Weijie Zhang, Zhou Lu, Cailing Chen, Peter Vannatta, Chenxin Yang, Abdullah M. Al-Enizi, Ayman Nafady, Shengqian Ma
Despite recent progress in 3D covalent organic frameworks (3D-COFs), their design and synthesis still pose significant challenges, mainly due to a limited mechanistic understanding of their synthesis. Herein, a linker exchange approach has been utilized to synthesize a series of new 3D-COFs by first preparing an imine-linked 3D-COF followed by exchanging with selected linear diamine linkers. This approach can be widely applicable to different types of diamines, enabling rational-designed synthesis of 3D frameworks that are previously inaccessible via direct polymerization in a one-pot reaction. Mechanistic aspects associated with the improved 3D-COF synthesis via the linker exchange approach, are investigated by density functional theory calculations, in which the possibility of the departure of the leaving linker is a spontaneous process with a decrease in enthalpy. Catalytic and computational results revealed that incorporating benzoxazole moiety into the 3D-COF frameworks enables a significant increase in the capability of visible-light-driven catalysis. The overall findings of the present study will pave the way toward the development of 3D-COFs with tunable structures and functions for other promising and challenging applications.
{"title":"Expanded Synthesis of 3D Covalent Organic Frameworks via Linker Exchange for Efficient Photocatalytic Aerobic Oxidation","authors":"Weijie Zhang, Zhou Lu, Cailing Chen, Peter Vannatta, Chenxin Yang, Abdullah M. Al-Enizi, Ayman Nafady, Shengqian Ma","doi":"10.1002/smll.202502316","DOIUrl":"https://doi.org/10.1002/smll.202502316","url":null,"abstract":"Despite recent progress in 3D covalent organic frameworks (3D-COFs), their design and synthesis still pose significant challenges, mainly due to a limited mechanistic understanding of their synthesis. Herein, a linker exchange approach has been utilized to synthesize a series of new 3D-COFs by first preparing an imine-linked 3D-COF followed by exchanging with selected linear diamine linkers. This approach can be widely applicable to different types of diamines, enabling rational-designed synthesis of 3D frameworks that are previously inaccessible via direct polymerization in a one-pot reaction. Mechanistic aspects associated with the improved 3D-COF synthesis via the linker exchange approach, are investigated by density functional theory calculations, in which the possibility of the departure of the leaving linker is a spontaneous process with a decrease in enthalpy. Catalytic and computational results revealed that incorporating benzoxazole moiety into the 3D-COF frameworks enables a significant increase in the capability of visible-light-driven catalysis. The overall findings of the present study will pave the way toward the development of 3D-COFs with tunable structures and functions for other promising and challenging applications.","PeriodicalId":228,"journal":{"name":"Small","volume":"56 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660677","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}
Shasha Guo, Mohamed Ait Tamerd, Changyuan Li, Xinyue Shi, Menghao Yang, Jingrong Hou, Jie Liu, Mingxue Tang, Shu-Chih Haw, Chien-Te Chen, Ting-Shan Chan, Chang-Yang Kuo, Zhiwei Hu, Long Yang, Jiwei Ma
Magnetite (Fe3O4), a conversion-type anode material, possesses high capacity, cost-effectiveness and environmental friendliness, positioning it as a promising candidate for the large-scale energy storage applications. However, the multi-electron reactions in sodium-ion batteries face challenges originated from the electrochemical inactivity of Na+ intercalation in the conversion-type oxides. In this work, controllable Fe vacancies are tailored in Fe3O4 lattice through the gradient Mo doping. The pair distribution function local structure analysis reveals that the key to stabilizing more Fe vacancies lies in the uniform occupation of Mo dopants at both tetrahedral (8a) and octahedral (16d) sites. The vacancy-rich structure, featuring 7.3% Fe vacancies, achieves a significantly enhanced capacity of 127 mAh g−1 after 150 cycles at 100 mA g−1, in comparison with the 37 mAh g−1 for defect-free Fe3O4. A comprehensive understanding of how the defective structure relates to electrochemical performance is presented, combining physical-electrochemical characterizations with theoretical calculations. The occurred Mo-O interactions enhances electronic conductivity and diminishes electrostatic interactions between intercalated Na+ and lattice O2−. Concurrently, Fe vacancies facilitate bulk Na+ migration with lower energy barrier. This study presents a prospect for modulating the defective structure in transition metal oxides to activate fast and reversible sodium intercalation toward high-performance sodium-ion batteries.
