Nazari Sahar, Najmi Ali, Kumar Priyank, Zavabeti Ali, Allioux Francois-Marie, Natarajan Anirudh Raju, Esrafilzadeh Dorna, Jalili Ali R
School of Chemical Engineering, University of New South Wales (UNSW), Sydney, NSW, 2033, Australia.
School of Civil and Environmental Engineering, University of New South Wales (UNSW), Sydney, NSW, 2033, Australia.
Small. 2025 Aug;21(32):e2504087. doi: 10.1002/smll.202504087. Epub 2025 Jun 17.
A high-entropy liquid metal alloy (Ga-Fe-Zn-Sn-Bi-Ni) is developed to address the multi-step complexity of green ammonia electrosynthesis from nitrate. Guided by molecular dynamics, design of experiments, and density functional theory, this alloy exploits high configurational entropy to form diverse, atomically dispersed active sites. The liquid state eliminates endothermic barriers by enabling nitrogen intermediates to move freely to the most energetically favorable sites. Crucially, a hydrogen shuttling mechanism is uncovered where Fe acts as a proton hub while Sn, Ni, and Zn store and transfer hydrogen to Fe, enhancing reaction kinetics and preventing catalyst saturation. This synergy boosts ammonia production rates up to sevenfold while maintaining high Faradaic efficiency (FE). By integrating entropy-driven design, dynamic site reconfiguration, and hydrogen management, this work establishes a robust foundation for efficient, scalable ammonia electrosynthesis in pursuit of NetZero targets.
一种高熵液态金属合金（镓-铁-锌-锡-铋-镍）被开发出来，以解决从硝酸盐中进行绿色氨电合成的多步复杂性问题。在分子动力学、实验设计和密度泛函理论的指导下，这种合金利用高组态熵形成了多样的、原子分散的活性位点。液态通过使氮中间体能够自由移动到能量最有利的位点，消除了吸热障碍。至关重要的是，发现了一种氢穿梭机制，其中铁充当质子中心，而锡、镍和锌储存并将氢转移到铁上，增强了反应动力学并防止催化剂饱和。这种协同作用将氨的生产率提高了七倍，同时保持了高法拉第效率（FE）。通过整合熵驱动设计、动态位点重新配置和氢管理，这项工作为追求净零目标的高效、可扩展氨电合成奠定了坚实基础。
