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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Molecularly-regulating oxygen-containing functional groups of ramie activated carbon for high-performance supercapacitors

Zhenyu Chen,Yuyang Chen,Qing Wang,Ting Yang,Qitian Luo,Kai Gu,Weiqing Yang

Effectively managing oxygen-containing functional groups (OCFGs) within activated carbon and methodically elucidating their intricate types and proportions are essential for considerably improving the electrochemical performance of carbon-based supercapacitors . Herein, we designed a ZnCl 2 -based molecular regulation strategy to introduce OCFGs into ramie-activated carbon (RAC), managing different OCFGs and revealing their structure–activity relationship with electrochemical performance. Thus, this regulated RAC, with a 3.5-fold enhancement in advantageous OCFGs (a-OCFGs: C O and COO), exhibits a supreme specific capacitance of 286.4F g −1 at 1 A/g and an excellent capacitance retention rate of 89.7 % at 20 A/g in an aqueous electrolyte, considerably surpassing that of nonregulated RAC (212.0F g −1 and 81.9 %). This confirms that a-OCFGs provide ample ion-storage accommodation and suppress solvent electronic oxidation, thereby enhancing electrochemical performance. Furthermore, its electrochemical performance is competitive with that of the commercial YP-50F (129.2F g −1 at 1 A/g). Therefore, this work not only highlights the contributions of specific OCFGs to high electrochemical performance but also designs a promising commercial electrode material to meet the demands of OCFGs-adequate carbon-based energy storage devices.

研究领域: 材料科学 · 能源存储
✓ 已验证 DOI PubMed 高影响因子
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MACROMOLECULES · 2024 · IF 5.1

Methyl Matters: Molecular Regulation of the Soft-to-Rigid Transition of Shape Memory Hydrogels for Programmable Deformation

Zhiye Yuan,Yijie Jin,Yu Wu,Xinjun Wu,Nan Hai,Jianlei Lu,Chuanzhuang Zhao,Jiawei Zhang

The properties of intelligent polymeric materials are essentially determined by their chemical structures. Shape memory hydrogels that utilize hydrophobic aggregation at elevated temperatures to stabilize temporary shapes, the association of polymer networks is similar to that of thermoresponsive polymers. To realize a precise control on the shape memory function of these materials and broaden their practical applications, it is essential to build up a structure–property relationship on a molecular level. In this study, we fabricated a series of poly(acrylic acid–methacrylic acid)/Ca(CH3COO)2 shape memory hydrogels with cooling-induced shape transformation behavior. The results showed that the incorporation of α-methyl groups would restrict the hydrophobic aggregation of hydrogel networks, and the soft-to-stiff transition temperature of the hydrogels would shift to elevated temperatures with the increasing density of α-methyl groups. Therefore, the shape recovery process could be regulated by adjusting the association degree of the polymer networks. Finally, the hydrogels were explored as smart capsules with sequential drug delivery capacity and as dredging devices capable of removing thrombus. This study reveals the influence of α-methyl groups on the association dynamics of the poly(acrylic acid–methacrylic acid)/Ca(CH3COO)2 hydrogels, which would promote the design of novel shape memory polymers guided by the relationship between chemical structure and properties.

研究领域: 材料科学 · 生物医学工程
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Environmentally adaptive self-healing hydrogels via multiscale control of water molecules for human-machine interaction

Liping Li,Yang Yang,Wanhui Shi,Yunzhen Chang,Ying Zhang,Wenjing Hou,Sheng Zhu,Gaoyi Han

Self-healing hydrogels can autonomously restore their structural integrity and functionality after injury. However, their self-repair capability is often compromised by water evaporation at high temperatures (> 30 °C) or crystallization at cryogenic conditions (< −20 °C). Here, we introduce a “Li + -hydration-coordination synergistic water-locking” strategy, which immobilizes water molecules within the hydrogel network via water-locking structures formed by a robust hydration shell ([Li(H 2 O) 4 ] + ) and polymer-ionic-water complexes ([Li(CO-PAM)(H 2 O) 4 ] + ). Under this water-locking mode, the Li + -hydrogels maintain their softness even under harsh enviromental conditions, which facilitates the dynamic reconfiguration of self-healing bonds within the polymer network. As a result, the healed Li + -hydrogels exhibit a stretchability/tensile strength of up to 780 %/30 kPa, 1024 %/193 kPa, and 620 %/525 kPa at −60 °C, 25 °C, and 80 °C, corresponding to healing efficiencies of 75 %, 98 %, and 60 %, respectively. Additionally, it also demonstrates wide strain-sensing range (0.1 %–600 %), rapid response time (80 ms) and excellent cycle stability (2000 cycles), which can be successfully employed in human-machine interaction. This strategy establishes a design paradigm for environmentally adaptive composite materials through multiscale control of ion-mediated water molecules.

