ACS Applied Polymer Materials最新文献

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Impact of Alkali Metal Coordination on the Photoluminescence Quantum Efficiency Trend in Hybrid Supramolecular Trimetallic Halides 碱金属配位对混合超分子三金属卤化物光量子效率趋势的影响
IF 7.2 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-22 DOI: 10.1021/acs.chemmater.4c0212810.1021/acs.chemmater.4c02128
Pan Wang, Jiawei Lin, Zhu Guo and Lingling Mao*, 
{"title":"Impact of Alkali Metal Coordination on the Photoluminescence Quantum Efficiency Trend in Hybrid Supramolecular Trimetallic Halides","authors":"Pan Wang,&nbsp;Jiawei Lin,&nbsp;Zhu Guo and Lingling Mao*,&nbsp;","doi":"10.1021/acs.chemmater.4c0212810.1021/acs.chemmater.4c02128","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02128https://doi.org/10.1021/acs.chemmater.4c02128","url":null,"abstract":"<p >Hybrid supramolecular trimetallic halides with a double-shell clathrate structure belong to a type of functional material with complex compositions and wide tunability. The double-shell structure is generally composed of a crown ether molecule sandwiched between different metal halide units. Here, we synthesize six new hybrid trimetallic halides and their solid solutions with the general formula [(<i>A</i>18C6)<sub>3</sub><i>MX</i><sub>4</sub>][<i>BX</i><sub>4</sub>] (where <i>A</i> = K<sup>+</sup>, Rb<sup>+</sup>, Cs<sup>+</sup>; M = Mn<sup>2+</sup> or Mn<sub>1–<i>x</i></sub>Zn<sub><i>x</i><sup>2+</sup></sub>; <i>B</i> = In<sup>3+</sup>; <i>X</i> = Cl<sup>–</sup> or Br<sup>–</sup>), abbreviated as <i>A</i>-<i>M</i>-<i>X</i>. Through the structural analysis of the crystal structure and characterizations of the optical properties of these materials, we have found a direct correlation between the photoluminescence quantum yield (PLQY) and the suitability of the coordination between the <i>A</i>-site metal and the crown ether. Specifically, as the radius of the alkali metal increases (from K to Rb), the PLQY decreases due to poorer suitability. The suitability of the coordination has been analyzed in detail by quantifying the structural parameters (i.e., <i>A</i>–O bond distance, O–<i>A</i>–O bond angle, and distance from <i>A</i> metal to the crown ether center). This trend has been further confirmed via two independent systems using solid solutions through <i>M</i>-site alloying and comparing the chloride and bromide analogs. Surprisingly, a selective coordination mode has surfaced when alloying on the A-site, where the larger alkali metal preferentially coordinates with the connected crown ether instead of the isolated one. This effective approach leads to a wide range of tunability of the PLQY from 21.7 to 95.2% within the total 12 materials. Through further analysis, we have found that the substitution of the <i>A</i>-site metal from K to Cs increases the Mn–<i>X</i> distance, which weakens the crystal field strength of Mn and aligns with the observed trend in PLQY. Our work has further expanded the material space of hybrid trimetallic double-shell clathrates and provides determining insights into controlling the structure and PLQY.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"36 21","pages":"10651–10660 10651–10660"},"PeriodicalIF":7.2,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Nitrogen Defective Engineering of a Metal-Free Carbon Catalyst for Ammonia Electrosynthesis from Nitrate 用于硝酸电合成氨的无金属碳催化剂的氮缺陷工程设计
IF 7.1 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-22 DOI: 10.1021/acssuschemeng.4c0585910.1021/acssuschemeng.4c05859
Shengjun Du, Jun Fang, Minglong Guo, Guangxing Yang, Qiao Zhang, Zhiting Liu and Feng Peng*, 
