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Synergistic Dual Dynamic Bonds in Covalent Adaptable Networks

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CCS Chemistry 2024年第1期6卷 41-56页

作者： Jun Zhao Zhaoming Zhang Chunyu Wang Xuzhou Yan School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai

Covalent adaptable networks(CANs),comprising polymer networks crosslinked by dynamic covalent bonds(DCBs),have garnered considerable attention as sustainable *** the stress relaxation of CANs is essential for controlling their viscoelastic *** unexpected acceleration of stress relaxation has been observed in CANs containing dual dynamic *** dynamic behavior of the second dynamic bonds can accelerate stress relaxation and lower the relaxation activation energy of dual dynamic CANs compared to analogous CANs that rely on only one type of *** findings complement current approaches that utilize catalysts or adjust network *** this minireview,we summarize the synergistic acceleration effects in various CANs containing dual dynamic *** classify these effects based on the second dynamic bonds,including noncovalent bonds,mechanical bonds,and the second *** also discuss the mechanisms behind this ***,we highlight the challenges and offer perspectives on harnessing the synergistic effects of these dual dynamic systems to expand the chemistry and applications of CANs.

关键词： covalent adaptable networks dynamic covalent bonds dynamic materials stress relaxation synergistic effect

Highlights of mainstream solar cell efficiencies in 2023

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frontiers in Energy 2024年第1期18卷 8-15页

作者： Wenzhong SHEN Yixin ZHAO Feng LIU Institute of Solar Energy and Key Laboratory of Artificial Structures and Quantum Control(Ministry of Education)School of Physics and AstronomyShanghai Jiao Tong UniversityShanghai 200240China School of Environmental science and Engineering and Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China School of Chemistry and Chemical Engineering and Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China

This article continues our highlights last two years[1,2]on the highest independently confirmed mainstream(silicon,perovskite,and organic)solar cell efficiencies in *** world record power conversion efficiency(PCE)of the single-junction silicon and perovskite/silicon tandem solar cells has reached over 27%and close to 34%,respectively,in *** have also witnessed the rapid mass-production development of the silicon passivating contact and silicon back contact solar cells,as well as further progress with perovskite solar cells(PSCs).

关键词： perovskite mainstream fir

Strengthening and toughening styrene-butadiene rubber by mechanically interlocked cross-links

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science China Chemistry 2024年第10期67卷 3414-3422页

作者： Yuanhao Wang Li Yang Lin Cheng Jun Zhao Ruixue Bai Wenbin Wang Shaolei Qu Zhaoming Zhang Wei Yu Xuzhou Yan School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Key Laboratory of Electrical Insulation and Thermal AgingShanghai Jiao Tong University

Styrene-butadiene rubber(SBR) is an indispensable material in modern society, and the necessity for enhanced mechanical properties in SBR persists, particularly to withstand the rigors of challenging environmental conditions. To surmount the limitations of conventional cross-linking modes, mechanical bonds stabilized by host-guest recognition are incorporated as the cross-linking points of SBR to form mechanically interlocked networks(MINs). Compared with covalently cross-linked network, the representative MIN exhibits superior mechanical performance in terms of elongation(1392%) and breaking strength(4.6 MPa), whose toughness has surged by 17 times. Dissociation of host-guest recognition and subsequent sliding motion provide an effective energy dissipation mechanism, and the release of hidden length is also beneficial to enhance ***, the introduction of the rotaxane cross-links made the network more pliable and possess damping and elastic properties, which can return to initial state with one minute rest interval. We aspire that this direct introduction method can serve as a blueprint, offering valuable insights for the enhancement of mechanical properties in conventional commercial polymer materials.

关键词： mechanically interlocked molecules host-guest chemistry styrene-butadiene rubber mechanical properties dynamic materials

Chiral liquid crystals based on pillararene and supramolecular self-assembly-induced chirality amplification

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science China Chemistry 2024年第10期67卷 3373-3381页

作者： Bicong Liang Yujie Cheng Xiong Liu Lan Jia Xuehong Wei Qiang Zheng Pi Wang Danyu Xia Xuzhou Yan College of Materials science and Engineering Taiyuan University of Technology Scientific Instrument Center Shanxi University School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong University

