材料科学最新文献

{"title":"Engineering semiconductor quantum dots for co-upcycling of CO2 and biomass-derived alcohol","authors":"Lin-Xing Zhang, Zi-Rong Tang, Ming-Yu Qi, Yi-Jun Xu","doi":"10.1039/d4ta01996b","DOIUrl":"https://doi.org/10.1039/d4ta01996b","url":null,"abstract":"Utilizing semiconductor quantum dots (QDs) to construct a bifunctional reaction system of coupling CO<small>₂</small> reduction with biomass valorization represents an appealing approach for the production of usable fuels and value-added chemicals. Herein, we present an efficient cooperative photocatalytic process for simultaneously achieving the reduction of CO<small>₂</small> to syngas and the oxidation of biomass-derived furfuryl alcohol to furfural and hydrofuroin over SiO<small>₂</small>-supported CdSe/CdS QDs (CdSe/CdS-SiO<small>₂</small>). The type-II band alignment in CdSe/CdS core/shell heterostructures enables effective charge separation and interfacial charge migration concurrently. By further assembly onto spherical SiO<small>₂</small> support, the optimized CdSe/CdS-SiO<small>₂</small> composite exhibits remarkably enhanced activities for syngas and furfural/hydrofuroin production, which are 2.3 and 3.5 times higher than those of binary CdSe/CdS core/shell QDs, and 90.4 and 18.5 times higher than those of bare CdSe QDs, along with good stability. In particular, by altering the thickness of CdS shell, the syngas CO/H<small>₂</small> ratio can be precisely modulated within a wide range (1.6 to 7.1), which serves as a crucial feedstock for the production of liquid fuels. This work is expected to develop core/shell QDs-based photocatalysts for versatile and available photoredox-catalyzed reaction systems that integrate CO<small>₂</small> valorization with biomass upgrading.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462386","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}

{"title":"Ultrahigh energy storage capacities in high-entropy relaxor ferroelectrics","authors":"Yunyao Huang, Kaili Shang, Yule Yang, Wenjing Shi, Leiyang Zhang, Vladimir Laletin, Vladimir Shur, Ruiyi Jing, Li Jin","doi":"10.1039/d4ta03637a","DOIUrl":"https://doi.org/10.1039/d4ta03637a","url":null,"abstract":"Realizing ultrahigh recoverable energy-storage density (<em>W</em><small>_rec</small>) alongside giant efficiency (<em>η</em>) remains a significant challenge for the advancement of dielectrics in next-generation pulse power energy-storage (ES) devices. In this study, we introduce an entropy engineering approach, manipulating local polar fluctuations and tailoring microstructure evolution through a high-entropy design strategy, to effectively regulate the ES performance of lead-free (Bi<small>_0.5</small>Na<small>_0.5</small>)TiO<small>₃</small> (BNT)-based dielectrics. By intricately designing a high-entropy matrix, (Bi<small>_0.375</small>Na<small>_0.3</small>Sr<small>_0.25</small>K<small>_0.075</small>)TiO<small>₃</small> (BNSKT), and enhancing configurational entropy with the Bi(Mg<small>_0.5</small>Sn<small>_0.5</small>)O<small>₃</small> (BMS) end member, we developed multi-cation substituted BNT relaxor ceramics based on a viscous polymer process (VPP) method. Our findings reveal that modulating atomic configurational entropy yields favorable and stable microstructural characteristics, contributing to an improved breakdown electric field (<em>E</em>-field), reduced hysteresis and delayed polarization saturation. The VPP-synthesized high-entropy 0.85BNSKT-0.15BMS (BNT-H15<small>_VPP</small>) ceramics achieved a significant ES density <em>W</em><small>_rec</small> of 11.24 J cm<small>⁻³</small>, <em>η</em> of 88.3%, and responsivity (<em>ξ</em>, defined as <em>W</em><small>_rec</small>/<em>E</em>) of 184 J kV<small>⁻¹</small> cm<small>⁻²</small> under 610 kV cm<small>⁻¹</small>. Additionally, pulse charging/discharging measurements indicated a large discharge energy density (<em>W</em><small>_dis</small>) of 6.6 J cm<small>⁻³</small>, a short discharge time of 2.2 μs, and remarkable temperature stability over 20–120 °C. This work underscores the feasibility of the high-entropy strategy for designing robust dielectric ceramics, heralding promising advancements in advanced ES capacitors with comprehensive ES performance.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462395","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}

