ACS Applied Energy Materials最新文献

{"title":"Flexible Thermoelectric Energy Harvester with Stacked Structure of Thermoelectric Composite Films Made of PVDF and Bi2Te3-Based Particles","authors":"Da Eun Shin, Nagamalleswara Rao Alluri, Kwi-Il Park","doi":"10.1021/acsaem.4c01772","DOIUrl":"https://doi.org/10.1021/acsaem.4c01772","url":null,"abstract":"Flexible thermoelectric energy harvesters (f-TEHs) enable wearable sensors or electronic devices to be attached on curved objects with a thermal source. We demonstrated a stacked-structured f-TEH that generates thermal energy without increasing its cross-sectional area. The device consists of thermoelectric composite films fabricated by p- and n-type Bi₂Te₃ and poly(vinylidene fluoride), Al foil and polyethylene terephthalate film. The output performance improved as the number of thermoelectric film layers (L) increased, and the L = 8 f-TEH generated maximum voltage, current, and power. Multiphysics simulations and bending tests were adopted for further investigation. This study demonstrates a distinctive configuration and comprehension of its energy generation mechanism.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264300","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mechanical and Thermoelectric Properties of Na-Intercalated SnSe2 Crystals","authors":"Zhiping Liu, Tingting Deng, Pengfei Qiu, Wenwen Zheng, Zhi Li, Zhengyang Zhou, Xun Shi","doi":"10.1021/acsaem.4c01928","DOIUrl":"https://doi.org/10.1021/acsaem.4c01928","url":null,"abstract":"Recently, two-dimensional (2D) van der Waals (vdW) SnSe₂-based crystals have attracted great attention due to their metal-like plasticity and good thermoelectric (TE) performance at room temperature. The halogen elements have been successfully doped at Se sites in SnSe₂ crystals to greatly improve the TE properties while maintaining good plasticity. As a typical layered material, the space among the vdW layers in SnSe₂ is quite large and can be intercalated by guest elements to tune various physical properties. In this work, we successfully prepared a series of Na-intercalated SnSe₂ crystals by using the temperature gradient method. The effects of intercalating Na into the vdW gaps on the crystal structure and mechanical and TE properties are systematically investigated. Intercalating Na in SnSe₂ has little influence on the crystal structure and band gap. The electrical conductivity is enhanced by Na-intercalation, but the doping efficiency is lower than those of Br and Cl. A maximum power factor (PF) of 5.6 μW cm^–1 K^–2 is obtained for Na_0.02SnSe₂ at 300 K, comparable with most Ag₂S- and AgCuSe-based plastic inorganic TE materials. The plasticity of SnSe₂ is well maintained when the Na-intercalating content is below 0.05. This work provides more understanding of SnSe₂-based plastic TE materials.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264188","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Cobalt-Atom Active Sites Grafted UiO-66-NH2 via EDTA for the Enhanced Production of Syngas in CO2 Photoreduction","authors":"Toan-Anh Quach, Minh-Khoa Duong, Sakar Mohan, Trong-On Do","doi":"10.1021/acsaem.4c01729","DOIUrl":"https://doi.org/10.1021/acsaem.4c01729","url":null,"abstract":"In recent years, the use of photocatalysts has emerged as a promising research direction to transform harmful CO₂ molecules into renewable fuels. In this work, the chelating agent ethylenediaminetetraacetic acid (EDTA) containing a central metal atom like Co was attached to the UiO-66-NH₂ metal–organic frameworks (MOFs) through a one-pot synthesis. Several samples with different molar ratios of UiO-66-NH₂–Co and EDTA (molar ratios of UiO-66-NH₂–Co/EDTA is 1.2; 0.6; and 0.4) were synthesized and assessed for photocatalytic CO₂ reduction to produce syngas (the mixture of CO and H₂), which can be used for generating liquid fuels. Among these samples, the highest syngas production rate was achieved by sample U-E-0.6, yielding around 776.40 and 1217.29 μmol g^–1 h^–1 of CO and H₂, respectively, at the end of 4 h. Multiple investigations, including electrochemical impedance, time-resolved, steady state photoluminescence, linear sweep voltammetry, and photocurrent measurements, revealed that the addition of EDTA-metal to UiO-66-NH₂ improved the photoelectrochemical properties of the system, thereby enhancing its photocatalytic activity under solar irradiation. This research paves the way for the development of a single atom encapsulated in the MOF material for photocatalytic CO₂ reduction.