Macrocyclic liquid crystals combine the unique property of liquid crystals and excellent supramolecular assembly ability of macrocyclic compounds. It is a significant challenge to make rational use of the advantages of macrocyclic compounds to prepare new macrocyclic mesogens. Pillararenes, a type of macrocycles with rigid pillar-shaped frameworks and easy-tofunctionalize property, are excellent building blocks to fabricate liquid crystal materials. However, the site-selective modification property of pillararene has been rarely exploited to tailor liquid crystal behaviors. Previously reported pillararene-based liquid crystal systems are almost prepared by per-functionalized pillararenes. Herein, we report the regulation of chiral liquid crystal behaviors by different derivatization of pillararene. Lyotropic and thermotropic liquid crystals with different chirality were obtained by self-assembly of pillararene with different numbers of cholesterol groups. The bridge between thermotropic liquid crystal and lyotropic liquid crystal based on pillararene is built. In addition, the chirality of the mesogens can be amplified through supramolecular self-assembly driven by noncovalent interactions. Based on the different liquid crystal behaviors, the optical signal of the pillararene-based chiral liquid crystals was used to fabricate an information encryption system. This work provides a simple strategy to regulate liquid crystal behaviors via pillararene-based mesogens and realizes information encryption through the combination of different types of liquid crystals.

关键词： chiral liquid crystal pillararene self-assembly cholesterol information encryption

Recent advancements and perspectives of fast-charging composite anodes for lithium-ion batteries

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science China Chemistry 2024年

作者： Qinghui Zeng Yongteng Dong Yuanmao Chen Xinyang Yue Zheng Liang frontiers science Center for Transformative molecules Zhang Jiang Institute for Advanced Study Shanghai Jiao Tong University

The escalating demand for fast-charging lithium-ion batteries(LIBs) has mirrored the rapid proliferation and widespread adoption of electric vehicles and portable electronic devices. Nonetheless, the sluggish diffusion kinetics of lithium ions and electrode degradation in conventional graphite-based anodes pose formidable hurdles in achieving optimal fast-charging capabilities for LIBs. To overcome these challenges, the innovative concept of fast-charging composite anodes, a paradigm shift from traditional single-component designs, has emerged as a promising avenue to enhance the overall performance of LIBs under rapid charging conditions. This paper provides a comprehensive review of the recent advancements in fast-charging composite anodes for LIBs, with a pivotal emphasis on the design principles and material selection strategies employed in various composite anode formulations. Furthermore, it outlines the future prospects and research trajectories in this burgeoning field, offering insights into potential breakthroughs and directions for further exploration.

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Synthesis of Polyethylenes with In-Chain Isolated Carbonyls from CO_(2)and Ethylene via a Tandem Photoreduction/Polymerization Protocol

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CCS Chemistry 2024年第6期6卷 1591-1599页

作者： Fulin Zhou Haojie Dai Shan Tang Yongfeng Zhou frontiers science Center for Transformative molecules Shanghai Key Laboratory for Molecular Engineering of Chiral DrugsSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240

Aiming at accessing polyethylene-bearing in-chain degradable functionality,copolymerization of carbon dioxide(CO_(2))with ethylene has long been recognized as a significant but highly challenging ***,most trials have resulted in ethylene homopolymerization because of the endothermic property and high energy barriers of CO_(2)insertion during polymer chain *** we report an unprecedented tandem reaction protocol for the synthesis of polyethylenes with in-chain carbonyls from CO_(2)and ethylene by the combination of photocatalytic CO_(2)reduction and palladium-catalyzed coordination/insertion *** protocol provides an easy way to adjust the carbonyl content(from 0.13 to 12 mol%)and insertion selectivity(up to 99%isolated carbonyls)of the polyethylene copolymers,which enables the polymers tomaintain the main properties of highdensity polyethylene and simultaneously endows them with good *** addition,besides apolar polyethylene copolymers,polar-functionalized polyethylenes with in-chain isolated carbonyls can also be synthesized from CO_(2),ethylene and a polar monomer using the same *** believe our present work sheds new light on the synthesis of degradable polyethylenes by employing CO_(2)as a green carbonyl source.

