Hydrophobicity modulation on a ferriporphyrin-based metal–organic framework for enhanced ambient electrocatalytic nitrogen fixation

电化学 化学 材料科学 氮气 固氮 金属有机骨架 电催化剂 金属 无机化学 化学工程 纳米技术 电极 有机化学 冶金 吸附 物理化学 工程类
作者
Hongming He,Hongkai Li,Qianqian Zhu,Cheng‐Peng Li,Zhihong Zhang,Miao Du
出处
期刊:Applied Catalysis B-environmental [Elsevier]
卷期号:316: 121673-121673 被引量:36
标识
DOI:10.1016/j.apcatb.2022.121673
摘要

Electrocatalytic N 2 fixation represents an energy-efficient and long-term sustainable approach, which can convert N 2 to NO 3 – or NH 3 via the electrochemical N 2 oxidation reaction (NOR) or N 2 reduction reaction (NRR). However, the inert N 2 molecule, low activity of electrocatalysts, and predisposed competitive reactions result in the poor yields and Faradaic efficiencies of N 2 fixation reactions, which greatly restrict the application of such green synthesis technology. In this work, a molecular-level post-modification strategy has been explored to integrate diverse alkyl chains on a ferriporphyrin-based metal–organic framework (MOF) PCN-222(Fe), which provides adjustable hydrophobicity and highly dispersed active sites. The increased lengths of alkyl groups can gradually improve the hydrophobicity of decorated MOFs, which effectively suppress the competitive reactions and boost the electrocatalytic NOR and NRR performances. Significantly, the highest Faradaic efficiency of 70.7% so far and a state-of-the-art NO 3 − yield of 110.9 μg h –1 mg cat. –1 can be achieved for NOR, which are attributed to the synergistic effect of FeN 4 active sites, high porosity, and strong hydrophobicity for n -octadecylphosphonic acid (OPA) decorated PCN-222(Fe). The hydrophobicity of ferriporphyrin-based MOF can be modulated using the molecular-level post-modification strategy, which remarkably boosts the electrocatalytic performances for N 2 oxidation to NO 3 – or N 2 reduction to NH 3 under ambient conditions. The highest Faradaic efficiency of 70.7% by far and a state-of-the-art of NO 3 − yield of 110.9 μg h –1 mg cat. –1 are realized for nitrogen oxidation reaction, in virtue of the synergistic effect of ferriporphyrin active sites, high porosity, and enhanced hydrophobicity. • The hydrophobicity of a ferriporphyrin-based MOF can be well modulated by the molecular-level post-modification strategy. • The enhanced hydrophobicity remarkably boosts the electrocatalytic performances for ambient N 2 oxidation or N 2 reduction reaction. • The Faradaic efficiency of 70.7% and a NO 3 − yield of 110.9 μg h –1 mg cat. –1 are realized for nitrogen oxidation reaction.
最长约 10秒,即可获得该文献文件

科研通智能强力驱动
Strongly Powered by AbleSci AI
科研通是完全免费的文献互助平台,具备全网最快的应助速度,最高的求助完成率。 对每一个文献求助,科研通都将尽心尽力,给求助人一个满意的交代。
实时播报
2秒前
悦耳的母鸡完成签到,获得积分10
2秒前
luffy189完成签到 ,获得积分10
2秒前
4秒前
4秒前
4秒前
4秒前
5秒前
小白菜完成签到 ,获得积分10
5秒前
森sen发布了新的文献求助10
6秒前
7秒前
7秒前
wang完成签到,获得积分10
8秒前
Wang Mu发布了新的文献求助10
8秒前
mmm发布了新的文献求助10
9秒前
makimaki发布了新的文献求助10
10秒前
MaoMao发布了新的文献求助10
10秒前
10秒前
10秒前
长尾巴的人类完成签到,获得积分10
11秒前
着急的笑旋完成签到,获得积分10
14秒前
周杰完成签到,获得积分10
14秒前
科研通AI5应助阿光采纳,获得10
15秒前
gezid完成签到 ,获得积分10
16秒前
16秒前
贪玩半蕾发布了新的文献求助10
17秒前
xx发布了新的文献求助10
17秒前
hanleiharry1发布了新的文献求助10
18秒前
18秒前
tutu完成签到,获得积分10
19秒前
Lucas应助wanhe采纳,获得10
20秒前
21秒前
21秒前
21秒前
Shell完成签到,获得积分10
21秒前
科目三应助科研猫采纳,获得10
21秒前
22秒前
喜悦香薇完成签到,获得积分10
22秒前
研友_VZG7GZ应助doctor_loong采纳,获得10
22秒前
Garra9822完成签到 ,获得积分10
24秒前
高分求助中
Production Logging: Theoretical and Interpretive Elements 2700
Mechanistic Modeling of Gas-Liquid Two-Phase Flow in Pipes 2500
Kelsen’s Legacy: Legal Normativity, International Law and Democracy 1000
Handbook on Inequality and Social Capital 800
Conference Record, IAS Annual Meeting 1977 610
Interest Rate Modeling. Volume 3: Products and Risk Management 600
Interest Rate Modeling. Volume 2: Term Structure Models 600
热门求助领域 (近24小时)
化学 材料科学 生物 医学 工程类 有机化学 生物化学 物理 纳米技术 计算机科学 内科学 化学工程 复合材料 基因 遗传学 物理化学 催化作用 量子力学 光电子学 冶金
热门帖子
关注 科研通微信公众号,转发送积分 3546536
求助须知:如何正确求助?哪些是违规求助? 3123667
关于积分的说明 9356348
捐赠科研通 2822331
什么是DOI,文献DOI怎么找? 1551314
邀请新用户注册赠送积分活动 723326
科研通“疑难数据库(出版商)”最低求助积分说明 713699