首页|载体调控增强PtFe氢氧化催化剂的抗CO中毒性能

载体调控增强PtFe氢氧化催化剂的抗CO中毒性能

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以质子交换膜燃料电池(PEMFC)为代表的氢能技术是我国能源转换战略的重要基石,对于实现双碳目标并缓解我们面临的能源与环境问题发挥着至关重要的作用.目前PEMFC阳极侧主要使用纯化氢气,使用成本高昂,推进含CO的低成本灰氢在阳极端应用,有利于加快PEMFC技术的商业化进程.阳极氢氧化反应(HOR)催化剂多为Pt/C,即使在CO浓度低于10 ppm(1 ppm=10-6)的情况下也很容易失活,开发耐CO中毒的Pt基催化剂成为关键问题.通过合金化策略缓解三相界面处CO吸附可提高Pt基电催化剂的CO耐受性,但载体对CO耐受性的影响鲜见报道.为了探究金属一载体相互作用与催化剂CO耐受性之间的关系,采用共浸渍法探究了碳载体及氧化物载体对于PtFe合金形貌、金属价态及抗中毒性能的影响.结果表明,碳载体有利于提高PtFe合金颗粒的均一性,提高Pt的表面价态,进而展现出优异的抗中毒性能.PtFe/C催化剂在1 000 ppm H2/CO中的活性衰减仅为5.2%,商业Pt/C的活性衰减则高达66.1%.PtFe/C催化剂在1 000 ppm H2/CO中2 000 s测试后氢氧化(HOR)活性保持率高达98%,而商业Pt/C催化剂2 000 s无HOR活性.PtFe/C催化剂中的Pt具有高的表面价态,其d带中心位置下降;活性位点Pt对于CO的吸附减弱,催化剂展现出优异的CO耐受能力.
Support regulation for enhancing CO-tolerance performance of the PtFe HOR electrocatalyst
Hydrogen energy technology,which is represented by proton exchange membrane fuel cell(PEMFC),is an important cornerstone of our energy strategy,playing crucial role in realizing the double carbon goal and alleviating the energy-related and environmental problems.The purified hydrogen with high cost is currently used in the anode side of PEMFC,promoting the application of low-cost gray hydrogen with CO residue is beneficial for accelerating the commercialization process of PEMFC technology.Pt/C is widely utilized as the anodic HOR electroacatalyst,but it can be deactivated even when the CO concentration is less than 10 ppm(1 ppm=10-6),rendering the development of CO-tolerant Pt-based catalysts to be pivotal issue.Alleviating the CO adsorption at the triple-phase interferface by alloying strategy can improve the CO tolerance of Pt-based electrocatalysts,but the effect of supports on the CO tolerance is rarely reported.The effects of carbon and oxide support on the morphology,metal valence and CO-resistance of PtFe alloy were investigated by co-impregnation method,aiming for investigating the relationship between the metal-support interaction and the CO tolerance of designed electrocatalysts.The carbon support can improve the homogeneity of PtFe alloy particles,improve the surface valence of Pt,thus PtFe/C can exhibit excellent anti-CO poisoning performance.The PtFe/C electrocatalyst only showed 5.2%HOR activity decline at 1 000 ppm H2/CO,while the HOR activity of the commercial Pt/C decreased by 66.1%.The HOR activity retention rate of PtFe/C electrocatalyst was 98%after 2 000 s in 1000 ppm H2/CO,while the commercial Pt/C catalyst had no HOR activity after 2000 s.Pt in the PtFe/C electrocatalyst has higher valence state,which means a lower d-band center and weakened CO adsorption on the HOR-active Pt sites,thus the PtFe/C electrocatalyst reveals excellent CO tolerance.

Pt-based catalystsmetal-support interactiontriple-phase interfaceinterfacial stabilityanti-CO poisoningproton exchange membrane fuel cell

董子豪、金纯、刘亚飞

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矿冶科技集团有限公司,北京 100160

北京当升材料科技股份有限公司,北京 100160

Pt基催化剂 金属-载体相互作用 三相界面 界面稳定性 抗CO中毒 质子交换膜燃料电池

2024

矿冶
北京矿冶研究总院

矿冶

CSTPCD
影响因子:0.78
ISSN:1005-7854
年,卷(期):2024.33(6)