关键词： carbon dioxide coordination polymerization polyethylene photoreduction photodegradation

Chiral mesostructured hematite with temperature-independent magnetism due to spin confinement

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Nano Research 2024年第3期17卷 2019-2024页

作者： Baiwen Zhang Jing Ai Yingying Duan Te Bai Lu Han Shunai Che School of Physics science and Engineering Tongji UniversityShanghai 200092China School of Chemistry and Chemical Engineering Tongji UniversityShanghai 200092China Wuxi Vocational College of science and Technology Wuxi 214028China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200240China

Hematite(α-Fe_(2)O_(3))is known to undergo conversion from weak ferromagnetic to antiferromagnetic as the temperature decreases below the Morin temperature(TM=250 K)due to spin moment rotation occurring during the Morin transition(MT).Herein,we endowed hematite with mesostructured chirality to maintain weak ferromagnetism without *** mesostructured hematite(CMH)nanoparticles were prepared by a hydrothermal method with glutamic acid(Glu)as the symmetry-breaking *** triangular bipyramidal CMH nanoparticles were composed of helically cleaved nanoflakes with twisted crystal ***-cooled(FC)magnetization measurements showed that the magnetic moments of CMH were stabilized without MT within the temperature range of 10–300 *** loop measurements confirmed the weak ferromagnetism of *** enhanced Dzyaloshinskii–Moriya interaction(DMI)was speculated to be responsible for the temperature-independent weak ferromagnetism,in which the spin configuration would be confined with canted antiferromagnetic coupling due to the mesostructured chirality of CMH.

关键词： hematite chiral mesostructure Dzyaloshinskii–Moriya interaction weak ferromagnetism antiferromagnetic material temperature-independent magnetism

Insight into the mechanism of 5-hydroxymethylfurfural electroreduction to 2,5-bis(hydroxymethyl)furan over Cu anchored N-doped carbon nanosheets

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Nano Research 2024年第9期17卷 7991-7999页

作者： Haoran Wu Xinwei Chen Haishan Xu Runlu Yang Xin Wang Junying Chen Zhenbing Xie Liang Wu Yiyong Mai School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Tangshan Normal UniversityTangshan 063000China

Design of non-noble metal electrocatalysts for biomass conversion to high-value chemicals and understanding the related catalytic mechanisms are of profound significance but have remained a major ***,we developed a novel biomass-derived electrocatalyst(denoted as Cu/NC),featuring with electron-deficient copper nanoparticles anchored on N-doped carbon nanosheets,for the electrochemical reduction of 5-hydroxymethylfurfural(HMF)to 2,5-bis(hydroxymethyl)furan(BHMF,a vital precursor of functional polymers).The optimized Cu/NC electrocatalyst exhibited an excellent performance with high Faradaic efficiency(89.5%)and selectivity(90.8%)of BHMF at a low concentration of HMF(18.1 mM).Even at a very high HMF concentration(108.6 mM),the Faraday efficiency and selectivity of BHMF could still reach 74.8%and 81.1%,*** performance approached those of the reported noble metal-based *** study revealed that the N doping in the Cu/NC catalyst could regulate the electronic structure of Cu,strengthening the adsorption of the HMF carbonyl group,and thus boosting the selectivity of ***,strong electronic metal-support interactions of Cu and the N-doped carbon support optimized the charge transfer rate,thus promoting the dissociation of water to the active hydrogen(H^(*))species and boosting the reaction kinetic rate of H^(*)and HMF.

关键词： biomass 5-hydroxymethylfurfural electrochemical reduction N-doped carbon materials 2,5-bis(hydroxymethyl)furan

Water-Driven Malleable,Weldable and Eco-Friendly Recyclable Carbon Fiber Reinforced Dynamic Composites

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Chinese Journal of Chemistry 2024年第5期42卷 516-522页

作者： Ping Yu Qirui Huang Yi Wang Wan Peng Zichen Jia Haiyue Wang Juanjuan Ma Chunyu Wang Xuzhou Yan School of Environmental and Chemical Engineering Jiangsu Key Laboratory of Function Control Technology for Advanced MaterialsJiangsu Ocean UniversityLianyungangJiangsu222005 China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai200240 China

Traditional carbon fiber-reinforced polymers based on thermoset matrix have been extensively used in the fields of wind turbine blades,automotive sector,and aerospace,among many ***,there is still a major challenge of recycling those polymers due to the high cost and adverse impacts on the *** this work,we apply a polyimine network as matrix,which possess considerable tensile and thermal properties,to prepare the carbon fiber reinforced polyimine materials with trifluoromethyl diphenoxybenzene units(CFRFP)using a prepreg-based compression molding *** CFRFP can be reshaped or reprocessed by heat or with water rapidly,and exhibited multifunction,including welding,chemical recycling,*** unique findings gained from our study will facilitate the manufacturing capability and enrich the types of fiber-reinforced composites.

关键词： Dynamic chemistry Green chemistry Fiber-reinforced composites Fluoropolyimine Welding Reshaping Recycling Renewable resources