哈工大王振波教授:制备高活性与高稳定性兼备的锰基催化剂
作者:Jiazhan Li, Mengjie Chen, David A. Cullen, Sooyeon Hwang, Maoyu Wang, Boyang Li, Kexi Liu, Stavros Karakalos, Marcos Lucero, Hanguang Zhang, Chao Lei, Hui Xu, George E. Sterbinsky, Zhenxing Feng, Dong Su, Karren L. More, Guofeng Wang, Zhenbo Wang, Gang Wu
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2018-11-08 10:12:52
高性能(活性、稳定性)非贵金属催化剂的研究制备是实现燃料电池技术大规模商业化应用的关键,也是该领域面临的难题。Fe-N-C催化剂是目前活性最好的非贵金属催化剂,但仍然面临稳定性差的问题,而铁离子的Fenton效应进一步限制了其实际应用。哈工大化工与化学学院王振波教授课题组另辟蹊径,采用化学掺杂和物理吸附相结合的两步法逐步提高MOF衍生的氮掺杂纳米碳载体活性位点的密度,制备了高活性与高稳定性兼备的单原子分散的Mn-N-C催化剂。其催化活性与传统的Fe-N-C催化剂相当(0.8V vs.
RHE),但具有更加优异的稳定性。同时,燃料电池中的测试结果进一步证实了Mn-N-C催化剂的应用前景。原子级分辨率的STEM和X-射线吸收光谱证实单原子分散的MnN4为主要的催化活性位点,DFT理论计算进一步研究了该活性位点的催化路径与反应机理。该研究从实践和理论两个层面上证实了锰基催化剂的活性与稳定性,为高性能催化剂的研究制备开辟了新的方向。
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Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells
作者:Jiazhan Li, Mengjie Chen, David A. Cullen, Sooyeon Hwang, Maoyu Wang, Boyang Li, Kexi Liu, Stavros Karakalos, Marcos Lucero, Hanguang Zhang, Chao Lei, Hui Xu, George E. Sterbinsky, Zhenxing Feng, Dong Su, Karren L. More, Guofeng Wang, Zhenbo Wang, Gang Wu
●
2018-11-08 10:12:52
导语
Platinum group metal (PGM)-free catalysts that are also iron free are highly desirable for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells, as they avoid possible Fenton reactions. Here we report an efficient ORR catalyst that consists of atomically dispersed nitrogen-coordinated single Mn sites on partially graphitic carbon (Mn-N-C). Evidence for the embedding of the atomically dispersed MnN4 moieties within the carbon surface-exposed basal planes was established by X-ray absorption spectroscopy and their dispersion was confirmed by aberration-corrected electron microscopy with atomic resolution. The Mn-N-C catalyst exhibited a half-wave potential of 0.80 V versus the reversible hydrogen electrode, approaching that of Fe-N-C catalysts, along with significantly enhanced stability in acidic media. The encouraging performance of the Mn-N-C catalyst as a PGM-free cathode was demonstrated in fuel cell tests. First-principles calculations further support the MnN4 sites as the origin of the ORR activity via a 4e− pathway in acidic media.
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