Single-atom catalysts templated by metal–organic frameworks for electrochemical nitrogen reduction

Zhang, Rui; Jiao, Long; Yang, Weijie; Wan, Gang; Jiang, Hai-Long

doi:10.1039/C9TA10206J

Title: Single-atom catalysts templated by metal–organic frameworks for electrochemical nitrogen reduction

Journal Article · Thu Oct 24 00:00:00 EDT 2019 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/C9TA10206J· OSTI ID:1583128

Zhang, Rui ^[1]; Jiao, Long ^[1];

^[2]; Wan, Gang ^[3];

^[4]

Univ. of Science and Technology of China, Hefei (China)
Univ. of Science and Technology of China, Hefei (China); North China Electric Power Univ., Baoding (China)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Univ. of Science and Technology of China, Hefei (China); Chinese Academy of Sciences (CAS), Fuzhou (China)

The electrocatalytic nitrogen reduction reaction (NRR) offers much prospect for substituting the energy-consuming Haber–Bosch process. Nevertheless, its sluggish reaction kinetics and the competing hydrogen evolution reaction always result in limited ammonia yield and low faradaic efficiency (FE). Here, an Fe-decorated porphyrinic metal–organic framework (MOF) is employed as a precursor to construct single-atom Fe implanted nitrogen-doped carbon catalysts (Fe₁-N-C) through a mixed ligand strategy. Benefiting from the highly dispersed single-atom Fe sites, hierarchically porous structure and good conductivity, Fe₁-N-C shows a FE of 4.51% and an ammonia yield rate of 1.56 × 10^-11 mol cm^-2 s^-1 at -0.05 V versus the reversible hydrogen electrode, superior to those of Co₁-N-C and Ni₁-N-C. Theoretical calculations show that Fe₁-N-C shows the lowest energy barrier of the rate-determining step during the NRR process, consistent with its highest activity obtained in experiments. This work reveals the unique potential of single-atom catalysts for the electrochemical NRR and provides in-depth insights into the catalytic mechanism of the NRR.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515; 21725101, 21871244, 21521001; 2019TQ0298; WK2060030029

OSTI ID:: 1583128

Journal Information:: Journal of Materials Chemistry. A, Vol. 7, Issue 46; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 103 works

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