Enabling Efficient Oxygen Evolution via Anchoring Carbon-Layer-Confined RuOx on a Well-Matched Substrate

IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Liming Zeng, Bang Yuan, Qing Zhou
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Abstract

Oxygen evolution reaction (OER) is a multistep proton-coupled four-electron process with sluggish kinetics, which seriously limits the hydrogen production efficiency, thus it is of great importance to develop an efficient and stable OER catalyst. In this study, a two-step differential pyrolysis strategy is employed to design a three-dimensional porous microstructured material consisting of RuOx nanoparticles coated by a thin-layer carbon, where the active particles were isolated in separate chambers and the RuOx nanoparticles mainly existed in the form of a heterogeneous interface between RuO2 and partial metallic Ru. The preparation parameters of the catalysts are optimized via combining transient and steady-state polarization properties, and the target catalyst Cat-500–1.5t shows the best OER catalytic performance after ca. 60 h of a chronopotentiometry test in an acidic medium with a much smaller performance change than other samples. The unique design of adopting a carbon layer to form separate reaction chambers largely mitigates the excessive oxidation loss of the active components under strong oxidation potential. The suitability of the catalyst with the loaded substrate and test media is explored, and in an acidic medium, the carbon paper is much better than the titanium fiber, while in an alkaline medium, the titanium fiber is obviously superior to the carbon paper. On both carbon paper and titanium fiber, the performance in an alkaline medium outperforms that in an acidic medium, and the possible reasons for the performance difference are analyzed. Herein, to obtain the actual electrocatalytic performance, the optimal design of the catalyst structure and matching suitable conductive substrate in a specific medium are quite necessary, which provides a feasible strategy for the acquisition of efficient and stable electrocatalysts and the desirable presentation of performance.

Abstract Image

通过在匹配良好的基底上锚定碳层限制的 RuOx,实现高效氧气进化
氧进化反应(OER)是一个多步骤质子耦合四电子过程,其动力学缓慢,严重限制了制氢效率,因此开发一种高效稳定的 OER 催化剂具有重要意义。本研究采用两步差热分解策略设计了一种由纳米 RuOx 粒子包覆薄层碳组成的三维多孔微结构材料,其中活性粒子被隔离在不同的腔室中,纳米 RuOx 粒子主要以 RuO2 和部分金属 Ru 的异质界面形式存在。通过结合瞬态和稳态极化特性,对催化剂的制备参数进行了优化,目标催化剂 Cat-500-1.5t 在经过约 60 h 的慢动作催化后显示出最佳的 OER 催化性能。目标催化剂 Cat-500-1.5t 在酸性介质中经过约 60 小时的计时电位测试后,显示出最佳的 OER 催化性能,其性能变化远远小于其他样品。采用碳层形成独立反应室的独特设计在很大程度上减轻了活性成分在强氧化电位下的过度氧化损失。在酸性介质中,碳纸的性能远优于钛纤维,而在碱性介质中,钛纤维则明显优于碳纸。碳纸和钛纤维在碱性介质中的性能均优于酸性介质,并分析了造成性能差异的可能原因。由此可见,要获得实际的电催化性能,催化剂结构的优化设计和在特定介质中匹配合适的导电基底是十分必要的,这为获得高效稳定的电催化剂和理想的性能表现提供了可行的策略。
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来源期刊
Langmuir
Langmuir 化学-材料科学:综合
CiteScore
6.50
自引率
10.30%
发文量
1464
审稿时长
2.1 months
期刊介绍: Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).
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