{"title":"Activating Sodium Intercalation in Cation-Deficient Fe3O4 Through Mo Substitution","authors":"Shasha Guo, Mohamed Ait Tamerd, Changyuan Li, Xinyue Shi, Menghao Yang, Jingrong Hou, Jie Liu, Mingxue Tang, Shu-Chih Haw, Chien-Te Chen, Ting-Shan Chan, Chang-Yang Kuo, Zhiwei Hu, Long Yang, Jiwei Ma","doi":"10.1002/smll.202408212","DOIUrl":"https://doi.org/10.1002/smll.202408212","url":null,"abstract":"Magnetite (Fe<sub>3</sub>O<sub>4</sub>), a conversion-type anode material, possesses high capacity, cost-effectiveness and environmental friendliness, positioning it as a promising candidate for the large-scale energy storage applications. However, the multi-electron reactions in sodium-ion batteries face challenges originated from the electrochemical inactivity of Na<sup>+</sup> intercalation in the conversion-type oxides. In this work, controllable Fe vacancies are tailored in Fe<sub>3</sub>O<sub>4</sub> lattice through the gradient Mo doping. The pair distribution function local structure analysis reveals that the key to stabilizing more Fe vacancies lies in the uniform occupation of Mo dopants at both tetrahedral (8<i>a</i>) and octahedral (16<i>d</i>) sites. The vacancy-rich structure, featuring 7.3% Fe vacancies, achieves a significantly enhanced capacity of 127 mAh g<sup>−1</sup> after 150 cycles at 100 mA g<sup>−1</sup>, in comparison with the 37 mAh g<sup>−1</sup> for defect-free Fe<sub>3</sub>O<sub>4</sub>. A comprehensive understanding of how the defective structure relates to electrochemical performance is presented, combining physical-electrochemical characterizations with theoretical calculations. The occurred Mo-O interactions enhances electronic conductivity and diminishes electrostatic interactions between intercalated Na<sup>+</sup> and lattice O<sup>2−</sup>. Concurrently, Fe vacancies facilitate bulk Na<sup>+</sup> migration with lower energy barrier. This study presents a prospect for modulating the defective structure in transition metal oxides to activate fast and reversible sodium intercalation toward high-performance sodium-ion batteries.","PeriodicalId":228,"journal":{"name":"Small","volume":"25 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660957","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 irreconcilable camouflage mechanisms of radar and infrared spectroscopy present substantial challenges to integrating multi-physics field cloaking technology. Although aerogels possess both microwave dissipation and thermal insulation, higher infrared emissivity restrict further amelioration in compatible stealth field. Herein, we propose a bilayer configuration comprised of aramid nanofiber (ANF) aerogel and infrared shielding meta-surface (ISM). The top ISM with low-pass filtering capabilities is engineered to regulate emissivity while remaining transparent to microwaves. While the bottom quaternary ANF aerogels with radar dissipation and thermal insulation are synthesized by multi-scale design strategy and heterogeneous surface engineering. Through theoretical and experimental optimization, the assembled compatible stealth composite achieves a near-perfect absorption in X-band, while the synergy of low emissivity and thermal insulation facilitates concealment in infrared windows. Specifically, the minimum reflection loss (RL) reaches −32.44 dB, effective absorption bandwidth (EAB) expands to 3.69 GHz (8.71–12.40 GHz), and the integration of effective reflection loss value (ΔH) increases to 9.92 dB GHz mm−1. Additionally, low thermal conductivity (0.0288 W (m K)−1) and average infrared emissivity (0.23 in 3–5 µm and 0.25 in 8–14 µm) can reduce infrared radiation energy by 68.1%. This research provides a new thought for the design of multispectral camouflage and demonstrates enormous potential in stealth technologies.