{"title":"Nitrogen Defective Engineering of a Metal-Free Carbon Catalyst for Ammonia Electrosynthesis from Nitrate","authors":"Shengjun Du,&nbsp;Jun Fang,&nbsp;Minglong Guo,&nbsp;Guangxing Yang,&nbsp;Qiao Zhang,&nbsp;Zhiting Liu and Feng Peng*,&nbsp;","doi":"10.1021/acssuschemeng.4c0585910.1021/acssuschemeng.4c05859","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c05859https://doi.org/10.1021/acssuschemeng.4c05859","url":null,"abstract":"<p >Electrocatalytic nitrate reduction reaction (ENO<sub>3</sub>RR) to NH<sub>3</sub> provides an appealing route to valorize pollutants needed to close the nitrogen cycle. The development of metal-free carbon catalysts with high stability and well-developed active sites for ENO<sub>3</sub>RR is highly desirable, while the role of structural defects (such as vacancies or functional groups) on NH<sub>3</sub> electrosynthesis is not fully understood. Herein, we developed a group of carbon-based catalysts with regulated quaternary-N and N vacancies, and the effect of dual defect sites on the ENO<sub>3</sub>RR to NH<sub>3</sub> process was systematically investigated. The as-prepared NHC-1000 catalyst with atomic-level engineered active sites exhibited a NH<sub>3</sub> Faradaic efficiency of 91.2% associated with a NH<sub>3</sub> yield rate of 2.6 mmol h<sup>–1</sup> g<sup>–1</sup> at –0.5 V (vs RHE), better than most of the reported metal-free carbon electrocatalysts. According to the structure characterization and theoretical calculations, the yielded NH<sub>3</sub> was dependent on the nitrogen defective involved catalytic sites. The quaternary-N moiety facilitated the potential-determining step of *NO protonation to *NHO and further contributed to the formation of *NH<sub>2</sub> intermediates by the synergistic action of N-vacancies, which enhanced the NO<sub>3</sub><sup>–</sup> to NH<sub>3</sub> activity effectively. This work provides a fundamental principle and deeper understanding for designing advanced carbon-based catalysts by defect engineering applied in the ENO<sub>3</sub>RR process effectively.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16320–16328 16320–16328"},"PeriodicalIF":7.1,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571024","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Non-noble Ni@NbOx Catalyst for Selective Hydrodehydroxylation of 5-Hydroxymethylfurfural to 5-Methylfurfural 将 5-羟甲基糠醛选择性加氢羟化为 5-甲基糠醛的非贵金属 Ni@NbOx 催化剂
IF 7.1 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-22 DOI: 10.1021/acssuschemeng.4c0468410.1021/acssuschemeng.4c04684
Ye Liu, Haiyang Yuan, Bin Zhang*, Lei Zhang, Qingling Xu, Minghua Dong, Tianjiao Wang, Xiaomeng Cheng, Haifeng Qi, Zhijuan Zhao, Lihua Chen*, Baolian Su, Buxing Han and Huizhen Liu*, 
{"title":"Non-noble Ni@NbOx Catalyst for Selective Hydrodehydroxylation of 5-Hydroxymethylfurfural to 5-Methylfurfural","authors":"Ye Liu,&nbsp;Haiyang Yuan,&nbsp;Bin Zhang*,&nbsp;Lei Zhang,&nbsp;Qingling Xu,&nbsp;Minghua Dong,&nbsp;Tianjiao Wang,&nbsp;Xiaomeng Cheng,&nbsp;Haifeng Qi,&nbsp;Zhijuan Zhao,&nbsp;Lihua Chen*,&nbsp;Baolian Su,&nbsp;Buxing Han and Huizhen Liu*,&nbsp;","doi":"10.1021/acssuschemeng.4c0468410.1021/acssuschemeng.4c04684","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c04684https://doi.org/10.1021/acssuschemeng.4c04684","url":null,"abstract":"<p >Selective hydrogenation of substrates containing multiple unsaturated bonds (C═C and C═O) is a crucial catalytic process in the production of high-value chemicals. The development of nonprecious metal catalytic systems is of importance for hydrogenation processes due to the high cost and scarcity of noble metals. In this study, we have developed a straightforward and versatile encapsulation technique for the synthesis of Ni@NbO<sub><i>x</i></sub> catalysts, which enables highly selective hydrodehydroxylation of 5-hydroxymethylfurfural (HMF) to 5-methylfurfural (MF) under H<sub>2</sub>. Mechanistic studies revealed that metallic Ni<sup>0</sup> encapsulated within NbO<sub><i>x</i></sub> facilitates hydrogen dissociation through an energy quasi-barrierless process (&lt;0.1 eV), while simultaneously avoiding the adsorption of furan or C═O groups over Ni nanoparticles, therefore enhancing the selective hydrodehydroxylation of HMF to MF. Furthermore, the Ni@NbO<sub><i>x</i></sub> catalyst was tolerant to different conditions for selective hydrogenation, such as crude H<sub>2</sub> containing CO, substrates contaminated with various metal salts, etc.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16202–16211 16202–16211"},"PeriodicalIF":7.1,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Comparison of Lithium Diffusion in Isostructural Ta12MoO33 and Nb12MoO33: Experimental and Computational Insights from Single Crystals 等结构 Ta12MoO33 和 Nb12MoO33 中的锂扩散比较:来自单晶体的实验和计算见解
