氮掺杂介孔碳负载钴催化剂的制备及其脱除富氢气体CO性能研究

Preparation of Nitrogen Doped Mesoporous Carbon Supported Cobalt Catalyst and Its Performance for Removal of CO in Hydrogen-Rich Gas

为有效脱除富氢气体中的CO,制备了氮掺杂的有序介孔碳及其负载纳米钴颗粒的催化剂,采用N2吸附-脱附、X射线衍射(X-ray diffraction,XRD)、拉曼光谱、X射线光电子能谱(X-ray photoelectron spectroscopy,XPS)、热重-质谱联用(thermogravimetry-mass spectrometry,TGMS)等手段进行表征,研究了氮掺杂对有序介孔碳负载钴基催化剂的自还原行为和CO甲烷化反应性能的影响规律。结果表明,在介孔碳骨架中引入的氮原子主要作为氧化钴的成核位点,与氧化物载体产生较强的相互作用,大大提高了钴物种的分散度,从而形成颗粒尺寸均匀的小纳米钴颗粒,显著促进了其自还原反应,进而提高了催化剂的还原度。催化剂评价结果表明,与未掺杂氮的介孔碳载体相比,氮掺杂介孔碳载体使催化剂的CO脱除效率明显提升。

In order to effectively remove CO from hydrogen-rich gas,cobalt-based nano-particle catalyst supported on nitrogen-doped ordered mesoporous carbon was prepared and characterized by X-ray diffraction(XRD),Raman spectrum,X-ray photoelectron spectroscopy(XPS)and thermogravimetry-mass spectrometry(TG-MS).The effects of nitrogen doping on the self-reduction behavior of the catalyst and CO methanation reaction performance were studied.The characterization results show that the nitrogen atoms introduced into the mesoporous carbon skeleton are mainly used as the nucleation sites of cobalt oxide,which have a strong interaction with the oxide carrier,and greatly improve the dispersion of cobalt species.Thus,small nanocobalt particles with uniform particle size are formed,which significantly promote self-reduction reaction and thereby improve the reduction degree of the catalyst.The catalyst evaluation results show that,compared with the mesoporous carbon carrier without doping,the CO removal efficiency of the catalyst doped by nitrogen is much higher.