GIANT最新文献

{"title":"Influence of activation/deactivation process on surface-initiated atom transfer radical polymerization: An in silico investigation","authors":"Zhongyan Zhang ,&nbsp;Hui Li ,&nbsp;Yuqi Guo ,&nbsp;Yao-Hong Xue ,&nbsp;Hong Liu","doi":"10.1016/j.giant.2024.100345","DOIUrl":"10.1016/j.giant.2024.100345","url":null,"abstract":"<div><div>We propose a simulation approach to explore surface-initiated atom transfer radical polymerization (SI-ATRP), in which how the chain growth is affected by activation/deactivation process could be considered explicitly. Our findings indicate that these activation and deactivation mechanisms provide all polymer chains with equal growth opportunities. This process leads to a significant increase of grafting density while concurrently reducing the dispersity of the grafted chains. The ratio of activated and dormant chains is theoretically proved to eventually reach equilibrated within the activation/deactivation process. The shorter lifetime of activation/deactivation cycle leads to an even equal opportunity and a faster “stop-continue” pace for the growth of all chains. Our study is helpful for better understanding the role of activation/deactivation process in SI-ATRP from a microscopic perspective.</div></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"21 ","pages":"Article 100345"},"PeriodicalIF":5.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142653876","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}

{"title":"Homochiral “8″-shaped nanotoroids assembled from polypeptides","authors":"Ruiqi Jin,&nbsp;Yue Du,&nbsp;Jiaping Lin,&nbsp;Chunhua Cai","doi":"10.1016/j.giant.2024.100343","DOIUrl":"10.1016/j.giant.2024.100343","url":null,"abstract":"<div><div>Figure eight-shaped (“8″-shaped) nanotoroids have been observed in DNA and proteins, however, they are rarely reported in synthetic polymer systems. Reported here is the formation of homochiral “8″-shaped nanotoroids from poly(γ-benzyl glutamate) (PBG) homopolymers. The L-type and D-type PBGs, i.e., PBLG and PBDG respectively, form left-handed and right-handed “8″-shaped chiral nanotoroids. The formation of the nanotoroids is achieved in a two-step route. Nanofibers are first self-assembled by the PBG homopolymers, which, with changing solvent nature, break into short nanofibers and twist into “8″-shaped nanotoroids. In such processes, the pendant phenyl groups of PBGs change from an extended to a contract form, which generates the internal stress driving the transition of nanofibers to “8″-shaped nanotoroids. This work not only enriches the topology and preparation method of nanotoroids, but also enhances our ability in controlling polymer nanostructures.</div></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100343"},"PeriodicalIF":5.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657154","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}

{"title":"Small dop of comonomer, giant shift of dynamics: α-methyl-regulated viscoelasticity of poly(methacrylamide) hydrogels","authors":"Xin Guan ,&nbsp;Zhiheng Zhou ,&nbsp;Xinzhen Fan ,&nbsp;Wenchao Xu ,&nbsp;Yijie Jin ,&nbsp;Chuanzhuang Zhao","doi":"10.1016/j.giant.2024.100342","DOIUrl":"10.1016/j.giant.2024.100342","url":null,"abstract":"<div><div><em>α</em>-Methyl groups play significant roles in the regulation of water molecules within both small molecular systems and bio-macromolecular systems. Systematically studying the influence of <em>α</em>-methyl on the dynamics of water molecules within hydrogel systems is therefore worthwhile. In this study, we prepared a series of hydrogen-bonded (H-bonded) hydrogels with varying densities of <em>α</em>-methyl groups by copolymerizing methacrylamide (MAm) with its <em>α</em>-methyl-absent analogue, acrylamide (Am). Introducing a small amount of Am (≤6 mol%) into the polymer chain resulted in significant shifts in the viscoelasticity of the hydrogels. The hydrogels exhibit a “time-temperature-<em>α</em>-methyl equivalence”, meaning that introduction of <em>α</em>-methyl-absent monomer has effects similar to elevating temperature and prolonging observation time on the dynamic properties. Based on low-field nuclear magnetic resonance spectroscopy and Raman scattering, a “hydrophilic defects-assisted H-bonds dissociation” mechanism is proposed, depicting that the <em>α</em>-methyl-absent monomer can disturb the rearrangement of water molecules surrounding the polymer chain and accelerate chain dissociation. These findings enabled the copolymer hydrogels with functions such as fast self-healing and tunable interface adhesion.</div></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100342"},"PeriodicalIF":5.4,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142418054","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}

