Synthesis of Metal-Nitrogen-Carbon Electrocatalysts with Atomically Regulated Nitrogen-Doped Polycyclic Aromatic Hydrocarbons

Chen, Shaoqing1,2,3; Yan, Hui-Min4; Tseng, Jochi5; Ge, Shijie1; Li, Xia3; Xie, Lin6; Xu, Zian1; Liu, Pengfei7,8; Liu, Chongxuan9; Zeng, Jie10; Wang, Yang-Gang4; Wang, Hsing-Lin1,11,12

2024-04-18

10.1021/jacs.4c01770

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY   影响因子和分区

0002-7863

1520-5126

Tuning the active site structure of metal-nitrogen-carbon electrocatalysts has recently attracted increasing interest. Herein, we report a bottom-up synthesis strategy in which atomically regulated N-doped polycyclic aromatic hydrocarbons (N-PAHs) of NxC42-x (x = 1, 2, 3, 4) were used as ligands to allow tuning of the active site's structures of M-N-x and establish correlations between the structures and electrocatalytic properties. Based on the synthesis process, detailed characterization, and DFT calculation results, active structures of Nx-Fe-1-Nx in Fe-1-Nx/RGO catalysts were constructed. The results demonstrated that the extra uncoordinated N atoms around the Fe-1-N-4 moieties disrupted the pi-conjugated NxC42-x ligands, which led to more localized electronic state in the Fe-1-N-4 moieties and superior catalytic performance. Especially, the Fe-1-N4/RGO exhibited optimized performance for ORR with E-1/2 increasing by 80 mV and J(k) at 0.85 V improved 18 times (compared with Fe-1-N1/RGO). This synthesis strategy utilizing N-PAHs holds significant promise for enhancing the controllability of metal-nitrogen-carbon electrocatalyst preparation.

SCI ; EI

英语

第一 ; 通讯

Guangdong Provincial Pearl River Talents Program[2017ZT07Z479] ; Department of Science and Technology of Guangdong Province[2018B030322001] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2019B010941001] ; Key-Area Research and Development Program of Guangdong Province["2205153","22022504"] ; NSFC[2019QN01L353] ; Guangdong "Pearl River" Talent Plan[JCYJ20210324103608023] ; Shenzhen Science and Technology Program[CYJ20170817110652558]

Chemistry

Chemistry, Multidisciplinary

WOS:001230569800001

AMER CHEMICAL SOC

Web of Science

1.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
2.Soochow Univ, Coll Energy, Suzhou 215006, Peoples R China
3.Soochow Univ, Coll Chem Chem Engn & Mat Sci, Innovat Ctr Chem Sci, Suzhou 215006, Peoples R China
4.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
5.Japan Synchrotron Radiat Res Inst JASRI, Diffract & Scattering Div, Sayo, Hyogo 6795198, Japan
6.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
7.Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
8.Spallat Neutron Source Sci Ctr, Dongguan 523808, Peoples R China
9.Southern Univ Sci & Technol, Sch Environm Sci & Engn, Shenzhen 518055, Peoples R China
10.Univ Sci & Technol China, Dept Chem Phys, Hefei Natl Lab Phys Sci Microscale, Hefei 230000, Peoples R China
11.Southern Univ Sci & Technol, Key Univ Lab Highly Efficient Utilizat Solar Energ, Shenzhen 518055, Peoples R China
12.Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China

Chen, Shaoqing,Yan, Hui-Min,Tseng, Jochi,et al. Synthesis of Metal-Nitrogen-Carbon Electrocatalysts with Atomically Regulated Nitrogen-Doped Polycyclic Aromatic Hydrocarbons[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146(20).

Chen, Shaoqing.,Yan, Hui-Min.,Tseng, Jochi.,Ge, Shijie.,Li, Xia.,...&Wang, Hsing-Lin.(2024).Synthesis of Metal-Nitrogen-Carbon Electrocatalysts with Atomically Regulated Nitrogen-Doped Polycyclic Aromatic Hydrocarbons.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146(20).

Chen, Shaoqing,et al."Synthesis of Metal-Nitrogen-Carbon Electrocatalysts with Atomically Regulated Nitrogen-Doped Polycyclic Aromatic Hydrocarbons".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146.20(2024).