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  • Guiyang Zheng, Xuelian Kang, Haoran Ye, Wei Fan, Christian Sonne, Su Shiung Lam, Rock Keey Liew, Changlei Xia, Yang Shi, Shengbo Ge
    Chinese Chemical Letters. 2024, 35(4): 108817-.

    Humans have relied on biomass for survival and development since the Stone Age. All aspects of human needs for materials are covered by tools, fuel, and buildings. Nowadays, metals and petroleum-based materials are widely used in highly developed industries. Unfortunately, environmental contamination and the loss of natural resources have led to the reemergence of biomass resources as efficient and sustainable energy sources. Notably, simple and direct applications can no longer meet the demand for functionalization, high performance of materials and construction materials. Therefore, it is imperative to modify biomass and combine its utilisation to produce functionalization and high performance materials. For example, construction materials with superior mechanical properties and water resistance can be produced by reinforcing fibres to facilitate crosslinking. Water-oil separation or adsorption effects of hydrogels and aerogels are determined by the porosity and lightness of biomass, biocomposite conductor is prepared by chimaeric conductive material. Here, we review the approaches that have been taken to devise an environmentally friendly yet fully recyclable and sustainable functionalised biocomposites from biomass and its potential directions for future research.

  • Xinyue Lan, Junguang Liang, Churan Wen, Xiaolong Quan, Huimin Lin, Qinqin Xu, Peixian Chen, Guangyu Yao, Dan Zhou, Meng Yu
    Chinese Chemical Letters. 2024, 35(4): 108616-.

    Despite the synergy of immune checkpoint blockade (ICB) therapy and photodynamic therapy (PDT) holds great promise as countermeasures against breast cancer, exploring long-term or flexible short-time therapeutic strategies in "cold" tumors remains a great challenge. Here, we present a polyunsaturated fatty acid-doped liposomal hydrogel Lp(DHA)@CP Gel loaded with photosensitizer chlorin e6 (Ce6) and programmed death-ligand 1 antibody (αPD-L1) for flexible local photoimmunotherapy with merely single-dosed administration. The presence of polyunsaturated fatty acid (docosahexaenoic acid, DHA) doped in particle membrane endows liposomes with flexibly reactive oxygen species (ROS)-responsive release capability, which was attributed to the presence of abundant unsaturated groups. The αPD-L1 was repeatedly induced to in situ release in response to the PDT under photo-exposure. The immunogenic cell death (ICD) effect of PDT evoked "cold" breast tumor to "hot" one, and then assisted the cascade released αPD-L1 to synergistically boost the immunotherapy. After a single dose of peritumoral administration of Lp(DHA)@CP Gel, the on-demand treatment can maximize patient compliance and safety by adjusting therapeutic behaviors via a photo on-off switch. This work presents a flexible medication platform, showing promise in improving the objective response rate of ICB therapy and minimizing its systemic toxicity.

  • Zhe Wang, Li-Peng Hou, Qian-Kui Zhang, Nan Yao, Aibing Chen, Jia-Qi Huang, Xue-Qiang Zhang
    Chinese Chemical Letters. 2024, 35(4): 108570-.

    Electrolyte design is essential for stabilizing lithium metal anodes and localized high-concentration electrolyte (LHCE) is a promising one. However, the state-of-the-art LHCE remains insufficient to ensure long-cycling lithium metal anodes. Herein, regulating the solvation structure of lithium ions in LHCE by weakening the solvating power of diluents is proposed for improving LHCE performance. A diluent, 1,1,2,2,3,3,4,4-octafluoro-5-(1,1,2,2-tetrafluoroethoxy) pentane (OFE), with weaker solvating power is introduced to increase the proportion of aggregates (an anion interacts with more than two lithium ions, AGG-n) in electrolyte compared with the commonly used 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE). The decomposition of AGG-n in OFE-based LHCE intensifies the formation of anion-derived solid electrolyte interphase and improves the uniformity of lithium deposition. Lithium metal batteries with OFE-based LHCE deliver a superior lifespan of 190 cycles compared with 90 cycles of TTE-based LHCE under demanding conditions. Furthermore, a pouch cell with OFE-based LHCE delivers a specific energy of 417 Wh/kg and undergoes 49 cycles. This work provides guidance for designing high-performance electrolytes for lithium metal batteries.

