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Xiaolei Li Zifeng Lin Na Jin Lei Sun Xiaojiao Yang Ying Liu 《Advanced functional materials》2023,33(20):2214667
Polyoxometalates are intriguing high-capacity anode materials for alkali-metal-ion storage due to their multi-electron redox capabilities and flexible structure. However, their poor electrical conductivity and high working voltage severely restrict their practical application. Herein, the dinuclear polyoxovanadate Sr2V2O7·H2O with unusually high electrical conductivity is reported as a promising anode material for lithium-ion batteries. During the initial lithiation process, the Sr2V2O7·H2O anode experiences an electrochemically induced crystalline-to-amorphous transition. The resulting amorphous structure provides high redox activity and fast reaction kinetics via reversible V4.9+/V2.8+ redox couple through the intercalation mechanism. Furthermore, when coupled with the LiFePO4 cathode, the strong V O bonds of the amorphous anode provide excellent structural stability, with the full-cell capable of performing >12 000 cycles with a capacity retention of 72%. Another advantage of Sr2xV2O7-δ·yH2O (0.5 ≤ x ≤ 1.0) is its composition adjustability, which enables delicately regulating the Sr vacancy content without destroying the structure. The defect Sr2xV2O7-δ·yH2O (x = 0.5) electrodes show significantly improved specific capacity and rate capability without sacrificing other key properties, delivering a high specific capacity of 479 mAh g-1 at 0.1 mA cm-2 and 41.9% of its capacity in 2 min. Overall, the preliminary study points the way forward for the facile preparation of high-quality polyoxometalates for advanced energy storage applications and beyond. 相似文献
95.
Shiyu Huang Yuan Chang Zhuwei Li Jiaqi Cao Yurou Song Junfeng Gao Licheng Sun Jungang Hou 《Advanced functional materials》2023,33(21):2211631
Photoredox catalysis is a green solution for organics transformation and CO2 conversion into valuable fuels, meeting the challenges of sustainable energy and environmental concerns. However, the regulation of single-atomic active sites in organic framework not only influences the photoredox performance, but also limits the understanding of the relationship for photocatalytic selective organic conversion with CO2 valorization into one reaction system. As a prototype, different single-atomic metal (M) sites (M2+ = Fe2+, Co2+, Ni2+, Cu2+, and Zn2+) in hydrogen-bonded organic frameworks (M-HOF) backbone with bridging structure of metal-nitrogen are constructed by a typical “two-in-one” strategy for superior photocatalytic C N coupling reactions integrated with CO2 valorization. Remarkably, Zn-HOF achieves 100% conversion of benzylamine oxidative coupling reactions, 91% selectivity of N-benzylidenebenzylamine and CO2 conversion in one photoredox cycle. From X-ray absorption fine structure analysis and density functional theory calculations, the superior photocatalytic performance is attributed to synergic effect of atomically dispersed metal sites and HOF host, decreasing the reaction energy barriers, enhancing CO2 adsorption and forming benzylcarbamic acid intermediate to promote the redox recycle. This work not only affords the rational design strategy of single-atom active sites in functional HOF, but also facilitates the fundamental insights upon the mechanism of versatile photoredox coupling reaction systems. 相似文献
96.
Jiajia Deng Xin Wang Weihua Zhang Liangyan Sun Xinxin Han Xianqin Tong Liming Yu Jiandong Ding Lin Yu Yuehua Liu 《Advanced functional materials》2023,33(21):2211664
Extracellular vesicles (EVs) derived from mesenchymal stem cells (MSCs) have emerged as an appealing alternative to cell therapy in regenerative medicine. Unlike bone marrow MSCs (BMSCs) cultured in vitro with normoxia, bone marrow in vivo is exposed to a hypoxic environment. To date, it remains unclear whether hypoxia preconditioning can improve the function of BMSC-derived EVs and be more conducive to bone repair. Herein, it is found that hypoxia preconditioned BMSCs secrete more biglycan (Bgn)-rich EVs via proteomics analysis, and these hypoxic EVs (Hypo-EVs) significantly promote osteoblast proliferation, migration, differentiation, and mineralization by activating the phosphatidylinositide 3-kinase/protein kinase B pathway. Subsequently, an injectable bioactive hydrogel composed of poly(ethylene glycol)/polypeptide copolymers is developed to improve the stability and retention of Hypo-EVs in vivo. The Hypo-EVs-laden hydrogel shows continuous liberation of Hypo-EVs for 3 weeks and substantially accelerates bone regeneration in 5-mm rat cranial defects. Finally, it is confirmed that Bgn in EVs is a pivotal protein regulating osteoblast differentiation and mineralization and exerts its effects through paracrine mechanisms. Therefore, this study shows that hypoxia stimulation is an effective approach to optimize the therapeutic effects of BMSC-derived EVs and that injectable hydrogel-based EVs delivery is a promising strategy for tissue regeneration. 相似文献
97.