{"title":"Size effect of nickel from nanoparticles to clusters to single atoms for electrochemical CO2 reduction","authors":"Qin Pan, Yang Chen, Hui Li, Guanghuan Ma, Shuoshuo Jiang, Xin Cui, Lei Zhang, Yuxin Bao, Tianyi Ma","doi":"10.1039/d4ta03404j","DOIUrl":"https://doi.org/10.1039/d4ta03404j","url":null,"abstract":"Electrochemical CO2 reduction to value-added chemicals is a promising solution for alleviating environmental issues. Nickel-nitrogen-carbon catalysts have been considered as a potential candidate for CO2 reduction. However, the size effect of Ni-based catalysts in the electrochemical CO2 reduction reaction (CO2RR) remains elusive. Here, we precisely controlled the size of nitrogen-doped-carbon anchored Ni from nanoparticles to clusters to single atoms and systematically investigated the size effect of Ni on the CO2 electroreduction performance for the first time. The Faradaic efficiency of CO varies from 59% over Ni nanoparticles to 85% over single atoms at -0.8 V vs. RHE, along with an excellent turnover frequency for CO production (3554.5 h-1) and a current density of 12 mA cm-2, surpassing most other state-of-the-art catalysts. The formation of H* for competitive hydrogen evolution reaction is facile on Ni nanoparticles and clusters, which enable syngas production with a wide range of CO/H2 ratios (1.1-6.3). The characterization results reveal that the electronic state of Ni species can be tuned by varying the particle sizes. The unique electronic nature of single-atom Ni optimizes the adsorption of CO2 and the formation of *COOH intermediates, thus promoting CO2 electroreduction. This work elucidates the importance of the particle sizes on the electrochemical CO2 reduction performance.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462443","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}

{"title":"Constructing sodiophilic interconnected ion-transport channels towards stable Na-metal anode","authors":"Yi Ding, Min Guo, Yawei Zhang, Song Lu, Jiadi Ying, Yeqing Wang, Tiancun Liu, Zhixin Yu","doi":"10.1039/d4ta03489a","DOIUrl":"https://doi.org/10.1039/d4ta03489a","url":null,"abstract":"Electrochemical cells utilizing metals (e.g., Li, Na, K) as anodes have sparked significant interest in both academia and industry. However, the rapid growth of sodium dendrite and irregular deformation are limiting the usage of sodium metal anode. Fast ion transport is crucial for metal deposition and stripping. Herein, we fabricated a hybrid metal anode by physically mixing superionic conductor Na3V2(PO4)3 particles with sodium metal using a facile and scalable rolling and folding method. The superionic conductor particles with high affinity for Na+ are beneficial for charged Na-ion channels formation. These channels serve as reservoirs to continuously release and deliver sodium ions, compensating for the ionic flux of electrolyte. Moreover, the percolated Na+-conducting channels also reduce the diffusion barrier and accelerate Na+ migration, thereby homogenizing the local Na-ion flux and steering uniform Na deposition. These characteristics collectively contribute to dendrite-free Na electrodeposition and long cycle life (over 1000 h for 2 mAh cm-2 at 0.5 mA cm-2) in symmetric cells. Remarkably, when paired with Na3V2(PO4)3 cathodes, the full cell delivers high capacity retention (87.8% after 1000 cycles at a current density of 5C) and excellent rate performance (57.3 mAh g-1 at 50C).","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462489","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}

{"title":"Stabilizing LAGP/Li interface and in-situ visualizing the interfacial structure evolution for high-performance solid-state lithium metal batteries","authors":"Jin Li, Junjie Chen, Xiaosa Xu, Jing Sun, Baoling Huang, Tianshou Zhao","doi":"10.1039/d4ee02075h","DOIUrl":"https://doi.org/10.1039/d4ee02075h","url":null,"abstract":"LAGP/Li interface, Lithium metal batteries, In-situ visualizing, Structure evolution, Multilayer structure electrolyte","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":null,"pages":null},"PeriodicalIF":32.5,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462505","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}

