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通过多尺度催化剂优化在酸性介质中实现高效的析氧电合成

Efficient HO Electrosynthesis in Acidic media via Multiscale Catalyst Optimization.

作者信息

Shim Jaehyuk, Lee Jaewoo, Shin Heejong, Mok Dong Hyeon, Heo Sungeun, Paidi Vinod K, Lee Byoung-Hoon, Lee Hyeon Seok, Yang Juhyun, Shin Dongho, Moon Jaeho, Kim Kang, Jung Muho, Lee Eungjun, Bootharaju Megalamane S, Kim Jeong Hyun, Park Subin, Kim Mi-Ju, Glatzel Pieter, Yoo Sung Jong, Back Seoin, Lee Kug-Seung, Sung Yung-Eun, Hyeon Taeghwan

机构信息

Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul, 08826, Republic of Korea.

School of Chemical and Biological Engineering, Institute of Chemical Processes, Seoul National University, Seoul, 08826, Republic of Korea.

出版信息

Adv Mater. 2025 Apr;37(17):e2418489. doi: 10.1002/adma.202418489. Epub 2025 Mar 18.

DOI:10.1002/adma.202418489
PMID:40099574
Abstract

Electrochemically generating hydrogen peroxide (HO) from oxygen offers a more sustainable and cost-effective alternative to conventional anthraquinone process. In alkaline conditions, HO is unstable as HO , and in neutral electrolytes, alkali cation crossover causes system instability. Producing HO in acidic electrolytes ensures enhanced stability and efficiency. However, in acidic conditions, the oxygen reduction reaction mechanism is dominated by the inner-sphere electron transfer pathway, requiring careful consideration of both reaction and mass transfer kinetics. These stringent requirements limit HO production efficiency, typically below 10-20% at industrial-relevant current densities (>300 mA cm). Using a multiscale approach that combines active site tuning with macrostructure tuning, this work presents an octahedron-like cobalt structure on interconnected hierarchical porous nanofibers, achieving a faradaic efficiency exceeding 80% at 400 mA cm and stable operation for over 120 h at 100 mA cm. At 300 mA cm, the optimized catalyst demonstrates a cell potential of 2.14 V, resulting in an energy efficiency of 26%.

摘要

通过电化学方法将氧气转化为过氧化氢(HO),为传统蒽醌法提供了一种更具可持续性且成本效益更高的替代方案。在碱性条件下,HO 会以 HO 的形式变得不稳定,而在中性电解质中,碱金属阳离子的交叉会导致系统不稳定。在酸性电解质中生产 HO 可确保更高的稳定性和效率。然而,在酸性条件下,氧还原反应机制以内层电子转移途径为主导,需要仔细考虑反应动力学和传质动力学。这些严格的要求限制了 HO 的生产效率,在与工业相关的电流密度(>300 mA cm)下,通常低于 10 - 20%。本研究采用多尺度方法,将活性位点调控与宏观结构调控相结合,在相互连接的分级多孔纳米纤维上构建了八面体状钴结构,在 400 mA cm 时实现了超过 80%的法拉第效率,并在 100 mA cm 下稳定运行超过 120 小时。在 300 mA cm 时,优化后的催化剂的电池电位为 2.14 V,能量效率为 26%。

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