Wang Tianwei, Zhang Quan, Lian Kang, Qi Gaocan, Liu Qian, Feng Ligang, Hu Guangzhi, Luo Jun, Liu Xijun
Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China.
Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China.
J Colloid Interface Sci. 2024 Feb;655:176-186. doi: 10.1016/j.jcis.2023.10.157. Epub 2023 Nov 2.
Metal-organic frameworks (MOF) derived carbon materials are considered to be excellent conductive mass transfer substrates, and the large specific surface area provides a favorable platform for loading metal nanoparticles. Tuning the coordination of metals through polyacid doping to change the MOF structure and specific surface area is an advanced strategy for designing catalysts. Modification of Fe-doped ZIF-8 pre-curing by pyrolysis of phosphomolybdic acid hydrate (PMo), Fe nanoparticles confined by Mo and N co-doped carbon frameworks (Fe-NP/MNCF) were fabricated, and the impact of PMo doping on the shape and functionality of the catalysts was investigated. The Zn-air battery (ZAB) driven CO electrolysis was realized by using Fe-NP/MNCF, which was used as bifunctional oxygen reduction reaction (ORR) and carbon dioxide reduction reaction (CORR) catalysts. The results show that the half-wave potential (E) of Fe-NP/MNCF is 0.89 V, and the limiting diffused current density (j) is 6.4 mA cm. The ZAB constructed by Fe-NP/MNCF shows a high specific capacity of 794.8 mAh g, a high open-circuit voltage (OCV) of 1.475 V, and a high power density of 111.6 mW cm. Fe-NP/MNCF exhibited efficient CORR performance with high CO Faraday efficiency (FE) of 87.5 % and current density for the generation of carbon dioxide (j) of 10 mA cm at -0.9 V vs RHE. ZAB-driven CORR had strong catalytic stability. These findings provide new methods and techniques for the preparation of advanced carbon-based catalysts from MOFs.
金属有机框架（MOF）衍生的碳材料被认为是优异的导电传质基底，其大比表面积为负载金属纳米颗粒提供了良好的平台。通过多元酸掺杂调节金属配位以改变MOF结构和比表面积是设计催化剂的一种先进策略。采用水合磷钼酸（PMo）热解对铁掺杂ZIF-8预固化体进行改性，制备了Mo和N共掺杂碳骨架限制的铁纳米颗粒（Fe-NP/MNCF），并研究了PMo掺杂对催化剂形状和功能的影响。利用Fe-NP/MNCF作为双功能氧还原反应（ORR）和二氧化碳还原反应（CORR）催化剂，实现了锌空气电池（ZAB）驱动的CO电解。结果表明，Fe-NP/MNCF的半波电位（E）为0.89 V，极限扩散电流密度（j）为6.4 mA cm。由Fe-NP/MNCF构建的ZAB具有794.8 mAh g的高比容量、1.475 V的高开路电压（OCV）和111.6 mW cm的高功率密度。Fe-NP/MNCF表现出高效的CORR性能，在相对于可逆氢电极（RHE）为-0.9 V时，CO法拉第效率（FE）高达87.5%，二氧化碳生成电流密度（j）为10 mA cm。ZAB驱动的CORR具有很强的催化稳定性。这些发现为从MOF制备先进的碳基催化剂提供了新的方法和技术。
