Edge-Site Engineering of Atomically Dispersed Fe-N4 by Selective C-N Bond Cleavage for Enhanced Oxygen Reduction Reaction Activities

Journal of the American Chemical Society
Rui JiangLeyu Wang

Abstract

Single-atom metal-nitrogen-carbon (M-N-C) catalysts have sparked intense interests, but the catalytic contribution of N-bonding environment neighboring M-N4 sites lacks attention. Herein, a series of Fe-N-C nanoarchitectures have been prepared, which confer adjustable numbers of atomically dispersed Fe-N4 sites, tunable hierarchical micro-mesoporous structures and intensified exposure of interior active sites. The optimization between Fe-N4 single sites and carbon matrix delivers superior oxygen reduction reaction activity (half-wave potential of 0.915 V vs RHE in alkaline medium) with remarkable stability and high atom-utilization efficiency (almost 10-fold enhancement). Both experiments and theoretical calculations verified the selective C-N bond cleavage adjacent to Fe center induced by porosity engineering could form edge-hosted Fe-N4 moieties, and therefore lower the overall oxygen reduction reaction barriers comparing to intact atomic configuration. These findings provide a new pathway for the integrated engineering of geometric and electronic structures of single-atom materials to improve their catalytic performance.

References

Oct 28, 2011·Angewandte Chemie·Dang Sheng Su, Gongquan Sun
May 29, 2012·Nature Nanotechnology·Yanguang LiHongjie Dai
Nov 29, 2013·Angewandte Chemie·Zhicheng ZhangXun Wang
Feb 6, 2015·Chemical Society Reviews·Yao NieZidong Wei
Aug 8, 2015·Nature Communications·Hai-Wei LiangKlaus Müllen
Dec 15, 2015·Journal of the American Chemical Society·Ulrike I KrammPeter Bogdanoff
Dec 13, 2016·Journal of the American Chemical Society·Vanessa ArmelFrédéric Jaouen
Feb 22, 2017·Journal of the American Chemical Society·Yao ZhengShi-Zhang Qiao
Mar 25, 2017·Chemical Society Reviews·S M J RoggeJ Gascon
May 26, 2017·Journal of the American Chemical Society·Jiashen MengLiqiang Mai
Jun 9, 2017·Journal of the American Chemical Society·Changming ZhaoYadong Li
Aug 2, 2017·Journal of the American Chemical Society·Maolin ZhangYadong Li
Sep 14, 2017·Journal of the American Chemical Society·Hanguang ZhangGang Wu

❮ Previous
Next ❯

Citations

Apr 18, 2019·Chemical Communications : Chem Comm·Ying WangXiaoqiang Cui
Oct 2, 2019·Chemical Society Reviews·Huilong FeiXiangfeng Duan
Sep 20, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Xiaoying ZhangYongkui Shan
Mar 25, 2020·Physical Chemistry Chemical Physics : PCCP·Mengyao LvMinghui Yang
Jul 16, 2020·Advanced Materials·Hui ChenXiaoxin Zou
Sep 2, 2020·Chemical Society Reviews·Lulu LiJinlong Gong
Jan 9, 2020·Angewandte Chemie·Yongpeng LeiYadong Li
Dec 20, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Xinxin YangYongliang Li
Mar 7, 2020·Advanced Materials·Xin WangXiangdong Yao
Apr 1, 2020·Nanoscale Horizons : the Home for Rapid Reports of Exceptional Significance in Nanoscience and Nanotechnolgy·Zongkui KouJohn Wang
Aug 31, 2020·Research : a Science Partner Journal·Junxing HanChunwen Sun
Oct 21, 2020·Nature Communications·Travis Marshall-RothYogesh Surendranath
Nov 5, 2020·Chemical Communications : Chem Comm·Peng DuYang Yang Li
Jan 2, 2021·Journal of Hazardous Materials·Yu MaoLei Zheng

❮ Previous
Next ❯

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.