Self-Supporting Electrocatalyst Film Based on Self-Assembly of Heterogeneous Bottlebrush and Polyoxometalate for Efficient Hydrogen Evolution Reaction,Macromolecular Rapid Communications

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Self-Supporting Electrocatalyst Film Based on Self-Assembly of Heterogeneous Bottlebrush and Polyoxometalate for Efficient Hydrogen Evolution Reaction
Macromolecular Rapid Communications ( IF 4.2 ) Pub Date : 2022-02-05 , DOI: 10.1002/marc.202100915
Yayu Lin ₁ , Youlong Zhu ₁ , Qian Ma ₂ , Xianlan Ke ₁ , Pengwei Ma ₁ , Rongfeng Liao ₁ , Shaohong Liu ₁ , Dingcai Wu ₁

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Developing efficient electrocatalysts to promote the hydrogen evolution reaction (HER) is essential for a green and sustainable future energy supply. For practical applications, it is a challenge to achieve the self-assembly of electrocatalyst from microscopic to macroscopic scales. Herein, a facile strategy is proposed to fabricate a self-supporting electrocatalyst film (CNT-g-PSSCo/PW₁₂) for HER by electrostatic interaction-induced self-assembly of cobalt polystyrene sulfonate-grafted carbon nanotube heterogeneous bottlebrush (CNT-g-PSSCo) and polyoxometalate (PW₁₂). Co²⁺ ions of CNT-g-PSSCo can function as junctions for interconnecting neighboring bottlebrushes to form the 3D nanonetwork structure and enable electrostatic capture of negatively charged PW₁₂ nanodots. Moreover, CNT backbones can provide highly conductive pathways to CNT-g-PSSCo/PW₁₂. Such a self-assembled CNT-g-PSSCo/PW₁₂ displays a low overpotential of 31 mV at a current density of 10 mA cm⁻² and a small Tafel slope of 25 mV dec⁻¹, showing high efficiency toward HER. Furthermore, CNT-g-PSSCo/PW₁₂ with a stable self-supporting film morphology exhibits long-term electrocatalytic stability over 1000 CV cycles without noticeable overpotential change in acidic media. The findings may provide a new avenue for constructing self-assembled functional nanonetwork materials with well-orchestrated structural hierarchy for many applications in energy, environment, catalysis, medicine, and others.

中文翻译：

基于多相瓶刷和多金属氧酸盐自组装高效析氢反应的自支撑电催化剂膜

开发高效的电催化剂以促进析氢反应 (HER) 对于绿色和可持续的未来能源供应至关重要。对于实际应用，实现电催化剂从微观到宏观的自组装是一个挑战。在此，本文提出了一种简便的策略，通过聚苯乙烯磺酸钴接枝碳纳米管异质瓶刷_（ CNT- g - PSSCo) 和多金属氧酸盐 (PW ₁₂ )。CNT- g的Co ²⁺离子-PSSCo 可以作为连接相邻瓶刷的连接点，以形成 3D 纳米网络结构，并能够静电捕获带负电的 PW ₁₂纳米点。此外，CNT 主链可以为 CNT- g -PSSCo/PW ₁₂提供高导电通路。这种自组装的CNT- g - PSSCo/PW ₁₂在 10 mA cm ^{-2的电流密度和 25 mV dec}^-1的小塔菲尔斜率下显示出 31 mV 的低过电位，显示出对 HER 的高效率。此外， CNT- g -PSSCo/PW ₁₂具有稳定的自支撑薄膜形态在 1000 CV 循环中表现出长期的电催化稳定性，而在酸性介质中没有明显的过电位变化。这些发现可能为构建具有良好协调结构层次的自组装功能纳米网络材料提供了一条新途径，用于能源、环境、催化、医学等领域的许多应用。

更新日期：2022-02-05

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