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Synergetic Porous Insulating and Passivation Layer Design for High-Efficiency and Stable Perovskite Solar Cells
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-23 DOI: 10.1021/acsmaterialslett.4c0209910.1021/acsmaterialslett.4c02099
Jiashun Li, Jing Liao, Tianhe Dong, Hongyu Li, Ze Li, Li Tan, Xu Chen, Wenfeng Zhang and Haijin Li*, 
{"title":"Synergetic Porous Insulating and Passivation Layer Design for High-Efficiency and Stable Perovskite Solar Cells","authors":"Jiashun Li,&nbsp;Jing Liao,&nbsp;Tianhe Dong,&nbsp;Hongyu Li,&nbsp;Ze Li,&nbsp;Li Tan,&nbsp;Xu Chen,&nbsp;Wenfeng Zhang and Haijin Li*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0209910.1021/acsmaterialslett.4c02099","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02099https://doi.org/10.1021/acsmaterialslett.4c02099","url":null,"abstract":"<p >Perovskite solar cells have attracted extensive attention due to their simple manufacturing process and high efficiency. However, defects between the perovskite and hole transport layer can lead to nonradiative recombination of photogenerated carriers and severe ion migration, which accelerates the degradation of such devices. Here, we chose to deposit an Al<sub>2</sub>O<sub>3</sub> porous insulating layer on the surface of the perovskite film. At the same time, we chose to introduce NMABr (1-Naphthylmethylamine Bromide) into Al<sub>2</sub>O<sub>3</sub> as a modifier to overcome the issue that applying Al<sub>2</sub>O<sub>3</sub> alone may hinder interfacial carrier transport due to the uncontrolled morphology. The addition of NMABr not only has a passivation effect but also changes the morphology of the Al<sub>2</sub>O<sub>3</sub> layer. Under the synergistic effect of Al<sub>2</sub>O<sub>3</sub> and NMABr, a porous insulating contact layer is better formed, which is conducive to carrier transport and improves the stability and efficiency.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"350–358 350–358"},"PeriodicalIF":9.6,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143085949","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Stepwise Structural Relaxation in Battery Active Materials
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-22 DOI: 10.1021/acsmaterialslett.4c0205810.1021/acsmaterialslett.4c02058
Amalie Skurtveit*, Erlend Tiberg North, Heesoo Park, Dmitry Chernyshov, David S. Wragg* and Alexey Y. Koposov*, 
{"title":"Stepwise Structural Relaxation in Battery Active Materials","authors":"Amalie Skurtveit*,&nbsp;Erlend Tiberg North,&nbsp;Heesoo Park,&nbsp;Dmitry Chernyshov,&nbsp;David S. Wragg* and Alexey Y. Koposov*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0205810.1021/acsmaterialslett.4c02058","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02058https://doi.org/10.1021/acsmaterialslett.4c02058","url":null,"abstract":"<p >Whenever the cycling of Li-ion batteries is stopped, the electrode materials undergo a relaxation process, but the structural changes that occur during relaxation are not well-understood. We have used operando synchrotron X-ray diffraction with a time resolution of 1.24 s to observe the structural changes that occur when the lithiation of graphite and LiFePO<sub>4</sub> electrodes are interrupted. Assessing the kinetics of the relaxation processes coupled with molecular dynamics simulations allows us to identify three relaxation stages in graphite. The atomistic origin for the relaxation process within the partially lithiated graphite structure is driven by the reorganization of Li ions into Li clusters. Relaxation in LiFePO<sub>4</sub> electrodes is considerably slower than for graphite, but the observed structural changes is also attributed to reorganization of Li ions. These insights highlight the nature of the structural changes that occur during relaxation and the importance of using operando structural studies to avoid misleading conclusions about the reaction mechanisms in battery materials.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"343–349 343–349"},"PeriodicalIF":9.6,"publicationDate":"2024-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialslett.4c02058","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143085842","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Establishing Active Cu+–O–Mg2+ Sites at the Cu2O/CuO Interface for Efficient Electroreduction of CO2 to C2+ Products
