College of Geography and Environmental Sciences, Key laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science, Zhejiang Normal University, Jinhua, 321004, P. R. China.
Zhejiang Engineering Laboratory for Green Syntheses and Applications of Fluorine-Containing Specialty Chemicals, Institute of Advanced Fluorine-Containing Materials, Zhejiang Normal University, Jinhua, 321004, P. R. China.
Small. 2023 Jul;19(27):e2300136. doi: 10.1002/smll.202300136. Epub 2023 Mar 27.
Transition metal catalysts are regarded as one of promising alternatives to replace traditional Pt-based catalysts for oxygen reduction reaction (ORR). In this work, an efficient ORR catalyst is synthesized by confining Fe C nanoparticles into N, S co-doped porous carbon nanosheets (Fe C/N,S-CNS) via high-temperature pyrolysis, in which 5-sulfosalicylic acid (SSA) demonstrates as an ideal complexing agent for iron (ΙΙΙ) acetylacetonate while g-C N behaves as a nitrogen source. The influence of the pyrolysis temperature on the ORR performance is strictly examined in the controlled experiments. The obtained catalyst exhibits excellent ORR performance (E = 0.86 V; E = 0.98 V) in alkaline electrolyte, coupled by exhibiting the superior catalytic activity and stability (E = 0.83 V, E = 0.95 V) to Pt/C in acidic media. In parallel, its ORR mechanism is carefully illustrated by the density functional theory (DFT) calculations, especially the role of the incorporated Fe C played in the catalytic process. The catalyst-assembled Zn-air battery also exhibits a much higher power density (163 mW cm ) and ultralong cyclic stability in the charge-discharge test for 750 h with a gap increase down to 20 mV. This study provides some constructive insights for preparation of advanced ORR catalysts in green energy conversion units correlated systems.
过渡金属催化剂被认为是替代传统的 Pt 基催化剂用于氧还原反应（ORR）的有前途的替代品之一。在这项工作中，通过高温热解将 FeC 纳米颗粒封装在 N、S 共掺杂多孔碳纳米片中（FeC/N，S-CNS），合成了一种高效的 ORR 催化剂，其中 5-磺基水杨酸（SSA）作为铁（III）乙酰丙酮的理想络合剂，而 g-CN 则作为氮源。在对照实验中严格考察了热解温度对 ORR 性能的影响。所得催化剂在碱性电解质中表现出优异的 ORR 性能（E = 0.86 V；E = 0.98 V），并且在酸性介质中表现出优于 Pt/C 的优异催化活性和稳定性（E = 0.83 V，E = 0.95 V）。同时，通过密度泛函理论（DFT）计算仔细说明了其 ORR 机制，特别是掺杂的 FeC 在催化过程中的作用。组装的锌空气电池在充放电测试中也表现出更高的功率密度（163 mW cm-2）和超长的循环稳定性，在 750 h 的测试中，间隙下降到 20 mV。这项研究为在绿色能源转换相关系统中制备先进的 ORR 催化剂提供了一些有建设性的见解。
