Delicate Control over Electron Distribution and Water Dissociation Kinetics in Strongly Coupled Ru@NMoC Hybrid Catalyst Realizes Efficient Seawater Electrolysis
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引用次数: 0
Abstract
Delicate control over electron distribution in hybrid catalysts is crucial for improving hydrogen evolution catalysis, which remains an aspirational target in advancing efficient hydrogen production. Herein, we optimize the local electronic structures and balance the reaction steps by incorporating Ru clusters into nitrogen-doped molybdenum carbide (denoted as Ru@NMoC), addressing performance limitations in alkaline seawater. The Ru@NMoC catalyst demonstrates ultra-low overpotentials of 8, 17, and 20 mV at 10 mA cm⁻² in 1 M KOH, 1 M KOH + 0.5 M NaCl, and 1 M KOH seawater, respectively, significantly outperforming conventional HER catalysts. Operando spectroscopic techniques reveal strong ability for interface water dissociation and stable local charge structure in Ru@NMoC. Theoretical simulations demonstrate that N-doping of Ru clusters self-optimizes their electronic states and lowering the energy barrier for water dissociation. Self-powered H2 production system can be achieved using Zn-H₂O batteries to drive anion exchange membrane water electrolysis cell, demoinstrating its practicability.
杂化催化剂中电子分布的精细控制对于改善析氢催化是至关重要的,这仍然是推进高效制氢的理想目标。在此,我们通过将Ru团簇掺入氮掺杂碳化钼(表示为Ru@NMoC)来优化局部电子结构并平衡反应步骤,以解决碱性海水中的性能限制。Ru@NMoC催化剂在1 M KOH, 1 M KOH + 0.5 M NaCl和1 M KOH海水中表现出10 mA cm⁻²时的超低过电位,分别为8、17和20 mV,显著优于传统的HER催化剂。Operando光谱技术揭示了Ru@NMoC具有较强的界面水解离能力和稳定的局部电荷结构。理论模拟表明,钌簇的n掺杂使其电子态自优化,降低了水解离的能垒。采用Zn-H₂O电池驱动阴离子交换膜电解池,实现了自供电制氢系统,证明了其实用性。
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.