Gao Xintong, Wang Pengtang, Sun Xiaogang, Jaroniec Mietek, Zheng Yao, Qiao Shi-Zhang
School of Chemical Engineering, The University of Adelaide, Adelaide, SA, 5005, Australia.
Department of Chemistry and Biochemistry & Advanced Materials, Liquid Crystal Institute, Kent State University, Kent, OH, 44242, United States of America.
Angew Chem Int Ed Engl. 2025 Feb 3;64(6):e202417987. doi: 10.1002/anie.202417987. Epub 2024 Nov 16.
Conventional water electrolysis relies on expensive membrane-electrode assemblies and sluggish oxygen evolution reaction (OER) at the anode, which makes the cost of green hydrogen (H) generation much higher than that of grey H. Here, we develop an innovative and efficient membrane-free water electrolysis system to overcome these two obstacles simultaneously. This system utilizes the thermodynamically more favorable urea oxidation reaction (UOR) to generate clean N over a new class of Cu-based catalyst (CuO) for replacing OER, fundamentally eliminating the explosion risk of H and O mixing while removing the need for membranes. Notably, this membrane-free electrolysis system exhibits the highest H Faradaic efficiency among reported membrane-free electrolysis work. In situ spectroscopic studies reveal that the new NH intermediate-mediated UOR mechanism on the CuO catalyst ensures its unique N selectivity and OER inertness. More importantly, an industrial-type membrane-free water electrolyser (MFE) based on this system successfully reduces electricity consumption to only 3.78 kWh Nm, significantly lower than the 5.17 kWh Nm of commercial alkaline water electrolyzers (AWE). Comprehensive techno-economic analysis (TEA) suggests that the membrane-free design and reduced electricity input of the MFE plants reduce the green H production cost to US$1.81 kg, which is lower than those of grey H while meeting the technical target (US$2.00-2.50 kg) set by European Commission and United States Department of Energy.
传统的水电解依赖于昂贵的膜电极组件以及阳极上缓慢的析氧反应(OER),这使得绿色氢气(H)的生产成本远高于灰色氢气。在此,我们开发了一种创新且高效的无膜水电解系统,以同时克服这两个障碍。该系统利用热力学上更有利的尿素氧化反应(UOR),在一类新型铜基催化剂(CuO)上生成清洁的氮气来替代OER,从根本上消除了氢气和氧气混合的爆炸风险,同时无需使用膜。值得注意的是,在已报道的无膜电解工作中,这种无膜电解系统展现出最高的氢气法拉第效率。原位光谱研究表明,CuO催化剂上由新型NH中间体介导的UOR机制确保了其独特的氮选择性和对OER的惰性。更重要的是,基于该系统的工业型无膜水电解槽(MFE)成功地将电耗降低至仅3.78 kWh Nm⁻³,显著低于商业碱性水电解槽(AWE)的5.17 kWh Nm⁻³。综合技术经济分析(TEA)表明,MFE装置的无膜设计和降低的电力输入将绿色氢气的生产成本降至1.81美元/千克,低于灰色氢气的成本,同时满足了欧盟委员会和美国能源部设定的技术目标(2.00 - 2.50美元/千克)。