Zhang Ge, Zhou Jia, Liu Jiang, Ma Tian, Chen Yu, Xu Chunli
Key Laboratory of Applied Surface and Colloid Chemistry (Shaanxi Normal University), Ministry of Education, Xi'an 710119, People's Republic of China.
School of Chemistry and Chemical Engineering, Shaanxi Normal University, Chang'an West Street 620, Xi'an 710119, People's Republic of China.
Nanotechnology. 2021 Feb 26;32(9):095401. doi: 10.1088/1361-6528/abc6df.
Hollow structure and pore size are considered to be crucial to the performance of nitrogen-doped carbon materials. In this paper, a lipstick-like hollow and mesoporous nitrogen-doped carbon (HNC-1000) material is prepared using a bottom-up template participation strategy. The images by scanning electron microscopy and transmission electron microscopy show that the precursor ZnO particles, the intermediate ZnO@ZIF-8 core-shell particles, and the target HNC-1000 particles all maintain a lipstick-like morphology, and HNC-1000 is a hollow nitrogen-doped carbon material. The specific surface area and pore size analyses show that the synthesized HNC-1000 has a very rich mesoporous structure with Vmeso+macro/Vtotal of 94.8% and mean mesopore size at 13.67 nm. X-ray photoelectron spectroscopy results show that the nitrogen in the catalyst HNC-1000 is mainly pyridine nitrogen and graphite nitrogen. The prepared HNC-1000 has excellent ORR catalytic activity with onset potential (0.98 V versus RHE), half-wave potential (0.85 V versus RHE), and limiting current density (5.51 mA cm), which is comparable to that of commercial Pt/C (20 wt%) and superior to NC-1000 derived from pristine ZIF-8. HNC-1000 also has good stability and strong methanol tolerance, which is superior to commercial Pt/C catalyst. The improved performance of HNC-1000 is attributed to its hollow and mesoporous morphology. These findings demonstrate a stratage for the rational design and synthesis of practical electrocatalysts.
中空结构和孔径被认为对氮掺杂碳材料的性能至关重要。本文采用自下而上的模板参与策略制备了一种口红状的中空介孔氮掺杂碳(HNC-1000)材料。扫描电子显微镜和透射电子显微镜图像表明,前驱体ZnO颗粒、中间产物ZnO@ZIF-8核壳颗粒以及目标HNC-1000颗粒均保持口红状形态,且HNC-1000是一种中空氮掺杂碳材料。比表面积和孔径分析表明,合成的HNC-1000具有非常丰富的介孔结构,介孔和大孔体积占总体积的比例为94.8%,平均介孔尺寸为13.67 nm。X射线光电子能谱结果表明,催化剂HNC-1000中的氮主要为吡啶氮和石墨氮。制备的HNC-1000具有优异的氧还原反应催化活性,起始电位(相对于可逆氢电极,0.98 V)、半波电位(相对于可逆氢电极,0.85 V)和极限电流密度(5.51 mA cm),与商业Pt/C(20 wt%)相当,且优于由原始ZIF-8衍生的NC-1000。HNC-1000还具有良好的稳定性和较强的甲醇耐受性,优于商业Pt/C催化剂。HNC-1000性能的提升归因于其中空和介孔形态。这些发现展示了一种合理设计和合成实用电催化剂的策略。