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Atomic Precision CoCu Heterodimers with Pseudo-D3h Symmetry Enable Tandem Nitrate Reduction
Akash Prabhu Sundar Rajan1, Jayaraman Theerthagiri1, Piyapa Junmon2
1Department of Chemistry (BK21 FOUR), Research Institute of Advanced Chemistry, Gyeongsang National University, Jinju, Republic of Korea.
None:
The electrochemical reduction of nitrate (eNO3RR) to ammonia (NH3) is an efficient method for mitigating nitrate (NO3 -) pollutant while offering sustainable NH3 generation under ambient environments. However, optimizing NO3 - adsorption on catalytic surfaces and promoting adsorbed hydrogen formation remain challenging. Herein, we introduce pulsed laser irradiation in liquid for the first time to design a metal-metal-ligand-coordinated CoCu heterodimer catalyst with a pseudo-D3h symmetry anchored on nitrogen-doped graphene oxide (CoCu-HeD/NGO), enabling a tandem catalytic effect for the eNO3RR. The catalyst reaches a remarkable Faradaic efficiency of 91% at -0.4 V vs. RHE and a high NH3 production rate of 25 mg h-1 cm-2 at -0.5 V vs. RHE. Combined theoretical and in situ spectroelectrochemical analyses reveal that the synergistic interaction among Co and Cu dual sites enhances NO3 - adsorption, weakens N─O bonds, and facilitates the establishment of Langmuir-Hinshelwood-type hydrogenation intermediates, steering the tandem reaction pathway toward selective NH3 formation. Furthermore, a Zn-nitrate battery with a CoCu-HeD/NGO cathode integrates energy generation and NH3 synthesis with environmental remediation, delivering 5.26 mW cm-2 power density and stable discharge performance. Practical NH3 production is verified via Ar stripping-acid-trapping methods. This work establishes a new paradigm for the rational design of site-selective electrocatalysts for hybrid energy-to-chemical platforms.
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