IF 7.2 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-22 DOI: 10.1021/acs.chemmater.4c0211810.1021/acs.chemmater.4c02118
Md Abdullah Al Muhit, Sean C. Wechsler, Zachary J. L. Bare, CJ Sturgill, Navindra Keerthisinghe, Matthias A. Grasser, Gregory Morrison, Christopher Sutton*, Morgan Stefik* and Hans-Conrad zur Loye*, 
{"title":"Comparison of Lithium Diffusion in Isostructural Ta12MoO33 and Nb12MoO33: Experimental and Computational Insights from Single Crystals","authors":"Md Abdullah Al Muhit,&nbsp;Sean C. Wechsler,&nbsp;Zachary J. L. Bare,&nbsp;CJ Sturgill,&nbsp;Navindra Keerthisinghe,&nbsp;Matthias A. Grasser,&nbsp;Gregory Morrison,&nbsp;Christopher Sutton*,&nbsp;Morgan Stefik* and Hans-Conrad zur Loye*,&nbsp;","doi":"10.1021/acs.chemmater.4c0211810.1021/acs.chemmater.4c02118","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02118https://doi.org/10.1021/acs.chemmater.4c02118","url":null,"abstract":"<p >The demand for fast charging requires high-performance battery materials with improved ionic transport. Wadsley–Roth (WR) structures have garnered attention, where the combination of blocks and shear planes addresses ionic and electronic conductivity, respectively. An improved understanding of structure–property relationships could lead to higher-performance materials. Herein, we report the first single-crystal structures of Nb<sub>12</sub>MoO<sub>33</sub> and Ta<sub>12</sub>MoO<sub>33</sub> that are consistent with other (3 × 4 × ∞) WR phases. The lithiation of Ta<sub>12</sub>MoO<sub>33</sub> is reported to enable an isostructural comparison with Nb<sub>12</sub>MoO<sub>33</sub>. These two compounds have similar unit cell volumes and atomic radii, where the Ta<sub>12</sub>MoO<sub>33</sub> unit cell is 0.2 vol % smaller. Despite the similarities in structure, the lithiation capacities, voltage windows, C rate-dependent capacities, and ionic diffusivities are distinctly different. These experimental trends align well with density functional theory calculations showing (1) a lower activation energy for Li transport within Ta<sub>12</sub>MoO<sub>33</sub> consistent with its measured 1.5–4.9-fold higher diffusion coefficients (lithiation) and (2) an ∼25% greater measured lithiation stoichiometry for Nb<sub>12</sub>MoO<sub>33</sub>, which is attributed to the calculated smaller octahedral distortions (compared to Ta<sub>12</sub>MoO<sub>33</sub>). These findings reveal that smaller channels in Ta<sub>12</sub>MoO<sub>33</sub> stabilize the transition state with 5-fold coordination, which both decreases the activation energy for diffusion and limits the extent of lithiation. Such structure–property trends help in the search for next-generation battery materials.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"36 21","pages":"10626–10639 10626–10639"},"PeriodicalIF":7.2,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608763","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Fine-Tuning of Acidity in Hierarchical Zeolites for the Efficient Prins Cyclization Yielding Florol 微调分层沸石中的酸度以实现高效的普林斯环化反应,产生弗洛里酚
IF 7.1 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-22 DOI: 10.1021/acssuschemeng.4c0553510.1021/acssuschemeng.4c05535
Julián E. Sánchez-Velandia, Mykhailo Kurmach, Oleksiy Shvets, Hermenegildo Garcia Baldoví, Eduardo García-Verdugo, Dmitry Yu. Murzin* and Nataliya Shcherban*, 
{"title":"Fine-Tuning of Acidity in Hierarchical Zeolites for the Efficient Prins Cyclization Yielding Florol","authors":"Julián E. Sánchez-Velandia,&nbsp;Mykhailo Kurmach,&nbsp;Oleksiy Shvets,&nbsp;Hermenegildo Garcia Baldoví,&nbsp;Eduardo García-Verdugo,&nbsp;Dmitry Yu. Murzin* and Nataliya Shcherban*,&nbsp;","doi":"10.1021/acssuschemeng.4c0553510.1021/acssuschemeng.4c05535","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c05535https://doi.org/10.1021/acssuschemeng.4c05535","url":null,"abstract":"<p >In this contribution, several hierarchical zeolites comprising mainly Brønsted acid sites with different morphologies (nanosheets, nanoparticles, nanorods) were synthesized and applied to the efficient synthesis of the perfume Florol (2-isobutyl-4-methyl-tetrahydro-2H-pyran-4-ol) via Prins cyclization of isoprenol and isovaraldehyde. Tuning the acidity