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通过MoC-MoN异质结构的协同性能促进电化学氨合成。

Promoting electrochemical ammonia synthesis by synergized performances of MoC-MoN heterostructure.

作者信息

An Tae-Yong, Surendran Subramani, Jesudass Sebastian Cyril, Lee Hyunjung, Moon Dae Jun, Kim Jung Kyu, Sim Uk

机构信息

Hydrogen Energy Technology Laboratory, Korea Institute of Energy Technology (KENTECH), Naju, Republic of Korea.

Department of Science and Engineering, Chonnam National University, Gwangju, Republic of Korea.

出版信息

Front Chem. 2023 Feb 16;11:1122150. doi: 10.3389/fchem.2023.1122150. eCollection 2023.

DOI:10.3389/fchem.2023.1122150
PMID:36874069
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9980907/
Abstract

Hydrogen has become an indispensable aspect of sustainable energy resources due to depleting fossil fuels and increasing pollution. Since hydrogen storage and transport is a major hindrance to expanding its applicability, green ammonia produced by electrochemical method is sourced as an efficient hydrogen carrier. Several heterostructured electrocatalysts are designed to achieve significantly higher electrocatalytic nitrogen reduction (NRR) activity for electrochemical ammonia production. In this study, we controlled the nitrogen reduction performances of MoC-MoN heterostructure electrocatalyst prepared by a simple one pot synthesis method. The prepared MoC-MoN heterostructure nanocomposites show clear phase formation for MoC and MoN, respectively. The prepared MoC-MoN electrocatalysts deliver a maximum ammonia yield of about 9.6 μg h cm and a Faradaic efficiency (FE) of about 10.15%. The study reveals the improved nitrogen reduction performances of MoC-MoN electrocatalysts due to the combined activity of the MoC and MoN phases. In addition, the ammonia production from MoC-MoN electrocatalysts is intended by the associative nitrogen reduction mechanism on MoC phase and by Mars-van-Krevelen mechanism on MoN phase, respectively. This study suggests the importance of precisely tuning the electrocatalyst by heterostructure strategy to substantially achieve higher nitrogen reduction electrocatalytic activity.

摘要

由于化石燃料的枯竭和污染的加剧,氢气已成为可持续能源中不可或缺的一部分。由于储氢和运输是扩大其适用性的主要障碍,通过电化学方法生产的绿色氨被视为一种高效的氢载体。人们设计了几种异质结构电催化剂,以实现显著更高的电化学氨生产电催化氮还原(NRR)活性。在本研究中,我们通过简单的一锅合成法控制了MoC-MoN异质结构电催化剂的氮还原性能。制备的MoC-MoN异质结构纳米复合材料分别显示出清晰的MoC和MoN相形成。制备的MoC-MoN电催化剂的最大氨产率约为9.6 μg h cm,法拉第效率(FE)约为10.15%。该研究揭示了由于MoC和MoN相的联合活性,MoC-MoN电催化剂的氮还原性能得到了改善。此外,MoC-MoN电催化剂的氨生产分别通过MoC相上的缔合氮还原机制和MoN相上的Mars-van-Krevelen机制实现。这项研究表明了通过异质结构策略精确调整电催化剂以大幅提高氮还原电催化活性的重要性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/845cee5bdee7/fchem-11-1122150-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/59826a6a2130/fchem-11-1122150-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/205bf9d184ff/fchem-11-1122150-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/15f8588da6ff/fchem-11-1122150-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/6fe7a2e8adee/fchem-11-1122150-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/845cee5bdee7/fchem-11-1122150-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/59826a6a2130/fchem-11-1122150-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/205bf9d184ff/fchem-11-1122150-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/15f8588da6ff/fchem-11-1122150-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/6fe7a2e8adee/fchem-11-1122150-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1b80/9980907/845cee5bdee7/fchem-11-1122150-g005.jpg

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