{"title":"Binary blends of poly(lactic acid) and poly(methyl methacrylate) for high energy density and charge/discharge efficiency capacitors","authors":"Shuo Zhao ,&nbsp;Le Zhou ,&nbsp;Junshang Zhang,&nbsp;Yang Shen,&nbsp;Ce-Wen Nan","doi":"10.1016/j.giant.2024.100340","DOIUrl":"10.1016/j.giant.2024.100340","url":null,"abstract":"<div><p>Polymer dielectrics are widely used in modern power electronics due to their high flexibility and high breakdown strength. However, the limited energy density of current polymer dielectrics limits their wider applications, and there is an urgent need to develop novel polymer dielectric materials. Poly(lactic acid) (PLA) is favored for biological applications due to its biocompatibility and biodegradability. In general, PLA has three optical isomers, namely poly(L-lactide) (PLLA), poly(D-lactide) (PDLA), and poly(DL-lactide) (PDLLA), but the investigation of their dielectric properties remains limited. In this study, a significant increase in energy storage density and charge/discharge efficiency in poly(methyl methacrylate) (PMMA) was achieved by incorporating isomers of PLA into PMMA. Experimental results indicate that the introduction of PLA creates a phase-separated structure within PMMA, and in particular, the introduction of the crystalline region significantly improved the breakdown strength (<em>E</em>_b). Finally, PLLA/PMMA 50/50 and PDLA/PMMA 50/50 exhibit the discharged energy densities of 8.55 J cm⁻³ and 8.18 J cm⁻³, respectively, with charge/discharge efficiencies of 89.6% and 90.9%. This work enables the achievement of all-organic dielectrics with high energy storage density and high efficiency through the construction of phase-separated structures and demonstrates the great potential of biodegradable polymers in electronic devices.</p></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100340"},"PeriodicalIF":5.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666542524001048/pdfft?md5=5fdaadba5fe8c446d394f5b0099d8249&pid=1-s2.0-S2666542524001048-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142270615","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}

{"title":"The effect of dynamic cross-links and mesogenic groups on the swelling and collapse of polymer gels","authors":"Daniil E. Larin ,&nbsp;Andrey V. Shibaev ,&nbsp;Ch.-Y. Liu ,&nbsp;Alexander V. Emelyanenko","doi":"10.1016/j.giant.2024.100341","DOIUrl":"10.1016/j.giant.2024.100341","url":null,"abstract":"<div><p>The polymer gels containing dynamic cross-links and mesogenic groups are among the key candidates for the development of soft actuators and detectors, displays, sensors and other programmable and self-healing materials. In this article, firstly, the collapse of polymer networks with irreversible cross-links in the presence of a dynamic cross-linker is investigated by means of Flory-type theory. It is shown that, at not a very poor solvent quality (near the theta-conditions), the swelling ratio for a gel containing irreversible and dynamic cross-links is less than for a gel with irreversible cross-links only, whereas at poor or good solvent qualities sizes of these gels are close to each other. The number of dynamic cross-links monotonically increases with worsening the solvent quality. The gel contraction can be also achieved by increasing the dynamic cross-linker concentration, which allows one to change the transition point in a wide range of solvent conditions. Secondly, polymer networks containing irreversible and dynamic cross-links and incorporating mesogenic side groups is studied using the Maier–Saupe theory. With decreasing in the temperature, the continuous transition from a swollen to collapsed state occurs. With further increase in the temperature, the swelling ratio discontinuously decreases and the nematic order parameter sharply increases from zero to a value ​​close to one. By increasing the dynamic cross-linker concentration, the swelling-to-collapse transition and, then, the isotropic-nematic transition are observed. A phase diagram of the gel is constructed and, depending on the dynamic cross-linker concentration and temperature, the swollen gel with the zero nematic order parameter, the collapsed gel with the zero nematic order parameter, and the collapsed gel with the nematic ordering can be formed. A growth of the length of the mesogenic side group leads to an increase in the area of ​​existence of the collapsed gel with the nematic ordering in the phase diagram. The obtained theoretical results are in agreement with corresponding experimental data from the literature.</p></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100341"},"PeriodicalIF":5.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S266654252400105X/pdfft?md5=3f12b4db5dbdfa4da62fa4ae992677ca&pid=1-s2.0-S266654252400105X-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255055","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}

