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使用钌单原子催化剂实现5,5'-偶氮四唑含能材料的绿色电合成及高效产氢

Green Electrosynthesis of 5,5'-Azotetrazolate Energetic Materials Plus Energy-Efficient Hydrogen Production Using Ruthenium Single-Atom Catalysts.

作者信息

Li Jiachen, Zhang Cong, Zhang Chi, Ma Huijun, Guo Zhaoqi, Zhong Chenglin, Xu Ming, Wang Xuanjun, Wang Yaoyu, Ma Haixia, Qiu Jieshan

机构信息

Xi'an Key Laboratory of Special Energy Materials, School of Chemical Engineering, Northwest University, Xi'an, 710069, China.

Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry & Materials Science, Northwest University, Xi'an, 710127, China.

出版信息

Adv Mater. 2022 Aug;34(32):e2203900. doi: 10.1002/adma.202203900. Epub 2022 Jul 5.

Abstract

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 thermodynamically 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 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 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.

摘要

水电解涉及两个平行反应,即析氧反应(OER)和析氢反应(HER),其中缓慢的析氧反应是导致高能耗的一个重要限制步骤。将有机替代物进行热力学有利的电氧化与析氢反应耦合,以同时经济高效地生产增值化学品和氢气,是一种很有前景的方法。在此,介绍了一种使用单原子催化剂进行有机含能材料(EMs)绿色电化学合成与制氢的新型耦合系统。这些催化剂通过将钌单原子简便地恒电流沉积在硒化钼上制备而成,在碱性介质中,于-10 mA cm时显示出38.9 mV的低析氢过电位。重要的是,通过将水分解与5-氨基-1H-四唑的电氧化耦合以合成5,5'-偶氮四唑含能材料,在10 mA cm的电流下,水电解的电池电压可显著降低至仅1.35 V。这些材料传统上是在涉及强氧化剂、高温条件以及副产物难以分离的苛刻条件下合成的。本研究提供了一种绿色高效的合成有机含能材料的方法,同时还能制氢。

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