Highly Active and Stable Nitrogen-Doped Ruthenium Oxide/Titanium Nitride Composite Anode Electrocatalyst for Practical Proton Exchange Membrane Water Electrolyzers
Heng Zhang, Lili Liu, Liu Pei, Dongdong Wang, Xingdong Wang
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引用次数: 0
Abstract
The application of ruthenium-based catalysts in proton-exchange membrane water electrolyzers is impeded by lattice oxygen mechanism and the subsequent structural collapse. Herein, a design strategy for the preparation of N-doped RuO₂ using TiN nanoparticles as the nitrogen source is presented. The in- situ characterization and theoretical calculation reveal the optimized oxygen evolution reaction (OER) mechanism on the resulting N-RuO2/TiN catalyst. The incorporation of low-electronegativity N and the formation of interfacial Ru−O−Ti bridge structure lead to the redistribution of electron density on adjacent Ru sites, weakening the Ru–O covalency and inhibiting the reactivity of lattice oxygen during electrocatalytic OER. Meanwhile, the altered electronic structures also optimize the adsorption energy of intermediates, consequently facilitating the formation of the pivotal intermediate *OOH and enhancing the electrocatalytic activity. The N-RuO2/TiN electrocatalyst displays a extremely low OER overpotential of 159 mV at 10 mA cm−2 in 0.5 m H2SO4. Particularly, the water electrolysis single cell with N-RuO2/TiN as anode electrocatalyst conveys an extremely low voltage of 1.78 V at 3A cm−2 and degradation rate of 26 µV h−1 during a 1100 h operation at 1 A cm−2. This work also provides an excellent catalyst for industrial-level electrolysis.
钌基催化剂在质子交换膜水电解槽中的应用受到晶格氧机制和随后的结构崩溃的阻碍。本文提出了一种以TiN纳米颗粒为氮源制备氮掺杂的RuO₂的设计策略。原位表征和理论计算揭示了优化后的N-RuO2/TiN催化剂的析氧反应机理。在电催化OER过程中,低电负性N的加入和界面Ru - O - Ti桥结构的形成导致电子密度在相邻的Ru位点上重新分布,削弱了Ru - O共价,抑制了晶格氧的反应活性。同时,改变的电子结构也优化了中间体的吸附能,从而促进了关键中间体*OOH的形成,提高了电催化活性。N-RuO2/TiN电催化剂在0.5 m H2SO4中,在10 mA cm−2条件下显示出极低的OER过电位,为159 mV。特别是,以N-RuO2/TiN为阳极电催化剂的水电解单体电池在3A cm−2下的电压极低,为1.78 V,在1a cm−2下运行1100小时,降解率为26 μ V h−1。这项工作也为工业电解提供了一种极好的催化剂。
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.