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Energy Storage Materials · 2024 · IF 18.9

Synergistic interaction between amphiphilic ion additive groups for stable long-life zinc ion batteries

Qiaoyi Yan,Zhengqiang Hu,Zhengzheng Liu,Feng Wu,Yi Zhao,Renjie Chen,Li Li

The uneven deposition of zinc and hydrogen generation at the zinc anode interface constitute major impediments to the lifespan of aqueous zinc-ion batteries. Herein, an amphoteric ion additive, choline phosphate (CP), is proposed to stabilize the battery anode interface. The remarkable interplay between choline ions and phosphate groups assumes a pivotal role in homogenizing zinc ion deposition and regulating the behavior of free water molecules. Due to the negative electric field adsorption on the surface of the zinc anode, the positively charged choline ions will be adsorbed on its surface preferentially and prevent the approach of water molecules. The phosphate group interacts strongly with the zinc ion, permeating the solvated structure of these ions, regulating zinc ion flux, and immobilizing free water molecules through hydrogen bonding to impede unwanted side reactions. In summary, using CP additives yields a profound enhancement in enabling significantly extended cycle lifespans of both Zn//Zn symmetric batteries and LiFePO 4 full batteries.

研究领域: 电化学 · 能源材料 · 电极界面工程 · 储能技术 · 电池化学
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Nanoscale · 2025 ·Vol. 17 ·期 38 ·22122-22133 · IF 5.1

Rigid support–molecular regulation–interface reinforcement synergistic strategy enables PEO-based electrolytes for solid-state lithium batteries

Yingtai Zhao,Xiangping Feng,Xin Sun,Lei Zhang,Zhishuang Song,Jinzhu Zhao,Zhiyuan Wang,Runguo Zheng,Hongyu Sun,Yanguo Liu

Poly(ethylene oxide) (PEO)-based solid polymer electrolytes have broad application prospects due to their flexibility, high lithium salt solubility, and low cost. However, low ionic conductivity, low Li+ transference number, poor electrochemical stability, and inadequate mechanical strength restrict their application in solid-state lithium batteries (SSLBs). Herein, a composite solid-state electrolyte (CSE), PEO@GFC-15, is prepared using a simple and scalable solution casting method, incorporating glass fiber cloth (GFC) and Li6.4Al0.1La3Zr1.7Ta0.3O12 (LALZTO) particles. LALZTO can enhance Li+ transport kinetics by increasing the amorphous region, constructing a Li–O–C dynamic coordination network, and providing more free Li+. It can also promote the decomposition of lithium salt to generate abundant LiF and fix TFSI−, enhancing interface stability, with the oxidation potential increasing to 5.2 V. The high elastic modulus of GFC and the strong hydrogen bond network endow PEO@GFC-15 with good flexibility. Additionally, the three-dimensional rigid network and non-flammable inorganic LALZTO particles improve its thermal stability. Therefore, the Li plating/stripping stability and electrochemical performance of SSLBs are effectively enhanced by the rigid support–molecular regulation–interface reinforcement synergistic modification strategy. This work provides practical insights for the development of high-performance SSLBs.

研究领域: 材料科学 · 电化学 · 高分子化学 · 能源存储 · 固态电池 · 界面科学 · 无机非金属材料
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Polystyrene microplastics enhanced the effect of PFOA on Chlorella sorokiniana: Perspective from the cellular and molecular levels

Zhilin Zhao,Xiaoying Zheng,Zongshuo Han,Yue Li,Haidong He,Tao Lin,Hang Xu

Microplastics (MPs) commonly coexist with other contaminants and alter their toxicity. Perfluorooctanoic acid (PFOA), an emerging pollutant, may interact with MPs but remain largely unknown about the joint toxicity of PFOA and MPs. Hence, this research explored the single and joint effects of PFOA and polystyrene microplastics (PS-MPs) on microalgae ( Chlorella sorokiniana ) at the cellular and molecular levels. Results demonstrated that PS-MPs increased PFOA bioavailability by altering cell membrane permeability, thus aggravating biotoxicity (synergistic effect). Meanwhile, the defense mechanisms (antioxidant system modulation and extracellular polymeric substances secretion) of Chlorella sorokiniana were activated to alleviate toxicity. Additionally, transcriptomic analysis illustrated that co-exposure had more differential expression genes (DEGs; 4379 DEGs) than single-exposure (PFOA: 2533 DEGs; PS-MPs: 492 DEGs), which were mainly distributed in the GO terms associated with the membrane composition and antioxidant system. The molecular regulatory network further revealed that PS-MPs and PFOA primarily regulated the response mechanisms of Chlorella sorokiniana by altering the ribosome biogenesis, photosynthesis, citrate cycle, oxidative stress , and antioxidant system (antioxidant enzyme, glutathione-ascorbate cycle). These findings elucidated that PS-MPs enhanced the effect of PFOA, providing new insights into the influences of MPs and PFOA on algae and the risk assessment of multiple contaminants. Environmental implication MPs and PFAS, emerging contaminants , are difficult to degrade and pose a non-negligible threat to organisms. Co-pollution of MPs and PFAS is ubiquitous in the aquatic environment, while risks of co-existence to organisms remain unknown. The present study revealed the toxicity and defense mechanisms of microalgae exposure to PS-MPs and PFOA from cellular and molecular levels. According to biochemical and transcriptomic analyses, PS-MPs increased PFOA bioavailability and enhanced the effect of PFOA on Chlorella sorokiniana , showing a synergistic effect. This research provides a basis for assessing the eco-environmental risks of MPs and PFAS.

