Bifunctional 2D superlattice electrocatalysts of alternating layered double hydroxide (LDH)–transition metal dichalcogenide (TMD) heterolayers were synthesized by interstratification of the exfoliated nanosheets. Density functional theory calculations predict an increased interfacial charge transfer between interstratified LDH and TMD nanosheets, which would lead to enhanced electrocatalytic activity. The electrostatically driven self-assembly of oppositely charged 2D building blocks, i.e., exfoliated Ni–Al-LDH/Ni–Fe-LDH and MoS₂ nanosheets, yields mesoporous heterolayered Ni–Al-LDH–MoS₂/Ni–Fe-LDH–MoS₂ superlattices. The synthesized superlattices show improved electrocatalytic activity with enhanced durability for oxygen and hydrogen evolution reactions and water splitting. The interstratification improves the chemical stability of LDH in acidic media, thus expanding its possible applications. The high electrocatalytic activity of the superlattices may be attributed to an enhanced affinity for OH^–/H⁺, improved electrical conduction and charge transfer, and the increase of active sites. This study indicates that the formation of superlattices via self-assembly of 2D nanosheets provides useful methodology to explore high-performance electrocatalysts with improved stability.

中文翻译：

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层状双氢氧化物-过渡金属二硫属元素化物的双功能二维超晶格活性催化剂可用于总水分解

通过分层剥离的纳米片，合成了交替层状双氢氧化物（LDH）-过渡金属二卤化硅（TMD）杂层的双功能二维超晶格电催化剂。密度泛函理论计算预测，层状的LDH和TMD纳米片之间的界面电荷转移会增加，这将导致增强的电催化活性。带有相反电荷的2D构建块的静电驱动自组装，即，剥落的Ni-Al-LDH / Ni-Fe-LDH和MoS ₂纳米片，产生了介孔杂层Ni-Al-LDH-MoS ₂ / Ni-Fe-LDH-硫化钼₂超晶格。合成的超晶格显示出改进的电催化活性，并且对氧和氢的逸出反应和水分解具有增强的耐久性。互层化提高了LDH在酸性介质中的化学稳定性，从而扩展了其可能的应用。超晶格的高电催化活性可能归因于对OH的增强的亲和力^- / H ⁺，改进的电传导和电荷转移，并且活性位点的增加。这项研究表明，通过2D纳米片的自组装形成超晶格提供了探索具有改进稳定性的高性能电催化剂的有用方法。