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用于在氮化钛上负载亚2纳米钌纳米团簇的热冲击合成法,作为一种用于析氢反应的卓越电催化剂。

Thermal Shock Synthesis for Loading Sub-2 nm Ru Nanoclusters on Titanium Nitride as a Remarkable Electrocatalyst toward Hydrogen Evolution Reaction.

作者信息

Zong Lingbo, Lu Fenghong, Li Ping, Fan Kaicai, Zhan Tianrong, Liu Porun, Jiang Lixue, Chen Dehong, Zhang Ruiyong, Wang Lei

机构信息

International Cooperation United Laboratory of Eco-chemical Engineering and Green Manufacturing, Technology Innovation Center of Battery Safety and Energy Storage Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China.

Centre for Catalysis and Clean Energy Gold Coast Campus, Griffith University, Gold Coast, QLD, 4222, Australia.

出版信息

Adv Mater. 2024 Aug;36(32):e2403525. doi: 10.1002/adma.202403525. Epub 2024 Jun 7.

DOI:10.1002/adma.202403525
PMID:38762765
Abstract

Heterogeneous catalysts embracing metal entities on suitable supports are profound in catalyzing various chemical reactions, and substantial synthetic endeavors in metal-support interaction modulation are made to enhance catalytic performance. Here, it is reported the loading of sub-2 nm Ru nanocrystals (NCs) on titanium nitride support (HTS-Ru-NCs/TiN) via a special Ru-Ti interaction using the high-temperature shock (HTS) method. Direct dechlorination of the adsorbed RuCl, ultrafast nucleation process, and short coalescence duration at ultrahigh temperatures contribute to the immobilization of Ru NCs on TiN support via producing the Ru-Ti interfacial perimeter. HTS-Ru-NCs/TiN shows remarkable activity toward hydrogen evolution reaction (HER) in alkaline solution, yielding ultralow overpotentials of 16.3 and 86.6 mV to achieve 10 and 100 mA cm, respectively. The alkaline and anion exchange membrane water electrolyzers assembled using HTS-Ru-NCs/TiN yield 1.0 A cm at 1.65 and 1.67 V, respectively, which validate its applicability in the hydrogen production industry. Theoretical simulations reveal the favorable formation of Ru─O and Ti─H bonds at the interfacial perimeters between Ru NCs and TiN, which accelerates the prerequisite water dissociation kinetics for enhanced HER activity. This exemplified work motivates the design of specific interfacial perimeters via the HTS strategy to improve the performance of diverse catalysis.

摘要

包含在合适载体上的金属实体的多相催化剂在催化各种化学反应方面具有深远意义,并且人们在调节金属-载体相互作用方面进行了大量的合成努力以提高催化性能。在此,报道了通过高温冲击(HTS)方法利用特殊的Ru-Ti相互作用将亚2纳米Ru纳米晶体(NCs)负载在氮化钛载体上(HTS-Ru-NCs/TiN)。吸附的RuCl的直接脱氯、超快成核过程以及在超高温下的短聚并持续时间有助于通过产生Ru-Ti界面周长将Ru NCs固定在TiN载体上。HTS-Ru-NCs/TiN在碱性溶液中对析氢反应(HER)表现出显著活性,分别产生16.3和86.6 mV的超低过电位以达到10和100 mA cm⁻²。使用HTS-Ru-NCs/TiN组装的碱性和阴离子交换膜水电解槽分别在1.65和1.67 V下产生1.0 A cm⁻²,这验证了其在制氢工业中的适用性。理论模拟揭示了在Ru NCs和TiN之间的界面周长处有利地形成Ru─O和Ti─H键,这加速了增强HER活性所需的水离解动力学。这项示例工作推动了通过HTS策略设计特定的界面周长以提高各种催化的性能。

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引用本文的文献

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