The development of new proton-conducting materials through a convenient and low-cost method is crucial in fuel cell technology. Supramolecular hydrogen-bonded organic networks (SHONs) are constructed by self-assembly of multi-component organic molecules through hydrogen bond interactions, in which the intermolecular hydrogen bond bridge constructed by Brønsted acid–base pairs and water molecules can accelerate the process of protonation and deprotonation for efficient proton conduction. The particle state and hydrophilicity of SHONs directly affect the grain boundary conductivity and the stability of the hydrogen bond network, which play a decisive role in the proton conduction. In this study, cellulose fibers were used as carrier to induce the in-situ growth of SHONs, constructed by melamine and 1,2-ethanedisulfonic acid, to prepare composite paper for a promising proton exchange membrane. Cellulose fibers exhibited significant regulation on the particle state and hydrophilicity of SHONs. Scanning electron microscopy and surface area analysis showed that the introduction of cellulose fiber changed the particle state of SHONs. Compared with pure SHONs, SHONs grown in-situ on cellulose fibers exhibited a smaller particle size and a more continuous arrangement, which was beneficial to improve the grain boundary conductivity. Contact angle measurements proved that the introduction of cellulose fibers improved the hydrophilicity of SHONs. This contributed to improving the stability of the hydrogen bond networks and the smoothness of the proton conduction channel. The regulation effect of cellulose fibers on SHONs improved the proton conduction efficiency of SHONs. The formed composite paper with SHONs grown in-situ on cellulose fibers exhibited a proton conduction value of up to 6.46 × 10^–2 S cm⁻¹ at 75 °C and 85% RH. This work provides a novel strategy for preparing highly efficient proton conducting composite paper for potential application in proton-exchange membrane fuel cells.

通过方便且低成本的方法开发新的质子传导材料在燃料电池技术中至关重要。超分子氢键有机网络（SHONs）是由多组分有机分子通过氢键相互作用自组装构建的，其中由布朗斯台德酸碱对和水分子构建的分子间氢键桥可以加速质子化和去质子化以实现有效的质子传导。SHONs的颗粒状态和亲水性直接影响晶界电导率和氢键网络的稳定性，对质子传导起决定性作用。本研究以纤维素纤维为载体诱导 SHONs 的原位生长，由三聚氰胺和 1,2-乙二磺酸构成，为有前途的质子交换膜制备复合纸。纤维素纤维对SHONs的颗粒状态和亲水性表现出显着的调节作用。扫描电子显微镜和表面积分析表明，纤维素纤维的引入改变了SHONs的颗粒状态。与纯SHONs相比，在纤维素纤维上原位生长的SHONs粒径更小，排列更连续，有利于提高晶界电导率。接触角测量证明，纤维素纤维的引入提高了 SHON 的亲水性。这有助于提高氢键网络的稳定性和质子传导通道的平滑度。纤维素纤维对SHONs的调控作用提高了SHONs的质子传导效率。^–2 S cm ^-1在 75 °C 和 85% RH 下。这项工作为制备用于质子交换膜燃料电池潜在应用的高效质子传导复合纸提供了一种新策略。