A New Balancer for H Production and Consumption in Nitrate Reduction Reaction

Major Contributions
 

1.Universal Synthesis of High-Entropy Aerogels: Development of a seed-mediated synthetic strategy that overcomes thermodynamic immiscibility and nucleation disparities, enabling the first successful fabrication of structurally uniform, single-phase high-entropy metallene aerogels (HEMAs) such as PdCuSnCoNi.

2.Superior Electrocatalytic Performance: Demonstration of exceptional nitrate reduction activity, where the optimized HEMA achieves a near-unity ammonia Faradaic efficiency of 99.5% and an ultrahigh yield rate, significantly outperforming conventional monometallic counterparts and commercial catalysts.

3.Mechanistic Resolution of Kinetic Balance: Elucidation of a kinetic balancing mechanism where multi-metallic electronic modulation optimizes the Pd d-band center to enhance *NO₂ adsorption and precisely matches *H production with consumption, effectively suppressing hydrogen evolution while accelerating ammonia synthesis.

主要貢獻
 

1.高熵氣凝膠的通用合成：開發一種晶種介導的合成策略，克服熱力學不互溶與成核差異，首次成功製備出結構均勻的單相高熵金屬烯氣凝膠（HEMAs），如 PdCuSnCoNi。

2.卓越的電催化性能：展現出優異的硝酸鹽還原活性，優化後的 HEMA 實現了接近 100%（99.5%）的氨法拉第效率以及超高的產率，性能顯著超越傳統單金屬材料與商用催化劑。

3.動力學平衡的機制解析：闡明動力學平衡機制，揭示多金屬電子調控能優化 Pd d-帶中心以增強 *NO₂ 吸附，並精確匹配活性氫的生成與消耗，從而在有效抑制析氫反應的同時加速氨的合成。