Modulating the proton transfer kinetics via Ru single atoms for highly efficient ammonia synthesis
Chem Catalysis(2023)
摘要
The electrochemical nitrate reduction reaction (eNO3RR) is an appealing technology for converting environmentally toxic NO3- to ammonia (NH3). This approach was usually obstructed by the multi-proton/electron involved process. Here, we report a catalyst with Ru single atoms supported on Co3O4 (Ru SAsCo3O4). The as-developed Ru SAs-Co3O4 catalyst shows a remarkable NH3-evolving activity with a faradic efficiency of 94.92% +/- 4.02% at the potential of -0.2 V (vs. RHE) and a generation rate of 1,843.45 +/- 57.14 mmol h-1 cm -2 at the potential of -0.5 V. Further investigations revealed that the Ru SAs play a dual role in simultaneously accelerating the proton transfer and modulating the d-electron structures of the neighboring Co sites, which led to a lower energy barrier of the rate-determining step. Eventually, by combining the eNO3RR and electrosynthesis of 5,5'-azotetrazolate at a two-electrode system, an energy-saving NH3 synthesis, while simultaneously producing value-added chemicals, was successfully achieved.
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关键词
nitrate reduction reaction,Ru single atoms,proton transfer,proton inventory studies,coupling system
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