ACS Materials Letters最新文献

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Polymorphism of [Cu15(PhCH2CH2S)13(PPh3)6][BF4]2 and Double-Helical Assembly of [Cu18H(PhCH2CH2S)14(PPh3)6Cl3]: Origin of Two Chiral Nanoclusters with Triple-Helical Core from Intermediates.
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2025-01-02 eCollection Date: 2025-02-03 DOI: 10.1021/acsmaterialslett.4c02148
Abhijit Nag, Abdul Mannan Butt, Moon Young Yang, Praveen B Managutti, Bilal Masood Pirzada, M Infas H Mohideen, Ahmed L Abdelhady, Mohamed Abu Haija, Sharmarke Mohamed, Boris V Merinov, William A Goddard, Ahsanulhaq Qurashi
{"title":"Polymorphism of [Cu<sub>15</sub>(PhCH<sub>2</sub>CH<sub>2</sub>S)<sub>13</sub>(PPh<sub>3</sub>)<sub>6</sub>][BF<sub>4</sub>]<sub>2</sub> and Double-Helical Assembly of [Cu<sub>18</sub>H(PhCH<sub>2</sub>CH<sub>2</sub>S)<sub>14</sub>(PPh<sub>3</sub>)<sub>6</sub>Cl<sub>3</sub>]: Origin of Two Chiral Nanoclusters with Triple-Helical Core from Intermediates.","authors":"Abhijit Nag, Abdul Mannan Butt, Moon Young Yang, Praveen B Managutti, Bilal Masood Pirzada, M Infas H Mohideen, Ahmed L Abdelhady, Mohamed Abu Haija, Sharmarke Mohamed, Boris V Merinov, William A Goddard, Ahsanulhaq Qurashi","doi":"10.1021/acsmaterialslett.4c02148","DOIUrl":"10.1021/acsmaterialslett.4c02148","url":null,"abstract":"<p><p>Here, we report the solvent-induced polymorphism in [Cu<sub>15</sub>(PET)<sub>13</sub>(TPP)<sub>6</sub>][BF<sub>4</sub>]<sub>2</sub>(Cu<sub>15</sub>) (TPP = triphenylphosphine, PET = 2-phenylethanthiol), and double-helical assembly of the [Cu<sub>18</sub>H(PET)<sub>14</sub>(TPP)<sub>6</sub>Cl<sub>3</sub>] (Cu<sub>18</sub>) nanocluster (NC) from reaction intermediates. Both copper NCs have an intrinsically chiral triple-stranded helicate metal core, unlike traditional copper NCs with a polyhedral-based kernel. The chiral structure of Cu<sub>15</sub> resembles an enantiomeric pair in the unit cell. Moreover, Cu<sub>18</sub> has a three-layered 3D chirality of a sandwich constructed of sulfur-bridged copper NCs aligned in a top-middle-down configuration. Furthermore, the Cu<sub>18</sub> NC self-hierarchically assembles into a complex double-stranded helix secondary structure sustained by noncovalent interactions. Electrospray ionization mass spectrometry (ESI-MS), density functional theory (DFT), and X-ray photoelectron spectroscopy (XPS) were utilized to validate the single-crystal X-ray diffraction (SCXRD) data. Overall, this study provides an interesting example of polymorphism, chirality, and hierarchical double-helical assembly of NCs, allowing for extensive understanding of complicated structures at the atomic level.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 2","pages":"442-449"},"PeriodicalIF":9.6,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11795624/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363258","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
Integrating Multiple Functional Moieties toward Environmentally Friendly and Highly Efficient Interfacial Mediator for Rubber/Silica Composites
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2025-01-01 DOI: 10.1021/acsmaterialslett.4c0212710.1021/acsmaterialslett.4c02127
Yeqing Li, Haixin Yang, Shuangjian Yu*, Siwu Wu, Zhenghai Tang, Baochun Guo*, Danling Wang, Huiming Ren, Ming Tian and Liqun Zhang, 
{"title":"Integrating Multiple Functional Moieties toward Environmentally Friendly and Highly Efficient Interfacial Mediator for Rubber/Silica Composites","authors":"Yeqing Li,&nbsp;Haixin Yang,&nbsp;Shuangjian Yu*,&nbsp;Siwu Wu,&nbsp;Zhenghai Tang,&nbsp;Baochun Guo*,&nbsp;Danling Wang,&nbsp;Huiming Ren,&nbsp;Ming Tian and Liqun Zhang,&nbsp;","doi":"10.1021/acsmaterialslett.4c0212710.1021/acsmaterialslett.4c02127","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02127https://doi.org/10.1021/acsmaterialslett.4c02127","url":null,"abstract":"<p >The problems of high volatile organic compound (VOC) emission and low efficiency of silane coupling agents (SCAs) used in the rubber/silica composites for “green tires” have been troubling the rubber industry. A unique silane (MFSi) integrating hydroxyls, tertiary nitrogen, and norbornenyl were prepared by a solvent-free/catalyst-free one-pot method. MFSi can graft onto the rubber chain through a highly efficient norbornenyl/sulfur reaction, while the dangling hydroxyls in MFSi can improve its affinity with silica and tertiary nitrogen has a significant internal catalytic effect on the silanization of silica. As a result, MFSi shows a significantly higher coupling efficiency of silica-filled composites compared to the most widely used SCAs. Consequently, MFSi-modified composites exhibit excellent environmental friendliness, including significantly reduced heat buildup (∼55%) and abrasion loss (∼53%) and VOC emissions (∼42%). We envision that the design of the multifunctional mediator will provide valuable insights into the development of high-performance “green tires” in a more environmentally friendly manner.