  • Botao Gao, He Qi, Hui Liu, Jun Chen
    Chinese Chemical Letters. 2024, 35(4): 108598-.

    The electric field-induced irreversible domain wall motion results in a ferroelectric (FE) hysteresis. In antiferroelectrics (AFEs), the irreversible phase transition is the main reason for the hysteresis effects, which plays an important role in energy storage performance. Compared to the well-demonstrated FE hysteresis, the structural mechanism of the hysteresis in AFE is not well understood. In this work, the underlying correlation between structure and the hysteresis effect is unveiled in Pb(Zr, Sn, Ti)O3 AFE system by using in-situ electrical biasing synchrotron X-ray diffraction. It is found that the AFE with a canting dipole configuration, which shows a continuous polarization rotation under the electric field, tends to have a small hysteresis effect. It presents a negligible phase transition, a small axis ratio, and electric field-induced lattice changing, small domain switching. All these features together lead to a slim hysteresis loop and a high energy storage efficiency. These results offer a deep insight into the structure-hysteresis relationship of AFEs and are helpful for the design of energy storage material.

  • Pingping Wang, Huixian Miao, Kechuan Sheng, Bin Wang, Fan Feng, Xuankun Cai, Wei Huang, Dayu Wu
    Chinese Chemical Letters. 2024, 35(4): 108600-.

    The blue-light-excitable phosphors play a crucial role in the high-performance white LEDs. Here, we report on two new Cu(Ⅰ) coordination network materials as yellow-emitting phosphors prepared by suitably expanded π-conjugated triazole ligands. Upon blue-light irradiation, these complexes exhibit efficient solid-state emission and enhanced photostability. Through incorporating the yellow phosphor and a commercial blue-green powder (BaSi2N2O2:Eu2+) with a blue LED chip, the phosphor-converted LED devices display remarkable white emission properties. The experimental results demonstrate that the Cu(Ⅰ) coordination network materials function as promising blue-light excitable phosphors with great application potential for full-spectrum white LEDs.

  • Yuan Zhang, Shenghao Gong, A.R. Mahammed Shaheer, Rong Cao, Tianfu Liu
    Chinese Chemical Letters. 2024, 35(4): 108587-.

    MOF-based core-shell structures with high surface area, abundant active sites, and broad absorption bands are viable alternatives to traditional single-component photocatalysts. In this report, we describe the design and construction of delicate Ag nanowires@NH2-UiO-66 with a core-shell structure for use as photocatalysts in imine synthesis under light. The optimized composites exhibited 80% imine production, which was higher than both MOF and Ag NWs. The significant improvement in photocatalytic activity under light may be attributed to the plasmonic effect of silver nanowires and their core-shell structure, which promotes the separation of electron-hole pairs. Moreover, the photocatalytic activity of the core-shell nanostructure may provide valuable insight into the design and construction of MOF-based composite photocatalysts for oxidative coupling of amines.

  • Caixia Li, Yi Qiu, Yufeng Zhao, Wuliang Feng
    Chinese Chemical Letters. 2024, 35(4): 108846-.

    The poor interfacial contact is one of the biggest challenges that solid-state lithium batteries suffer from. Reducing the solid-state electrolyte surface energy by transforming the interface from lithiophobic to lithiophilic is effective to promote the interfacial contact, but electronic conductive interphases usually increase the risk of electron attack, thus leading to uncontrollable Li dendrite growth. Herein, we propose a self-assembled thermodynamic stable LiI interphase to simultaneously improve the interfacial contact between the garnet electrolyte Li7La3Zr2O12 (LLZO) and Li anode, and prohibit the electron attack. The direct contact between LLZO and Li and the high temperature Li melting process was ascribed to Zr4+ reduction, which facilitated Li dendrite formation and propagation. With the modification of the high lithiophilic I2 thin film, the area specific interfacial resistance of LLZO/Li was reduced from 1525 Ω/cm2 to 57 Ω/cm2. More importantly, LLZO was protected from being reduced due to the outstanding electronic insulativity of the LiI interphase, which leaded to a high critical current density of 1.2/7.0 mA/cm2 in the time/capacity-constant modes, respectively.