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-20 DOI: 10.1021/acsmaterialslett.4c0231910.1021/acsmaterialslett.4c02319
Qinyuan Ji, Hu Zang, Changjiang Liu, Haiyan Lu, Nan Yu and Baoyou Geng*, 
{"title":"Establishing Active Cu+–O–Mg2+ Sites at the Cu2O/CuO Interface for Efficient Electroreduction of CO2 to C2+ Products","authors":"Qinyuan Ji,&nbsp;Hu Zang,&nbsp;Changjiang Liu,&nbsp;Haiyan Lu,&nbsp;Nan Yu and Baoyou Geng*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0231910.1021/acsmaterialslett.4c02319","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02319https://doi.org/10.1021/acsmaterialslett.4c02319","url":null,"abstract":"<p >Cu-based materials are regarded as effective electrocatalysts for CO<sub>2</sub>RR; however, Cu<sup>+</sup>, the active site for C–C coupling, is unstable under reduction conditions. Herein, Mg<sup>2+</sup> is doped into the Cu<sub>2</sub>O/CuO interface and generates high-activity Cu<sup>+</sup>–O-Mg<sup>2+</sup> sites following electrochemical activation. The electron-withdrawing effect of Mg<sup>2+</sup> in the Cu<sup>+</sup>–O-Mg<sup>2+</sup> site stabilizes Cu<sup>+</sup> and optimizes the reaction pathway for CO<sub>2</sub>RR. At a partial current density of 567.21 ± 5.18 mA cm<sup>–2</sup>, the Faraday efficiency (FE) for C<sub>2+</sub> products can reach 81.03 ± 0.74%. In situ Raman and in situ infrared spectroscopy reveal that the Cu<sup>+</sup>–O-Mg<sup>2+</sup> site significantly enhances the coverage and stability of *CO, which contributes to the ultrahigh selectivity of CO<sub>2</sub> toward C<sub>2+</sub> products. Density functional theory (DFT) studies indicate that *CO<sub>2</sub> is readily adsorbed on the Cu<sup>+</sup>–O-Mg<sup>2+</sup> site, facilitating the more effective generation of *CO, which subsequently promotes the electrochemical C–C coupling step and accelerates the production of C<sub>2+</sub> products.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"333–342 333–342"},"PeriodicalIF":9.6,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143084983","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Far-From-Equilibrium Processing Opens Kinetic Paths for Engineering Novel Materials by Breaking Thermodynamic Limits
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-20 DOI: 10.1021/acsmaterialslett.4c0195210.1021/acsmaterialslett.4c01952
Yihong Yu, Zhengpeng Qin, Xuefeng Zhang, Yanan Chen, Gaowu Qin and Song Li*, 
{"title":"Far-From-Equilibrium Processing Opens Kinetic Paths for Engineering Novel Materials by Breaking Thermodynamic Limits","authors":"Yihong Yu,&nbsp;Zhengpeng Qin,&nbsp;Xuefeng Zhang,&nbsp;Yanan Chen,&nbsp;Gaowu Qin and Song Li*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0195210.1021/acsmaterialslett.4c01952","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01952https://doi.org/10.1021/acsmaterialslett.4c01952","url":null,"abstract":"<p >Thermodynamic metastable nanomaterials display attractive properties due to their unique atom configuration and microstructure, distinct from their counterparts found in equilibrium phase diagrams. However, their fabrication remains a grand challenge because conventional methods are generally operated under near-equilibrium conditions. To break the thermodynamic limits for discovering novel materials, numerous fabrication methods by adopting extreme strategies have been developed, including ultrafast synthesis, Joule heating, carbon thermal shock, pulse heating, extreme temperature gradients, and rapid solidification. A common feature of these methods is that the target material is processed under a far-from-equilibrium (FFE) thermodynamic state, where a new kinetic route is created for the evolution of an unprecedented composition/structure. In this review, we provide a unifying view and guiding strategies for engineering FFE environments during materials synthesis, categorized within both temporal and spatial dimensions of the thermodynamic landscape. Furthermore, we highlight the potential of FFE materials, not only as platforms for deeper understanding nonequilibrium behaviors, but also as a framework for designing innovative materials for advanced technologies.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"319–332 319–332"},"PeriodicalIF":9.6,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143085804","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Framework-Isomeric Metal–Organic Frameworks Built from Supermolecular Building Blocks for High Iodine Capture