{"title":"Advanced Multiphysics Camouflage Based on Low-Emissivity Meta-surface Coupled with Wave-Absorbing and Thermal-Insulating Aerogel","authors":"Wenqing Hai, Siyi Bi, Lili Yang, Jiatong Wu, Wenlong Huang, Mengting Cui, Xin Zhang, Jing Meng, Chunhui Chen, Huiqi Shao, Guangwei Shao, Jinhua Jiang, Nanliang Chen","doi":"10.1002/smll.202500155","DOIUrl":"https://doi.org/10.1002/smll.202500155","url":null,"abstract":"The irreconcilable camouflage mechanisms of radar and infrared spectroscopy present substantial challenges to integrating multi-physics field cloaking technology. Although aerogels possess both microwave dissipation and thermal insulation, higher infrared emissivity restrict further amelioration in compatible stealth field. Herein, we propose a bilayer configuration comprised of aramid nanofiber (ANF) aerogel and infrared shielding meta-surface (ISM). The top ISM with low-pass filtering capabilities is engineered to regulate emissivity while remaining transparent to microwaves. While the bottom quaternary ANF aerogels with radar dissipation and thermal insulation are synthesized by multi-scale design strategy and heterogeneous surface engineering. Through theoretical and experimental optimization, the assembled compatible stealth composite achieves a near-perfect absorption in X-band, while the synergy of low emissivity and thermal insulation facilitates concealment in infrared windows. Specifically, the minimum reflection loss (RL) reaches −32.44 dB, effective absorption bandwidth (EAB) expands to 3.69 GHz (8.71–12.40 GHz), and the integration of effective reflection loss value (<i>ΔH</i>) increases to 9.92 dB GHz mm<sup>−1</sup>. Additionally, low thermal conductivity (0.0288 W (m K)<sup>−1</sup>) and average infrared emissivity (0.23 in 3–5 µm and 0.25 in 8–14 µm) can reduce infrared radiation energy by 68.1%. This research provides a new thought for the design of multispectral camouflage and demonstrates enormous potential in stealth technologies.","PeriodicalId":228,"journal":{"name":"Small","volume":"37 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143661000","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}
Tamanna Mallick, Anushree Mondal, Shubham Das, Priyadarsi De
Amyloid aggregation, intricately related to various neurodegenerative and metabolic diseases, presents a significant growing health challenge. Dopamine, a potent antioxidant, plays a pivotal role in modulating protein misfolding by leveraging its potent anti-amyloidogenic and neuroprotective properties. However, its biological applications are limited by poor aqueous solubility and suboptimal biocompatibility. To address these challenges, water-soluble copolymers (DP1-DP3) featuring dopamine and glucose side-chain pendants are fabricated and investigated for their efficacy in inhibiting amyloid fibril formation from insulin and amyloid beta (Aβ42) peptide. The effects of DP1-DP3 copolymers on amyloid fibrillation are assessed using several biophysical techniques, which demonstrate excellent radical scavenging properties and the remarkable efficacy of DP3 copolymer in suppressing insulin amyloid fibrillation, achieving ≈97% inhibition. Isothermal titration calorimetry (ITC) and fluorescence binding experiments are carried out to quantify the insulin-DP3 complex formation. Molecular dynamics simulations validate the ability of DP3 to prevent amyloid fibrillogenesis of both insulin and Aβ42. These studies demonstrate beneficial interactions between DP3 and amyloidogenic protein/peptide, facilitating the stability of the resulting complexes. Overall, the present findings suggest that dopamine-based antioxidant polymers hold significant potential as advanced therapeutic agents for preventing amyloidogenic disorders.