Yu Cheng Xinnan Xu Mengfan Wang Chengwei Deng Yi Sun Chenglin Yan Tao Qian 《Advanced functional materials》2023,33(44):2302332
As a promising energy carrier, ammonia synthesis by electrocatalytic nitrogen reduction reaction (eNRR) is a promising green and low-carbon ammonia synthesis strategy that can replace the traditional Haber–Bosch process. However, the development of eNRR processes is mainly severely constrained by competitive hydrogen evolution reaction (HER), and the corresponding strategies to inhibit this adverse side reaction to obtain high eNRR selectivity are still limited. In addition, for this complex reaction involving gas–liquid–solid three-phase interface and proton/electron transfer, it is great significance to analyze and summarize the existing inhibition HER strategies from the viewpoint of dynamics. In view of this, this work reviews proton supply/filtration regulation strategy in catalytic system, allowing a systematic survey of the literature focusing on interface membrane regulation (inorganic membrane and organic membrane), electrolyte regulation (metal-mediated strategy and electrolyte ion regulation strategy) and system device design (electrode structure design and electrolytic cell device design). Constructive catalytic system design guidance is also suggested to inhibit hydrogen evolution and improve NH3 selectivity, aiming for scalable and economically feasible applications. 相似文献
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Jiayang Liao Xiang Lv Xi-xi Sun Junhua Li Haomin Wang Qiang Chen Hanpeng Lu Duan Wang Jian Bi Jiagang Wu 《Advanced functional materials》2023,33(34):2303637
Although the piezo-catalysis is promising for the environmental remediation and biomedicine, the piezo-catalytic properties of various piezoelectric materials are limited by low carrier concentrations and mobility, and rapid electron-hole pair recombination, and reported regulating strategies are quite complex and difficult. Herein, a new and simple strategy, integrating phase boundary engineering and defect engineering, to boost the piezo-catalytic activity of potassium sodium niobate ((K, Na)NbO3, KNN) based materials is innovatively proposed. Tur strategy is validated by exampling 0.96(K0.48Na0.52)Nb0.955Sb0.045O3-0.04(BixNa4-3x)0.5ZrO3-0.3%Fe2O3 material having phase boundary engineering and conducted the defect engineering via the high-energy sand-grinding. A high reaction rate constant k of 92.49 × 10−3 min−1 in the sand-grinding sample is obtained, which is 2.40 times than that of non-sand-grinding one and superior to those of other representative lead-free perovskite piezoelectric materials. Meanwhile, the sand-grinding sample has remarkable bactericidal properties against Escherichia coli and Staphylococcus aureus. Superior piezo-catalytic activities originate from the enhanced electron-hole pair separation and the increased carrier concentration. This study provides a novel method for improving the piezo-catalytic activities of lead-free piezoelectric materials and holds great promise for harnessing natural energy and disease treatment. 相似文献
100.
Hui Zhang Yinkun Sun Junjie Yang Zhiyu Sun Yanxin Zhao Xin Li Wei Wang Dongwei Lu Jun Ma 《Advanced functional materials》2023,33(40):2302816
Precise adjustment of the pore size, damage repair, and efficient cleaning is all challenges for the wider application of inorganic membranes. This study reports a simple strategy of combining dry-wet spinning and electrosynthesis to fabricate stainless-steel metal–organic framework composite membranes characterized by customizable pore sizes, targeted reparability, and high catalytic activity for membrane cleaning. The membrane pore size can be precisely customized in the range of 14–212 nm at nanoscale, and damaged membranes can be repaired by targeted treatment in 120 s. In addition, advanced oxidation processes can be used to quickly clean the membrane and achieve 98% flux recovery. The synergistic actions of the membrane matrix and the selective layer increase the adsorption energy of active sites to oxidant, shorten the electron transfer cycle, and enhance the overall catalytic performance. This study can provide a new direction for the development of advanced membranes for water purification and high-efficiency membrane cleaning methods. 相似文献