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3. Hollow Multishelled Structure: Synthesis Chemistry and Application

Author

Mao, Dan, Wang, Chao, Li, Wei, Zhou, Liang, Liu, Jian, Zheng, Zijian, Zhao, Yong, Cao, An-min, Wang, Shutao, Huang, Jiaxing, Huo, Fengwei, Chen, Hongyu, Mai, Liqiang, Yu, Ranbo, Wang, Lianzhou, Lu, Yunfeng, Yu, Chengzhong, Yang, Qihua, Yang, Zhenzhong, Zeng, Hua Chun, Zhao, Huijun, Tang, Zhiyong, Zhao, Dongyuan, and Wang, Dan

Published
2024
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24. Biomimetic Superstructured Interphase for Aqueous Zinc-Ion Batteries

Author

Ai, Yan, primary, Yang, Chaochao, additional, Yin, Ziqing, additional, Wang, Tong, additional, Gai, Tianyu, additional, Feng, Jiayou, additional, Li, Kailin, additional, Zhang, Wei, additional, Li, Yefei, additional, Wang, Fei, additional, Chao, Dongliang, additional, Wang, Yonggang, additional, Zhao, Dongyuan, additional, and Li, Wei, additional

Published
2024
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30. Fluorine Doping Mediated Epitaxial Growth of NaREF4 on TiO2 for Boosting NIR Light Utilization in Bioimaging and Photodynamic Therapy.

Author

Kou, Yufang, Liu, Minchao, Zhou, Qiaoyu, Lin, Runfeng, Yu, Hongyue, Hou, Mengmeng, Ming, Jiang, Tang, Yi, Elzatahry, Ahmed A., Zhang, Fan, Zhao, Dongyuan, and Li, Xiaomin

Subjects
ENERGY levels (Quantum mechanics), EPITAXY, BAND gaps, ENERGY transfer, PHOTODYNAMIC therapy
Abstract

By integrating TiO2 with rare earth upconversion nanocrystals (NaREF4), efficient energy transfer can be achieved between the two subunits under near‐infrared (NIR) excitation, which hold tremendous potential in the fields of photocatalysis, photodynamic therapy (PDT), etc. However, in the previous studies, the combination of TiO2 with NaREF4 is a non‐epitaxial random blending mode, resulting in a diminished energy transfer efficiency between the NaREF4 and TiO2. Herein, we present a fluorine doping‐mediated epitaxial growth strategy for the synthesis of TiO2‐NaREF4 heteronanocrystals (HNCs). Due to the epitaxial growth connection, NaREF4 can transfer energy through phonon‐assisted pathway to TiO2, which is more efficient than the traditional indirect secondary photon excitation. Additionally, F doping brings oxygen vacancies in the TiO2 subunit, which further introduces new impurity energy levels in the intrinsic band gap of TiO2 subunit, and facilitates the energy transfer through phonon‐assisted method from NaREF4 to TiO2. As a proof of concept, TiO2‐NaGdF4 : Yb,Tm@NaYF4@NaGdF4 : Nd@NaYF4 HNCs were rationally constructed. Taking advantage of the dual‐model up‐ and downconversion luminescence of the delicately designed multi‐shell structured NaREF4 subunit, highly efficient photo‐response capability of the F‐doped TiO2 subunit and the efficient phonon‐assisted energy transfer between them, the prepared HNCs provide a distinctive nanoplatform for bioimaging‐guided NIR‐triggered PDT. [ABSTRACT FROM AUTHOR]

Published
2024
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31. A Library of Nanocrystal‐Inserted Ordered Mesoporous Frameworks with Ultrahigh Density and Spatial Dispersity.

Author

Zhang, Wei, Shi, Wenxiong, Wang, Jinxiu, Zhu, Kerun, Tian, Yong, He, Haili, Duan, Linlin, Fang, Huang, Liu, Yupu, Wang, Biwei, Ma, Yuzhu, Zhao, Tiancong, Zhang, Xingmiao, Lv, Zirui, Zu, Lianhai, Tang, Yun, Dong, Angang, Kong, Biao, and Zhao, Dongyuan

