>S; it is subsequently confirmed experimentally. This method not only enhances the understanding of the gas sensing mechanism, but also has a universal nature, making it suitable for the development of various new gas-sensitive materials.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"193 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141934966","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}
Lijie Liu, Huajian Liu, Zifen Fan, Jie Liu, Xueying Wen, Huiyue Wang, Yan She, Guixin Hu, Ran Niu, Jiang Gong
The integrated technology of interfacial solar steam generation and photo-Fenton oxidation has emerged as a promising way to simultaneously mitigate freshwater scarcity and degrade organic pollutants. However, fabricating low-cost, multi-functional evaporators with high water evaporation and catalytic ability still presents a significant challenge. Herein, we report the functional upcycling of waste polyimide into semiconducting Fe-BTEC and subsequently construct Fe-BTEC-based composite evaporators for simultaneous freshwater production and photo-Fenton degradation of pollutants. Firstly, through a two-step solvothermal-solution stirring method, Fe-BTEC nanoparticles with the size of 20–100 nm are massively produced from waste polyimide, with a band gap energy of 2.2 eV. The composite evaporator based on Fe-BTEC and graphene possesses wide solar-spectrum absorption capacity, high photothermal conversion capacity, rapid delivery of water, and low enthalpy of evaporation. Benefiting from the merits above, the composite evaporator achieves a high evaporation rate of 2.72 kg m−2 h−1 from tetracycline solution, as well as the photothermal conversion efficiency of 97% when exposed to irradiation of 1 Sun, superior to many evaporators. What is more, the evaporator exhibits the tetracycline degradation rate of 99.6% with good recycling stability, ranking as one of the most powerful heterogeneous Fenton catalysts. COMSOL Multiphysics and density functional theory calculation results prove the synergistic effect of the concentrated heat produced by interfacial solar steam generation and catalytic active sites of Fe-BTEC on promoting H2O2 activation to form reactive oxidation radicals. This work not only provides a green strategy for upcycling waste polyimide, but also proposes a new approach to fabricate multi-functional evaporators.
{"title":"Simultaneous Solar-Driven Interfacial Evaporation and Photo-Fenton Oxidation by Semiconducting Metal–Organic Framework From Waste Polyimide","authors":"Lijie Liu, Huajian Liu, Zifen Fan, Jie Liu, Xueying Wen, Huiyue Wang, Yan She, Guixin Hu, Ran Niu, Jiang Gong","doi":"10.1002/eem2.12812","DOIUrl":"https://doi.org/10.1002/eem2.12812","url":null,"abstract":"The integrated technology of interfacial solar steam generation and photo-Fenton oxidation has emerged as a promising way to simultaneously mitigate freshwater scarcity and degrade organic pollutants. However, fabricating low-cost, multi-functional evaporators with high water evaporation and catalytic ability still presents a significant challenge. Herein, we report the functional upcycling of waste polyimide into semiconducting Fe-BTEC and subsequently construct Fe-BTEC-based composite evaporators for simultaneous freshwater production and photo-Fenton degradation of pollutants. Firstly, through a two-step solvothermal-solution stirring method, Fe-BTEC nanoparticles with the size of 20–100 nm are massively produced from waste polyimide, with a band gap energy of 2.2 eV. The composite evaporator based on Fe-BTEC and graphene possesses wide solar-spectrum absorption capacity, high photothermal conversion capacity, rapid delivery of water, and low enthalpy of evaporation. Benefiting from the merits above, the composite evaporator achieves a high evaporation rate of 2.72 kg m<sup>−2</sup> h<sup>−1</sup> from tetracycline solution, as well as the photothermal conversion efficiency of 97% when exposed to irradiation of 1 Sun, superior to many evaporators. What is more, the evaporator exhibits the tetracycline degradation rate of 99.6% with good recycling stability, ranking as one of the most powerful heterogeneous Fenton catalysts. COMSOL Multiphysics and density functional theory calculation results prove the synergistic effect of the concentrated heat produced by interfacial solar steam generation and catalytic active sites of Fe-BTEC on promoting H<sub>2</sub>O<sub>2</sub> activation to form reactive oxidation radicals. This work not only provides a green strategy for upcycling waste polyimide, but also proposes a new approach to fabricate multi-functional evaporators.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"57 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141884187","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}
A heteronuclear dual transition metal atom catalyst is a promising strategy to solve and relieve the increasing energy and environment crisis. However, the role of each atom still does not efficiently differentiate due to the high activity but low detectability of each transition metal in the synergistic catalytic process when considering the influence of heteronuclear induced atomic difference for each transition metal atom, thus seriously hindering intrinsic mechanism finding. Herein, we proposed coordinate environment vary induced heterogenization of homonuclear dual-transition metal, which inherits the advantage of heteronuclear transition metal atom catalyst but also controls the variable of the two atoms to explore the underlying mechanism. Based on this proposal, employing density functional theory study and machine learning, 23 kinds of homonuclear transition metals are doping in four asymmetric C3N for heterogenization to evaluate the underlying catalytic mechanism. Our results demonstrate that five catalysts exhibit excellent catalytic performance with a low limiting potential of −0.28 to −0.48 V. In the meantime, a new mechanism, “capture–charge distribution–recapture–charge redistribution”, is developed for both side-on and end-on configuration. More importantly, the pronate site of the first hydrogenation is identified based on this mechanism. Our work not only initially makes a deep understanding of the transition dual metal-based heteronuclear catalyst indirectly but also broadens the development of complicated homonuclear dual-atom catalysts in the future.