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264181","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-Density Arrangement of Nanoscale Regions with Tellurium Interstitial Atoms and Silver/Copper Vacancies in AgCuTe Thermoelectric Materials","authors":"Bin Xiao, He Yang, Jianbo Li, Jun Wang","doi":"10.1021/acsaem.4c01701","DOIUrl":"https://doi.org/10.1021/acsaem.4c01701","url":null,"abstract":"The rigid crystalline sublattice of Te ions in AgCuTe provides an effective electrical transport channel, enabling AgCuTe to exhibit good electrical properties. However, the appearance of vacancies or interstitial atoms within the Te^2– rigid anionic framework poses significant challenges both theoretically and experimentally. Here, we are the first to discover the existence of localized Te_i, V_Cu, and V_Ag multiple defects in the AgCuTe phase, as well as a highly ordered arrangement of V_Cu in the Cu₂Te phase of AgCuTe_1–<i>z</i> samples, by only fine-tuning the Te stoichiometric ratio. The formation of these localized defects arises from the excess precipitation of Ag and Cu during the process, which enhances phonon scattering and reduces thermal conductivity. Simultaneously, the total cation content in AgCuTe_1–<i>z</i> samples increases relative to the anion, thereby optimizing total intrinsic vacancies and carrier concentration. As a result, there is a 311% increase in the power factor and a 44% decrease in the lattice thermal conductivity at room temperature, leading to a 54% net increase in <i>ZT</i> compared to that of pristine AgCuTe. This approach is expected to be a universal modification strategy for enhancing the thermoelectric properties of other Te-based anionic framework superionic conductor materials.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264185","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Specific Capacitance Enhancement of Metal–Organic Framework (MOF) by Boosting Intramolecular Charge Transfer Mechanism","authors":"Ramkumar Vanaraj, Bharathi Arumugam, Gopiraman Mayakrishnan, Rajakumar Kanthapazham, Seong-Cheol Kim","doi":"10.1021/acsaem.4c01241","DOIUrl":"https://doi.org/10.1021/acsaem.4c01241","url":null,"abstract":"Energy storage is very important for the forthcoming future; hence, the overview of innovative materials in this research area is necessary. Here, two metal–organic framework (MOF) materials are described thoroughly, which is highly required because few MOFs are available only on high-performance supercapacitors. The melamine-, manganese-, and molybdenum-based MOF materials, such as Me-Mn-MOFs and Me-Mo-MOFs, were prepared and applied for supercapacitor applications. The MOF materials are validated and characterized using conventional characterization procedures. The physicochemical properties of the materials were analyzed through sophisticated instrumental analysis. The surface morphological results reveal that the melamine and manganese-based MOFs (Me-Mn-MOFs) display a cubic-like structure, whereas the melamine and molybdenum-based MOFs (Me-Mo-MOFs) portray rod-like structures. The P-XRD, XPS, and BET results confirm the formation of the MOF materials from the starting materials. The electrochemical analysis reveals that the prepared materials could be a potential material for high-performance supercapacitor applications. The specific capacitances of Me-Mn-MOFs and Me-Mo-MOFs are 653.54 and 312.63 F/g. The asymmetric devices demonstrate that the power densities of Me-Mn-MOFs and Me-Mo-MOFs are 3048.7 and 2376.6 W/kg. The suggested materials could provide an original viewpoint on MOFs for use in high-performance supercapacitor applications.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264187","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Impact of TiO2 at the Grain Boundaries in Lithium Lanthanum Titanate Solid Electrolytes","authors":"Jose Carlos Madrid Madrid, Antranik Jonderian, Eric McCalla, Kulbir Kaur Ghuman","doi":"10.1021/acsaem.4c00883","DOIUrl":"https://doi.org/10.1021/acsaem.4c00883","url":null,"abstract":"The enhancement of Li-ion conductivity within the perovskite Li–La–Ti-O samples (LLTO) by the addition of TiO₂ remains unexplained in the literature. Herein, microscopy shows that TiO₂ appears at the grain boundaries (GB) of the perovskite, prompting a comprehensive molecular dynamics investigation. In this work, we analyzed symmetric and mixed LLTO GBs, as well as LLTO/TiO₂ interfaces, to understand the impact of the secondary phase on Li-ion conductivity compared to other factors, such as disorder or strain present in the samples due