CAS / MDL: 335-67-1
研究领域: 环境科学 · 毒理学 · 分子生物学 · 生态学
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Molecular Catalysis · 2023 · IF 4.6

A metal–free porous organic polymer with high CO2 adsorption for robust aqueous CO2 photoreduction via molecular regulation

Xinyue Hong,Youting Fang,Duobin Chao

Development of photocatalysts with both high CO 2 adsorption capacity and robust CO 2 reduction performance is promising toward carbon capture and utilization (CCU). Herein, a porous organic polymer (POP) based on molecular monomers 1,2,3,5–Tetrakis(carbazol–9–yl)–4,6–dicyanobenzene (4CzIPN) and 9–(4–([2,2′:6′,2′'–terpyridin]–4′–yl)phenyl)–9H–carbazole (CzTPY) has been prepared for metal–free photocatalytic reduction of CO 2 to CO with 94.7% selectivity in 100% aqueous medium. The POP displays a yield of CO up to 265.7 mmol g –1 , which is among the highest yields for POPs–based photocatalytic systems. More importantly, the POP also shows a high CO 2 uptake of 109.1 cm 3 g –1 (21.4 wt%) at 273 K and 1 atm. External photosensitizers or catalysts are not required in this photocatalytic system. Mechanistic studies indicate the introduction of CzTPY improved the electron transfer and charge separation. These results show a feasible way to construct POP–based photocatalysts not only capturing CO 2 efficiently but also catalyzing CO 2 reduction with a high yield by rational regulation of molecular monomers.

研究领域: 化学 · 材料科学 · 环境科学 · 能源科学
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Advanced Energy Materials · 2023 ·Vol. 13 ·期 10 ·2203547 · IF 27.8

Enabling All-Solid-State Li Metal Batteries Operated at 30 °C by Molecular Regulation of Polymer Electrolyte

Ying Wei,Te-Huan Liu,Wenjiang Zhou,Hang Cheng,Xueting Liu,Jia Kong,Yue Shen,Henghui Xu,Yunhui Huang

The low ionic conductivity of poly(ethylene oxide) (PEO)-based polymer electrolytes at room temperature and the undesired lithium-dendrite growth at Li|PEO interface impede their further application. Herein, a PEO polymer is regulated at the molecular level through a copper ion (Cu 2+ ) coordination effect with both PEO and Li salts to achieve a high Li + conductivity of 0.2 mS cm −1 and a transference number of 0.42 at 30 °C. Moreover, the Cu-coordinated PEO electrolyte is neither sticky nor hygroscopic because the hydrophilic oxygen groups in PEO are terminated by Cu ions. Furthermore, the in situ formed F/Li-rich inorganic layer induced by CuF 2 additive accelerates Li + transport kinetics and enables uniform Li + deposition during Li plating/stripping. As a result, the Cu 2+ -coordinated PEO electrolytes deliver a high critical current density of 1.5 mA cm −2 at 30 °C. An all-solid-state Li-LiNi 0.83 Co 0.12 Mn 0.05 O 2 (NCM83) battery with such a copper coordinated PEO electrolyte exhibits a long cycle life over 500 cycles with a capacity retention of 71% under 0.6 C at 30 °C. When the mass loading increases to a record high of 7 mg cm −2 , the Li-NCM83 cell delivers a high areal capacity of 1.07 mAh cm −2 under 0.1 C at 30 °C.

研究领域: 材料科学 · 电化学 · 储能技术 · 聚合物化学 · 电池技术
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Kinetic Molecular Modulation of Highly-Aligned Self-Locking Nanofibers for Strong, Tough, and Transparent Bioplastic Films

Shi-Peng Chen,Jing Wang,Dan-Yang Zhao,Jin-Long Zhu,Jia-Cheng Lv,Gan-Ji Zhong,Hua-Dong Huang,Zhong-Ming Li

Cellulose-based bioplastic films have long been considered a promising alternative to unrecyclable plastics. However, the failure to harness their full potential of hydroxyl-rich nature causes weakness and brittleness, restricting their successful applications. Inspired by natural bamboo, a supramolecular engineering strategy is proposed to modulate the self-assembly kinetics of cellulose chains for simultaneously reinforcing and toughening cellulose films. A loosely-structured amorphous molecular network is first constructed to enable dynamic rearrangement, and then the stretching field induce the formation of highly-aligned nanofibers, resembling a natural snap-fit self-locking system. As a result, the highly-aligned and tightly-stacked nanofiber imparts transparent cellulose films with an increase of exceeding 300% in fracture toughness to 6.82 MJ·m −3 and an impressive tensile strength of 176 MPa, surpassing the most previously reported fully regenerated cellulose films. This pioneering approach of kinetic molecular modulation opens up a new perspective for high-performance, transparent, and truly sustainable bioplastic films and beyond.

CAS / MDL: 80-70-6
研究领域: 材料科学 · 高分子科学 · 生物材料 · 纳米技术 · 可持续工程
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