Searching for low-cost non-Pt catalysts for oxygen reduction reaction (ORR) has been a key scientific issue in the development of fuel cells. In this work, the potential of utilizing the experimentally available two-dimensional (2D) Fe-phthalocyanine (Fe-Pc) monolayer with precisely-controlled distribution of Fe atoms as a catalyst of ORR was systematically explored by means of comprehensive density functional theory computations. The computations revealed that O2 molecules can be sufficiently activated on the surface of the Fe-Pc monolayer, and the subsequent ORR steps prefer to proceed on the Fe-Pc monolayer through a more efficient 4e pathway with a considerable limiting potential of 0.68 V. Especially, the Fe-Pc monolayer is more stable than the Fe-Pc molecule in acidic medium, and can present good catalytic performance for ORR on the addition of axial ligands. Therefore, the Fe-Pc monolayer is quite a promising single-atom-catalyst with high efficiency for ORR in fuel cells.
Background
Microbial electrosynthesis (MES) is a biocathode-driven process, in which electroautotrophic microorganisms can directly uptake electrons or indirectly via H
2
from the cathode as energy sources and CO
2
as only carbon source to produce chemicals.
Results
This study demonstrates that a hydrogen evolution reaction (HER) catalyst can enhance MES performance. An active HER electrocatalyst molybdenum carbide (Mo
2
C)-modified electrode was constructed for MES. The volumetric acetate production rate of MES with 12 mg cm
−2
Mo
2
C was 0.19 ± 0.02 g L
−1
day
−1
, which was 2.1 times higher than that of the control. The final acetate concentration reached 5.72 ± 0.6 g L
−1
within 30 days, and coulombic efficiencies of 64 ± 0.7% were yielded. Furthermore, electrochemical study, scanning electron microscopy, and microbial community analyses suggested that Mo
2
C can accelerate the release of hydrogen, promote the formation of biofilms and regulate the mixed microbial flora.
Conclusion
Coupling a HER catalyst to a cathode of MES system is a promising strategy for improving MES efficiency.
Electronic supplementary material
The online version of this article (10.1186/s13068-019-1413-z) contains supplementary material, which is available to authorized users.
pH-gated ion channels in cell membranes play important roles in the cell's physiological activities. Many artificial nanochannels have been fabricated to mimic the natural phenomenon of pH-gated ion transport. However, these nanochannels show pH sensitivity only within certain pH ranges. Wide-range pH sensitivity has not yet been achieved. Herein, for the first time, we provide a versatile strategy to increase the pH-sensitive range by using dual amphoteric nanochannels. In particular, amphoteric polymeric nanochannels with carboxyl groups derived from a block copolymer (BCP) precursor and nanochannels with hydroxyl groups made from anodic alumina oxide (AAO) were used. Due to a synergistic effect, the hybrid nanochannels exhibit nanofluidic diode properties with single rectification direction over a wide pH range. The novel strategy presented here is a scalable, low-cost, and robust alternative for the construction of large-area membranes for nanofluidic applications, such as the separation of biomolecules.
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