{"title":"Understanding the Intrinsic Mechanism of High-Performance Electrocatalytic Nitrogen Fixation by Heterogenization of Homonuclear Dual-Atom Catalysts","authors":"Yuefei Zhang, Yu Yang, Yu Zhang, Xuefei Liu, Wenjun Xiao, Degui Wang, Gang Wang, Zhen Wang, Jinshun Bi, Jincheng Liu, Xun Zhou, Wentao Wang","doi":"10.1002/eem2.12803","DOIUrl":"https://doi.org/10.1002/eem2.12803","url":null,"abstract":"A heteronuclear dual transition metal atom catalyst is a promising strategy to solve and relieve the increasing energy and environment crisis. However, the role of each atom still does not efficiently differentiate due to the high activity but low detectability of each transition metal in the synergistic catalytic process when considering the influence of heteronuclear induced atomic difference for each transition metal atom, thus seriously hindering intrinsic mechanism finding. Herein, we proposed coordinate environment vary induced heterogenization of homonuclear dual-transition metal, which inherits the advantage of heteronuclear transition metal atom catalyst but also controls the variable of the two atoms to explore the underlying mechanism. Based on this proposal, employing density functional theory study and machine learning, 23 kinds of homonuclear transition metals are doping in four asymmetric C<sub>3</sub>N for heterogenization to evaluate the underlying catalytic mechanism. Our results demonstrate that five catalysts exhibit excellent catalytic performance with a low limiting potential of −0.28 to −0.48 V. In the meantime, a new mechanism, “capture–charge distribution–recapture–charge redistribution”, is developed for both side-on and end-on configuration. More importantly, the pronate site of the first hydrogenation is identified based on this mechanism. Our work not only initially makes a deep understanding of the transition dual metal-based heteronuclear catalyst indirectly but also broadens the development of complicated homonuclear dual-atom catalysts in the future.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"54 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141884189","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 rapid development of nanotechnology has significantly revolutionized wearable electronics and expanded their functionality. Through introducing innovative solutions for energy harvesting and autonomous sensing, this research presents a cost-effective strategy to enhance the performance of triboelectric nanogenerators (TENGs). The TENG was fabricated from polyvinylidene fluoride (PVDF) and N, N′-poly(methyl methacrylate) (PMMA) blend with a porous structure via a novel optimized quenching method. The developed approach results in a high β-phase content (85.7%) PVDF/3wt.%PMMA porous blend, known for its superior piezoelectric properties. PVDF/3wt.%PMMA modified porous TENG demonstrates remarkable electrical output, with a dielectric constant of 40 and an open-circuit voltage of approximately 600 V. The porous matrix notably increases durability, enduring over 36 000 operational cycles without performance degradation. Moreover, practical applications were explored in this research, including powering LEDs and pacemakers with a maximum power output of 750 mW m−2. Also, TENG served as a self-powered tactile sensor for robotic applications in various temperature conditions. The work highlights the potential of the PVDF/PMMA porous blend to utilize the next-generation self-powered sensors and power small electronic devices.
