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Updated: Aug 15, 2026

Synthesis of Metal Nanoparticles Supported on Carbon Nanotube with Doped Co and N Atoms and its Catalytic Applications in Hydrogen Production
Published on: December 6, 2021
Functional differentiation of active hydrogen on Pd/Cu catalysts for efficient electrocatalytic nitrate reduction to
Chunhong Fu1, Chaohui Zhang1, Jiangli Sun1
1Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution, Nankai University, Tianjin 300350, China; Tianjin Advanced Water Treatment Technology International Joint Research Center, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
None:
Electrocatalytic nitrate reduction (NO3RR) offers a promising strategy to remediate NO3- pollution and synthesize value-added ammonia (NH3), but its efficiency is limited by the sluggish nitrite reduction and insufficient NH3 selectivity over Cu catalysts. Herein, Pd nanoparticle-decorated Cu submicron particles (PdNPs/Cu SPs) were developed to enhance the conversion of NO3- to NH3 through promoting active hydrogen (*H) generation. PdNPs/Cu SPs achieved a high conversion of 95.05% for NO3- to NH3 with a Faradaic efficiency of 95.65%. Mechanistic investigations revealed the generation of *H species with distinct binding states on PdNPs/Cu SPs. Lattice-associated hydrogen (*Hlat) was found to modify the local electronic structure of Pd and strengthen NO3- adsorption, whereas adsorbed hydrogen on the surface (*Hads) served as the primary reactive *H species participating in reduction and hydrogenation of nitrogen intermediates. The cooperative functions of *Hlat and *Hads promoted both NO3- adsorption and subsequent hydrogenations. DFT calculations further showed that *H accumulation on PdNPs/Cu SPs rendered the critical *NO → *HNO thermodynamically favorable (ΔG = -0.13 eV), thereby shifting the potential-determining step from *NO hydrogenation to NH3 desorption. In-situ mass spectrometry and spectroscopy elucidate the dominant reaction pathway and confirm the proposed synergy: *NO3→*NO2→*NO→*HNO→*NH2OH→*NH2→*NH3→NH3. This work provides an efficient catalyst for sustainable nitrogen cycling and offers a novel reference for leveraging distinct *H species with different binding states in multi-step electrocatalytic reactions.
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