{"title":"Systematic anode engineering enabling universal efficiency improvements in organic solar cells","authors":"Kwok Kiu Tsang ,&nbsp;Han Yu ,&nbsp;Joshua Yuk Lin Lai ,&nbsp;Ho Ming Ng ,&nbsp;Chung Hang Kwok ,&nbsp;Wenzhao Xiong ,&nbsp;Huawei Hu ,&nbsp;He Yan","doi":"10.1016/j.giant.2024.100338","DOIUrl":"10.1016/j.giant.2024.100338","url":null,"abstract":"<div><p>Anode modification and optimization is crucial towards improving performance of organic solar cells (OSCs). PEDOT:PSS is the most common choice as a hole transport layer (HTL) material, but suffers from issues including low conductivity. In this work, three alkyl amine derivatives - methylamine hydrochloride (MA), ethylamine hydrochloride (EA) and propylamine hydrochloride (PA) are doped into the commercially available Al 4083 PEDOT:PSS to form PEDOT:PSS-MA, PEDOT:PSS-EA and PEDOT:PSS-PA, as modified HTLs. All these modified HTLs exhibit improved chemical and electrical properties including work functions (WF), conductivities and charge carrier motilities. The alkyl amine doping shows compatibility in both Small Molecular Acceptors and All-Polymer OSCs. With PEDOT:PSS-MA demonstrates a highest PCE of 18.49 % compared to the 17.84 % of OSC devices prepared with pristine PEDOT:PSS with the PM6:L8-BO system, while PM6:PY-IT all-polymer OSCs improve PCE from 14.53 % to 15.22 %. AFM characterizations reveal that the introduction of the dopants have smoothened the surface morphology of spin-coated HTL films, which contributes towards more efficient charge extraction. In summary, this study not only presents a method of improving OSC efficiencies, but also provides insight and further possible directions towards anode optimization of OSCs.</p></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100338"},"PeriodicalIF":5.4,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666542524001024/pdfft?md5=7cffed61bf70a5c9878f9cd5534aaefe&pid=1-s2.0-S2666542524001024-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142149481","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}

{"title":"Thermal response color-tunable electroluminescent device for real-time visual temperature monitoring","authors":"Xiaohui Sun ,&nbsp;Jiuyue Zhang ,&nbsp;Xu Li ,&nbsp;Xuelei Gong ,&nbsp;Debin Kong ,&nbsp;Linjie Zhi","doi":"10.1016/j.giant.2024.100339","DOIUrl":"10.1016/j.giant.2024.100339","url":null,"abstract":"<div><p>Alternating current electroluminescent (ACEL) devices have attracted tremendous attention due to their significant applications in bioinspired electronics, smart wearables, and human-machine interfaces. However, it still faces limitations in real-time visual temperature sensing. Herein, a universal strategy is established to achieve real-time temperature dynamic visualization by integrating a thermochromic layer through a simple spin coating procedure. Such elaborate integration permits the device to display a wide array of luminous colors and achieve high-contrast color transitions in response to ambient temperature variations. More importantly, a quantitative relationship can be established between the temperatures and the luminous color changes. This advancement not only enhances multi-color emission capabilities but also enables the display of diverse information, marking a significant stride in the development of dynamic temperature sensing in ACEL devices.</p></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100339"},"PeriodicalIF":5.4,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666542524001036/pdfft?md5=f2d65086e3041e0a2e41046b0682031a&pid=1-s2.0-S2666542524001036-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122706","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}

{"title":"Giant molecule acceptors for high performance polymer solar cells","authors":"Hongmei Zhuo ,&nbsp;Beibei Qiu ,&nbsp;Xiaojun Li ,&nbsp;Zhi-Guo Zhang ,&nbsp;Yongfang Li","doi":"10.1016/j.giant.2024.100336","DOIUrl":"10.1016/j.giant.2024.100336","url":null,"abstract":"<div><p>Giant molecule acceptors (GMAs) are composed of two or more narrow bandgap small molecule acceptors (SMAs) subunits connected by conjugated or non-conjugated linking units, which possesses the advantages of the SMAs with broad absorption, appropriate electronic energy levels and fixed molecular weight (with good photovoltaic performance reproducibility), and the polymerized SMAs (PSMAs) with good film-forming property and high morphology stability and photo-stability. So that the GMAs are promising for future commercial application in polymer solar cells (PSCs). Therefore, the GMAs have attracted great attention recently. In this review, we will briefly introduce the development of the narrow bandgap SMAs, especially the A-DA’D-A structured SMAs, and the PSMAs. Then we will focus on the recent research progress of the GMAs, including the synthetic method of GMAs and the effect of number of the SMA subunits on the photovoltaic performance of the GMAs. Finally, we present our perspectives and offer a concise outlook on the further advancement of the GMAs.</p></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100336"},"PeriodicalIF":5.4,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666542524001000/pdfft?md5=10ab1653557cd9ed723c0a165fe256fe&pid=1-s2.0-S2666542524001000-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142087606","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}

