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Boosted Photoelectrochemical N2 Reduction over Mo2C In Situ Coated with Graphitized Carbon
Langmuir ( IF 3.9 ) Pub Date : 2020-11-24 , DOI: 10.1021/acs.langmuir.0c02770
Xia Li 1 , Weiqiang Fan 1 , Dongbo Xu 1 , Jinrui Ding 1 , Hongye Bai 1 , Weidong Shi 1
Affiliation  

Photoelectrochemical N2 reduction reaction (PEC NRR) is a promising method to solve the problems of environmental protection and energy sustainability. However, the strong chemical stability of the N≡N bond and competitive hydrogen evolution reaction (HER) cause the nonideal efficiency of N2 → NH3 conversion in actual operation. For the first time, a Mo2C/C heterostructure was fabricated as a PEC cathode for N2 reduction under environmental conditions. The Mo2C/C heterostructure could effectively decrease the coverage of hydrogen spillover and inhibit the competitive HER, resulting in a desirable selectivity for N2 activation. Meanwhile, the decoration of the C shell further promoted the stability and conductivity of Mo2C. Mo sites of Mo2C were considered as activation centers, which played a dominant role in the final PEC performance. An optimal NH3 yield rate of up to 6.6 μg h–1 mg–1 was achieved with the Mo2C/C heterostructure, which was almost 3 times that with pristine C. The faradic efficiency (FE) of the Mo2C/C heterostructure was 37.2% at 0.2 V (vs Ag/AgCl). This work not only provides an insight into the interplay between the Mo2C/C heterostructure and N2 activation, but also reveals its great potential in NH3 synthesis by a green route.

中文翻译:

石墨化碳原位包覆Mo 2 C促进光电化学N 2还原

光电化学N 2还原反应(PEC NRR)是解决环保和能源可持续性问题的一种有前途的方法。然而,N≡N键的强化学稳定性和竞争性的氢释放反应(HER)导致实际操作中N 2 →NH 3转化的非理想效率。首次制造了Mo 2 C / C异质结构作为PEC阴极,用于在环境条件下还原N 2。Mo 2 C / C异质结构可有效减少氢溢出的覆盖范围并抑制竞争性HER,从而对N 2具有理想的选择性激活。同时,C shell中的装饰进一步促进莫的稳定性和导电性2莫C. Mo位2 C下视为激活中心,其中在决赛中表现PEC起到了主导作用。Mo 2 C / C异质结构的最佳NH 3产率最高可达6.6μgh –1 mg –1,几乎是原始C的3倍。Mo 2 C / C的法拉第效率(FE)C异质结构在0.2 V(vs Ag / AgCl)下为37.2%。这项工作不仅提供了对Mo 2 C / C异质结构和N 2之间相互作用的深刻理解。活化,但也显示了其通过绿色途径在NH 3合成中的巨大潜力。
更新日期:2020-12-08
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