{"title":"Inhibition of Insulin Amyloid Fibrillogenesis Using Antioxidant Copolymers with Dopamine Pendants","authors":"Tamanna Mallick, Anushree Mondal, Shubham Das, Priyadarsi De","doi":"10.1002/smll.202501206","DOIUrl":"https://doi.org/10.1002/smll.202501206","url":null,"abstract":"Amyloid aggregation, intricately related to various neurodegenerative and metabolic diseases, presents a significant growing health challenge. Dopamine, a potent antioxidant, plays a pivotal role in modulating protein misfolding by leveraging its potent anti-amyloidogenic and neuroprotective properties. However, its biological applications are limited by poor aqueous solubility and suboptimal biocompatibility. To address these challenges, water-soluble copolymers (<b>DP1</b>-<b>DP3</b>) featuring dopamine and glucose side-chain pendants are fabricated and investigated for their efficacy in inhibiting amyloid fibril formation from insulin and amyloid beta (A<i>β</i><sub>42</sub>) peptide. The effects of <b>DP1</b>-<b>DP3</b> copolymers on amyloid fibrillation are assessed using several biophysical techniques, which demonstrate excellent radical scavenging properties and the remarkable efficacy of <b>DP3</b> copolymer in suppressing insulin amyloid fibrillation, achieving ≈97% inhibition. Isothermal titration calorimetry (ITC) and fluorescence binding experiments are carried out to quantify the insulin-<b>DP3</b> complex formation. Molecular dynamics simulations validate the ability of <b>DP3</b> to prevent amyloid fibrillogenesis of both insulin and A<i>β</i><sub>42</sub>. These studies demonstrate beneficial interactions between <b>DP3</b> and amyloidogenic protein/peptide, facilitating the stability of the resulting complexes. Overall, the present findings suggest that dopamine-based antioxidant polymers hold significant potential as advanced therapeutic agents for preventing amyloidogenic disorders.","PeriodicalId":228,"journal":{"name":"Small","volume":"183 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660998","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}
Lining Xu, Yingyu Zhang, Dingding Wang, Quanzhong Ren, Yi Wang, Zetong Zang, Anyi Guo, Jianxun Guo, Ling Wang, Renxian Wang, Yajun Liu
Macrophages are key innate immune cells in the muscle environment of sarcopenia patients, significantly influencing muscle stem cell (MuSC) proliferation and differentiation. However, prolonged activation of macrophages can hinder muscle recovery. In this study, it synthesizes lipoic acid-modified gold nanoparticles (LA-Au NPs) of varying sizes to evaluate their biocompatibility and immunomodulatory effects. The findings demonstrate that LA-Au NPs exhibit excellent biocompatibility with macrophages and promoted M2 polarization in a size-dependent manner. Mechanistically, LA-Au NPs facilitated metabolic reprogramming in macrophages by enhancing lysosomal autophagy and mitochondrial oxidative phosphorylation. Furthermore, macrophages are shown to chemotax toward MuSCs, regulating their proliferation via the chemokine system, inhibiting MuSC apoptosis, and enhancing differentiation under inflammatory conditions. In vivo studies have confirmed the safety and efficacy of LA-Au NPs in sarcopenia mice. To further enhance the effectiveness of LA-Au NPs, it investigates a delivery strategy that involves preconditioning macrophages with LA-Au NPs (Mac@Au NPs). Compared to the direct injection of LA-Au NPs, Mac@Au NPs demonstrate significantly greater benefits for muscle repair. This highlights the potential of macrophage therapy as a promising strategy for effective muscle regeneration and therapeutic intervention in sarcopenia.
