» Articles » PMID: 34138373

Folic Acid Self-Assembly Enabling Manganese Single-Atom Electrocatalyst for Selective Nitrogen Reduction to Ammonia

Overview
Journal Nanomicro Lett
Publisher Springer
Date 2021 Jun 17
PMID 34138373
Citations 5
Authors
Affiliations
Soon will be listed here.
Abstract

Efficient and robust single-atom catalysts (SACs) based on cheap and earth-abundant elements are highly desirable for electrochemical reduction of nitrogen to ammonia (NRR) under ambient conditions. Herein, for the first time, a Mn-N-C SAC consisting of isolated manganese atomic sites on ultrathin carbon nanosheets is developed via a template-free folic acid self-assembly strategy. The spontaneous molecular partial dissociation enables a facile fabrication process without being plagued by metal atom aggregation. Thanks to well-exposed atomic Mn active sites anchored on two-dimensional conductive carbon matrix, the catalyst exhibits excellent activity for NRR with high activity and selectivity, achieving a high Faradaic efficiency of 32.02% for ammonia synthesis at  - 0.45 V versus reversible hydrogen electrode. Density functional theory calculations unveil the crucial role of atomic Mn sites in promoting N adsorption, activation and selective reduction to NH by the distal mechanism. This work provides a simple synthesis process for Mn-N-C SAC and a good platform for understanding the structure-activity relationship of atomic Mn sites.

Citing Articles

Synthesis of Pd-Doped SnO and Flower-like Hierarchical Structures for Efficient and Rapid Detection of Ethanolamine.

Bi W, Zhu J, Zheng B, Liu S, Zhang L Molecules. 2024; 29(15).

PMID: 39125054 PMC: 11314598. DOI: 10.3390/molecules29153650.


Density Functional Theory Study of Triple Transition Metal Cluster Anchored on the CN Monolayer for Nitrogen Reduction Reactions.

Xiao S, Zhang D, Wang G, Zhou T, Wang N Molecules. 2024; 29(14).

PMID: 39064893 PMC: 11280456. DOI: 10.3390/molecules29143314.


Exploring the Roles of Single Atom in Hydrogen Peroxide Photosynthesis.

He K, Huang Z, Chen C, Qiu C, Zhong Y, Zhang Q Nanomicro Lett. 2023; 16(1):23.

PMID: 37985523 PMC: 10661544. DOI: 10.1007/s40820-023-01231-1.


Oxygen-Coordinated Single Mn Sites for Efficient Electrocatalytic Nitrate Reduction to Ammonia.

Zhang S, Zha Y, Ye Y, Li K, Lin Y, Zheng L Nanomicro Lett. 2023; 16(1):9.

PMID: 37932531 PMC: 10628069. DOI: 10.1007/s40820-023-01217-z.


Identification of Dynamic Active Sites Among Cu Species Derived from MOFs@CuPc for Electrocatalytic Nitrate Reduction Reaction to Ammonia.

Ji X, Sun K, Liu Z, Liu X, Dong W, Zuo X Nanomicro Lett. 2023; 15(1):110.

PMID: 37121962 PMC: 10149566. DOI: 10.1007/s40820-023-01091-9.

References
1.
Bao D, Zhang Q, Meng F, Zhong H, Shi M, Zhang Y . Electrochemical Reduction of N under Ambient Conditions for Artificial N Fixation and Renewable Energy Storage Using N /NH Cycle. Adv Mater. 2016; 29(3). DOI: 10.1002/adma.201604799. View

2.
Fang S, Zhu X, Liu X, Gu J, Liu W, Wang D . Uncovering near-free platinum single-atom dynamics during electrochemical hydrogen evolution reaction. Nat Commun. 2020; 11(1):1029. PMC: 7042219. DOI: 10.1038/s41467-020-14848-2. View

3.
Liu S, Wang M, Qian T, Ji H, Liu J, Yan C . Facilitating nitrogen accessibility to boron-rich covalent organic frameworks via electrochemical excitation for efficient nitrogen fixation. Nat Commun. 2019; 10(1):3898. PMC: 6715660. DOI: 10.1038/s41467-019-11846-x. View

4.
Kubin M, Guo M, Kroll T, Lochel H, Kallman E, Baker M . Probing the oxidation state of transition metal complexes: a case study on how charge and spin densities determine Mn L-edge X-ray absorption energies. Chem Sci. 2018; 9(33):6813-6829. PMC: 6115617. DOI: 10.1039/c8sc00550h. View

5.
Kresse , Furthmuller . Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys Rev B Condens Matter. 1996; 54(16):11169-11186. DOI: 10.1103/physrevb.54.11169. View