南方科技大学Hsing-Lin Wang小组经过不懈努力，实现了具有原子调控氮掺杂多环芳烃的金属-氮-碳电催化剂的合成。这一研究成果于2024年4月18日发表在国际顶尖学术期刊《美国化学会杂志》上。

调整金属-氮-碳电催化剂的活性位点结构近年来引起了越来越多的关注。

在该研究中，课题组人员报告了一种自下而上的合成策略，其中原子调节氮掺杂的N_xC_42-x (x = 1,2,3,4)的多环芳烃(N-PAHs)做为配体，以允许调整M-N_x的活性位点结构，并建立结构与电催化性能之间的相关性。基于合成过程、详细表征和DFT计算结果，构建了Fe₁-N_x /RGO催化剂中N_x-Fe₁-N_x的活性结构。

结果表明，Fe₁-N₄基团周围额外的不配位的N原子破坏了π共轭的N_xC_42-x配体，使得Fe₁-N₄基团的电子态更局域化，具有更好的催化性能。特别是Fe₁-N₄ /RGO表现出最佳的ORR性能，E_1/2提高了80 mV, 0.85 V的Jk提高了18倍(与Fe₁-N₁ /RGO相比)。这种利用N-多环芳烃的合成策略，对于提高金属-氮-碳电催化剂制备的可控性具有重要的前景。

附：英文原文

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

Author: Shaoqing Chen, Hui-Min Yan, Jochi Tseng, Shijie Ge, Xia Li, Lin Xie, Zian Xu, Pengfei Liu, Chongxuan Liu, Jie Zeng, Yang-Gang Wang, Hsing-Lin Wang

Issue&Volume: April 18, 2024

Abstract: 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–Nx and establish correlations between the structures and electrocatalytic properties. Based on the synthesis process, detailed characterization, and DFT calculation results, active structures of Nx–Fe1–Nx in Fe1–Nx/RGO catalysts were constructed. The results demonstrated that  the extra uncoordinated  N atoms around the Fe1–N4 moieties disrupted the π-conjugated NxC42–x ligands, which led to more localized electronic state in the Fe1–N4 moieties and superior catalytic performance. Especially, the Fe1–N4/RGO exhibited optimized performance for ORR with E1/2 increasing by 80 mV and Jk at 0.85 V improved 18 times (compared with Fe1–N1/RGO). This synthesis strategy utilizing N-PAHs holds significant promise for enhancing the controllability of metal–nitrogen–carbon electrocatalyst preparation.

DOI: 10.1021/jacs.4c01770

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c01770