{"title":"Thermally stable inorganic Bi0.4Sb1.6Te3/metal-organic frameworks (MOFs) composites with 1-by-1 nm pore engineering towards mid-temperature thermoelectrics","authors":"Wanjia Zhang, Bassem Maythalony, Fengxian Gao, Fanshi Wu, Wei Zhao, Pengfei Xu, Wenhua Zhang, Cailing Chen, Zhan Shi, Xiyang Wang, Yue Lou, Biao Xu","doi":"10.1039/d4ee01652a","DOIUrl":"https://doi.org/10.1039/d4ee01652a","url":null,"abstract":"Metal-organic frameworks (MOFs) exhibit substantial promise in the field of thermoelectrics, thanks to their adjustable porosity and modifiable physical/chemical characteristics. The widespread application of MOFs in thermoelectricity has been hampered by their low conductivity and limited thermal stability. In this work, a uniform dispersion of MOFs within the Bi0.4Sb1.6Te3 matrix is realized. This results in dual benefits: the assurance of microstructural stability of MOFs within the composites and a significant enhancement in electrical transport of Bi0.4Sb1.6Te3 induced by the organic-inorganic interfacial electron transfer and energy filtration effect. Meanwhile, the 1-by-1-nm-tuned-pore and intricate hierarchical architecture of MOFs play a crucial role in diminishing thermal conductivity of Bi0.4Sb1.6Te3. Consequently, the notable thermoelectric performance of the Bi0.4Sb1.6Te3/0.5 wt% ZIF-8 nanocomposite is achieved, including a peak zT of 1.65, a remarkable maximum cooling ΔT of 71.6 K at Th = 300 K, and a record-high thermoelectric conversion efficiency of 6.7% at ΔT = 238 K. This study utilizes the unique structural features of MOFs, broadening their applications into the mid-temperature range within the field of thermoelectrics.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":null,"pages":null},"PeriodicalIF":32.5,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462545","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}

{"title":"Theoretical probing monolayer BiI3 as electrolyte separator and 3d-TM doped BiI3 as electrocatalysts toward high performance Lithium-Sulfur batteries","authors":"Wentao Wu, Kaixin Zou, Li Wang, Boyan Li, Yang Wen, Chunlai Gao, Feng Lu, Weichao Wang, Weihua Wang","doi":"10.1039/d4ta02572e","DOIUrl":"https://doi.org/10.1039/d4ta02572e","url":null,"abstract":"Lithium-sulfur (Li-S) batteries are regarded as one kind of promising energy storage systems, but the present challenge is to achieve the desired energy density through resolving shuttle effect and sluggish electrochemical process. In this work, the pristine two-dimensional (2D) BiI<small>₃</small> with intrinsic atomic pore structures and its corresponding 3<em>d</em> transition metal (TM) doped systems have been proposed and examined to solve the above issues based on first principles calculations. Due to the uniquely atomic pores, 2D BiI<small>₃</small> monolayer can be served as an electrolyte separator to block dissolved lithium polysulfides (LiPSs) while ensuring an ultra-fast transport of Li ions. More significantly, the 3<em>d</em>-TM (TM=Ti, V) doped BiI<small>₃</small> systems extremely lower overpotentials to 0.16-0.17 V for sulfur reduction reaction and decrease energy barriers to 0.29-0.44 eV for decomposing insoluble Li<small>₂</small>S, indicating the promotion of electrochemical process of LiPSs conversion by 3<em>d</em>-TM doping. Electronic structure analysis shows that the charge redistribution on monolayer TM/BiI<small>₃</small> triggered by the hybridization of I-5<em>p</em> and TM-3<em>d</em> states is crucial to improve the adsorption and conversion of LiPSs for TM/BiI<small>₃</small> through stronger Li-I bonds. These findings provide the key electrolyte separator and electrocatalyst potentially and open up the possibility of multifunctional materials with similar structures to apply in high-performance Li-S batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462452","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}

