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In Situ Synthesis of MoS2 on C3N4 To Form MoS2/C3N4 with Interfacial Mo–N Coordination for Electrocatalytic Reduction of N2 to NH3
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-05-25 , DOI: 10.1021/acssuschemeng.0c02763
Ziming Zhao 1 , Sha Luo 1 , Ping Ma 1 , Yutong Luo 1 , Wei Wu 1 , Yu Long 1 , Jiantai Ma 1
Affiliation  

Electrocatalytic nitrogen reduction reaction (NRR), as an alternative to synthetic ammonia under mild condition, provides a promising method for storage and sustainable utilization of ammonia. However, the catalytic performance of the NRR electrocatalyst still requires a systematical investigation and improvement. Herein, this paper reports that MoS2/C3N4 is prepared by in situ controllable synthesis through a one-step pyrolysis process of thiourea and ammonium molybdate. A thorough characterization reveals that the strong interactions between MoS2 and C3N4 of MoS2/C3N4 lead to the formation of an interface with Mo–N coordination, which promotes electron transfer across the MoS2/C3N4 interface. Meanwhile, it is clarified that the formation of interfacial Mo–N coordination is beneficial to improve the catalytic activity and acts as the main active sites for catalyzing NRR. As a result, the as-prepared electrocatalyst exhibits an excellent NH3 yield rate of 19.86 μg h–1 mgcat.–1 and an enhanced faradaic efficiency of 6.87% at −0.5 V (vs reversible hydrogen electrode) in 0.1 M Na2SO4, placing it as one of the most promising NRR electrocatalysts.

中文翻译:

Mo 3界面配位在C 3 N 4上原位合成MoS 2形成MoS 2 / C 3 N 4,用于电催化还原N 2为NH 3

电催化氮还原反应(NRR)作为温和条件下合成氨的替代物,为氨的存储和可持续利用提供了一种有前途的方法。但是,NRR电催化剂的催化性能仍然需要系统的研究和改进。本文中,本文报道了MoS 2 / C 3 N 4是通过硫脲和钼酸铵的一步热解过程通过原位可控制合成制备的。彻底的表征表明,MoS 2 / C 3 N 4的MoS 2和C 3 N 4之间有很强的相互作用导致形成具有Mo–N配位的界面,从而促进电子跨MoS 2 / C 3 N 4界面的转移。同时,阐明了Mo-N界面配位的形成有利于提高催化活性,并作为催化NRR的主要活性中心。结果,所制备的电催化剂显示出出色的NH 3产率,为19.86μgh –1 mg cat。–1和在0.1 M Na 2 SO 4中在-0.5 V(相对于可逆氢电极)下的法拉第效率提高了6.87%,使其成为最有希望的NRR电催化剂之一。
更新日期:2020-05-25
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