Journal of Catalysis ( IF 6.5 ) Pub Date : 2023-09-27 , DOI: 10.1016/j.jcat.2023.115148
Cong Yong , Yipu Xu , Hui Yu , Peiran Wu , Jiansong Wang , Liu-Liu Shen , Gui-Rong Zhang , Donghai Mei
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ZIF-derived carbons (ZDCs) represent a novel category of non-precious metal catalysts (NPMCs) for the oxygen reduction reaction (ORR). Nevertheless, establishing the correlation between their structure and performance is challenging due to their diverse structural properties and ill-defined active site moieties. Here we investigate the effect of ZIF-67 derived carbon’s particle size and corresponding distribution of assorted nitrogen functionalities on the ORR. Our findings reveal a substantial increase in ORR activity with decreasing ZDC particle size, while the exact influence of nitrogen functionalities remains uncertain. Most importantly, the present work unveils a correlation between the ORR activity and the site density (SD) of Co-Nx within the ZDC materials, which can be attributed to the concurrently increasing SD and accessibility of Co-Nx on the ZDC particles with small sizes. The present work provides novel insights into the optimization of ZDCs as high-performance NPMCs for ORR in alkaline electrolytes.
中文翻译:

量化碱性电解质中 ZIF 衍生碳的活性位点密度和尺寸依赖性 ORR 活性
ZIF 衍生碳 (ZDC) 代表了一类用于氧还原反应 (ORR) 的新型非贵金属催化剂 (NPMC)。然而,由于其不同的结构特性和不明确的活性位点部分,建立它们的结构和性能之间的相关性具有挑战性。在这里,我们研究了 ZIF-67 衍生碳的粒径和各种氮官能团的相应分布对 ORR 的影响。我们的研究结果表明,随着 ZDC 粒径的减小,ORR 活性显着增加,而氮官能团的确切影响仍不确定。最重要的是,目前的工作揭示了 ORR 活性与 Co-N x的位点密度 (SD) 之间的相关性在 ZDC 材料中,这可归因于小尺寸 ZDC 颗粒上的SD 和 Co-N x的可及性同时增加。目前的工作为优化 ZDC 作为碱性电解质中 ORR 的高性能 NPMC 提供了新的见解。