Dynamic catalytic interface driven three-step synergistic mechanism for boosting ammonia and hydroxylamine synthesis.
basic_science · Level V
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- Record sourced from PubMed, PMID 42481488.
- Also identified by DOI 10.1038/s41467-026-75665-7.
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Abstract
Despite the short-term industrial landscape remaining unchanged, green synthesis technologies for ammonia (NH<sub>3</sub>) and hydroxylamine (NH<sub>2</sub>OH) are critical for carbon neutrality. Alternatively, electrocatalytic nitrate reduction (NIRR) can be integrated with membrane separation technology via a modular design, simultaneously achieving pollution control and resource recovery. However, the microscopic mechanism of NIRR remains ambiguous given the complex dynamic catalytic interface, hindering advanced catalyst development. Here, we propose a three-step synergistic mechanism at dynamic catalytic interface, which integrates interfacial microenvironment regulation, OH species cycle, and reverse hydrogen spillover for efficient NH<sub>3</sub> and NH<sub>2</sub>OH synthesis across different scenarios. Notably, dual-site heterostructure catalyst exhibits almost 100% NH<sub>3</sub>-Faradaic Efficiency (FE<sub>NH3</sub>) across a wide nitrate concentration range, reaching a maximum NH<sub>3</sub> yield of 10.27 mmol h<sup>-1</sup> cm<sup>-2</sup>. The simultaneous NH<sub>3</sub> synthesis-recovery system maintains almost 100% FE<sub>NH3</sub> and NH<sub>3</sub> recovery efficiency over 120 h, accompanied by long-term durability and negligible performance degradation. Additionally, cyclopentanone-mediated NIRR process delivers a satisfactory NH<sub>2</sub>OH-Faradaic Efficiency (83.48%), and the assembled zinc-nitrate battery achieves a high peak power density (57.6 mW cm<sup>-2</sup>).