The efficiency of splitting water into hydrogen and oxygen is highly depended on the catalyst used. Enhancing the thermodynamics and/or kinetics of electrocatalytic reactions and redox property through organic–inorganic nanohybrids represents one of the most powerful strategies to boost the electrocatalytic performance of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, a rational design of carbon-supported transition metal oxide grown on a nickel foam surface is reported, which synergistically integrates the thermodynamics and/or kinetics through modification of electronic structures with accelerated kinetics by adjusting electron-giving and electron-absorbing groups. SCN^– modification experiment and pre - and post-catalytic analysis manifest that the Co/Fe-N formed between the Co/Fe metal and amino functional group serve as the center of HER. Operando Raman spectroscopy was utilized to explore the OER active intermediates present under catalytic conditions. Specifically, the catalyst requires only an overpotential of 1.466 V to reach 10 mA cm⁻² with good stability over 100 h at various current densities between 20, 40, 60, 80 and 100 mA cm⁻², superior to controlled transition metal oxides and noble metals. This is a viable and systematic strategy to prepare metal organic framework catalysts with appropriate functional groups that can be used for energy storage and conversion in multiple applications.

将水分解为氢和氧的效率高度取决于所用的催化剂。通过有机-无机纳米杂化物增强电催化反应的热力学和/或动力学以及氧化还原特性是提高氢析出反应（HER）和氧析出反应（OER）的电催化性能的最有效策略之一。这里，报道了在泡沫镍表面上生长的碳负载的过渡金属氧化物的合理设计，其通过调节电子给予和电子吸收基团以加速的动力学通过修饰电子结构来协同地整合热力学和/或动力学。SCN ^–改性实验和催化前后分析表明，Co / Fe金属与氨基官能团之间形成的Co / Fe-N是HER的中心。利用Operando拉曼光谱研究催化条件下存在的OER活性中间体。具体而言，该催化剂仅需1.466 V的超电势即可达到10 mA cm ^-2，并在20、40、60、80和100 mA cm ^-2之间的各种电流密度下，在100 h内具有良好的稳定性，优于受控的过渡金属氧化物和贵金属。这是一种制备具有适当官能团的金属有机骨架催化剂的可行且系统的策略，该催化剂可用于多种应用中的能量存储和转化。