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Stably Immobilizing Sub-3 nm High-Entropy Pt Alloy Nanocrystals in Porous Carbon as Durable Oxygen Reduction Electrocatalyst
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-08-11 , DOI: 10.1002/adfm.202204110
Wenjing Zhang 1 , Xin Feng 2 , Zhan Xin Mao 1 , Jing Li 1 , Zidong Wei 1
Affiliation  

Immobilizing ultrafine high-entropy Pt alloy nanocrystals (HENs) in porous carbon (PC) with strong interface interaction, which is crucial to efficient and durable oxygen reduction reaction (ORR), remains a challenge. In this study, an anchoring-carbonization strategy for strongly bonding sub-3 nm HENs in ordered mesoporous carbon is reported. When heating the orderly assembled composites containing hydrophobic organometallic precursors, structure directing agent F127, and hydrophilic resol, F127 is first removed at moderate temperature region, leading to reduced metallic species directly anchored on partially carbonized resol framework. Then along further temperature increase, in situ carbonization of resol around the HENs, enables more effective plane bonding rather than a single point contact of HENs with carbon. It not only enhances the anchor strength, but also inhibits migration and size growth of HENs along the subsequent high-temperature carbonization. As a result, senary, septenary, octonary, and denary Pt-based HENs with average nanocrystal sizes of 2.2, 2.6, 2.9, and 2.8 nm, respectively, are successfully imbedded into porous carbon. In electrocatalytic ORR, porous carbon-supported senary Pt-based HENs (6-HENs/PC) exhibit superior activity and durability, representing a promising electrocatalyst. This strategy allows for the preparation of a range of ultrafine HENs strongly loaded on porous carbon for wide applications.

中文翻译:

在多孔碳中稳定固定亚 3 nm 高熵 Pt 合金纳米晶体作为耐用的氧还原电催化剂

将超细高熵 Pt 合金纳米晶体 (HEN) 固定在具有强界面相互作用的多孔碳 (PC) 中,这对于高效和持久的氧还原反应 (ORR) 至关重要,这仍然是一个挑战。在这项研究中,报道了一种在有序介孔碳中强键合亚 3 nm HEN 的锚定碳化策略。当加热有序组装的含有疏水性有机金属前体、结构导向剂 F127 和亲水性甲阶酚醛树脂的复合材料时,F127 首先在中等温度区域被去除,导致还原的金属物质直接锚定在部分碳化的甲阶酚醛树脂骨架上。然后随着温度的进一步升高,HEN 周围的甲阶酚醛树脂原位碳化,能够实现更有效的平面键合,而不是 HEN 与碳的单点接触。它不仅增强了锚固强度,而且抑制了 HENs 在随后的高温碳化过程中的迁移和尺寸增长。结果,平均纳米晶体尺寸分别为 2.2、2.6、2.9 和 2.8 nm 的 senary、septenary、octonary 和 denary Pt 基 HEN 成功地嵌入到多孔碳中。在电催化 ORR 中,多孔碳负载的 Senary Pt 基 HENs (6-HENs/PC) 表现出优异的活性和耐久性,是一种很有前途的电催化剂。该策略允许制备一系列强负载在多孔碳上的超细 HEN,用于广泛的应用。和 2.8 nm 分别成功地嵌入到多孔碳中。在电催化 ORR 中,多孔碳负载的 Senary Pt 基 HENs (6-HENs/PC) 表现出优异的活性和耐久性,是一种很有前途的电催化剂。该策略允许制备一系列强负载在多孔碳上的超细 HEN,用于广泛的应用。和 2.8 nm 分别成功地嵌入到多孔碳中。在电催化 ORR 中,多孔碳负载的 Senary Pt 基 HENs (6-HENs/PC) 表现出优异的活性和耐久性,是一种很有前途的电催化剂。该策略允许制备一系列强负载在多孔碳上的超细 HEN,用于广泛的应用。
更新日期:2022-08-11
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