天津大学化学系张兵课题组在氮化铁催化剂催化二氧化碳加氢反应机理方面取得新进展。2020年11月18日，国际知名学术期刊《德国应用化学》发表了这一成果。

在该研究中，团队发现Fe₂N@C纳米颗粒在二氧化碳选择性加氢形成C₂₊烃反应中具备优异的催化活性（C₂₊选择性53.96%，C₂-C₄⁼选择性31.03%），超过了相应的Fe@C纳米颗粒。原位X射线衍射、非原位穆斯堡尔谱和X射线光电子能谱表明，氮化铁在原位转化为高活性的碳化铁，后者才是真正的活性物质。此外，原位漫反射傅里叶变换红外光谱和对照实验的综合结果表明，原位形成的羰基铁介导了从氮化铁到碳化铁的转变过程。

据了解，开发高效催化剂和揭示其中的活性组分对二氧化碳选择性加氢制C₂₊烃有着非常重要的意义。

附：英文原文

Title: Unveiling the Activity Origin of Iron Nitride Catalyst for Efficient Hydrogenation of CO2 to C2+ Hydrocarbons

Author: Bohang Zhao, Mengyao Sun, Fanpeng Chen, Yanmei Shi, Yifu Yu, Xingang Li, Bin Zhang

Issue&Volume: November 18, 2020

Abstract: Developing efficient catalytic materials and unveiling the active species is significant for selective hydrogenation of CO  2  to C  2+  hydrocarbons. Fe  2  N@C nanoparticles were reported to exhibit outstanding performance toward selective CO  2  hydrogenation to C  2+  hydrocarbons (C  2+  selectivity: 53.96%; C  2  ‐C  4  =  selectivity, 31.03%), outperforming corresponding Fe@C. In situ X‐ray diffraction, ex situ  Mssbauer  and X‐ray photoelectron spectra revealed that iron nitrides were in situ converted to highly active iron carbides, which acted as the real active species. Moreover, the combined results of in situ diffuse reflectance infrared Fourier transform spectroscopy and control experiments suggested an in situ formed carbonyl iron‐mediated conversion mechanism from iron nitrides to iron carbides.

DOI: 10.1002/anie.202015017

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202015017