Abstract

It is a great challenge to integrate incompatible subunits into ordered macroscopic materials with tailored functionalities. Herein, a facile modular assembly strategy is demonstrated to link incompatible colloidal nanocrystals and polymer micelles by using the phenolic resol as the "molecule glue" for the synthesis of nanocrystal‐inserted mesoporous frameworks with diverse functionalities. It is found that the uniform nanocrystals can be inserted into the mesoporous frameworks with outstanding spatial dispersity, even in the case of high incorporation density. This modular assembly route is versatile, a library of nanocrystals with diverse diameters, shapes, and compositions can be integrated into various kinds of mesoporous frameworks (carbon, carbon‐SiO2, and carbon‐TiO2 composites). Unprecedently, this strategy also allows the controllable assembly of two, even three types of nanocrystals within the mesoporous frameworks to achieve multiple functionalities. The as‐prepared nanocomposites can simultaneously exhibit catalytic, magnetic, and adsorption properties independently, and show synergistic effects for tandem catalytic applications. [ABSTRACT FROM AUTHOR]

Published
2024
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32. High Capacitance Based on Vacancy Defective Porous Carbon in Ionic Liquid.

Author

Feng, Shihao, Zhao, Qian, Wang, Junjun, Zhang, Wei, Wang, Weixiao, Xu, Ming, Zhou, Liang, Mai, Liqiang, Zhao, Dongyuan, and Liu, Yong

Subjects
CARBON-based materials, ENERGY density, DENSITY functional theory, ACTIVATED carbon, ELECTRIC capacity
Abstract

Porous carbons have been extensively studied in electrochemical capacitors (ECs). However, low capacitance remains a limitation due to the electrical double layer (EDL) storage mechanism when porous carbons are used in ionic liquids (ILs) based ECs. Herein, the nitrogen‐derived vacancy defects in porous carbon nanospheres are found which can boost capacitive charge storage and present reversible high capacitance of 427 F g−1 in pure IL electrolyte, equal to a normalized area capacitance (CA) of 16 µF cm−2, surpassing the theoretical EDL CA (≈11 µF cm−2). When used as capacitive cathode, the assembled Lithium hybrid capacitor express high energy density of 635 Wh kg−1 based on active material under much high‐power density of 14.5 kW kg−1. A combination of control experiments and density functional theory investigation indicate that the EC's performance improvement mostly stems from strong interactions at vacancy defects, triggering extraordinary faradaic capacitance. The results shed light on defect engineering for realizing extra faradaic capacitance of carbon materials, and open up new opportunities for improving EC's energy density. [ABSTRACT FROM AUTHOR]

Published
2024
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35. The Rise of Xene Hybrids.

Author

Kumar, Prashant, Singh, Gurwinder, Guan, Xinwei, Roy, Soumyabrata, Lee, Jangmee, Kim, In Young, Li, Xiaomin, Bu, Fanxing, Bahadur, Rohan, Iyengar, Sathvik Ajay, Yi, Jiabao, Zhao, Dongyuan, Ajayan, Pulickel M., and Vinu, Ajayan

Published
2024
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36. Rescue of dead MnO2 for stable electrolytic Zn–Mn redox-flow battery: a metric of mediated and catalytic kinetics.

Author

Wang, Qi, Zhou, Wanhai, Zhang, Yanyan, Jin, Hongrun, Li, Xinran, Zhang, Tengsheng, Wang, Boya, Zhao, Ruizheng, Zhang, Junwei, Li, Wei, Qiao, Yu, Jia, Chuankun, Zhao, Dongyuan, and Chao, Dongliang

Subjects
DENSITY functional theory, ENERGY density, ENERGY storage, ELECTROLYSIS, OXIDATION-reduction reaction
Abstract

The virtues of electrolytic MnO2 aqueous batteries are high theoretical energy density, affordability and safety. However, the continuous dead MnO2 and unstable Mn2+/MnO2 electrolysis pose challenges to the practical output energy and lifespan. Herein, we demonstrate bifunctional cationic redox mediation and catalysis kinetics metrics to rescue dead MnO2 and construct a stable and fast electrolytic Zn–Mn redox-flow battery (eZMRFB). Spectroscopic characterizations and electrochemical evaluation reveal the superior mediation kinetics of a cationic Fe2+ redox mediator compared with the anionic ones (e.g. I– and Br–), thus eliminating dead MnO2 effectively. With intensified oxygen vacancies, density functional theory simulations of the reaction pathways further verify the concomitant Fe-catalysed Mn2+/MnO2 electrolysis kinetics via charge delocalization and activated O 2p electron states, boosting its rate capability. As a result, the elaborated eZMRFB achieves a coulombic efficiency of nearly 100%, ultra-high areal capacity of 80 mAh cm–2, rate capability of 20 C and a long lifespan of 2500 cycles. This work may advance high-energy aqueous batteries to next-generation scalable energy storage. [ABSTRACT FROM AUTHOR]