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 2","pages":"425–432 425–432"},"PeriodicalIF":9.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143087499","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
Old Bottles of New Wines: Dynamic Multimode Color-Tuning Long Afterglow and White Light Emission in Cost-Effective Metal-Organic Frameworks (MOFs)
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-30 DOI: 10.1021/acsmaterialslett.4c0233410.1021/acsmaterialslett.4c02334
Xin-Qi Chen, Shi-Cheng Wang, Meng An, Zhuo Chen and Zheng Wang*, 
{"title":"Old Bottles of New Wines: Dynamic Multimode Color-Tuning Long Afterglow and White Light Emission in Cost-Effective Metal-Organic Frameworks (MOFs)","authors":"Xin-Qi Chen,&nbsp;Shi-Cheng Wang,&nbsp;Meng An,&nbsp;Zhuo Chen and Zheng Wang*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0233410.1021/acsmaterialslett.4c02334","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02334https://doi.org/10.1021/acsmaterialslett.4c02334","url":null,"abstract":"<p >Metal–organic frameworks (MOFs) with long afterglow luminescence (LAL) have gained attention for applications in light-emitting devices and anticounterfeiting. However, developing cost-effective and high-performance dynamic multicolor LAL MOFs remains challenging. Here, the rigid organic ligand 5-fluoronicotinic acid (FL), which incorporates a F atom to form molecular interlocking and inhibit nonradiative transitions, was chosen to self-assemble with MCl<sub>2</sub> (M = Zn and Cd) to fabricate long-lived phosphorescent MOFs. The synthesized MOFs, namely, FLCd, FLZn, and FLCd-DMF, exhibit excitation-dependent luminescence, ranging from blue/cyan to green, with cold white light emissions under specific excitations. Furthermore, all MOFs achieve dynamic color-tuning LAL based on excitation wavelength and temperature. Photoluminescence properties and theoretical calculations indicate that the multicolor LAL arises from the emissions of FL and its aggregation state, while enhanced phosphorescence can be assigned to heavy-atom and interlocking effects, coordination, and noncovalent interactions. Additionally, by leveraging their LAL behavior, these MOFs are applied for encrypting/decrypting information.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 2","pages":"417–424 417–424"},"PeriodicalIF":9.6,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143087025","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
Unveiling the Critical Role of Spatial Organization on Enzymatic Cascade Reactions in a Crystalline Framework with Hierarchical Porosity
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-30 DOI: 10.1021/acsmaterialslett.4c0218510.1021/acsmaterialslett.4c02185
Fanrui Sha, Geunho Han, Kunhuan Liu, Milad Ahmadi Khoshooei, Yongwei Chen, Randall Q. Snurr, Justin M. Notestein and Omar K. Farha*, 
{"title":"Unveiling the Critical Role of Spatial Organization on Enzymatic Cascade Reactions in a Crystalline Framework with Hierarchical Porosity","authors":"Fanrui Sha,&nbsp;Geunho Han,&nbsp;Kunhuan Liu,&nbsp;Milad Ahmadi Khoshooei,&nbsp;Yongwei Chen,&nbsp;Randall Q. Snurr,&nbsp;Justin M. Notestein and Omar K. Farha*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0218510.1021/acsmaterialslett.4c02185","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02185https://doi.org/10.1021/acsmaterialslett.4c02185","url":null,"abstract":"<p >Enzymatic cascades are critical for energy conversion and chemical transformations in living organisms. Their ecofriendly nature and high selectivity in catalysis make them promising candidates for improving chemical transformations in cell-free systems. However, their applications have been limited by their poor stability. Immobilized cascades, which can enhance activity, remain underexplored due to challenges such as ambiguous support structures and difficulties in controlling enzyme distribution. In this work, we employed NU-1510, a novel metal–organic framework (MOF) with a crystalline hierarchical pore structure, to stabilize an enzyme cascade that oxidizes ethanol to acetaldehyde and subsequently to acetic acid. The impact of enzyme spatial organization on the cascade kinetics was further investigated thanks to the crystalline hierarchical pore structure of the MOF host. These findings pave the way for the design of advanced biocatalytic systems with improved efficiency and durability, potentially transforming applications in sustainable chemical manufacturing and energy conversion.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 2","pages":"409–416 409–416"},"PeriodicalIF":9.6,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143087018","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