{"title":"Chiral supramolecular polymer functionalized two-dimensional transition metal-based catalyst for enhancing the electrochemical water splitting via. spin-polarized charge transfer","authors":"Utkarsh Utkarsh, Sai Rachana Pramatha, Anujit Balo, Utpal Kumar Gosh, Venkata Rao Kotagiri, Koyel Banerjee Ghosh","doi":"10.1039/d4ta02665a","DOIUrl":"https://doi.org/10.1039/d4ta02665a","url":null,"abstract":"Water-splitting is one of the potential avenues to store electricity produced from renewable energy sources in the form of fuel, though the oxygen evolution reaction (OER) limits its extensive application as it requires a high overpotential. The rationale behind designing efficient catalysts is mainly governed by the electronic and crystal structure of the catalyst. However, optimization of the spin-polarized charge transfer during electrolysis reveals the improvement of catalytic activity for the OER process by enhancing the faradaic efficiency and reducing the overpotential. Here, we report enhancing the electrocatalytic efficiency of the state-of-the-art Ni, Fe-based OER catalyst by controlling the spin-polarization during electrolysis. This spin-polarization is introduced using the chiral-induced spin selectivity (CISS) effect by integrating the catalyst with the perylene diimides (PDI)-based chiral supramolecular polymers. The improvement in OER exhibits a decrease in reaction overpotential and minimizes the byproduct production compared to the only catalyst and its analogous achiral modification. Therefore, this study represents a viable strategy for improving the catalytic activity of the top-performing catalysts employing chirality to introduce spin-alignment into the anode.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462457","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}

{"title":"Outstanding Reviewers for Journal of Materials Chemistry A in 2023","authors":"","doi":"10.1039/d4ta90114b","DOIUrl":"https://doi.org/10.1039/d4ta90114b","url":null,"abstract":"We would like to take this opportunity to thank all of <em>Journal of Material Chemistry A</em>’s reviewers for helping to preserve quality and integrity in chemical science literature. As part of this we would like to highlight and thank our Outstanding Reviewers for <em>Journal of Materials Chemistry A</em> in 2023.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462520","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}

{"title":"Precise Control of Process Parameters for >23% Efficiency Perovskite Solar Cells in Ambient Air Using an Automated Device Acceleration Platform","authors":"Jiyun Zhang, Jianchang Wu, Anastasia Barabash, Tian Du, Shudi Qiu, Vincent Marc Le Corre, Yicheng Zhao, Kaicheng Zhang, Frederik Schmitt, Zijian Peng, Jingjing Tian, Chaohui Li, Chao Liu, Thomas Heumueller, Larry Lüer, Jens Hauch, Christoph J Brabec","doi":"10.1039/d4ee01432d","DOIUrl":"https://doi.org/10.1039/d4ee01432d","url":null,"abstract":"Achieving high-performance perovskite photovoltaics, especially in ambient air relies heavily on optimizing process parameters. However, traditional manual methods often struggle to effectively control the key variables. This inherent challenge requires a paradigm shift toward automated platforms capable of precise and reproducible experiments. Herein, we use a fully automated device acceleration platform (DAP) to optimize the process parameters for preparing full perovskite devices using a two-step sequential technique in ambient air. 10 process parameters that have the potential to significantly influence device performance are systematically optimized. Specifically, we delve into the impact of the dripping speed of organic ammonium halide, a parameter that is difficult to control manually, on both perovskite film and device performance. Through the targeted design of experiments, we reveal that the dripping speed significantly affects device performance primarily by adjusting the residual PbI2 content in the films. We find that moderate dripping speeds, e.g., 50 µL/s, contribute to top-performance devices. Conversely, too fast or too slow speeds result in devices with relatively poorer performance and lower reproducibility. The optimized parameter set enables us to establish a Standard Operation Procedure (SOP) for additive-free perovskite processing under ambient conditions, which yield devices with efficiencies surpassing 23%, satisfactory reproducibility, and state-of-the-art photo-thermal stability. This research underscores the importance of understanding the causality of process parameters in enhancing perovskite photovoltaic performance. Furthermore, our study highlights the pivotal role of automated platforms in discovering innovative workflows and accelerating the development of high-performing perovskite photovoltaic technologies.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":null,"pages":null},"PeriodicalIF":32.5,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462537","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}