Chao Ge, Jing Li, Bin He, Yunlan Gu, Yawen Tang, Tongfei Li
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In situ Raman spectroscopic analysis reveals that the strategic construction of the n-p heterojunction not only dramatically facilitates the surface reconstruction of NiO to yield authentic NiOOH active species, but also substantially lowers the formation energy barrier for oxygen-containing intermediates during the OER, thereby markedly enhancing the overall catalytic efficiency of the reaction. 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引用次数: 0
摘要
寻求通过可再生电力驱动的水分解高效“绿色”制氢面临着深刻的挑战,最明显的是催化性能的逐步恶化,以及在工业相关的高电流条件下大规模运输效率低下所带来的重大限制。为了克服这些艰巨的挑战,我们通过简单的静电纺丝和煅烧后介导的界面设计,设计了一种结构精致,富氧空位的SnO2/NiO n-p空心纳米管结构异质结构(称为SnO2/NiO HNTs)。基于中空纳米纤维结构,这种创新的界面协调形成了一种具有催化能力的结构,赋予了双重功能优点:(1)一个电子定制的富氧表面,精确地调节氧中间体的吸附能量;(2)一个精心设计的三维(3D)多孔框架,由一维(1D)纳米纤维组成,促进快速气泡释放和有效的电解质渗透。这种和谐的结构协同作用使SnO2/NiO HNTs电极在电流密度为10 mA cm-2时获得200 mV的超低析氧反应(OER)过电位,同时保持90小时以上的稳定运行。原位拉曼光谱分析表明,n-p异质结的战略性构建不仅极大地促进了NiO的表面重构,生成真正的NiOOH活性物质,而且大大降低了OER过程中含氧中间体的形成能垒,从而显著提高了反应的整体催化效率。所展示的具有n-p异质结的界面工程策略为克服高速率析气电催化的质量输运限制提供了一种通用的设计范式。
The quest for efficient “green” hydrogen generation through renewable electricity-powered water splitting confronts profound challenges, most notably the progressive deterioration of catalytic performance and significant constraints imposed by mass transport inefficiencies under industrially pertinent high-current conditions. To overcome these formidable challenges, we have engineered a structurally refined, oxygen-vacancy-enriched SnO2/NiO n-p hollow nanotube-structured heterostructure (denoted as SnO2/NiO HNTs) via a facile electrospinning and post-calcination-mediated interfacial design. Rooted in a hollow nanofibers structure, this innovative interface orchestrates the formation of a catalytically potent architecture, bestowing dual functional merits: (1) an electronically tailored oxygen-enriched surface that precisely tunes the adsorption energetics of oxygen intermediates, and (2) a meticulously engineered three-dimensional (3D) porous framework composed of one-dimensional (1D) nanofibers that promotes swift bubble release and efficient electrolyte penetration. This harmonious architectural synergy empowers the SnO2/NiO HNTs electrode to attain a remarkably low oxygen evolution reaction (OER) overpotential of 200 mV at a current density of 10 mA cm-2, while sustaining robust operational stability beyond 90 hours. In situ Raman spectroscopic analysis reveals that the strategic construction of the n-p heterojunction not only dramatically facilitates the surface reconstruction of NiO to yield authentic NiOOH active species, but also substantially lowers the formation energy barrier for oxygen-containing intermediates during the OER, thereby markedly enhancing the overall catalytic efficiency of the reaction. The demonstrated interface engineering strategy with n-p heterojunction provides a generalized design paradigm for overcoming mass transport limitations in high-rate gas evolution electrocatalysis.
期刊介绍:
Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.