中国科学院合肥物质科学研究院张海民团队报道了铁基双碱基上硝酸和二氧化碳环境电合成尿素。相关研究成果于2022年10月20日发表在国际顶尖学术期刊《德国应用化学》。
开发高效的电催化剂以制备关键的*NH2和*CO中间体,对于硝酸盐(NO3-)和二氧化碳(CO2)在环境下电合成尿素至关重要。
该文中,研究人员报道了一种液相激光辐照方法,以在碳纳米管(Fe(a)@C-Fe3O4/CNT)上制备共生石墨碳包封的非晶铁和氧化铁纳米颗粒。Fe(a)@C-Fe3O4/CNT对使用NO3-和CO2合成尿素表现出优异的电催化活性,在环境条件下,尿素产率为1341.3±112.6μg h-1 mg cat-1,法拉第效率为16.5±6.1%。
实验和理论结果均表明,CNT上形成的Fe(a)@C和Fe3O4为吸附和活化O3-和CO2提供了双活性位点,从而生成了具有较低能量势垒的用于尿素形成的关键*NH2和*CO中间体。
该项工作将有助于设计和开发用于尿素环境合成的高效双位点电催化剂。
附:英文原文
Title: Ambient Electrosynthesis of Urea with Nitrate and Carbon Dioxide over Iron-Based Dual-Sites
Author: Jing Geng, Sihan Ji, Meng Jin, Chao Zhang, Min Xu, Guozhong Wang, Changhao Liang, Haimin Zhang
Issue&Volume: 2022-10-20
Abstract: The development of efficient electrocatalysts to generate key *NH 2 and *CO intermediates is crucial for ambient urea electrosynthesis with nitrate (NO 3 - ) and carbon dioxide (CO 2 ). Here we report a liquid-phase laser irradiation method to fabricate symbiotic graphitic carbon encapsulated amorphous iron and iron oxide nanoparticles on carbon nanotubes (Fe(a)@C-Fe 3 O 4 /CNTs). Fe(a)@C-Fe 3 O 4 /CNTs exhibits superior electrocatalytic activity toward urea synthesis using NO 3 - and CO 2 , affording a urea yield of 1341.3±112.6 μg h -1 mg cat -1 and a faradic efficiency of 16.5±6.1% at ambient conditions. Both experimental and theoretical results indicate that the formed Fe(a)@C and Fe 3 O 4 on CNTs provide dual active sites for the adsorption and activation of NO 3 - and CO 2 , thus generating key *NH 2 and *CO intermediates with lower energy barriers for urea formation. This work would be helpful for design and development of high-efficiency dual-site electrocatalysts for ambient urea synthesis.
DOI: 10.1002/anie.202210958
Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202210958
Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:12.959
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx