催化作用
介孔材料
硝酸盐
吸附
化学
反硝化
无机化学
氮气
介孔二氧化硅
碳纤维
纳米技术
选择性
化学工程
材料科学
物理化学
有机化学
复合数
工程类
复合材料
作者
Jianwei Fan,Yanyan Chen,Xiaoqian Chen,Zhangxiong Wu,Wei Teng,Wei‐xian Zhang
标识
DOI:10.1016/j.apcatb.2022.121983
摘要
Conversion of nitrate to dinitrogen (N2) is a great challenge in environmental remediation, because it is difficult to control a complete N–N coupling reaction for N2 generation. Herein, we report an atomically dispersed iron coordinated with nitrogen on an ordered mesoporous carbon framework (Meso-Fe–N–C) by a multicomponent co-assembly to improve the selectivity of electrocatalytic denitrification. Impressively, the N2 conversion rate (2176 mg N h−1 g−1 Fe) is 1–3 orders of magnitude higher than that of other iron-based and previously reported materials. Both of N coordination and geometric distortion derived from mesostructure tune the electronic structure of Fe site. This leads to a modest adsorption binding strength with key intermediate to balance the amounts of the surface-bound and solvated nitric oxide (NO). Meanwhile, mesochannels confine solvated NO for dimerization via the Eley-Rideal mechanism to promote N2 formation. The applicability over a wide pH range and long-term stability demonstrates potential practical application.
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