Reversibly Switchable Topography Enabled by Melting and Crystallization of Melt-Electrowritten Polymer Fibers
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-29 DOI: 10.1021/acsmaterialslett.4c0205710.1021/acsmaterialslett.4c02057
Ilia Sadilov, Gissela Constante, Martin Dulle, Dennis Schönfeld, Thorsten Pretsch and Leonid Ionov*, 
{"title":"Reversibly Switchable Topography Enabled by Melting and Crystallization of Melt-Electrowritten Polymer Fibers","authors":"Ilia Sadilov,&nbsp;Gissela Constante,&nbsp;Martin Dulle,&nbsp;Dennis Schönfeld,&nbsp;Thorsten Pretsch and Leonid Ionov*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0205710.1021/acsmaterialslett.4c02057","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02057https://doi.org/10.1021/acsmaterialslett.4c02057","url":null,"abstract":"<p >We report the fabrication of topographically structured surfaces with reversibly switchable topography by using melt electrowriting (MEW). In particular, MEW was used to produce continuous high aspect ratio lamellae of semicrystalline polyester urethane with a poly(1,10-decylene adipate) soft segment. The switching of topography is achieved by the expansion and contraction of the polymer caused by the melting and crystallization of the soft segment that results in the buckling of lamellae. In the molten stage, lamellae can be buckled in a certain direction by capillary forces caused by water droplets between two lamellae. In addition, the interlamellar distance between neighbors’ lamellae can be managed by water droplets. Finally, we have demonstrated the possibility of creating electrically conductive surfaces with switchable conductivity achieved by the reversible buckling of the lamellae.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 2","pages":"401–408 401–408"},"PeriodicalIF":9.6,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143087083","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
Linker Length Engineering toward Enhanced Photocatalytic Aerobic Oxidation in Benzothiadiazole-Based Covalent Organic Frameworks
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-26 DOI: 10.1021/acsmaterialslett.4c0231510.1021/acsmaterialslett.4c02315
Chao-Qin Han, Ze-Yang Wang, Shuai Sun, Jia-Xin Guo, Xiaoxi Huang and Xiao-Yuan Liu*, 
{"title":"Linker Length Engineering toward Enhanced Photocatalytic Aerobic Oxidation in Benzothiadiazole-Based Covalent Organic Frameworks","authors":"Chao-Qin Han,&nbsp;Ze-Yang Wang,&nbsp;Shuai Sun,&nbsp;Jia-Xin Guo,&nbsp;Xiaoxi Huang and Xiao-Yuan Liu*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0231510.1021/acsmaterialslett.4c02315","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02315https://doi.org/10.1021/acsmaterialslett.4c02315","url":null,"abstract":"<p >The intrinsic structural advantages and tunability of covalent organic frameworks (COFs) have made them promising photocatalysts for various photocatalytic reactions. However, it remains a great challenge to systematically tune the linker lengths and to build a linker-length-dependent structure-performance relationship of COFs-based photocatalysts. Herein, five isoreticular COFs with sql underlying nets have been successfully synthesized using benzothiadiazole-based ditopic aldehydes with varied linker lengths and 1,3,6,8-tetrakis(4-aminophenyl)pyrene as organic building units. The five obtained COFs exhibit significantly different activities toward photocatalytic aerobic oxidation. Remarkably, the COF-containing vinyl group, HIAM-0020, exhibited the best photocatalytic performance with near-unity conversion and selectivity for photocatalytic oxidative benzylamine coupling within 2 h. The experimental and theoretical investigations indicate that HIAM-0020 exhibits faster charge separation ability and lower charge migration resistance compared with the other four COFs. This work represents promising guidance for the rational design and synthesis of COF-based photocatalysts to achieve efficient organic transformation.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 2","pages":"393–400 393–400"},"PeriodicalIF":9.6,"publicationDate":"2024-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086648","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
