Graphitized Carbon Veils Break the Activity-Durability Trade-Off in PEMFC Cathode Catalysts

IF 30.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Subin Park,Eungjun Lee,Jieun Baik,Myeong-Geun Kim,Jin Soo Kang,Sung Jong Yoo
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引用次数: 0

Abstract

Proton exchange membrane fuel cells (PEMFCs) require cathode catalysts that combine high Pt utilization, efficient mass transport and long-term durability under demanding practical operation. However, recent developed Pt-based catalysts with small particle sizes suffer from a persistent activity-durability trade-off because highly accessible Pt surfaces are vulnerable to oxidation and dissolution. Here, we present a scalable Co-tannic acid (TA) coordination strategy that directly upgrades commercial Pt/C into graphitized carbon veil (GCV) Pt3Co by thermally converting a complex into a Pt-Co surface alloy and thin GCV while modifying the carbon surface. This integrated structure improves oxygen reduction activity, lowers local oxygen transport resistance and facilitates water removal while preserving reactant accessibility. Under heavy-duty operation, GCV-Pt3Co achieves a peak efficiency of 72%, high rated power density (1.21 W/cm 2 @0.67V). Also, GCV-Pt3Co exhibits outstanding durability under long-term operation. After accelerated durability test (ADT) cycles, it retains a Pt utilization of 3.95 kW/gPt and markedly extends the ADT projected lifetime to 27,800 h. This work establishes polyphenol-metal coordination as a practical route for upgrading parent catalyst into active and durable PEMFC catalysts.
石墨化碳膜打破了PEMFC阴极催化剂活性与耐久性的权衡
质子交换膜燃料电池(pemfc)需要在苛刻的实际操作条件下兼具高Pt利用率、高效质量传输和长期耐用性的阴极催化剂。然而,最近开发的具有小颗粒尺寸的Pt基催化剂受到持续活性和耐久性权衡的影响,因为高度可接近的Pt表面容易被氧化和溶解。在这里,我们提出了一种可扩展的共鞣酸(TA)配位策略,通过在修改碳表面的同时将配合物热转化为Pt- co表面合金和薄GCV,直接将商用Pt/C升级为石墨化碳膜(GCV) Pt3Co。这种集成结构提高了氧还原活性,降低了局部氧运输阻力,促进了水的去除,同时保持了反应物的可及性。在高负荷工况下,GCV-Pt3Co可实现72%的峰值效率,高额定功率密度(1.21 W/ cm2 @0.67V)。此外,GCV-Pt3Co在长期使用下表现出出色的耐久性。在加速耐久性测试(ADT)循环后,其Pt利用率保持在3.95 kW/gPt,并将ADT预期寿命显著延长至27,800 h。该研究确立了多酚-金属配位是将母体催化剂升级为活性和耐用的PEMFC催化剂的可行途径。
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来源期刊
Energy & Environmental Science
Energy & Environmental Science 化学-工程:化工
CiteScore
50.50
自引率
2.20%
发文量
349
审稿时长
2.2 months
期刊介绍: Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences." Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).
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