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Boosting Oxygen Reduction Reaction Activity of Palladium by Stabilizing Its Unusual Oxidation States in Perovskite
Chemistry of Materials ( IF 7.2 ) Pub Date : 2015-04-14 00:00:00 , DOI: 10.1021/acs.chemmater.5b00450
Yinlong Zhu 1 , Wei Zhou 1 , Yubo Chen 1 , Jie Yu 1 , Xiaomin Xu 1 , Chao Su 2 , Moses O. Tadé 2 , Zongping Shao 2, 3
Chemistry of Materials ( IF 7.2 ) Pub Date : 2015-04-14 00:00:00 , DOI: 10.1021/acs.chemmater.5b00450
Yinlong Zhu 1 , Wei Zhou 1 , Yubo Chen 1 , Jie Yu 1 , Xiaomin Xu 1 , Chao Su 2 , Moses O. Tadé 2 , Zongping Shao 2, 3
Affiliation
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The high cost, scarcity, and poor stability of metallic platinum (Pt) as an oxygen reduction reaction (ORR) catalyst in fuel cells and metal-air batteries have limited the commercialization of these attractive clean-energy technologies. Thus, developing alternative electrocatalysts that are economical and achieve maximized efficiency of stably catalyzing ORR is of prime importance in the societal pursuit of sustainable energy. Metallic palladium (Pd) is an alternative electrocatalyst that is less expensive than Pt; however, its current performance remains insufficient. Here we report for the first time that the ORR activity of the different oxidation states of Pd increased in the following order: Pd0 < Pd2+ < perovskite-type ionic (Pi) Pd3/4+. Especially, the intrinsic activity on Pd active site of (Pi) Pd3/4+ is ∼84-fold higher than that of Pd0. By doping the Pd element as a cation into the perovskite oxide lattice to form LaFe0.95Pd0.05O3-δ and LaFe0.9Pd0.1O3-δ, unusual oxidation states of 3/4+ for Pd are stabilized, and the catalysts exhibit superior mass activity, durability, and tolerance to methanol compared with the benchmark commercial Pt/C catalyst.
中文翻译：
通过稳定钙钛矿中的异常氧化态来提高钯的氧还原反应活性
在燃料电池和金属空气电池中作为氧还原反应（ORR）催化剂的金属铂（Pt）的高成本，稀缺性和较差的稳定性限制了这些有吸引力的清洁能源技术的商业化。因此，在社会上对可持续能源的追求中，开发经济的并且实现稳定催化ORR的最大效率的替代电催化剂至关重要。金属钯（Pd）是一种替代性的电催化剂，其价格比Pt便宜。但是，其当前性能仍然不足。在这里，我们首次报告Pd不同氧化态的ORR活性按以下顺序增加：Pd 0 <Pd 2+ <钙钛矿型离子（Pi）Pd 3/4 +。特别地，（Pi）Pd 3/4 +在Pd活性位点上的固有活性比Pd 0高约84倍。通过将Pd元素作为阳离子掺杂到钙钛矿氧化物晶格中以形成LaFe 0.95 Pd 0.05 O3 -δ和LaFe 0.9 Pd 0.1 O3 -δ，Pd的3/4 +异常氧化态得以稳定，并且催化剂表现出与基准商用Pt / C催化剂相比，具有更高的质量活性，耐久性和对甲醇的耐受性。
更新日期：2015-04-14
中文翻译：
通过稳定钙钛矿中的异常氧化态来提高钯的氧还原反应活性
在燃料电池和金属空气电池中作为氧还原反应（ORR）催化剂的金属铂（Pt）的高成本，稀缺性和较差的稳定性限制了这些有吸引力的清洁能源技术的商业化。因此，在社会上对可持续能源的追求中，开发经济的并且实现稳定催化ORR的最大效率的替代电催化剂至关重要。金属钯（Pd）是一种替代性的电催化剂，其价格比Pt便宜。但是，其当前性能仍然不足。在这里，我们首次报告Pd不同氧化态的ORR活性按以下顺序增加：Pd 0 <Pd 2+ <钙钛矿型离子（Pi）Pd 3/4 +。特别地，（Pi）Pd 3/4 +在Pd活性位点上的固有活性比Pd 0高约84倍。通过将Pd元素作为阳离子掺杂到钙钛矿氧化物晶格中以形成LaFe 0.95 Pd 0.05 O3 -δ和LaFe 0.9 Pd 0.1 O3 -δ，Pd的3/4 +异常氧化态得以稳定，并且催化剂表现出与基准商用Pt / C催化剂相比，具有更高的质量活性，耐久性和对甲醇的耐受性。
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