Competitive Coordination-Oriented Monodispersed Ruthenium Sites in Conductive MOF/LDH Hetero-Nanotree Catalysts for Efficient Overall Water Splitting in Alkaline Media,Advanced Materials

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Competitive Coordination-Oriented Monodispersed Ruthenium Sites in Conductive MOF/LDH Hetero-Nanotree Catalysts for Efficient Overall Water Splitting in Alkaline Media
Advanced Materials ( IF 27.4 ) Pub Date : 2022-01-10 , DOI: 10.1002/adma.202107488
Ying Wang ₁ , Shuo Wang ₁ , Ze-Lin Ma ₂ , Li-Ting Yan ₃ , Xue-Bo Zhao ₃ , Ying-Ying Xue ₁ , Jia-Min Huo ₁ , Xiao Yuan ₁ , Shu-Ni Li ₁ , Quan-Guo Zhai ₁

Affiliation

Rational exploration of efficient, inexpensive, and robust electrocatalysts is critical for the efficient water splitting. Conjugated conductive metal–organic frameworks (cMOFs) with multicomponent layered double hydroxides (LDHs) to construct bifunctional heterostructure catalysts are considered as an efficient but complicated strategy. Here, the fabrication of a cMOF/LDH hetero-nanotree array catalyst (CoNiRu-NT) coupled with monodispersed ruthenium (Ru) sites via a controllable grafted-growth strategy is reported. Rich-amino hexaiminotriphenylene linkers coordinate with the LDH nanotrunk to form cMOF nanobranches, providing numerous anchoring sites to precisely confine and stabilize RuN₄ sites. Moreover, monodispersed and reduced Ru moieties facilitate H₂O adsorption and dissociation, and the heterointerface between the cMOF and the LDH further modifies the chemical and electronic structures. Optimized CoNiRu-NT displays a significant increase in electrochemical water-splitting properties in alkaline media, affording low overpotentials of 22 mV at 10 mA cm⁻² and 255 mV at 20 mA cm⁻² for the hydrogen evolution reaction and oxygen evolution reaction, respectively. In an actual electrochemical system, CoNiRu-NT drives an overall water splitting at a low cell voltage of 1.47 V to reach 10 mA cm⁻². This performance is comparable to that of pure noble-metal-based materials and superior to most reported MOF-based catalysts.

中文翻译：

导电 MOF/LDH 杂纳米树催化剂中的竞争性配位定向单分散钌位点用于碱性介质中的高效整体水分解

合理探索高效、廉价和稳健的电催化剂对于高效的水分解至关重要。共轭导电金属有机骨架（cMOFs）与多组分层状双氢氧化物（LDHs）构建双功能异质结构催化剂被认为是一种有效但复杂的策略。本文报道了通过可控接枝生长策略与单分散钌 (Ru) 位点耦合的 cMOF/LDH 异质纳米树阵列催化剂 (CoNiRu-NT) 的制备。富氨基六亚氨基苯并苯连接体与 LDH 纳米主干配合形成 cMOF 纳米支链，提供大量锚定位点来精确限制和稳定 Ru N 4_位点。此外，单分散和还原的Ru部分有利于H ₂O 吸附和解离，以及cMOF和LDH之间的异质界面进一步改变了化学和电子结构。优化的 CoNiRu-NT 在碱性介质中显示出显着提高的电化学水分解性能，分别在 10 mA cm ^{-2和 20 mA cm}^-2下提供 22 mV 的低过电位和 255 mV的析氢反应和析氧反应。 . 在实际的电化学系统中，CoNiRu-NT 在 1.47 V 的低电池电压下驱动整体水分解达到 10 mA cm ^-2。这种性能与纯贵金属基材料相当，优于大多数报道的 MOF 基催化剂。

更新日期：2022-01-10

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