Issue 4, 2022

Fabrication of an amorphous metal oxide/p-BiVO4 photocathode: understanding the role of entropy for reducing nitrate to ammonia

Abstract

The controllable design of chemical microenvironment with the expected thermodynamics and kinetics for boosting catalytic activity and selectivity presents a challenge. Herein, an amorphous metal oxide (A-MxOy) was employed to understand the polymetallic association of the effect of entropy, revealing the interplay between entropy and the NO3 reduction reaction (NITRR) in a photoelectrochemical (PEC) system. Based on ultrafast transient absorption spectroscopy, the signal recovery of an optimal heterostructure (CoFeMnO/BiVO4) was 9.1 ps, confirming that amorphous CoFeMnO effectively promotes the kinetic factor of electrons. Thus, the NH3 yield rate of the optimal heterostructure (CoFeMnO/BiVO4) is up to 17.82 μg h−1 cm−2 (at −0.1 V vs. RHE), which is almost twice that of p-BiVO4. Furthermore, isotope 1H nuclear magnetic resonance spectroscopy was used to further demonstrate the exactitude of the NH3 evolutionary process, using 15NO3 as the N resource. Therefore, desirable entropy regulation and NH3 production make the herein A-MxOy/BiVO4 heterostructure a promising NITRR catalyst for use in a future solar conversion system.

Graphical abstract: Fabrication of an amorphous metal oxide/p-BiVO4 photocathode: understanding the role of entropy for reducing nitrate to ammonia

Supplementary files

Article information

Article type
Research Article
Submitted
24 Nov 2021
Accepted
07 Jan 2022
First published
08 Jan 2022

Inorg. Chem. Front., 2022,9, 805-813

Fabrication of an amorphous metal oxide/p-BiVO4 photocathode: understanding the role of entropy for reducing nitrate to ammonia

F. Wang, Q. Ding, Y. Bai, H. Bai, S. Wang and W. Fan, Inorg. Chem. Front., 2022, 9, 805 DOI: 10.1039/D1QI01472B

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