Bimetallic metal–organic framework-derived MoFe-PC microspheres for electrocatalytic ammonia synthesis under ambient conditions†,Journal of Materials Chemistry A

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Bimetallic metal–organic framework-derived MoFe-PC microspheres for electrocatalytic ammonia synthesis under ambient conditions†
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2019-12-30 , DOI: 10.1039/c9ta10524g
Silong Chen _{1,

2,

3,

4,

5} , Haeseong Jang _{6,

7,

8,

9} , Jia Wang _{1,

2,

3,

4,

5} , Qing Qin _{1,

2,

3,

4,

5} , Xien Liu _{1,

2,

3,

4,

5} , Jaephil Cho _{6,

7,

8,

9}

Affiliation

Developing high-efficiency electrocatalysts for artificial nitrogen fixation at room temperature and atmospheric pressure is fundamentally important but challenging. Herein, MoFe-PC (PC, phosphorus-doped carbon) microspheres, synthesized by facile one-step pyrolysis–phosphating of bimetallic metal–organic framework (MOF) precursors, were used as a cost-efficient catalyst for the electrocatalytic nitrogen reduction reaction (NRR). With the advantageous characteristics of the multicomponent active sites and porous structure inherited from the MOF precursor, the MoFe-PC catalyst achieves a peak NH₃ yield rate of 34.23 μg h⁻¹ mg_cat.⁻¹ with a high faradaic efficiency (FE) of 16.83% at −0.5 V vs. a reversible hydrogen electrode (RHE) in 0.1 M HCl under ambient conditions, exceeding those of most of the previously reported noble metal- or non-noble metal-based NRR electrocatalysts under the same conditions. The changes of the surface composition and structure of the catalyst before and after NRR testing are monitored by ex situ XPS and XANES. The Mo and Fe oxides and PC in the hybrids are both active in the NRR, synergistically enhancing the NRR performance.

中文翻译：

双金属金属-有机骨架衍生的MoFe-PC微球在环境条件下用于电催化氨合成†

开发在室温和大气压下用于人工固氮的高效电催化剂从根本上来说很重要，但具有挑战性。在这里，通过简单的一步热解-双金属金属-有机骨架（MOF）前体的磷化反应合成的MoFe-PC（PC，掺磷碳）微球被用作电催化氮还原反应的经济高效催化剂（ NRR）。凭借从MOF前体继承的多组分活性位点和多孔结构的有利特性，MoFe-PC催化剂可实现34.23μgh ^-1 mg _cat的NH ₃峰值产率_。^-1与16.83％在-0.5伏的高法拉第效率（FE）与在环境条件下在0.1 M HCl中使用可逆氢电极（RHE），在相同条件下超过了大多数以前报道的基于贵金属或非贵金属的NRR电催化剂的可逆氢电极（RHE）。之前和NRR试验后的催化剂的表面的组成和结构的变化是由监控易地XPS和XANES。杂化物中的Mo和Fe氧化物以及PC均在NRR中具有活性，从而协同增强NRR的性能。

更新日期：2020-01-09

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