Zhu Shicheng, Yang Ruoou, Li Huang Jing Wei, Huang Sirui, Wang Haozhi, Liu Youwen, Li Huiqiao, Zhai Tianyou
State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, P. R. China.
State Key Laboratory of Marine Resource Utilization in South China Sea, and School of Materials Science and Engineering, Hainan University, Haikou, Hainan, 570228, P. R. China.
Angew Chem Int Ed Engl. 2024 Apr 22;63(17):e202319462. doi: 10.1002/anie.202319462. Epub 2024 Mar 21.
Developing highly active oxygen evolution reaction (OER) catalysts in acidic conditions is a pressing demand for proton-exchange membrane water electrolysis. Manipulating proton character at the electrified interface, as the crux of all proton-coupled electrochemical reactions, is highly desirable but elusive. Herein we present a promising protocol, which reconstructs a connected hydrogen-bond network between the catalyst-electrolyte interface by coupling hydrophilic units to boost acidic OER activity. Modelling on N-doped-carbon-layer clothed Mn-doped-CoO (Mn-CoO@CN), we unravel that the hydrogen-bond interaction between CN units and HO molecule not only drags the free water to enrich the surface of Mn-CoO but also serves as a channel to promote the dehydrogenation process. Meanwhile, the modulated local charge of the Co sites from CN units/Mn dopant lowers the OER barrier. Therefore, Mn-CoO@CN surpasses RuO at high current density (100 mA cm @ ~538 mV).
开发在酸性条件下具有高活性的析氧反应（OER）催化剂是质子交换膜水电解的迫切需求。控制带电界面处的质子特性，作为所有质子耦合电化学反应的关键，是非常可取的，但难以实现。在此，我们提出了一种有前景的方案，即通过耦合亲水性单元来重建催化剂-电解质界面之间的连通氢键网络，以提高酸性OER活性。以N掺杂碳层包覆的Mn掺杂CoO（Mn-CoO@CN）为模型，我们揭示了CN单元与HO分子之间的氢键相互作用不仅将游离水拖至Mn-CoO表面使其富集，还作为促进脱氢过程的通道。同时，来自CN单元/Mn掺杂剂对Co位点局部电荷的调制降低了OER势垒。因此，Mn-CoO@CN在高电流密度（100 mA cm@~538 mV）下超过了RuO。
