Thus, designing and synthesizing of efficient electrocatalysts for water splitting have attracted numerous attention all over the world. Moreover, EWS could also facilitate the efficient consumption of renewable energy and the energy redistribution as the buffer to enhance the resilience of the energy system. Nowadays, electrochemical water splitting (EWS) is considered as the most green and sustainable method for hydrogen production 9, 10. The large-scale application of hydrogen energy could reduce carbon emissions, generating revolutionary impact on all aspects of energy utilization 5, 6, 7, 8. Hydrogen energy, accepted as the ideal substitute for fossil fuels, plays an important role in energy transformation 1, 2, 3, 4. Our work not only develops a route towards efficient catalysts applicable across a wide range of pH values, it also provides a successful showcase of a model catalyst for in-depth mechanistic insight into electrochemical water splitting. At a current density of 10 mA cm −2, the overpotential for hydrogen evolution and oxygen evolution is 23/201 mV and 42/194 mV in 0.5 M H 2SO 4 and 1 M KOH, respectively. The as-prepared catalyst exhibits efficient catalytic capability for electrochemical water splitting in both acidic and alkaline electrolytes. The pyrolysis-free synthesis also ensured the formation of well-defined active sites within the framework structure, providing ideal platforms to understand the catalytic processes. Starting with a conjugated framework containing Fe sites, the addition of Ni atoms is used to weaken the adsorption of electrochemically generated intermediates, thus leading to more optimized energy level sand enhanced catalytic performance. This work develops bifunctional catalysts with single atom active sites through a pyrolysis-free route. Catalysts capable of electrochemical overall water splitting in acidic, neutral, and alkaline solution are important materials.
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