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-19 DOI: 10.1021/acsmaterialslett.4c0190810.1021/acsmaterialslett.4c01908
Shuting Chen, Yinyin Wang, Jieqiu Huang, Huanhuan Xie, Jingjing Yuan, Mengyao Song, Bin Yang, Qingqing Pang* and Binbin Tu*, 
{"title":"Framework-Isomeric Metal–Organic Frameworks Built from Supermolecular Building Blocks for High Iodine Capture","authors":"Shuting Chen,&nbsp;Yinyin Wang,&nbsp;Jieqiu Huang,&nbsp;Huanhuan Xie,&nbsp;Jingjing Yuan,&nbsp;Mengyao Song,&nbsp;Bin Yang,&nbsp;Qingqing Pang* and Binbin Tu*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0190810.1021/acsmaterialslett.4c01908","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01908https://doi.org/10.1021/acsmaterialslett.4c01908","url":null,"abstract":"<p >The supermolecular building block approach is powerful in constructing hierarchically porous metal–organic frameworks (MOFs). However, the structural diversity of these extended frameworks built from the same building blocks has never been explored. Herein, we propose a strategy by synergistically tuning the extending direction of metal–organic polyhedra (MOPs) and the linker conformation to achieve MOFs with framework isomerism. Six novel MOFs (CCNUF-1–6) based on an octahedral MOP and different tritopic pyridine-based linkers were successfully synthesized, among which the structural diversity increased with increasing linker flexibility. The topologies (<b>sql</b>, <b>kgd</b>, and <b>rtl</b>) of these materials are unprecedented in MOP-based MOFs. Moreover, highly porous CCNUF-2–6 showed remarkable iodine uptake capacities in the range of 2.51 to 3.11 g g<sup>–1</sup>. This study emphasizes the potential of MOPs containing open metal sites as versatile platforms for the development of diversified hierarchically porous MOFs with enhanced functional properties.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"304–311 304–311"},"PeriodicalIF":9.6,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143085469","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Probing the Design Rules for Optimizing Electron Spin Relaxation in Densely Packed Triplet Media for Quantum Applications. 探讨密装三重态介质中优化电子自旋弛豫的设计规则。
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-19 eCollection Date: 2025-01-06 DOI: 10.1021/acsmaterialslett.4c01465
Max Attwood, Yingxu Li, Irena Nevjestic, Phil Diggle, Alberto Collauto, Muskaan Betala, Andrew J P White, Mark Oxborrow
{"title":"Probing the Design Rules for Optimizing Electron Spin Relaxation in Densely Packed Triplet Media for Quantum Applications.","authors":"Max Attwood, Yingxu Li, Irena Nevjestic, Phil Diggle, Alberto Collauto, Muskaan Betala, Andrew J P White, Mark Oxborrow","doi":"10.1021/acsmaterialslett.4c01465","DOIUrl":"10.1021/acsmaterialslett.4c01465","url":null,"abstract":"<p><p>Quantum technologies using electron spins have the advantage of employing chemical qubit media with tunable properties. The principal objective of material engineers is to enhance photoexcited spin yields and quantum spin relaxation. In this study, we demonstrate a facile synthetic approach to control spin properties in charge-transfer cocrystals consisting of 1,2,4,5-tetracyanobenzene (TCNB) and acetylated anthracene. We find that the extent and position of acetylation control the degree of charge-transfer and the optical band gap by modifying crystal packing and electronic structure. We further reveal that while the spin polarization of the triplet state is slightly reduced compared to prototypical Anthracene:TCNB, the phase memory (<i>T</i> <sub>m</sub>) and, for 9-acetylanthracene:TCNB spin-lattice relaxation (<i>T</i> <sub>1</sub>) time, could be enhanced up to 2.4 times. Our findings are discussed in the context of quantum microwave amplifiers, known as masers, and show that acetylation could be a powerful tool for improving organic materials for quantum sensing applications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"286-294"},"PeriodicalIF":9.6,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11707738/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142941428","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