in a zeolite was done by either incorporating metal centers or changing the initial composition and crystallization time. Furthermore, the interplay among the pore structure, specific mesoporosity, and accessibility of acidic sites is crucial for optimizing Florol synthesis. Strong Brønsted acid sites enhance the formation of the dehydration products, while mild-acidic Brønsted acid sites with a medium strength of accessible acid sites improve the formation of Florol. A maximum Florol yield of ca. 80% was achieved with Al-MFI and Al-FER (only 30 min) with typical nanosheet (nsh) morphology; in addition, values of TOF in the order of 1121 and 2655 h<sup>–1</sup>, respectively, were also achieved. Al-FER-nsh showed itself to be robust, because it can be reused several times without any apparent loss of its catalytic activity. Finally, different green chemistry parameters were also applied to the studied zeolites in the synthesis of Florol, suggesting the high efficiency of the best catalyst (Al-MFI-nsh).</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16283–16296 16283–16296"},"PeriodicalIF":7.1,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571115","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Extended Toolboxes Enable Efficient Biosynthesis of Multiple Products from CO2 in Fast-Growing Synechococcus sp. PCC 11901 扩展工具箱使快速生长的 Synechococcus sp. PCC 11901 能够从二氧化碳中高效合成多种产品
IF 7.1 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-22 DOI: 10.1021/acssuschemeng.4c0449710.1021/acssuschemeng.4c04497
Tong Zhang, Shubin Li, Lei Chen, Weiwen Zhang* and Tao Sun*, 
{"title":"Extended Toolboxes Enable Efficient Biosynthesis of Multiple Products from CO2 in Fast-Growing Synechococcus sp. PCC 11901","authors":"Tong Zhang,&nbsp;Shubin Li,&nbsp;Lei Chen,&nbsp;Weiwen Zhang* and Tao Sun*,&nbsp;","doi":"10.1021/acssuschemeng.4c0449710.1021/acssuschemeng.4c04497","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c04497https://doi.org/10.1021/acssuschemeng.4c04497","url":null,"abstract":"<p >Cyanobacteria are known to be photoautotrophic cell factories capable of converting CO<sub>2</sub> into valuable chemicals. The newly discovered marine cyanobacterium <i>Synechococcus</i> sp. PCC 11901 (hereafter PCC 11901) offers several advantages like rapid growth, high biomass, and high salinity tolerance, representing a promising chassis. To promote its application, we developed genetic toolboxes applicable to PCC 11901 in this study. First, a cobalamin (V<sub>B12</sub>)-independent chassis was constructed, allowing for cheaper cultivation. Second, genome copy numbers and transformation methods were, respectively, measured and optimized. Then, 14 neutral sites were identified and characterized within the genome PCC 11901, providing locations for genetic integration of exogenous cassettes. Subsequently, promoter libraries were developed, reaching an expression range of approximately 800 folds for constitutive promoters and an induction fold of up to approximately 400 for inducible promotors, respectively. As a proof of concept, natural production of the total lipid and phycocyanin was investigated using V<sub>B12</sub>-independent chassis, which realized an increase of 14.91% with lipid content compared with that of the wild-type strain. Further, we engineered the synthetic pathways of glucosylglycerol (GG) into PCC 11901 using the established toolboxes, reaching 590.41 ± 21.48 mg/L for GG production and self-sedimentation in photoreactors with the highest OD<sub>750 nm</sub> at 17.57 ± 0.77. Finally, the GG-producing strain grew well in seawater, reaching 324.50 ± 5.34 mg/L in shaking flask, which provided new strategies for cyanobacteria cultivation and production. Our work here made it possible to develop the fast-growing PCC 11901 as efficient carbon-neutral cell factory in the future.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16186–16201 16186–16201"},"PeriodicalIF":7.1,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Toward Sustainable Adhesives with Biodegradability, Scalability, and Removability: Poly(butylene succinate)-Based Hot-Melt Adhesives 实现具有生物降解性、可扩展性和可去除性的可持续粘合剂:聚丁二酸丁二醇酯热熔胶
