基于高熵效应的多原子共掺杂碳作为直接液体燃料电池阴极催化剂的性能研究  

Study on the performance of multi-atoms co-doped carbon as cathodecatalyst for direct liquid fuel cells based on the high-entropy effect

作　　者：简李想 方园 吴昕 王晶弟 朱建锋[1] JIAN Li-xiang;FANG Yuan;WU Xin;WANG Jing-di;ZHU Jian-feng(School of Material Science and Engineering,Shaanxi University of Science&Technology,Xi′an 710021,China;AVIC Creative Robotic Co.,Ltd.,Xi′an 710000,China)

机构地区：[1]陕西科技大学材料科学与工程学院,陕西西安710021 [2]中航创世机器人(西安)有限公司,陕西西安710000

出　　处：《陕西科技大学学报》2024年第4期111-117,共7页Journal of Shaanxi University of Science & Technology

基　　金：中国博士后科学基金项目(2019M663607);陕西省科技厅自然科学基础研究计划项目(2022JM-285)。

摘　　要：燃料电池技术作为一种新型清洁能源,有希望成为传统化石燃料的替代品之一.氧还原反应(ORR)是燃料电池的阴极反应,研究更稳定、更经济的高活性电催化剂对实现燃料电池商业化发展具有重要意义.本研究基于高熵效应的优势,制备了多种过渡金属共掺杂NSC材料(M-NSC,M=Co、Fe、Ni、Mn、Ce),旨在提高直接液体燃料电池阴极催化剂的催化性能.实验采用高温热解法分别合成了三种M/C摩尔比的(CeMnFeCoNi)-NSC催化剂,研究了不同金属添加量对材料微观结构和催化性能的影响.(CeMnFeCoNi)-NSC呈现二维层状结构,拥有较大的比表面积,为催化反应提供了更多的活性位点.将(CeMnFeCoNi)-NSC作为直接甲醇燃料电池(DMFC)和直接硼氢化物燃料电池(DBFC)的阴极催化剂,单电池功率密度分别为19.86 mW·cm^(-2)和73.81 mW·cm^(-2),优于高温热解法制备的Fe-NC(DMFC:7.92 mW·cm^(-2);DBFC:52.12 mW·cm^(-2)).这主要归因于在(CeMnFeCoNi)-NSC催化剂中金属与N元素产生的M-N4基团可以作为催化位点,以及多种金属之间的协同作用共同提高了其阴极活性.并且研究发现当金属总量与碳的摩尔比例为1∶50时,表现出最优异的电池性能.研究结果为开展碳基电催化剂的成分设计和性能调控提供了新思路.Fuel cells as a new type of clean energy,have become the potential alternatives to traditional fossil fuels.Oxygen reduction reaction(ORR)is the cathode procedure of fuel cells.It is of great significance to study more stable and economical high-activity electrocatalysts for the commercial development of fuel cells.Based on the advantages of high entropy effect,this work prepared multiple transition metal co-doped NSC materials(M-NSC,M=Co,Fe,Ni,Mn,Ce),in order to improve the catalytic performance of cathode catalysts.(CeMnFeCoNi)-NSC catalysts with different metal/carbon ratio were synthesized by high-temperature pyrolysis,and the influence of metal addition amounts on the microstructure and catalytic performance were studied.(CeMnFeCoNi)-NSC shows two-dimensional layered structure,providing a larger specific surface area and more active sites.Then(CeMnFeCoNi)-NSC was used as the cathode catalyst of direct methanol fuel cells(DMFC)and direct borohydride fuel cells(DBFC),and the peak power densities were 19.86 and 73.81 mW·cm^(-2),respectively,Compared with that of Fe-NC based DMFC and DBFC,the peak power densities were 7.92 and 52.12 mW·cm^(-2),respectively.The high performance of(CeMnFeCoNi)-NSC is mainly attributed to the M-N_(4) groups formed by metals and nitrogen,and the synergistic effect among multiple metals.Furthermore,it was found that the superior cell performance was achieved with the metal-to-carbon ratio of 1∶50.This study provides a new idea for the composition design and performance regulation of carbon-based electrocatalysts.

关 键 词：燃料电池 阴极 氧还原反应 杂原子掺杂碳 

分 类 号：TB34[一般工业技术—材料科学与工程]