【作者】 程修艳； 章凡玉； 张建玲；

【Author】 Xiuyan Cheng;Fanyu Zhang;Jianling Zhang;CAS Key Laboratory of Colloid,Interface and Thermodynamics,Institute of Chemistry,Chinese Academy of Science;

【机构】 胶体界面与化学热力学院重点实验室中国科学院化学研究所；

【摘要】 金属-有机框架(MOFs),是一类由金属离子或金属团簇和有机配体通过价键作用形成的结晶多孔材料,在气体存储、气体吸附分离、传感以及催化等领域有着广泛的应用。但由于MOFs存在不稳定及导电性差等问题,将其作为非均相催化剂用于二氧化碳电化学还原受到很大的限制。离子液体(IL)因为具有很多独特的性质,如不燃性、蒸汽压低、电导率高、结构可设计性以及功能可调性等,受到了研究者的普遍关注。本工作提出利用ZIF-8/IL复合物作为前驱体合成杂原子掺杂锌/碳-氮材料。首先采用溶剂热法制备ZIF-8,然后通过浸渍法在离子液体(HmimBF4、HmimPF6等)中制得ZIF-8/IL复合材料,高温热解ZIF-8/IL复合物得到杂原子掺杂的锌/碳-氮材料。通过X-射线衍射(XRD)和透射电子显微镜(TEM)等表征手段对杂原子掺杂的锌/碳-氮材料的结构和形貌进行了表征。研究表明,杂原子掺杂的锌/碳-氮材料能有效地将二氧化碳电化学还原为一氧化碳,且具有优异的一氧化碳法拉第效率、高的电流密度和稳定性。该方法为制备多种杂原子掺杂的金属/碳-氮材料提供了新思路。更多还原

【Abstract】 Metal-organic frameworks(MOFs) are a class of porous crystalline materials constructed from metal ions or metal clusters and organic links by strong bond interactions, which have been studied extensively in the fields of gas storage, gas adsorption and separation, sensing and catalysis. However, as heterogeneous catalysts for the electrochemical reduction of carbon dioxide, MOFs are greatly restricted due to their instability and poor electrical conductivity. Ionic liquid(IL) has received increasing attention due to its peculiar properties such as non-flammable, negligible vapor pressure, high ionic conductivity, designable structure and tunable properties. Here we propose the utilization of ZIF-8/IL composite as a precursor for the synthesis of heteroatom-doped zinc/carbon-nitrogen materials. ZIF-8 was firstly prepared by solvent thermal method, then ZIF-8/IL composite was synthesized by dipping in ILs(HmimBF4, HmimPF6, etc.) and heteroatom-doped zinc/carbon-nitrogen(Zn/C-N) material was obtained through a pyrolysis of ZIF-8/IL composite at high temperature. The structure and morphology of heteroatom-doped Zn/C-N were characterized by X-ray diffraction and transmission electron microscope. Such a heteroatom-doped Zn/C-N catalyst exhibits outstanding electrocatalytic activity for CO2 reduction reaction, i.e., an excellent CO faradaic efficiency, high current density and stability. This method provides a new way for the synthesis of different kinds of heteroatom-doped M/C-N composites.更多还原