Published
2024
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42. Electron‐Donating Conjugation Effect Modulated Zn2+ Reduction Reaction for Separator‐Free Aqueous Zinc Batteries

Author

Sun, Zhihao, primary, Bu, Fanxing, additional, Zhang, Yanyan, additional, Zhou, Wanhai, additional, Li, Xinran, additional, Liu, Xin, additional, Jin, Hongrun, additional, Ding, Shixiang, additional, Zhang, Tengsheng, additional, Wang, Lipeng, additional, Li, Hongpeng, additional, Li, Wei, additional, Zhang, Chaofeng, additional, Zhao, Dongyuan, additional, Wang, Yonggang, additional, and Chao, Dongliang, additional

Published
2024
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47. Synthesis of Mesoporous Catechin Nanoparticles as Biocompatible Drug-Free Antibacterial Mesoformulation

Author

Lin, Runfeng, Li, Gaoyang, He, Qianfeng, Song, Junfeng, Ma, Yanming, Zhan, Yating, Yuan, Minjia, Li, Qi, Chao, Dongliang, Li, Xiaomin, Wang, Peiyuan, Zhao, Tiancong, and Zhao, Dongyuan

Abstract

While polyphenolic substances stand as excellent antibacterial agents, their antimicrobial properties rely on the auxiliary support of micro-/nanostructures. Despite offering a novel avenue for enhancing polymer performance, controllable fabrication of mesoporous polymeric nanomaterials encounters significant challenges due to intricate intermolecular forces. In this article, mesoporous catechin nanoparticles have been successfully fabricated using a balanced multivariate interaction approach. The harmonization of the water–ethanol ratio and ionic strength effectively balances the forces of hydrogen bonding and π–π stacking, facilitating the controlled assembly of mesostructures. The mesoporous catechin nanoparticles exhibit a uniform spherical structure (∼100 nm), open mesopores with a diameter of ∼15 nm, and a high surface area of ∼106 m2g–1. While exhibiting a good biocompatibility and negative surface charge, the mesoporous catechins possess outstanding antibacterial ability and function as an antibiotic mesoformulation without the necessity of loading any drugs. This mesoformulation inhibits 50% in vitro Staphylococcus aureusgrowth with a low concentration of ∼10 μg mL–1and achieves complete inhibition at ∼25 μg mL–1. In a mouse wound model, accelerated wound healing and complete closure within 6–8 days are achieved. Proteomics of bacteria reveals that the excellent antibacterial property is attributed to the synergetic effect of mesoformulation’s mesostructure and the catechin molecule intervening in bacterial metabolism. Overall, this work may pave a novel way for the future exploration of polymer nanomaterials and antibiotic formulations.

Published
2024
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48. High-Valent Thiosulfate Redox Electrochemistry for Advanced Sulfur-Based Aqueous Batteries

Author

Feng, Yutong, Wang, Boya, Zhou, Wanhai, Jin, Hongrun, Yu, Xiaoyu, Zhang, Tengsheng, Zhao, Jian, Li, Hongpeng, Zhao, Jingwen, Li, Wei, Ma, Chenyan, Chao, Dongliang, and Zhao, Dongyuan

Abstract

Sulfur-based aqueous batteries (SABs) are promising for safe, low-cost, and high-capacity energy storage. However, the low output voltage of sulfur cannot meet the demands of high-energy cathode applications due to its intrinsic negative potential (E0= −0.51 V vs SHE) of low-valent polysulfide redox (S2–/S0). Here, instead of relying on traditional aqueous polysulfide redox, for the first time, we demonstrate a high-valent thiosulfate redox (S2O32–/S4O62–) electrochemistry, exhibiting positive redox potential (E0> 0 V vs SHE) and reversible cation storage in aqueous environment. OperandoX-ray absorption fine structure spectroscopy, in situRaman spectroscopy, and density functional theory calculations reveal the high reversibility and dynamic charge transfer process of high-valent thiosulfate redox. Significantly, the aqueous thiosulfate redox exhibits a high operating voltage of approximately 1.4 V, a reversible capacity of 193 Ah L–1, and a long cycling life of over 1000 cycles (99.6% capacity retention). This work provides new insights into the high-valent S-based electrochemistry and opens a new pathway to achieve energetic aqueous batteries.

Published
2024
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