Liang Xingyou, Ren Xuefeng, Yang Qiyue, Gao Liguo, Gao Mengfan, Yang Yanan, Zhu Haiding, Li Guangxin, Ma Tingli, Liu Anmin
State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, China.
Nanoscale. 2021 Feb 7;13(5):2843-2848. doi: 10.1039/d0nr08744k. Epub 2021 Feb 1.
The conversion of nitrogen into ammonia is crucial for human activities. The electrochemical synthesis of ammonia from nitrogen and water is a green process with great application prospects; to this end, much effort has been made to improve the catalytic activity and selectivity. Here, a Co-based metal-organic framework (MOF), that is, zeolitic imidazolate framework-67 (ZIF-67), supported on a TiC MXene (defined as ZIF-67@TiC) was prepared via in situ growth. Due to the high porosity and large active surface area of the MOF and the superior conductivity of the TiC MXene, the composite could efficiently synthesize ammonia electrochemically. In particular, the prepared ZIF-67@TiC catalyst exhibited an excellent NH yield (6.52 μmol h cm), significantly higher than those achieved by TiC and ZIF-67 (2.77 and 1.61 μmol h cm, respectively) alone, and good Faraday efficiency (20.2%) at -0.4 V (vs. the reversible hydrogen electrode). This study not only expands the application of the MXene family in the electrochemical nitrogen reduction reaction but also provides ideas for the development of high-performance electrocatalysts for NRR.
氮转化为氨对人类活动至关重要。由氮和水进行电化学合成氨是一个具有巨大应用前景的绿色过程;为此,人们付出了很多努力来提高催化活性和选择性。在此,通过原位生长制备了一种负载在TiC MXene上的钴基金属有机框架(MOF),即沸石咪唑酯框架-67(ZIF-67)(定义为ZIF-67@TiC)。由于MOF的高孔隙率和大活性表面积以及TiC MXene的优异导电性,该复合材料能够高效地电化学合成氨。特别地,制备的ZIF-67@TiC催化剂表现出优异的NH产率(6.52 μmol h cm),显著高于单独的TiC和ZIF-67(分别为2.77和1.61 μmol h cm)所达到的产率,并且在-0.4 V(相对于可逆氢电极)时具有良好的法拉第效率(20.2%)。这项研究不仅扩展了MXene家族在电化学氮还原反应中的应用,还为开发用于NRR的高性能电催化剂提供了思路。