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  • Title: Optimized Intermediates Adsorption Configuration on Co-Doped Fe2P@NiP2 Heterojunction Interface for Enhanced Electrocatalytic Nitrate-To-Ammonia Conversion.
    Author: Zheng Y, Tan Y, Yu X, Yao H, Hu S, Hu J, Chen Z, Guo X.
    Journal: Small; 2024 Aug; 20(32):e2312136. PubMed ID: 38482968.
    Abstract:
    The extraction of ammonia (NH3) through electrocatalytic nitrate reduction reaction (NO3 -RR) represents a sustainable avenue in NH3 generation and utilization. However, the catalytic efficiency of the NO3 -RR is hindered by the sluggish kinetics. This study first theoretically found that phosphide-based heterostructure can alter the adsorption structure of intermediates in the nitrate-to-ammonia process, thereby achieving precise regulation of the energy barrier in the rate-determining step. Based on theoretical design, a novel Co-doped Fe2P@NiP2 heterojunction catalyst is successfully synthesized, which deliver a notable NH3 yield rate of 0.395 mmol h-1 cm-2 at -0.7 V versus RHE, as well as a remarkable ammonia Faraday efficiency of 97.2% at -0.6 V versus RHE. Experimental and theoretical results further confirm that redistributing electrons and shifting the center of the d-band upwards through interfacial doping modulate intermediates adsorption strength and inhibition of hydrogen evolution, leading to excellent performance in NO3 --to-NH3. Further integrating the Co-Fe2P@NiP2 catalyst into a Zn-nitrate battery exhibits a substantial voltage output of 1.49 V and a commendable power density of 13.2 mW cm-2. The heteroatom-doped heterojunction strategy provides a versatile route for developing advanced catalysts, thereby broadening the horizons of electrocatalytic methodologies for nitrate reduction and ammonia synthesis.
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