Shape Memory Vitrimer for Reversible Dry Adhesion Enabled by Multiscale Reprocessing and Shape Fixing
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-26 DOI: 10.1021/acsmaterialslett.4c0235710.1021/acsmaterialslett.4c02357
Agha Aamir Jan, Junhyung Kim, Uhyeon Kim, Seungbeom Kim and Seok Kim*, 
{"title":"Shape Memory Vitrimer for Reversible Dry Adhesion Enabled by Multiscale Reprocessing and Shape Fixing","authors":"Agha Aamir Jan,&nbsp;Junhyung Kim,&nbsp;Uhyeon Kim,&nbsp;Seungbeom Kim and Seok Kim*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0235710.1021/acsmaterialslett.4c02357","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02357https://doi.org/10.1021/acsmaterialslett.4c02357","url":null,"abstract":"<p >Existing shape memory polymer based dry adhesives lack the ability to be reprocessed and thus to form multiple permanent shapes, limiting their adaptability to various arbitrary surfaces. Here, we present a shape memory vitrimer (SMV) based reversible dry adhesive that is reprocessable, relying on transesterification. The SMV possesses a glass transition temperature (<i>T</i><sub>g</sub>) of ∼50 °C and a topology freezing transition temperature (<i>T</i><sub>v</sub>) of ∼100 °C and exhibits a significant drop in storage modulus across <i>T</i><sub>g</sub> and stress relaxation above <i>T</i><sub>v</sub>. Combined with surface microstructuring, these characteristics provide our SMV dry adhesive with excellent adhesion strength (∼1.75 MPa) and reversibility (∼1000) due to the shape memory effect. Such an outstanding adhesive capability is further highlighted by reprocessing the SMV dry adhesive, thus reforming its permanent shape to adapt to an arbitrary adherend shape. Moreover, the SMV can self-weld above <i>T</i><sub>v</sub>, enabling easy repairs and enhancing its versatility for dry adhesive applications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 2","pages":"385–392 385–392"},"PeriodicalIF":9.6,"publicationDate":"2024-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086342","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
Suppressing Nongeminate Charge Recombination Triggers 19.5% Efficiency Bilayer Organic Solar Cells
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-25 DOI: 10.1021/acsmaterialslett.4c0218110.1021/acsmaterialslett.4c02181
Lixing Tan, Zhenmin Zhao, Sein Chung, Jingjing Zhao, Chaofeng Zhu, Kilwon Cho and Zhipeng Kan*, 
{"title":"Suppressing Nongeminate Charge Recombination Triggers 19.5% Efficiency Bilayer Organic Solar Cells","authors":"Lixing Tan,&nbsp;Zhenmin Zhao,&nbsp;Sein Chung,&nbsp;Jingjing Zhao,&nbsp;Chaofeng Zhu,&nbsp;Kilwon Cho and Zhipeng Kan*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0218110.1021/acsmaterialslett.4c02181","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02181https://doi.org/10.1021/acsmaterialslett.4c02181","url":null,"abstract":"<p >Bilayer organic solar cells, composed of a donor and acceptor layer, provide independent optimization of each layer to enhance the photovoltaic performance. However, the power conversion efficiency remains lower than that of bulk heterojunction cells. Herein, we focus on suppressing nongeminate charge recombination by tuning the acceptor layer’s morphology with fullerene derivatives to improve the performance of bilayer organic solar cells. We use the PM6/Y6 derivatives as model systems and incorporate fullerenes such as PC<sub>71</sub>BM into the acceptor layer to enhance aggregation, improve crystallinity, increase electron mobility, and reduce trap density. Consequently, bilayer devices based on PM6/BTP-eC9 and PM6/L8-BO achieved efficiencies of 18.0% and 19.5%, respectively, approaching the performance of bulk heterojunction cells. The improved fill factor results from reduced bimolecular recombination and suppressed trap-assisted recombination, offering insights into optimizing the active layer morphology and designing high-mobility acceptor materials for efficient bilayer organic solar cells.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"376–384 376–384"},"PeriodicalIF":9.6,"publicationDate":"2024-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086228","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