{"title":"Nanoparticle-Driven Skeletal Muscle Repair and Regeneration Through Macrophage-Muscle Stem Cell Interaction","authors":"Lining Xu, Yingyu Zhang, Dingding Wang, Quanzhong Ren, Yi Wang, Zetong Zang, Anyi Guo, Jianxun Guo, Ling Wang, Renxian Wang, Yajun Liu","doi":"10.1002/smll.202412611","DOIUrl":"https://doi.org/10.1002/smll.202412611","url":null,"abstract":"Macrophages are key innate immune cells in the muscle environment of sarcopenia patients, significantly influencing muscle stem cell (MuSC) proliferation and differentiation. However, prolonged activation of macrophages can hinder muscle recovery. In this study, it synthesizes lipoic acid-modified gold nanoparticles (LA-Au NPs) of varying sizes to evaluate their biocompatibility and immunomodulatory effects. The findings demonstrate that LA-Au NPs exhibit excellent biocompatibility with macrophages and promoted M2 polarization in a size-dependent manner. Mechanistically, LA-Au NPs facilitated metabolic reprogramming in macrophages by enhancing lysosomal autophagy and mitochondrial oxidative phosphorylation. Furthermore, macrophages are shown to chemotax toward MuSCs, regulating their proliferation via the chemokine system, inhibiting MuSC apoptosis, and enhancing differentiation under inflammatory conditions. In vivo studies have confirmed the safety and efficacy of LA-Au NPs in sarcopenia mice. To further enhance the effectiveness of LA-Au NPs, it investigates a delivery strategy that involves preconditioning macrophages with LA-Au NPs (Mac@Au NPs). Compared to the direct injection of LA-Au NPs, Mac@Au NPs demonstrate significantly greater benefits for muscle repair. This highlights the potential of macrophage therapy as a promising strategy for effective muscle regeneration and therapeutic intervention in sarcopenia.","PeriodicalId":228,"journal":{"name":"Small","volume":"14 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143661058","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 rational construction of efficient and stable electrocatalysts for methanol oxidation reaction (MOR) in acidic and alkaline media affects the commercialization of direct methanol fuel cells (DMFCs). Here, poly(3,4-propylenedioxythiophene) (PProDOT)-embedded Ti3C2Tx flakes for the growth of platinum and palladium bimetallic nanoparticles (PtPd) by a chemically reduced hydrothermal process are assembled. The constructed Ti3C2Tx/PProDOT/PtPd hybrids exhibit 3D-layered stereoscopic structures. After the embedding of PProDOT, the re-stacking of MXene flakes is suppressed and the interlayer spacing between flakes is extended, allowing the Ti3C2Tx/PProDOT interface to promote nanoparticle deposition, active site exposure, and charge transport. The electrochemical test outcomes reveal that the catalytic activity of Ti3C2Tx/PProDOT/PtPd for MOR far exceeds that of Ti3C2Tx/PtPd and Pt/C. In acidic electrolytes, the mass activity (MA) of Ti3C2Tx/PProDOT/PtPd is 2206.1 mA mg−1, which is 4.4 and 5.8 times higher than that of Ti3C2Tx/PtPd and Pt/C, respectively. In alkaline electrolytes, the MA of Ti3C2Tx/PProDOT/PtPd reaches 4180 mA mg−1, which is 2.1 and 4.8 times higher than that of Ti3C2Tx/PtPd and Pt/C, respectively. Meanwhile, its stability and CO tolerance improve significantly. Besides, Ti3C2Tx/PProDOT/PtPd also exhibits enhanced catalytic activity toward ethanol oxidation.
{"title":"Stereo Assembly of Bimetallic PtPd on Ti3C2Tx/PProDOT for Efficient Methanol Oxidation Reaction in Both Acidic and Alkaline Media","authors":"Shuyue Xie, Tursun Abdiryim, Ruxangul Jamal, Guoliang Zhang, Xinsheng Tang, Yu Zhang, Yanyan Song, Nuramina Abdukirim","doi":"10.1002/smll.202500402","DOIUrl":"https://doi.org/10.1002/smll.202500402","url":null,"abstract":"The rational construction of efficient and stable electrocatalysts for methanol oxidation reaction (MOR) in acidic and alkaline media affects the commercialization of direct methanol fuel cells (DMFCs). Here, poly(3,4-propylenedioxythiophene) (PProDOT)-embedded Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> flakes for the growth of platinum and palladium bimetallic nanoparticles (PtPd) by a chemically reduced hydrothermal process are assembled. The constructed Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PProDOT/PtPd hybrids exhibit 3D-layered stereoscopic structures. After the embedding of PProDOT, the re-stacking of MXene flakes is suppressed and the interlayer spacing between flakes is extended, allowing the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PProDOT interface to promote nanoparticle deposition, active site exposure, and charge transport. The electrochemical test outcomes reveal that the catalytic activity of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PProDOT/PtPd for MOR far exceeds that of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PtPd and Pt/C. In acidic electrolytes, the mass activity (MA) of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PProDOT/PtPd is 2206.1 mA mg<sup>−1</sup>, which is 4.4 and 5.8 times higher than that of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PtPd and Pt/C, respectively. In alkaline electrolytes, the MA of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PProDOT/PtPd reaches 4180 mA mg<sup>−1</sup>, which is 2.1 and 4.8 times higher than that of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PtPd and Pt/C, respectively. Meanwhile, its stability and CO tolerance improve significantly. Besides, Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/PProDOT/PtPd also exhibits enhanced catalytic activity toward ethanol oxidation.","PeriodicalId":228,"journal":{"name":"Small","volume":"56 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654167","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}
