<br>NiMoO4 负载 Ru 纳米粒子的工程反键轨道占据增强氯析出反应,Journal of Colloid and Interface Science

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NiMoO4 负载 Ru 纳米粒子的工程反键轨道占据增强氯析出反应
Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2024-06-04 , DOI: 10.1016/j.jcis.2024.06.023
Dianzhi Zhang ₁ , Haiming Gong ₁ , Tao Liu ₁ , Jiaguo Yu ₁ , Panyong Kuang ₁

Affiliation

析氯反应 (CER) 对于工业规模生产高纯度 Cl 至关重要。尽管开发了经典的尺寸稳定阳极来提高 CER 效率，但竞争性析氧反应 (OER) 仍然是实现高 Cl 选择性的障碍。在此，设计了一种无粘合剂电极，即负载在泡沫钛上的 Ru 纳米颗粒 (NPs) 装饰的 NiMoO 纳米棒阵列 (NRA) (Ru-NiMoO/Ti)，用于饱和 NaCl 溶液（pH = 2）中的活性 CER。 Ru-NiMoO/Ti 电极在 10 mA cm 电流密度下表现出 20 mV 的低过电势、超过 90% 的高 Cl 选择性以及可运行 90 小时的强大耐用性。 CER 和 OER 之间塔菲尔斜率的显着差异表明 Ru-NiMoO/Ti 电极具有高 Cl 选择性和优异的反应动力学。进一步的研究揭示了Ru和NiMoO之间强烈的金属-载体相互作用（SMSI），促进电子通过Ru-O桥键转移并增加Ru 3d-Cl 2p反键轨道占据，最终导致Ru-Cl键减弱，促进Cl 解吸，并增强 Cl 的释放。我们的研究结果为通过反键轨道占用工程开发具有增强 CER 性能的电极提供了新的见解。

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Engineering antibonding orbital occupancy of NiMoO4-supported Ru nanoparticles for enhanced chlorine evolution reaction

Chlorine evolution reaction (CER) is crucial for industrial-scale production of high-purity Cl. Despite the development of classical dimensionally stable anodes to enhance CER efficiency, the competitive oxygen evolution reaction (OER) remains a barrier to achieving high Cl selectivity. Herein, a binder-free electrode, Ru nanoparticles (NPs)-decorated NiMoO nanorod arrays (NRAs) supported on Ti foam (Ru-NiMoO/Ti), was designed for active CER in saturated NaCl solution (pH = 2). The Ru-NiMoO/Ti electrode exhibits a low overpotential of 20 mV at 10 mA cm current density, a high Cl selectivity exceeding 90%, and robust durability for 90h operation. The marked difference in Tafel slopes between CER and OER indicates the high Cl selectivity and superior reaction kinetics of Ru-NiMoO/Ti electrode. Further studies reveal a strong metal-support interaction (SMSI) between Ru and NiMoO, facilitating electron transfer through the Ru–O bridge bond and increasing the Ru 3d–Cl 2p antibonding orbital occupancy, which eventually results in weakened Ru–Cl bonding, promoted Cl desorption, and enhanced Cl evolution. Our findings provide new insights into developing electrodes with enhanced CER performance through antibonding orbital occupancy engineering.

更新日期：2024-06-04

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