纳米技术的飞速发展极大地革新了可穿戴电子设备并拓展了其功能。通过引入能量收集和自主传感的创新解决方案，本研究提出了一种具有成本效益的策略来提高三电纳米发电机（TENG）的性能。该 TENG 由具有多孔结构的聚偏氟乙烯（PVDF）和 N，N′-聚甲基丙烯酸甲酯（PMMA）混合物通过一种新颖的优化淬火方法制成。所开发的方法产生了一种高 β 相含量（85.7%）的 PVDF/3wt.%PMMA 多孔共混物，这种共混物因其卓越的压电特性而闻名。PVDF/3wt.%PMMA 改性多孔 TENG 具有出色的电气输出，介电常数为 40，开路电压约为 600 V。多孔基质显著提高了耐久性，可经受 36 000 次以上的工作循环而不会出现性能下降。此外，这项研究还探索了实际应用，包括为 LED 和心脏起搏器供电，最大输出功率为 750 mW m-2。此外，TENG 还可作为自供电触觉传感器，用于各种温度条件下的机器人应用。这项工作突出了 PVDF/PMMA 多孔混合物在利用下一代自供电传感器和为小型电子设备供电方面的潜力。
{"title":"Quenched PVDF/PMMA Porous Matrix for Triboelectric Energy Harvesting and Sensing","authors":"Assem Mubarak, Bayandy Sarsembayev, Yerzhigit Serik, Abdirakhman Onabek, Zhanat Kappassov, Zhumabay Bakenov, Kazuyoshi Tsuchiya, Gulnur Kalimuldina","doi":"10.1002/eem2.12808","DOIUrl":"https://doi.org/10.1002/eem2.12808","url":null,"abstract":"The rapid development of nanotechnology has significantly revolutionized wearable electronics and expanded their functionality. Through introducing innovative solutions for energy harvesting and autonomous sensing, this research presents a cost-effective strategy to enhance the performance of triboelectric nanogenerators (TENGs). The TENG was fabricated from polyvinylidene fluoride (PVDF) and <i>N</i>, <i>N′</i>-poly(methyl methacrylate) (PMMA) blend with a porous structure via a novel optimized quenching method. The developed approach results in a high <i>β</i>-phase content (85.7%) PVDF/3wt.%PMMA porous blend, known for its superior piezoelectric properties. PVDF/3wt.%PMMA modified porous TENG demonstrates remarkable electrical output, with a dielectric constant of 40 and an open-circuit voltage of approximately 600 V. The porous matrix notably increases durability, enduring over 36 000 operational cycles without performance degradation. Moreover, practical applications were explored in this research, including powering LEDs and pacemakers with a maximum power output of 750 mW m<sup>−2</sup>. Also, TENG served as a self-powered tactile sensor for robotic applications in various temperature conditions. The work highlights the potential of the PVDF/PMMA porous blend to utilize the next-generation self-powered sensors and power small electronic devices.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"184 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141884270","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}
Huiyan Zeng, Zhongfei Liu, Jun Qi, Jiajun Chen, Yanquan Zeng, Chengyan Yang, Zhenzhong Li, Chao Wang, Long Gu, Yan Zhang, Miao Shu, Chunzhen Yang
A comprehensive understanding of the dynamic processes at the catalyst/electrolyte interfaces is crucial for the development of advanced electrocatalysts for the oxygen evolution reaction (OER). However, the chemical processes related to surface corrosion and catalyst degradation have not been well understood so far. In this study, we employ LiCoO2 as a model catalyst and observe distinct OER activities and surface stabilities in different alkaline solutions. Operando X-ray diffraction (XRD) and online mass spectroscopy (OMS) measurements prove the selective intercalation of alkali cations into the layered structure of LiCoO2 during OER. It is proposed that the dynamic cation intercalations facilitate the chemical oxidation process between highly oxidative Co species and adsorbed water molecules, triggering the so-called electrochemical-chemical reaction mechanism (EC-mechanism). The results of this study emphasize the influence of cations on OER and provide insights into new strategies for achieving both high activity and stability in high-performance OER catalysts.
全面了解催化剂/电解质界面的动态过程对于开发先进的氧进化反应（OER）电催化剂至关重要。然而，迄今为止，与表面腐蚀和催化剂降解相关的化学过程还没有得到很好的理解。在本研究中，我们以 LiCoO2 为模型催化剂，观察其在不同碱性溶液中不同的 OER 活性和表面稳定性。操作性 X 射线衍射 (XRD) 和在线质谱 (OMS) 测量证明，在 OER 过程中，碱阳离子选择性地插层到 LiCoO2 的层状结构中。研究认为，动态阳离子插层促进了高氧化性 Co 物种与吸附水分子之间的化学氧化过程，引发了所谓的电化学-化学反应机制（EC-机制）。该研究结果强调了阳离子对 OER 的影响，并为实现高性能 OER 催化剂的高活性和稳定性的新策略提供了启示。
{"title":"Dynamic Cation Intercalation Facilitating Chemical Oxidation of Water and Surface Stabilization During the Oxygen Evolution Reaction","authors":"Huiyan Zeng, Zhongfei Liu, Jun Qi, Jiajun Chen, Yanquan Zeng, Chengyan Yang, Zhenzhong Li, Chao Wang, Long Gu, Yan Zhang, Miao Shu, Chunzhen Yang","doi":"10.1002/eem2.12813","DOIUrl":"https://doi.org/10.1002/eem2.12813","url":null,"abstract":"A comprehensive understanding of the dynamic processes at the catalyst/electrolyte interfaces is crucial for the development of advanced electrocatalysts for the oxygen evolution reaction (OER). However, the chemical processes related to surface corrosion and catalyst degradation have not been well understood so far. In this study, we employ LiCoO<sub>2</sub> as a model catalyst and observe distinct OER activities and surface stabilities in different alkaline solutions. <i>Operando</i> X-ray diffraction (XRD) and online mass spectroscopy (OMS) measurements prove the selective intercalation of alkali cations into the layered structure of LiCoO<sub>2</sub> during OER. It is proposed that the dynamic cation intercalations facilitate the chemical oxidation process between highly oxidative Co species and adsorbed water molecules, triggering the so-called electrochemical-chemical reaction mechanism (EC-mechanism). The results of this study emphasize the influence of cations on OER and provide insights into new strategies for achieving both high activity and stability in high-performance OER catalysts.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"75 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141887313","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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