Nowadays, the development of novel technology for economical and efficient reclamation of waste acid containing metal ions is still the top priority. The graphene oxide (GO)-based membrane has gained attention in the relevant membrane processes driven by pressure gradient, concentration difference and even Donnan potential because of its special two-dimension (2D) structure and abundant hydrophilic sites. However, its work performances for electrodialysis (ED)-based acid recovery process are still unknown. In this work, GO-based proton permselective membranes (PPM) are designed and applied in the ED-based acid recovery. Above all, the possibility of selective separating protons from metal cations by GO membrane under a direct electric field and the related influencing factors are comprehensively explored by molecular dynamic simulation. Furthermore, a series of GO-based PPMs with designed thickness, interlayer spacing and charged state are prepared by adjusting GO loading, employing different crosslinking agents and attaching the relevant polyelectrolytes. Therein, the work performances of GO-based PPMs in a typical ion substitution ED process, including the metal cation leakage, water transport phenomenon and nonideal migration of anions are investigated and compared with those of commercial membrane. Results show that GO membranes prepared and used according to the optimized conditions embrace sharp separating property between protons and metal ions which is hardly deteriorated along with the change of their relative content. On the other hand, it is noticed that the leakage of organic anions and water transport seem to be unavoidable due to the exploitation of the porous support. Obviously, this work can contribute to not only developing a novel PPM for ED but extending the applications of the 2D nanomaterial as well.

目前，开发经济高效回收含金属离子废酸的新技术仍是当务之急。氧化石墨烯（GO）基膜由于其特殊的二维（2D）结构和丰富的亲水位点，在压力梯度、浓度差甚至唐南电位驱动的相关膜过程中受到关注。然而，其在基于电渗析（ED）的酸回收过程中的工作性能仍然未知。在这项工作中，基于 GO 的质子选择性渗透膜 (PPM) 被设计并应用于基于 ED 的酸回收。首先，通过分子动力学模拟综合探索了GO膜在直接电场下选择性分离质子与金属阳离子的可能性及相关影响因素。此外，通过调整GO负载量、使用不同的交联剂并连接相关的聚电解质，制备了一系列具有设计厚度、层间距和带电状态的基于GO的PPM。其中，研究了基于 GO 的 PPMs 在典型的离子取代 ED 过程中的工作性能，包括金属阳离子泄漏、水传输现象和阴离子的非理想迁移，并与商业膜进行了比较。结果表明，按照优化条件制备和使用的GO膜具有明显的质子和金属离子分离特性，并且几乎不随其相对含量的变化而劣化。另一方面，值得注意的是，由于多孔载体的开发，有机阴离子的泄漏和水的传输似乎是不可避免的。显然，这项工作不仅有助于开发用于 ED 的新型 PPM，还有助于扩展二维纳米材料的应用。