Hyun-Geun Oh, Younghyun You, Seungyun Lee, Sangheon Lee, Fan Ren, Stephen J. Pearton, Jihyun Kim, Gwan-Hyoung Lee
Multilayer transition metal dichalcogenides (ML-TMDs) with commensurate, incommensurate, and reconstructed structures, have emerged as a class of 2D materials with unique properties that differ significantly from their monolayer counterparts. While previous research has focused on monolayers, the discovery of various novel properties has sparked interest in multilayers with diverse structures engineered through stacking. These materials are characterized by interactions between layers and exhibit remarkable tunability in their structural, optical, and electronic behaviors depending on stacking order, twist angle, and interlayer coupling. This review provides an overview of ML-TMDs and explores their properties such as electronic band structure, optical responses, ferroelectricity, and anomalous Hall effect. Various synthetic methods employed to fabricate ML-TMDs, including mechanical stacking and chemical vapor deposition techniques, with an emphasis on achieving precise control of the twist angles and layer configurations, are discussed. This study further explores potential applications of ML-TMDs in nanoelectronics, optoelectronics, and quantum devices, where their unique properties can be harnessed for next-generation technologies. The critical role played by these materials in the development of future electronic and quantum devices is highlighted.
{"title":"Commensurate, Incommensurate, and Reconstructed Structures of Multilayer Transition Metal Dichalcogenide and Their Applications","authors":"Hyun-Geun Oh, Younghyun You, Seungyun Lee, Sangheon Lee, Fan Ren, Stephen J. Pearton, Jihyun Kim, Gwan-Hyoung Lee","doi":"10.1002/smll.202412737","DOIUrl":"https://doi.org/10.1002/smll.202412737","url":null,"abstract":"Multilayer transition metal dichalcogenides (ML-TMDs) with commensurate, incommensurate, and reconstructed structures, have emerged as a class of 2D materials with unique properties that differ significantly from their monolayer counterparts. While previous research has focused on monolayers, the discovery of various novel properties has sparked interest in multilayers with diverse structures engineered through stacking. These materials are characterized by interactions between layers and exhibit remarkable tunability in their structural, optical, and electronic behaviors depending on stacking order, twist angle, and interlayer coupling. This review provides an overview of ML-TMDs and explores their properties such as electronic band structure, optical responses, ferroelectricity, and anomalous Hall effect. Various synthetic methods employed to fabricate ML-TMDs, including mechanical stacking and chemical vapor deposition techniques, with an emphasis on achieving precise control of the twist angles and layer configurations, are discussed. This study further explores potential applications of ML-TMDs in nanoelectronics, optoelectronics, and quantum devices, where their unique properties can be harnessed for next-generation technologies. The critical role played by these materials in the development of future electronic and quantum devices is highlighted.","PeriodicalId":228,"journal":{"name":"Small","volume":"91 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654173","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}
Xueqiu Chen, Jing-Jing Lv, Limin Zhou, Xiaoruizhuo Lin, Mingming Zhang, Zeqiang Cui, Bingtao Sun, Dan Shi, Yong Lei, Ning Wang, Huile Jin, Haibo Ke, Shun Wang, Shaoan Cheng, Zheng-Jun Wang
Cu-based materials can electrocatalytically reduce CO2 or CO into high-value-added multi-carbon (C2+) products. The features, including morphology, crystal plane, etc., have a great influence on their electrocatalytic performance. Herein, the 3D Cu microbuds (3D Cu MBs) are finely synthesized with enriched grain boundaries by controlling the reaction temperature, time, and pH. The obtained Cu MBs can work as an efficient catalyst for electrocatalytic CO reduction reaction (eCORR) in a flow cell. As compared to the commercial micron Cu, Cu MBs exhibit a significantly higher C2+ product selectivity (≈83% at −0.58 V vs reversible hydrogen electrode-RHE), higher partial current density (410 mA cm−2), and a lower overpotential. The typical 3D hierarchical structure and polycrystalline feature endow the Cu MBs with abundant active grain boundaries for eCORR to form C2+ products. This study offers a new insight into the crystalline-controlled synthesis of 3D Cu catalyst for CO electrolysis.
