1. A Cascade Jet Plasma Oxidation─electroreduction System Using Pd‐Ni Dual‐Site Catalyst for Sustainable Ammonia Production from Air.
- Author
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Ding, Jun, Li, Wenyi, Zhang, Heng, Tang, Shu, Mao, Zhixian, Zhang, Shengbo, Jin, Meng, Lin, Qifu, Zhang, Yunxia, Wang, Guozhong, and Zhang, Haimin
- Subjects
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PLASMA jets , *SUSTAINABILITY , *JETS (Fluid dynamics) , *ELECTROLYTIC reduction , *ENERGY consumption , *CARBON nanotubes - Abstract
Electrocatalytic N2 reduction reaction (eNRR) has been deemed as an alternative approach to the Haber‐Bosch (H‐B) process for ammonia (NH3) production, but it remains a huge challenge. Here jet plasma oxidation of N2 is reported in air into NOx and subsequently NO2− coupling with electrochemical NO2− reduction reaction (pN2─eNO2−RR) over PdNi alloying nanoparticles on N‐doped carbon nanotubes (PdNi/N‐CNTs) for NH3 synthesis. The results demonstrate that the jet plasma reactor possesses excellent gas reforming capacity to achieve the largest NO2− yield rate of 30.46 mmol h−1 with a low energy consumption of 2.66 kWh molN−1. For subsequent eNO2−RR, PdNi/N‐CNTs can afford an NH3 yield of 34.96 mg h−1 mgcat.−1 and a faradaic efficiency (FE) of 98.21% at −0.38 and 0.02 V (vs RHE), respectively. In situ spectroscopic characterizations combined with theoretical calculations unveil that PdNi/N‐CNTs provide Pd and Ni dual active sites, enabling NO2− activation on the Ni site and active H* provision on the Pd site to facilitate eNO2−RR. A cascade pN2‐eNO2−RR system is constructed for sustainable NH3 production, achieving a stable NH3 yield rate of 25.56 mmol h−1, an average FE >85%, as well as NOx to NH3 conversion efficiency of 44.62% at constant ampere‐level current with finally collection of gram‐level (NH4) 2SO4 product. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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