Green Electrosynthesis of 5,5′-Azotetrazolate Energetic Materials Plus Energy-Efficient Hydrogen Production Using Ruthenium Single-Atom Catalysts
Green Electrosynthesis of 5,5′-Azotetrazolate Energetic Materials Plus Energy-Efficient Hydrogen Production Using Ruthenium Single-Atom Catalysts
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DOI：
10.1002/adma.202203900
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发表时间：
2022-07-05
影响因子：
29.4
通讯作者：
Qiu, Jieshan
中科院分区：
文献类型：
--
作者：
Li, Jiachen;Zhang, Cong;Qiu, Jieshan
水电解涉及两个并行的反应，即析氧（OER）和析氢（HER），其中缓慢的OER是导致高能耗的显著限制步骤。将有机替代品的热动力学有利的电氧化与增值精细化学品HER相结合是同时具有成本效益地生产增值化学品和氢气的有前途的方法。介绍了一种新的有机含能材料绿色电化学合成与单原子催化制氢耦合体系。该催化剂通过简单的钌单原子在硒化钼上的恒电流沉积而制备，并且在碱性介质中在-10 mA cm（-2）下显示出38.9 mV的低HER过电位。更重要的是，通过将水裂解与5-氨基-1H-四唑的电氧化耦合来合成5，5 '-偶氮四唑含能材料，可以将水电解的槽电压在10 mA cm（-2）的电流下显著降低到仅1.35 V。这些材料传统上是在苛刻的条件下合成的，包括强氧化剂、高温条件和难以分离的副产物。本研究提供了一种绿色高效的合成有机EM同时制氢的方法。
Water electrolysis involves two parallel reactions, that is, oxygen evolution (OER) and hydrogen evolution (HER), in which sluggish OER is a significant limiting step that results in high energy consumption. Coupling the thermo-dynamically favorable electrooxidation of organic alternatives to value-added fine chemicals HER is a promising approach for the simultaneous cost-effective production of value-added chemicals and hydrogen. Here, a new coupling system for the green electrochemical synthesis of organic energetic materials (EMs) plus hydrogen production using single-atom catalysts is introduced. The catalysts are prepared by the facile galvanostatic deposition of ruthenium single atoms on the molybdenum selenide and reveal a low HER overpotential of 38.9 mV at -10 mA cm(-2) in an alkaline medium. Importantly, the cell voltage of water electrolysis can be significantly reduced to only 1.35 V at a current of 10 mA cm(-2) by coupling water splitting with the electrooxidation of 5-amino-1H-tetrazole to synthesize 5,5'-azotetrazolate energetic material. These materials are traditionally synthesized under harsh conditions involving a strong oxidizing agent, high-temperature conditions, and difficult separation of by-products. This study provides a green and efficient method of synthesizing organic EMs while simultaneously producing hydrogen.