to the GBs. The rigid-ion Buckingham-type potential combined with a long-range Coulombic term was used to accurately model ionic interactions. The investigation of diffusion mechanisms through mean squared displacement (MSD) analysis unveiled that disordered TiO₂ phases significantly enhance Li-ion mobility compared with more orderly Sigma 5 or mixed GBs. This suggests that the disorder may create additional pathways for ion diffusion not present in symmetric GBs or crystalline LLTO samples. Furthermore, the enhanced Li-ion diffusion through LLTO/TiO₂ interfaces was indeed observed in the calculations and is attributed to the presence of TiO₂ phases and, to a lesser extent, to the highly disordered interface formed between them. These insights into the intricate migration mechanisms of Li ions through the exceptionally complex microstructures present in LLTO could advance the development of efficient solid-state electrolytes for Li-ion battery applications.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264297","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hydrogen Storage in Mg–Ni-Type Alloys with La and Sm Incorporation","authors":"Yiwan Chen, Hui Yong, Shuai Wang, Xiuzhi Zhang, Wei Zhang, Kai Feng, Jifan Hu, Yanghuan Zhang","doi":"10.1021/acsaem.4c01850","DOIUrl":"https://doi.org/10.1021/acsaem.4c01850","url":null,"abstract":"The addition of rare earth elements lanthanum and samarium to Mg–Ni-type alloys enhanced the hydrogen absorption and desorption kinetics. The microstructures of these alloys were characterized by using XRD, SEM, TEM, HTREM, and SAED methods. PCT equipment was employed to test the hydrogen storage performance. It was observed that Mg₉₆NiLa₃ alloys exhibited a more uniform and refined phase distribution, credited to the grain refinement effect triggered by Mg₁₇La₂. Additionally, the Mg₉₆NiLa₃ alloy demonstrated a significant hydrogen storage capacity, with hydrogen release reaching 6.2 wt % at 593 K, compared to 5.4 wt % for the Mg₉₆NiSm₃ alloy at the same temperature. The activation energies of dehydrogenation for Mg₉₆NiLa₃ and Mg₉₆NiSm₃ were 99.69 and 97.53 kJ/mol, respectively, with no significant difference considering errors. Similarly, the enthalpies of dehydrogenation were 72.9 kJ/mol of H₂ for Mg₉₆NiLa₃ and 78 kJ/mol of H₂ for Mg₉₆NiSm₃, indicating no notable distinction in the thermodynamic properties of the two alloys. Thus, the enhancement of the thermodynamic properties of Mg–Ni-type alloys by rare earth elements La and Sm appears to be insignificant.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264299","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tetraalkyl/Alkyltriphenylphosphonium Hexatungstates for Efficient Electrocatalytic Hydrogen Evolution Reaction in Alkaline Media: An Experimental and In Silico-Based Synchronization Approach","authors":"Debojyoti Kundu, Gajiram Murmu, Sanjukta Zamindar, Naresh Chandra Murmu, Priyabrata Banerjee, Sumit Saha","doi":"10.1021/acsaem.4c01315","DOIUrl":"https://doi.org/10.1021/acsaem.4c01315","url":null,"abstract":"The development of stable, cost-effective, noble metal-free, and highly efficient electrocatalysts embraces great potential for efficient hydrogen production through water electrolysis. Herein, tetraalkyl/alkyltriphenylphosphonium hexatungstate-based Lindqvist polyoxometalates named <b>HTC-1</b> and <b>HTC-2</b>, respectively, have been synthesized and characterized as promising electrocatalysts for effectual water-splitting reactions. The inclusion of tetrabutyl- and allyltriphenylphosphonium bromides as precursors into hexatungstate ions (W₆O₁₉^2–) exhibited a synergistic effect that promoted a notable improvement in the hydrogen evolution reaction (HER) performance. It also imposes extra surface-active sites and facilitates the electronic transition to boost HER activity in alkaline medium with a lower overpotential value of 136 and 185 mV at benchmark current density and a Tafel slope of 88 and 121 mV dec^–1, respectively. Density functional theory (DFT) calculations also corroborated the experimental finding that <b>HTC-1</b> acts as a more efficient electrocatalyst due to the presence of a more electron-rich center than <b>HTC-2</b>. The experimental results are further unequivocally corroborated by the <i>in silico</i> approaches, which include density functional theory, reactive site analysis, electronic property analysis, and Gibbs free energy analysis. These results conclusively demonstrate that <b>HTC-1</b> exhibits a lower energy barrier in promoting the adsorption of HER intermediates, particularly, hydrogen adsorption. These observations represent an auspicious “proof of concept” for developing more efficient hexatungstate-based electrocatalysts in the future.