中山大学廖培钦研究团队开发出连续电合成医用级浓度纯H₂O₂溶液的，导电镍酞菁基共价有机框架。相关研究成果于2024年11月4日发表于国际顶尖学术期刊《美国化学会杂志》。

H₂O₂的电合成为工业中使用的传统蒽醌方法提供了一种环保的替代方案，但存在杂质、H₂O₂产率和浓度受限的问题。

该文中，研究人员展示了一种基于酞菁镍的共价有机框架（COF，表示为BBL-PcNi），其固有电导率为1.14×10^-5Sm^-1，在3.5V的低电池电压下，其具有530mAcm^-2的超高电流密度和～100%的法拉第效率（H₂O₂）。值得注意的是，这种高水平的性能在200小时的连续运行中保持不变，没有明显的退化。

当集成到放大的膜电极组件电解槽中，并在2 V的极低电池电压下以～3300 mA的电流运行时，BBL PcNi连续产生医用级浓度（3.5 wt%）的纯H₂O₂溶液，这至少是之前报道的催化剂的3.5倍，是传统蒽醌工艺产量的1.5倍。

机理研究表明，增强π共轭以减少集成到COF中的分子催化位点的带隙，可以更有效地增强其固有的电子传输能力，从而显著提高H₂O₂生成的电催化性能。

附：英文原文

Title: Continuous Electrosynthesis of Pure H2O2 Solution with Medical-Grade Concentration by a Conductive Ni-Phthalocyanine-Based Covalent Organic Framework

Author: Meng-Di Zhang, Jia-Run Huang, Cheng-Peng Liang, Xiao-Ming Chen, Pei-Qin Liao

Issue&Volume: November 4, 2024

Abstract: Electrosynthesis of H2O2 provides an environmentally friendly alternative to the traditional anthraquinone method employed in industry, but suffers from impurities and restricted yield rate and concentration of H2O2. Herein, we demonstrated a Ni-phthalocyanine-based covalent-organic framework (COF, denoted as BBL-PcNi) with a higher inherent conductivity of 1.14 × 10–5 S m–1, which exhibited an ultrahigh current density of 530 mA cm–2 with a Faradaic efficiency (H2O2) of ～100% at a low cell voltage of 3.5 V. Notably, this high level of performance is maintained over a continuous operation of 200 h without noticeable degradation. When integrated into a scale-up membrane electrode assembly electrolyzer and operated at ～3300 mA at a very low cell voltage of 2 V, BBL-PcNi continuously yielded a pure H2O2 solution with medical-grade concentration (3.5 wt %), which is at least 3.5 times higher than previously reported catalysts and 1.5 times  the output of the traditional anthraquinone process. A mechanistic study revealed that enhancing the π-conjugation to reduce the band gap of the molecular catalytic sites integrated into a COF is more effective to enhance its inherent electron transport ability, thereby significantly improving the electrocatalytic performance for H2O2 generation.

DOI: 10.1021/jacs.4c10675

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c10675