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    Interfacial Covalent Bonds Regulated Electron-Deficient 2D Black Phosphorus for Electrocatalytic Oxygen Reactions
    (Weinheim : Wiley-VCH, 2021) Wang, Xia; Raghupathy, Ramya Kormath Madam; Querebillo, Christine Joy; Liao, Zhongquan; Li, Dongqi; Lin, Kui; Hantusch, Martin; Sofer, Zdeněk; Li, Baohua; Zschech, Ehrenfried; Weidinger, Inez M.; Kühne, Thomas D.; Mirhosseini, Hossein; Yu, Minghao; Feng, Xinliang
    Developing resource-abundant and sustainable metal-free bifunctional oxygen electrocatalysts is essential for the practical application of zinc–air batteries (ZABs). 2D black phosphorus (BP) with fully exposed atoms and active lone pair electrons can be promising for oxygen electrocatalysts, which, however, suffers from low catalytic activity and poor electrochemical stability. Herein, guided by density functional theory (DFT) calculations, an efficient metal-free electrocatalyst is demonstrated via covalently bonding BP nanosheets with graphitic carbon nitride (denoted BP-CN-c). The polarized P-N covalent bonds in BP-CN-c can efficiently regulate the electron transfer from BP to graphitic carbon nitride and significantly promote the OOH* adsorption on phosphorus atoms. Impressively, the oxygen evolution reaction performance of BP-CN-c (overpotential of 350 mV at 10 mA cm−2, 90% retention after 10 h operation) represents the state-of-the-art among the reported BP-based metal-free catalysts. Additionally, BP-CN-c exhibits a small half-wave overpotential of 390 mV for oxygen reduction reaction, representing the first bifunctional BP-based metal-free oxygen catalyst. Moreover, ZABs are assembled incorporating BP-CN-c cathodes, delivering a substantially higher peak power density (168.3 mW cm−2) than the Pt/C+RuO2-based ZABs (101.3 mW cm−2). The acquired insights into interfacial covalent bonds pave the way for the rational design of new and affordable metal-free catalysts. © 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH
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    Freestanding MXene‐based macroforms for electrochemical energy storage applications
    (Hoboken, NJ : Wiley, 2023) Lu, Qiongqiong; Liu, Congcong; Zhao, Yirong; Pan, Wengao; Xie, Kun; Yue, Pengfei; Zhang, Guoshang; Omar, Ahmad; Liu, Lixiang; Yu, Minghao; Mikhailova, Daria
    Freestanding MXene-based macroforms have gained significant attention as versatile components in electrochemical energy storage applications owing to their interconnected conductive network, strong mechanical strength, and customizable surface chemistries derived from MXene nanosheets. This comprehensive review article encompasses key aspects related to the synthesis of MXene nanosheets, strategies for structure design and surface medication, surface modification, and the diverse fabrication methods employed to create freestanding MXene-based macroform architectures. The review also delves into the recent advancements in utilizing freestanding MXene macroforms for electrochemical energy storage applications, offering a detailed discussion on the significant progress achieved thus far. Notably, the correlation between the macroform's structural attributes and its performance characteristics is thoroughly explored, shedding light on the critical factors influencing efficiency and durability. Despite the remarkable development, the review also highlights the existing challenges and presents future perspectives for freestanding MXene-based macroforms in the realms of high-performance energy storage devices. By addressing these challenges and leveraging emerging opportunities, the potential of freestanding MXene-based macroforms can be harnessed to enable groundbreaking advancements in the field of energy storage.