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Ammonia is the main precursor for the production of fertilizers, a hydrogen energy carrier and an emerging clean fuel that plays a crucial role in sustaining life on the globe.

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Hierarchical CoFe-LDH@g-C3N4 heterostructures have been synthesized via a facile and easily scalable in situ solvothermal method for efficient overall water splitting.

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The development of durable, low-cost, and efficient photo-/electrolysis for the oxygen and hydrogen evolution reactions (OER and HER) is important to fulfill increasing energy requirements. Herein, highly efficient and active photo-/electrochemical catalysts, that is, CoMn-LDH@g-C N hybrids, have been synthesized successfully through a facile in situ co-precipitation method at room temperature. The CoMn-LDH@g-C N composite exhibits an obvious OER electrocatalytic performance with a current density of 40 mA cm at an overpotential of 350 mV for water oxidation, which is 2.5 times higher than pure CoMn-LDH nanosheets. For HER, CoMn-LDH@g-C N (η =-448 mV) requires a potential close to Pt/C (η =-416 mV) to reach a current density of 50 mA cm . Furthermore, under visible-light irradiation, the photocurrent density of the CoMn-LDH@g-C N composite is 0.227 mA cm , which is 2.1 and 3.8 time higher than pristine CoMn-LDH (0.108 mA cm ) and g-C N (0.061 mA cm ), respectively. The CoMn-LDH@g-C N composite delivers a current density of 10 mA cm at 1.56 V and 100 mA cm at 1.82 V for the overall water-splitting reaction. Therefore, this work establishes the first example of pure CoMn-LDH and CoMn-LDH@g-C N hybrids as electrochemical and photoelectrochemical water-splitting systems for both OER and HER, which may open a pathway to develop and explore other LDH and g-C N nanosheets as efficient catalysts for renewable energy applications.

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