Monodisperse Os-O-Co Modules Enable Ampere-Level Hydrazine-Assisted Seawater Splitting in Membraneless Electrolyzers

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yafei Feng, Shao Wang, Yin Zhu, Hui Xie, Yangyang Zhang, Mingyu Cheng, Xiaoyue He, Yanxu Chen, Chong Xiao, Genqiang Zhang, Yi Xie
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Abstract

Hydrazine oxidation-assisted seawater electrolysis (HzOR-SWE) is critical for addressing freshwater scarcity and energy crises. However, the development of this technology has been significantly impeded by the absence of efficient catalysts capable of cleaving N─H bonds during the hydrazine oxidation reaction (HzOR). Herein, Monodispersed Os-O-Co modules are constructed within a cobalt hydroxide structure via an in situ osmium (Os) single-atom modification strategy to serve as a bifunctional catalyst. The d-p orbital hybridization in the structure shifts the d-band center of Os sites away from the Fermi level, weakening the adsorption energy of reaction intermediates and exhibiting the lowest N─H dehydrogenation energy barrier for HzOR and moderate active hydrogen adsorption energy for hydrogen evolution reaction (HER). When integrated into a membraneless flow cell (MFC), the catalyst demonstrates exceptional performance in HzOR-SWE, requiring only 0.768 V to deliver 1.0 A cm−2 with a remarkable rate of 31.9 moles of hydrogen per kilowatt-hour (kWh). This represents a 70.7% energy saving compared to conventional seawater splitting systems (2.62 V, 7.6 kWh mol−1). This work holds significant importance for advancing the economic viability of low-energy seawater electrolysis for hydrogen production.

Abstract Image

单分散Os-O-Co模块可在无膜电解槽中实现安培级肼辅助海水分解
联氨氧化辅助海水电解是解决淡水短缺和能源危机的关键技术。然而,由于缺乏在肼氧化反应(HzOR)中能够切割N─H键的有效催化剂,该技术的发展受到了很大的阻碍。本文通过原位锇(Os)单原子修饰策略,在氢氧化钴结构中构建单分散Os- o - co模块,作为双功能催化剂。结构中的d-p轨道杂化使Os位的d带中心远离费米能级,削弱了反应中间体的吸附能,HzOR表现出最低的N─H脱氢能垒,而析氢反应(HER)表现出中等的活性氢吸附能。当集成到无膜流动电池(MFC)中时,该催化剂在HzOR-SWE中表现出优异的性能,仅需要0.768 V就可以提供1.0 a cm - 2,并且每千瓦时(kWh)的速率为31.9摩尔氢。与传统的海水分解系统(2.62 V, 7.6 kWh mol - 1)相比,这节省了70.7%的能源。这项工作对推进低能耗海水电解制氢的经济可行性具有重要意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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