  • Liliang Chu, Xiaoyan Zhang, Jianing Li, Xuelei Deng, Miao Wu, Ya Cheng, Weiping Zhu, Xuhong Qian, Yunpeng Bai
    Chinese Chemical Letters. 2024, 35(4): 108896-.

    Polysubstituted chiral γ-butyrolactones are the core structural units of many natural products and high value-added flavors and fragrances used in the food and cosmetic industry. Current enzymatic cascade synthesis of these molecules faces the problems of low enzyme activity and phase separation in batch reaction, resulting in low productivity. Herein, we report a new continuous-flow process to synthesize the optically pure Nicotiana tabacum lactone (3S,4S)-4a and whisky lactone (3R,4S)-4b from α,β-unsaturated γ-ketoesters. A new ene reductase (ER) from Swingsia samuiensi (SsER) and a carbonyl reductase (SsCR) were engineered by directed evolution to improve their activity and thermostability. The continuous-flow preparative reactions were performed in two 3D microfluidic reactors, generating (3S,4S)-4a (99% ee and 87% de) and (3R,4S)-4b (99% ee and 98% de) with space-time yields 3 and 7.4 times higher than those of the batch reactions. The significant enhancement in the productivity of enzyme cascade catalysis brought by cutting-edge continuous microfluidic technology will benefit the general multi-enzyme catalytic systems in the future.

  • Yuqing Zhu, Haohao Chen, Li Wang, Liqun Ye, Houle Zhou, Qintian Peng, Huaiyong Zhu, Yingping Huang
    Chinese Chemical Letters. 2024, 35(4): 108884-.

    Piezoelectric catalysis, a new catalytic method, is widely used in the field of environmental sanitation, including waste water treatment and dye degradation. However, in the face of the growing environmental pollution problem, the efficiency of piezoelectric catalysis is still hampered by the stress variation in the natural environment. Therefore, it is particularly important to improve the catalytic efficiency of piezoelectric materials. We divide piezoelectric materials into two categories: inorganic piezoelectric materials and organic piezoelectric materials. Then the mainstream inorganic piezoelectric materials are divided into four subcategories, namely: (1) MTiO3 (M = Ba, Sr), (2) bi-class catalytic materials, (3) MoX2 (X = S, Se), and (4) ZnO piezoelectric materials. The mainstream organic piezoelectric materials are divided into PVDF and g-C3N4 materials. At the same time, the above materials are summarized to explain the excellent performance of materials from the perspective of structure and piezoelectric principle. In addition, we summarized the modification methods that can be applied to piezoelectric materials: (1) Morphology methods, (2) composites with heterojunctions, and (3) surface modification. Finally, we summarized the prospects of piezoelectric materials in the field of environment and water treatment.

  • Jie Wu, Xiaoqing Yu, Guoxing Li, Su Chen
    Chinese Chemical Letters. 2024, 35(4): 109234-.

    Particle engineering has opened the floodgates to material science in both fundamental and application field. However, covalent interactions have not yet been adequately designed in the particle engineering for functional colloidal photonic crystals (CPCs). Herein, we achieved covalent coupling between carboxyl-rich poly(styrene-acrylic acid) (P(St-AA)) monodispersed colloidal particles and amine-rich carbon dots (CDs) based on an feasible and universal particle engineering strategy. The designed CDs-grafted P(St-AA) monodispersed colloidal particles initiate a hydrogen bond-driven assembly mode and ensure the construction of large-scale crack-free CPCs. Moreover, the CDs equipped with selective broad-band absorption capacity could improve the saturation of structural colors for high-visibility CPCs. Furthermore, an injectable photonic hydrogel (IPH) is developed to design CPC supraball hydrogel via integrating the CDs-grafted P(St-AA) CPC supraballs with supramolecular hydrogel. Combining superior flexibility, sufficient self-healing capacity of supramolecular hydrogel with visual optical information of our CPC supraballs, a cyclically reversible coding and decoding system was developed. Meanwhile, we firstly demonstrated the novel strategy of 3D supraballs-based passive cooling. The designed 3D CPC supraball hydrogel presents nearly full observation angle reflections behavior and excellent water evaporation capacity and achieves 3.6 ℃ temperature drops, showing the application advantages in 3D thermal management. This work not only provides a new insight for manipulating optical properties of CPCs, but also demonstrates an easy-to-perform platform, as well as indicates the direction for the promising application of CPCs.

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