Junwei Wu, Yan Zheng, Mengyan Huang, Peiyan Ma, Zhengyi Fu
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引用次数: 0
Abstract
The surging global energy demand, coupled with diminishing fossil fuel reserves, is accelerating the technological advancement of clean hydrogen production through water electrolysis. Although molybdenum disulfide (MoS2) has been widely recognized as an efficient electrocatalyst for the hydrogen evolution reaction (HER), its practical implementation in clean hydrogen energy systems remains constrained by the sluggish kinetics of the oxygen evolution reaction (OER). This study presents a synergistic optimization strategy aimed at concurrently enhancing electron and proton transfer kinetics within MoS2-based OER systems. Through a facile solid-state mechanochemical protocol involving direct ball milling of commercial MoS2 with silver nitrate precursors, we successfully synthesized NO3−-grafted MoS2@Ag nanohybrids. Electrochemical evaluation in alkaline medium (1 M KOH) revealed exceptional OER performance, achieving a current density of 10 mA cm−2 at an overpotential of merely 259 mV, coupled with a Tafel slope of 98.84 mV·dec−1. Notably, the engineered nanohybrid demonstrated exceptional operational stability. Systematic characterization elucidated that the performance enhancement originated from two complementary mechanisms: (i) accelerated electron transfer kinetics through partial phase transition from semiconducting 2H-MoS2 to metallic 1 T-MoS2 coupled with Ag-induced electronic structure modulation and (ii) optimized proton transfer dynamics enabled by NO3−-mediated buffer effects that promote deprotonation of critical reaction intermediates.
全球能源需求的激增,加上化石燃料储量的减少,正在加速通过水电解清洁制氢的技术进步。虽然二硫化钼(MoS2)已被广泛认为是析氢反应(HER)的有效电催化剂,但其在清洁氢能源系统中的实际应用仍然受到析氧反应(OER)动力学缓慢的限制。本研究提出了一种协同优化策略,旨在同时增强基于mos2的OER系统中的电子和质子转移动力学。通过简单的固态机械化学方案,包括直接球磨商用二硫化钼与硝酸银前驱体,我们成功地合成了NO3−接枝MoS2@Ag纳米杂化。在碱性介质(1 M KOH)中的电化学评价显示出优异的OER性能,在过电位仅为259 mV的情况下,电流密度达到10 mA cm−2,塔菲尔斜率为98.84 mV·dec−1。值得注意的是,这种工程纳米混合材料表现出了优异的操作稳定性。系统表征表明,性能增强源于两个互补机制:(i)从半导体2H-MoS2到金属1 T-MoS2的部分相变加速了电子转移动力学,加上ag诱导的电子结构调制;(ii) NO3−介导的缓冲效应优化了质子转移动力学,促进了关键反应中间体的去质子化。
期刊介绍:
Ionics is publishing original results in the fields of science and technology of ionic motion. This includes theoretical, experimental and practical work on electrolytes, electrode, ionic/electronic interfaces, ionic transport aspects of corrosion, galvanic cells, e.g. for thermodynamic and kinetic studies, batteries, fuel cells, sensors and electrochromics. Fast solid ionic conductors are presently providing new opportunities in view of several advantages, in addition to conventional liquid electrolytes.