La3(Ga3S3O3)(Si2O7): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-19 DOI: 10.1021/acsmaterialslett.4c0216210.1021/acsmaterialslett.4c02162
Ming-Shu Zhang, Shao-Min Pei, Xiao-Ming Jiang, Bin-Wen Liu* and Guo-Cong Guo*, 
{"title":"La3(Ga3S3O3)(Si2O7): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups","authors":"Ming-Shu Zhang,&nbsp;Shao-Min Pei,&nbsp;Xiao-Ming Jiang,&nbsp;Bin-Wen Liu* and Guo-Cong Guo*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0216210.1021/acsmaterialslett.4c02162","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02162https://doi.org/10.1021/acsmaterialslett.4c02162","url":null,"abstract":"<p >The exceptional structural plasticity and well-balanced properties of oxychalcogenides make them highly desirable as infrared nonlinear optical (IR NLO) materials. A breakthrough in the design of high-performance oxychalcogenides involves integrating and assembling multiple anionic units to maximize their functions. Following this approach, we developed La<sub>3</sub>(Ga<sub>3</sub>S<sub>3</sub>O<sub>3</sub>)(Si<sub>2</sub>O<sub>7</sub>) (LGSSO) by simultaneously incorporating [Ga<sub>3</sub>O<sub>3</sub>S<sub>6</sub>] and [Si<sub>2</sub>O<sub>7</sub>] groups. The potential of LGSSO as an IR NLO material is evident from its wide bandgap (4.82 eV, runner-up in NLO oxychalcogenides), high laser-induced damage threshold (8.7 × AgGaS<sub>2</sub> at 1064 nm), attractive birefringence (0.122 at 546 nm), and moderate phase-matching second-harmonic generation response (1.7 × KH<sub>2</sub>PO<sub>4</sub> at 1064 nm, 0.3 × AgGaS<sub>2</sub> at 1910 nm). Theoretical studies indicate that the [LaS<sub>2</sub>O<sub>6</sub>] and [GaO<sub>2</sub>S<sub>2</sub>] contribute significantly to the NLO coefficient, while the [Ga<sub>3</sub>O<sub>3</sub>S<sub>6</sub>] trimers with pronounced polarizability anisotropy play a pivotal role in providing a substantial birefringence. This work offers a tangible paradigm for exploring well-performed oxychalcogenide NLO material.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"312–318 312–318"},"PeriodicalIF":9.6,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143085543","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Probing the Design Rules for Optimizing Electron Spin Relaxation in Densely Packed Triplet Media for Quantum Applications
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-19 DOI: 10.1021/acsmaterialslett.4c0146510.1021/acsmaterialslett.4c01465
Max Attwood*, Yingxu Li, Irena Nevjestic, Phil Diggle, Alberto Collauto, Muskaan Betala, Andrew J. P. White and Mark Oxborrow, 
{"title":"Probing the Design Rules for Optimizing Electron Spin Relaxation in Densely Packed Triplet Media for Quantum Applications","authors":"Max Attwood*,&nbsp;Yingxu Li,&nbsp;Irena Nevjestic,&nbsp;Phil Diggle,&nbsp;Alberto Collauto,&nbsp;Muskaan Betala,&nbsp;Andrew J. P. White and Mark Oxborrow,&nbsp;","doi":"10.1021/acsmaterialslett.4c0146510.1021/acsmaterialslett.4c01465","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01465https://doi.org/10.1021/acsmaterialslett.4c01465","url":null,"abstract":"<p >Quantum technologies using electron spins have the advantage of employing chemical qubit media with tunable properties. The principal objective of material engineers is to enhance photoexcited spin yields and quantum spin relaxation. In this study, we demonstrate a facile synthetic approach to control spin properties in charge-transfer cocrystals consisting of 1,2,4,5-tetracyanobenzene (TCNB) and acetylated anthracene. We find that the extent and position of acetylation control the degree of charge-transfer and the optical band gap by modifying crystal packing and electronic structure. We further reveal that while the spin polarization of the triplet state is slightly reduced compared to prototypical Anthracene:TCNB, the phase memory (<i>T</i><sub>m</sub>) and, for 9-acetylanthracene:TCNB spin–lattice relaxation (<i>T</i><sub>1</sub>) time, could be enhanced up to 2.4 times. Our findings are discussed in the context of quantum microwave amplifiers, known as masers, and show that acetylation could be a powerful tool for improving organic materials for quantum sensing applications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"286–294 286–294"},"PeriodicalIF":9.6,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialslett.4c01465","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143085444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ultrafast Photoassisted Capture of Uranium over Cu2O/CuO Heterojunction Enabled by Rapid Interfacial Electron Transfer