{"title":"3D Cu Microbuds for Electrocatalytic CO Reduction Reaction","authors":"Xueqiu Chen, Jing-Jing Lv, Limin Zhou, Xiaoruizhuo Lin, Mingming Zhang, Zeqiang Cui, Bingtao Sun, Dan Shi, Yong Lei, Ning Wang, Huile Jin, Haibo Ke, Shun Wang, Shaoan Cheng, Zheng-Jun Wang","doi":"10.1002/smll.202412672","DOIUrl":"https://doi.org/10.1002/smll.202412672","url":null,"abstract":"Cu-based materials can electrocatalytically reduce CO<sub>2</sub> or CO into high-value-added multi-carbon (C<sub>2+</sub>) products. The features, including morphology, crystal plane, etc., have a great influence on their electrocatalytic performance. Herein, the 3D Cu microbuds (3D Cu MBs) are finely synthesized with enriched grain boundaries by controlling the reaction temperature, time, and pH. The obtained Cu MBs can work as an efficient catalyst for electrocatalytic CO reduction reaction (eCORR) in a flow cell. As compared to the commercial micron Cu, Cu MBs exhibit a significantly higher C<sub>2+</sub> product selectivity (≈83% at −0.58 V vs reversible hydrogen electrode-RHE), higher partial current density (410 mA cm<sup>−2</sup>), and a lower overpotential. The typical 3D hierarchical structure and polycrystalline feature endow the Cu MBs with abundant active grain boundaries for eCORR to form C<sub>2+</sub> products. This study offers a new insight into the crystalline-controlled synthesis of 3D Cu catalyst for CO electrolysis.","PeriodicalId":228,"journal":{"name":"Small","volume":"70 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654175","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}
Yixuan Liu, Wenhua Xue, Jian Ye, Ruilong Zhang, Akkammagari Putta Rangappa, Jun Zhao
The photocatalytic conversion of biomass feedstock represents a promising and environmentally friendly strategy for achieving selective transformation and value addition. The slow charge dynamics and sluggish hole transfer in the oxidation reactions severely limit the photocatalytic activity. Here, the heterojunction is fabricated by synthesizing ultra thin ZnIn2S4 nanoflower with spinel CuCo2O4. The internal and interfacial electric fields are successfully constructed, which shows superior 5-hydroxymethylfurfural (HMF) valorization. HMF undergoes severe mineralization when ZnIn2S4 is used as the catalyst, resulting in 0.9% 2,5-diformylfuran (DFF) yield in water, while the ZnIn2S4/CuCo2O4 heterojunction catalyst exhibits 77% DFF selectivity with 88.6% HMF conversion, The cascaded bulk and internal electric fields greatly reduce the oxidation potential of holes and enhance the charge separation efficiency, thus give a remarkable 70-fold increase in DFF yield. This work overcomes the limitations of ZnIn2S4 application for HMF and similar alcohol oxidation reactions that typically require organic solvents, achieving a high DFF evolution rate of 724.9 µmol·g−1·h−1 in water within the first hour of the reaction, surpassing most reports of photocatalytic HMF selective oxidation.
