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Encapsulation of metal precursor within ZIFs for bimetallic N-doped carbon electrocatalyst with enhanced oxygen reduction
International Journal of Hydrogen Energy ( IF 7.2 ) Pub Date : 2018-06-20 , DOI: 10.1016/j.ijhydene.2018.05.160
Mengchen Wu , Xianxiang Hu , Congling Li , Jian Li , Haijun Zhou , Xia Zhang , Rui Liu

High-performance non-precious metal-doped carbon catalysts for oxygen reduction reactions (ORR) are viable candidates in lieu of platinum-based catalysts. It has been universally reported that active Co–N sites combined with Fe–N sites embedded in carbon matrix represent the most promising active sites for ORR process. Benefiting from the cage-encapsulated-precursor pyrolysis strategy, herein, we fabricated a Fe–N and Co–N homogeneously doped carbon framework by one step. TEM demonstrated the ultimate product had well-defined morphology with Fe (0.54 at%), Co (0.31 at%) and N (2.94 at%) uniformly distributed into the carbon skeleton. The N2 absorption-desorption isotherms indicated the MOF-derived catalyst had a high specific surface area of 647.6 m2 g−1 and inherit hierarchical porosity. Significantly, such FeCo–NC catalyst outperformed a current density (5.6 mA cm−2) at 0.70 V (vs reversible hydrogen electrode) 1.18 times higher than that of a commercial 20 wt% Pt/C (5 mA cm−2) catalyst in alkaline medium, and more positive peak potential of 0.63 V than its counterparts. Its high cycling stability and immunity towards methanol crossover in a wide range pH value showed good potential to be used as cathodes in proton exchange membrane fuel cells (PEMFCs) for long term operation. This simple synthesis strategy would to some degree leverage a cage-encapsulated-precursor for tailored utility of active sites for ORR in a porous carbon framework.



中文翻译:

ZIFs中金属前驱物对双金属N掺杂碳电催化剂的增强氧还原作用

用于氧还原反应(ORR)的高性能非贵金属掺杂碳催化剂是替代铂基催化剂的可行选择。据普遍报道,活性Co-N位点与嵌入碳基质中的Fe-N位点相结合代表了ORR过程中最有希望的活性位点。得益于笼罩式前驱体的热解策略,我们在一个步骤中制备了Fe–N和Co–N均匀掺杂的碳骨架。TEM证明最终产品具有明确定义的形态,其中Fe(0.54 at%),Co(0.31 at%)和N(2.94 at%)均匀分布在碳骨架中。N 2吸收-解吸等温线表明,MOF衍生的催化剂具有647.6 m 2  g -1的高比表面积并继承分层孔隙度。值得注意的是,这种FeCo-NC催化剂在0.70 V(相对于可逆氢电极)下的电流密度(5.6 mA cm -2)优于在市场上20 wt%Pt / C(5 mA cm -2)催化剂的电流密度(5.6 mA cm -2)1.18倍。碱性介质,并且比其对应的正峰电位高0.63V。它的高循环稳定性和在很宽的pH值范围内对甲醇穿透的抵抗力显示出良好的潜力,可用作质子交换膜燃料电池(PEMFC)的阴极,可长期运行。这种简单的合成策略在某种程度上会利用笼罩封装的前体来定制多孔碳骨架中ORR活性位点的效用。

更新日期:2018-06-20
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