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264190","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Fluorobenzene-Diluted Localized Highly Concentrated Electrolyte for Enhanced Electrochemical Performance of Li–O2 Battery","authors":"Syed Shoaib Hassan Zaidi, Justin T. Douglas, Xianglin Li","doi":"10.1021/acsaem.4c01566","DOIUrl":"https://doi.org/10.1021/acsaem.4c01566","url":null,"abstract":"Highly concentrated electrolytes (HCEs), owing to their high thermal and chemical stability, wider electrochemical stability windows (ESWs), and enhanced stability with Li metal anode, have been under the spotlight as a potential electrolyte candidate for developing Li–O₂ batteries. Nonetheless, their high viscosity, poor wettability, and high cost pose great challenges in achieving the desired results. In this study, we designed an HCE diluted with a low-polarity hydrocarbon cosolvent, fluorobenzene, and investigated its electrochemical performance in a Li–O₂ battery. Raman spectroscopy analysis and self-diffusivity coefficients of electrolyte components determined by nuclear magnetic resonance (NMR) technique have confirmed that the fluorobenzene-based localized highly concentrated electrolyte (FB-LHCE) conserved the unique solvation structure of contact ion pairs and cation–anion aggregates formed in HCE. Incorporating fluorobenzene into HCE improved the self-diffusivity of electrolyte components by over a magnitude, lowered the viscosity by over 40 times, and increased the ionic conductivity 5-fold. Furthermore, FB-LHCE drastically improved the electrode wettability by yielding 3 and 5 orders of magnitude higher double-layer capacitances than those of low-concentration (LCE) and HCE, respectively. Additionally, when compared with LCE as the baseline, HCE and FB-LHCE have demonstrated wider anodic ESWs (&gt;4.6 V). Li||Li symmetric cell tests revealed significantly improved electrochemical stability of HCE and FB-LHCE with Li metal anode compared to LCE. HCE and FB-LHCE have yielded stable cycling for double the amount of time (1300 h) compared with LCE (650 h). FB-LHCE delivered the highest specific discharge capacity (6.0 Ah g^–1) followed by LCE (2.25 Ah g^–1) and HCE (1.07 Ah g^–1) in Li–O₂ cells. Full-cell cycling stability tests have shown enhanced cycling stability with FB-LHCE (11 cycles) compared with those with LCE (2 cycles) and HCE (2 cycles).","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264191","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Sr0.7R0.3CoO3-δ (R = Gd, Eu, and Sm) Perovskites Infiltrated with Pd: Enhancing the Performance as Cathode Materials in Solid Oxide Fuel Cells","authors":"Mónica Chivite Lacaba, Alberto García Fernandes, Jesús Prado-Gonjal, José Antonio Alonso, Vanessa Cascos","doi":"10.1021/acsaem.4c01683","DOIUrl":"https://doi.org/10.1021/acsaem.4c01683","url":null,"abstract":"Perovskites based on Sr_0.7R_0.3CoO_3-δ (R = Gd, Eu, and Sm) were prepared to be used as cathodes in solid oxide fuel cells (SOFC). The materials were synthesized using the citrate-nitrate route and thermal treatments in air atmosphere. The identification of the phases was performed using high-resolution synchrotron X-ray powder diffraction (SXRD) at room temperature to determine the features of the crystalline structure and to identify oxygen vacancies in the materials. SXRD data revealed a significant presence of long-range ordered oxygen vacancies concentrated at the O2 and O4 oxygen positions, exhibiting large displacement factors, defined in a tetragonal perovskite-type superstructures with <i>I</i>4<i>/mmm</i> space group. Subsequently, thermal properties were analyzed to determine the thermal expansion coefficients and their compatibility with the other components of the cell. Additionally, thermal analysis allowed us to identify a reduction in the oxygen content as the temperature increases. A single-cell test conducted in electrolyte-supported configuration at 800 and 850 °C with values surpassing 750 mW/cm² demonstrated the successful utilization of these perovskites as cathode materials in SOFCs. Furthermore, the materials were further optimized by improving the performance of the cells with an additional process: infiltration with a Pd(NO₃)₂ solution.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264298","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}