{"title":"Recent progress in gel polymer electrolyte for lithium metal batteries","authors":"Changxing Han ,&nbsp;Xiong Shui ,&nbsp;Guansheng Chen ,&nbsp;Gaojie Xu ,&nbsp;Jun Ma ,&nbsp;Shanmu Dong ,&nbsp;Shitao Wang ,&nbsp;Xinhong Zhou ,&nbsp;Zili Cui ,&nbsp;Lixin Qiao ,&nbsp;Guanglei Cui","doi":"10.1016/j.giant.2024.100337","DOIUrl":"10.1016/j.giant.2024.100337","url":null,"abstract":"<div><p>Lithium metal batteries (LMBs) with high energy density have been deemed as one of the promising alternatives to alleviate the “range anxiety” of current electric vehicles based on traditional lithium-ion batteries. However, LMBs using traditional liquid electrolytes (LEs) are always facing serious lithium dendrite growth and electrolyte leakage issues, which could usually cause serious safety concerns. Solid polymer electrolytes (SPEs) with high mechanical stability could suppress the lithium dendrites to some extent, however, they are suffering from low ionic conductivity and inferior interfacial contact with electrodes. Gel polymer electrolytes (GPEs) combining the advantages of traditional LEs and SPEs could be a promising choice to alleviate above issues. In this review, we systematically summarized and clarified very recent progress of various advanced GPEs for LMBs, which is mainly focusing on the advancement of different polymer matrices used for GPE-based LMBs as well as the development of methodologies for the preparation of GPEs. In addition, we also provide a perspective aiming at inspiring new ideas and directions to design reliable GPEs for advancing the performance of LMBs and boosting their practical application.</p></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100337"},"PeriodicalIF":5.4,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666542524001012/pdfft?md5=d1fe0b732e6ae08beaca706f53b1556c&pid=1-s2.0-S2666542524001012-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142097218","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}

{"title":"Backbone engineering and side group manipulation in covalent organic frameworks for overall solar-driven hydrogen peroxide production","authors":"Ying Zhang ,&nbsp;Hangxun Xu","doi":"10.1016/j.giant.2024.100335","DOIUrl":"10.1016/j.giant.2024.100335","url":null,"abstract":"<div><p>Covalent Organic Frameworks (COFs) have emerged as highly promising materials for the photocatalytic production of hydrogen peroxide (H₂O₂) due to their exceptional structural tunability, robust frameworks, and high porosity. The efficient overall photosynthesis of H₂O₂ hinges on the simultaneous occurrence of the oxygen reduction reaction (ORR) and water oxidation reaction (WOR). This review introduces recent progress in developing key approaches such as backbone engineering and the incorporation of side groups to facilitate these critical reaction pathways. For example, innovative COF designs, such as spatially separating redox centers, have demonstrated significant improvements in photocatalytic performance. Moreover, the introduction of thioether-decorated triazine-based COFs and hexavalent triphenylene knots has led to remarkable H₂O₂ production rates. Furthermore, this review also addresses the challenges associated with the practical implementation of COFs, including their stability under operational conditions and the necessity for innovative reactor designs. The future prospects of COFs in sustainable chemical synthesis are also discussed, emphasizing their potential for COFs to revolutionize H₂O₂ production through green and sustainable methodologies. This review aims to provide valuable insights into the design and development of high-performance COF photocatalysts, paving the way for their practical applications in the sustainable production of value-added chemicals.</p></div>","PeriodicalId":34151,"journal":{"name":"GIANT","volume":"20 ","pages":"Article 100335"},"PeriodicalIF":5.4,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666542524000997/pdfft?md5=81435ea98e51b2dffd6205e621840e54&pid=1-s2.0-S2666542524000997-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142077396","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}