IF 7.1 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-21 DOI: 10.1021/acssuschemeng.4c0323410.1021/acssuschemeng.4c03234
Kwang-Hyun Ryu, Ji-Hyun Cho, Tae-Hyung Lee, Hoon Kim, Gi-Yeon Han, Jong-Ho Back* and Hyun-Joong Kim*, 
{"title":"Toward Sustainable Adhesives with Biodegradability, Scalability, and Removability: Poly(butylene succinate)-Based Hot-Melt Adhesives","authors":"Kwang-Hyun Ryu,&nbsp;Ji-Hyun Cho,&nbsp;Tae-Hyung Lee,&nbsp;Hoon Kim,&nbsp;Gi-Yeon Han,&nbsp;Jong-Ho Back* and Hyun-Joong Kim*,&nbsp;","doi":"10.1021/acssuschemeng.4c0323410.1021/acssuschemeng.4c03234","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c03234https://doi.org/10.1021/acssuschemeng.4c03234","url":null,"abstract":"<p >Previous studies aiming to achieve sustainability in adhesive materials, primarily focused on the integration of bioderived or biodegradable components. However, existing sustainable adhesives often prioritize permanent adhesion over removability, which limits their recyclability. Herein, we introduce an innovative approach for producing scalable, biodegradable, and removable hot-melt adhesives, offering sustainability. Polybutylene succinate (PBS) was selected as the base polymer because of its excellent melt processability, biodegradability, and commercial availability. To impart adhesiveness, three biomass-derived tackifiers were incorporated; basic rosin, disproportionated rosin, and rosin ester. The use of a twin-screw extruder enabled the efficient mixing of the base polymer and tackifiers for large-scale production at the kilogram scale. Our investigation revealed that basic rosin exhibited optimal compatibility and wettability, which were attributed to its high acid value. The high acid value promoted rapid crystallization and minimized crystal defects. A correlation between the crystallization behavior and adhesion strength was also established, identifying the optimal composition. The optimal composition yields a satisfactory adhesion strength (2.5 N/25 mm) that makes it suitable for removable or repositionable adhesives. Additionally, our optimized adhesive exhibited sufficient biodegradability and was completely decomposed by lipase within 21 d, which has not been observed in previous sustainable hot-melt adhesive studies. This study provides a practical pathway for enhancing adhesive sustainability with the potential for further advancements in tailoring the adhesion strength for diverse applications in future research.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16165–16174 16165–16174"},"PeriodicalIF":7.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Renewables-Based Routes to Paracetamol: A Green Chemistry Analysis 基于可再生能源的扑热息痛生产工艺:绿色化学分析
IF 7.1 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-21 DOI: 10.1021/acssuschemeng.4c0535310.1021/acssuschemeng.4c05353
Jimin Park, Caria Evans, Jacob Maier, Marta Hatzell, Stefan France, Carsten Sievers and Andreas S. Bommarius*, 
{"title":"Renewables-Based Routes to Paracetamol: A Green Chemistry Analysis","authors":"Jimin Park,&nbsp;Caria Evans,&nbsp;Jacob Maier,&nbsp;Marta Hatzell,&nbsp;Stefan France,&nbsp;Carsten Sievers and Andreas S. Bommarius*,&nbsp;","doi":"10.1021/acssuschemeng.4c0535310.1021/acssuschemeng.4c05353","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c05353https://doi.org/10.1021/acssuschemeng.4c05353","url":null,"abstract":"<p >Three potential routes for paracetamol synthesis from renewable phenol feedstock were examined and compared to each other and existing industrial routes with respect to Green Chemistry metrics and industrial viability. The routes tested were the acetamidation of hydroquinone, the imination and reduction of benzoquinone, and the hydrogenation of 4-nitrophenol. The hydroquinone and benzoquinone routes suffered from poor conversion and selectivity. The 4-nitrophenol route achieved good conversion, yield, and Green Chemistry metrics and is the most industrially viable of the three routes. When compared to existing routes, the 4-nitrophenol route is comparable or superior in terms of reactor metrics, Green Chemistry considerations, and raw material costs.</p><p >This paper suggests sustainable and renewable routes for paracetamol synthesis through a rigorous Green Chemistry analysis.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16271–16282 16271–16282"},"PeriodicalIF":7.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acssuschemeng.4c05353","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Unlocking the Potential of Dolomite for Developing More Sustainable Cementitious Materials through Partial Calcination 通过部分煅烧释放白云石的潜力,开发更具可持续性的水泥基材料