{"title":"Cascade Electric Field in ZnIn2S4/CuCo2O4 Photocatalyst for the Selective Oxidation of Biomass-Derived 5-Hydroxymethylfurfural in Aqueous Solutions","authors":"Yixuan Liu, Wenhua Xue, Jian Ye, Ruilong Zhang, Akkammagari Putta Rangappa, Jun Zhao","doi":"10.1002/smll.202409005","DOIUrl":"https://doi.org/10.1002/smll.202409005","url":null,"abstract":"The photocatalytic conversion of biomass feedstock represents a promising and environmentally friendly strategy for achieving selective transformation and value addition. The slow charge dynamics and sluggish hole transfer in the oxidation reactions severely limit the photocatalytic activity. Here, the heterojunction is fabricated by synthesizing ultra thin ZnIn<sub>2</sub>S<sub>4</sub> nanoflower with spinel CuCo<sub>2</sub>O<sub>4</sub>. The internal and interfacial electric fields are successfully constructed, which shows superior 5-hydroxymethylfurfural (HMF) valorization. HMF undergoes severe mineralization when ZnIn<sub>2</sub>S<sub>4</sub> is used as the catalyst, resulting in 0.9% 2,5-diformylfuran (DFF) yield in water, while the ZnIn<sub>2</sub>S<sub>4</sub>/CuCo<sub>2</sub>O<sub>4</sub> heterojunction catalyst exhibits 77% DFF selectivity with 88.6% HMF conversion, The cascaded bulk and internal electric fields greatly reduce the oxidation potential of holes and enhance the charge separation efficiency, thus give a remarkable 70-fold increase in DFF yield. This work overcomes the limitations of ZnIn<sub>2</sub>S<sub>4</sub> application for HMF and similar alcohol oxidation reactions that typically require organic solvents, achieving a high DFF evolution rate of 724.9 µmol·g<sup>−1</sup>·h<sup>−1</sup> in water within the first hour of the reaction, surpassing most reports of photocatalytic HMF selective oxidation.","PeriodicalId":228,"journal":{"name":"Small","volume":"19 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654207","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 excessive CO2 emissions from human activities severely impact the natural environment and ecosystems. Among the various technologies available, electrocatalytic CO2 reduction is regarded as one of the most promising routes due to its exceptional environmental friendliness and sustainability. Covalent organic frameworks (COFs) are crystalline, porous organic networks that are formed through thermodynamically controlled reversible covalent polymerization of organic linkers via covalent bonding. These materials exhibit high porosity, large surface area, excellent chemical and thermal stability, sustainability, high electron transfer efficiency, and surface functionalization capabilities, making them particularly effective in electrocatalytic CO2 reduction. First, this review briefly introduces the fundamental principles of electrocatalysis and the mechanism of electrocatalytic CO2 reduction. Next, it discusses the composition, structure, and synthesis methods of COF-based materials, as well as their applications in electrocatalytic CO2 reduction. Furthermore, it reviews the research progress in this field from the perspective of different types of COF-based catalysts. Finally, in light of the current research status, the development prospects of COF-based catalysts are explored, providing a reference for the development of more efficient and stable COF electrocatalysts for CO2 reduction.
{"title":"Recent Progress of Covalent Organic Frameworks-Based Materials Used for CO2 Electrocatalytic Reduction: A Review","authors":"Heng-fei Cui, Feng Yang, Cong Liu, Hao-wen Zhu, Ming-yang Liu, Rui-tang Guo","doi":"10.1002/smll.202502867","DOIUrl":"https://doi.org/10.1002/smll.202502867","url":null,"abstract":"The excessive CO<sub>2</sub> emissions from human activities severely impact the natural environment and ecosystems. Among the various technologies available, electrocatalytic CO<sub>2</sub> reduction is regarded as one of the most promising routes due to its exceptional environmental friendliness and sustainability. Covalent organic frameworks (COFs) are crystalline, porous organic networks that are formed through thermodynamically controlled reversible covalent polymerization of organic linkers via covalent bonding. These materials exhibit high porosity, large surface area, excellent chemical and thermal stability, sustainability, high electron transfer efficiency, and surface functionalization capabilities, making them particularly effective in electrocatalytic CO<sub>2</sub> reduction. First, this review briefly introduces the fundamental principles of electrocatalysis and the mechanism of electrocatalytic CO<sub>2</sub> reduction. Next, it discusses the composition, structure, and synthesis methods of COF-based materials, as well as their applications in electrocatalytic CO<sub>2</sub> reduction. Furthermore, it reviews the research progress in this field from the perspective of different types of COF-based catalysts. Finally, in light of the current research status, the development prospects of COF-based catalysts are explored, providing a reference for the development of more efficient and stable COF electrocatalysts for CO<sub>2</sub> reduction.","PeriodicalId":228,"journal":{"name":"Small","volume":"183 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654176","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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