Encapsulating Gold Nanoclusters into Melamine–Formaldehyde Polymer Nanoparticles for Confinement Induced Enhanced Emission toward Ratiometric Sensing and Light-Emitting Diode Fabrication
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-25 DOI: 10.1021/acsmaterialslett.4c0197510.1021/acsmaterialslett.4c01975
Songrui Li, Huifeng Zhang, Zhenzhen Huang, Jiutong Ma and Qiong Jia*, 
{"title":"Encapsulating Gold Nanoclusters into Melamine–Formaldehyde Polymer Nanoparticles for Confinement Induced Enhanced Emission toward Ratiometric Sensing and Light-Emitting Diode Fabrication","authors":"Songrui Li,&nbsp;Huifeng Zhang,&nbsp;Zhenzhen Huang,&nbsp;Jiutong Ma and Qiong Jia*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0197510.1021/acsmaterialslett.4c01975","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01975https://doi.org/10.1021/acsmaterialslett.4c01975","url":null,"abstract":"<p >Low photoluminescence quantum yield (PLQY) has long been one of the key issues that impedes the versatile applications of gold nanoclusters (AuNCs). In this work, melamine–formaldehyde polymer nanoparticles were employed as carriers to encapsulate AuNCs (AuNCs-MF PNPs), which can trigger the confinement induced enhanced emission (CIEE) effect, remarkably enhancing the PLQY more than 25 times from 1.46% (AuNCs) to 36.90% (AuNCs-MF PNPs) and improving the stability toward pH. By simultaneously incorporating AuNCs-MF PNPs and CDs as sensing probes, ratiometric fluorescence detection of H<sub>2</sub>S with improved sensitivity was achieved. To realize the on-site detection of H<sub>2</sub>S, a portable sensing platform based on a smartphone was constructed. Considering the high PLQY of AuNCs-MF PNPs, a light-emitting device (LED) was fabricated based on AuNCs-MF PNPs with favorable characteristics. This work not only provides a novel strategy for preparing AuNCs with high PLQY but also highlights their potential in fluorescence sensing and the field of intelligent luminescence.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"368–375 368–375"},"PeriodicalIF":9.6,"publicationDate":"2024-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086296","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
Efficient Photoredox Co-Upcycling of CO2 and Plastic Waste by Band-Gap-Engineered ZnxCd1–xS Catalyst
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-12-24 DOI: 10.1021/acsmaterialslett.4c0214210.1021/acsmaterialslett.4c02142
Yi Zhang, Ming-Yu Qi, Marco Conte, Zi-Rong Tang* and Yi-Jun Xu*, 
{"title":"Efficient Photoredox Co-Upcycling of CO2 and Plastic Waste by Band-Gap-Engineered ZnxCd1–xS Catalyst","authors":"Yi Zhang,&nbsp;Ming-Yu Qi,&nbsp;Marco Conte,&nbsp;Zi-Rong Tang* and Yi-Jun Xu*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0214210.1021/acsmaterialslett.4c02142","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02142https://doi.org/10.1021/acsmaterialslett.4c02142","url":null,"abstract":"<p >Solar-driven CO<sub>2</sub> reduction combined with plastic waste valorization presents a versatile approach to simultaneously reset misaligned hydrocarbon resources and achieve a carbon-neutral cycle. Herein, we demonstrate a co-upcycling heterogeneous photoredox catalysis for efficient CO<sub>2</sub> reduction to tunable syngas, integrated with polyethylene terephthalate (PET) plastic conversion for accessing acetate, over the spherical band-gap-engineered Zn<sub><i>x</i></sub>Cd<sub>1–<i>x</i></sub>S catalyst. The key to steering the syngas H<sub>2</sub>/CO rate is to modulate the conduction band bottom potentials of the Zn<sub><i>x</i></sub>Cd<sub>1–<i>x</i></sub>S photocatalysts by altering the Zn/Cd ratio, which results in syngas H<sub>2</sub>/CO production over a wide range. Moreover, controlled variations in the molar ratio of Zn/Cd regulate the electron–hole separation capability, thereby endowing Zn<sub>0.8</sub>Cd<sub>0.2</sub>S with the optimum syngas and acetate production rates. The underlying mechanistic origin of such a redox reaction involving CO<sub>2</sub>-assisted PET plastic conversion has been systematically investigated. This win-win cooperative photoredox catalysis offers a tantalizing possibility for co-upcycling of CO<sub>2</sub> and PET into value-added feedstocks.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 1","pages":"359–367 359–367"},"PeriodicalIF":9.6,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086614","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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