IF 7.1 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-21 DOI: 10.1021/acssuschemeng.4c0648610.1021/acssuschemeng.4c06486
Yukun Qin, Xiong Qian*, Yong Tao, Chuanlin Hu* and Fazhou Wang, 
{"title":"Unlocking the Potential of Dolomite for Developing More Sustainable Cementitious Materials through Partial Calcination","authors":"Yukun Qin,&nbsp;Xiong Qian*,&nbsp;Yong Tao,&nbsp;Chuanlin Hu* and Fazhou Wang,&nbsp;","doi":"10.1021/acssuschemeng.4c0648610.1021/acssuschemeng.4c06486","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06486https://doi.org/10.1021/acssuschemeng.4c06486","url":null,"abstract":"<p >Waste dolomite powder, a widely available industrial byproduct, has recently gained attention as a potential supplementary cementitious material. However, its inert reactivity challenges its potential for substantial cement replacement. This study explores the effectiveness of partially calcined dolomite (PCD) integrated with calcined clay for a high cement substitution level. A novel partial calcination method is introduced to optimize the decomposition of MgCO<sub>3</sub> and CaCO<sub>3</sub> to produce a core–shell structure with a highly reactive external CaO/MgO layer and a dense internal core of CaCO<sub>3</sub> and MgO. This configuration significantly enhances the formation of calcium silicate hydrate gels and carboaluminate phases, improving the overall strength of the material by over 90% at both 7 and 28 days compared to the sample with uncalcined dolomite. Additionally, the formulation of the proposed materials reduces CO<sub>2</sub> emission by 43% and energy consumption by 47% without sacrificing compressive strength. This innovative calcination technique broadens the application of waste dolomite in the development of sustainable cementitious materials.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16378–16387 16378–16387"},"PeriodicalIF":7.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571197","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Visible Light Induced Synthesis of 2-Benzoxazolecarboxamides Promoted by a Conjugated Microporous Polymer 共轭微孔聚合物促进 2-苯并恶唑羧酰胺的可见光诱导合成
IF 7.1 2区 化学
ACS Applied Polymer Materials Pub Date : 2024-10-21 DOI: 10.1021/acssuschemeng.4c0527510.1021/acssuschemeng.4c05275
Yujie Zhang, Rui Wang, Cuifen Lu, Chao Ma, Feiyi Wang, Guichun Yang, Yuexing Zhang* and Junqi Nie*, 
{"title":"Visible Light Induced Synthesis of 2-Benzoxazolecarboxamides Promoted by a Conjugated Microporous Polymer","authors":"Yujie Zhang,&nbsp;Rui Wang,&nbsp;Cuifen Lu,&nbsp;Chao Ma,&nbsp;Feiyi Wang,&nbsp;Guichun Yang,&nbsp;Yuexing Zhang* and Junqi Nie*,&nbsp;","doi":"10.1021/acssuschemeng.4c0527510.1021/acssuschemeng.4c05275","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c05275https://doi.org/10.1021/acssuschemeng.4c05275","url":null,"abstract":"<p >A new and effective protocol driven by visible light has been introduced for the first time to synthesize 2-benzoxazolecarboxamides from benzoxazinones and amines in the presence of a conjugated microporous polymer, PATP. The reaction produced a variety of 2-benzoxazolecarboxamides in moderate to good yields while demonstrating excellent functional group tolerance under mild conditions. In comparison with transition metal complexes or organic dye molecules, PATP exhibited superior catalytic activity due to its extended π-conjugation system, porous structure, and electronic donor–acceptor (D-A) characteristics. Moreover, the polymer PATP showed consistent recyclability without any significant loss of photocatalytic efficiency after recovery.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16239–16248 16239–16248"},"PeriodicalIF":7.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571204","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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