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-19 DOI: 10.1021/acsmaterialslett.4c0212110.1021/acsmaterialslett.4c02121
Huanhuan Liu, Hongliang Guo, Dingping Huang, Li Zhou, Jia Lei*, Yan Liu* and Wenkun Zhu*, 
{"title":"Ultrafast Photoassisted Capture of Uranium over Cu2O/CuO Heterojunction Enabled by Rapid Interfacial Electron Transfer","authors":"Huanhuan Liu,&nbsp;Hongliang Guo,&nbsp;Dingping Huang,&nbsp;Li Zhou,&nbsp;Jia Lei*,&nbsp;Yan Liu* and Wenkun Zhu*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0212110.1021/acsmaterialslett.4c02121","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02121https://doi.org/10.1021/acsmaterialslett.4c02121","url":null,"abstract":"<p >Photoassisted capture of uranium provides a promising strategy for the sustainable utilization of nuclear energy. Herein, we constructed Cu<sub>2</sub>O/CuO heterojunctions in situ by a wet-etching method, showing ultrafast reaction kinetics and photocatalytic activity for U(VI) reduction. In 8 ppm of uranium-containing wastewater, the Cu<sub>2</sub>O/CuO heterojunctions exhibited a remarkable uranium extraction efficiency of 94.6% within 10 min under irradiation, which exceeded most recently reported photocatalysts. The photocatalytic reaction rate constant of Cu<sub>2</sub>O/CuO heterojunctions was 5.8-time larger than that of pure Cu<sub>2</sub>O. A mechanism study indicated that the photogenerated electrons reduced CuO species in Cu<sub>2</sub>O/CuO heterojunctions and <i>in situ</i> created the oxygen vacancy during the photocatalysis process, which strengthened the binding of UO<sub>2</sub><sup>2+</sup>. The rapid electron transfer rate over the <i>in situ</i> heterojunction interfaces and the enhanced UO<sub>2</sub><sup>2+</sup> binding strength by the <i>in situ</i> formed oxygen vacancy accounted for the ultrafast reaction kinetics.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"295–303 295–303"},"PeriodicalIF":9.6,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143084968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-Capacity C/Sn-Composites as Next-Generation Anodes for Sodium-Ion Batteries
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-18 DOI: 10.1021/acsmaterialslett.4c0203310.1021/acsmaterialslett.4c02033
Alexander Kempf*, Magdalena Graczyk-Zajac* and Ralf Riedel, 
{"title":"High-Capacity C/Sn-Composites as Next-Generation Anodes for Sodium-Ion Batteries","authors":"Alexander Kempf*,&nbsp;Magdalena Graczyk-Zajac* and Ralf Riedel,&nbsp;","doi":"10.1021/acsmaterialslett.4c0203310.1021/acsmaterialslett.4c02033","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02033https://doi.org/10.1021/acsmaterialslett.4c02033","url":null,"abstract":"<p >This work investigates carbon/tin composites as anode materials for high-performance sodium-ion batteries (SIBs). The material is prepared by dispersing SnO<sub>2</sub> nanopowder in fructose solution, followed by thermal treatment under inert gas, leading to fructose carbonization and carbothermal reduction of SnO<sub>2</sub> forming metallic Sn, confirmed by thermogravimetric analysis (TGA) and X-ray diffraction (XRD). Different thermal procedures, including a single-step with extended holding times and a two-step process, are explored; the latter separates fructose carbonization from carbothermal reduction, with the second step conducted under conventional heating conditions or via an ultrafast heating method. The composite with low carbon content exhibits a sodiation capacity of 749.2 mAh g<sup>–1</sup> in the first cycle with a high initial cycle efficiency (ICE) of 83.2%. After 100 cycles at 37.2 mA g<sup>–1</sup>, it retains a capacity of 351 mAh g<sup>–1</sup>. The material demonstrates excellent rate capability, maintaining a capacity of 344.5 mAh g<sup>–1</sup> at a rate of 2380 mA g<sup>–1</sup>.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"275–285 275–285"},"PeriodicalIF":9.6,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143085026","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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