N-Doped Hollow Carbon Sphere and Polyhedral Carbon Composite Supported Pt/Fe Nanoparticles as Highly Efficient Cathodic Catalysts of Proton-Exchange Membrane Fuel Cells,ACS Applied Energy Materials

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N-Doped Hollow Carbon Sphere and Polyhedral Carbon Composite Supported Pt/Fe Nanoparticles as Highly Efficient Cathodic Catalysts of Proton-Exchange Membrane Fuel Cells
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2023-01-23 , DOI: 10.1021/acsaem.2c02838
Yuebing Wang ₁ , Guanghua Tan ₁ , Qingfeng Yi _{1,

2} , Can Fang ₁ , Ruowei Yi ₃

Affiliation

With the growing energy crisis, people urgently need green energy sources to replace fossil ones. As a zero-emission clean energy source, the proton-exchange membrane fuel cell (PEMFC) has received growing attention from researchers due to its broad practical application. However, so far only noble metal Pt can be used as a mature cathodic catalyst for PEMFC to effectively promote the slow kinetic process of the oxygen reduction reaction (ORR). Herein, a low Pt-loading carbon-based catalyst (pCN@NHCS-Fe/Pt-280) with hollow carbon spheres (HCSs), metal–organic frameworks (MOFs), and carbon nanotubes (CNTs) structure was synthesized by the thermal reduction of platinum acetylacetonate and pCN@NHCS-Fe. Compared with the benchmark Pt/C catalyst, pCN@NHCS-Fe/Pt-280 presents low cost, and its ORR onset potential (E_onset = 0.971 V_RHE) and half-wave potential (E_1/2 = 0.883 V_RHE) in acidic media are comparable to those of 40% Pt/C (E_onset = 0.965 V_RHE, E_1/2 = 0.883 V_RHE). In the durability test for ORR, its current retention percentage (92.3%) is still higher than 40% Pt/C (86.7%) after 10 000 s of the constant potential test, and its cyclic voltammetry (CV) and linear scan voltammetry (LSV) profiles after 500 cycles exhibit outstanding stability. Moreover, pCN@NHCS-Fe/Pt-280 quickly recovers to 79.1% of the initial value after adding methanol, while 40% Pt/C can recover only to 72.3%, indicating a superior ability in antialcohol oxidation. In addition, the maximum power density of pCN@NHCS-Fe/Pt-280 (518.7 mW cm^–2) as the cathode catalyst of PEMFC in the H₂–air cell test is also higher than that of Pt/C (515.3 mW cm^–2), while its power density is lower than that of Pt/C in the H₂–O₂ cell test at different pressures due to the high-temperature influence at high current densities. This work provides a valuable idea for the design of multistructured (HCSs, MOFs, CNTs, etc.) electrocatalysts and a feasible strategy for the development of low-Pt-loaded ORR catalysts.

中文翻译：

N 掺杂空心碳球和多面体碳复合负载 Pt/Fe 纳米粒子作为质子交换膜燃料电池的高效阴极催化剂

随着能源危机的加剧，人们迫切需要绿色能源来替代化石能源。质子交换膜燃料电池（PEMFC）作为一种零排放的清洁能源，因其广泛的实际应用而越来越受到研究人员的关注。然而，到目前为止，只有贵金属 Pt 可以作为 PEMFC 的成熟阴极催化剂，以有效促进氧还原反应 (ORR) 的缓慢动力学过程。在此，通过热合成具有空心碳球（HCSs）、金属有机骨架（MOFs）和碳纳米管（CNTs）结构的低铂负载碳基催化剂（pCN@NHCS-Fe/Pt-280）乙酰丙酮铂和 pCN@NHCS-Fe 的还原。与基准 Pt/C 催化剂相比，pCN@NHCS-Fe/Pt-280 具有低成本、ORR 起始潜力（E_onset = 0.971 V _RHE ) 和酸性介质中的半波电位 ( E _1/2 = 0.883 V _RHE ) 与 40% Pt/C 相当 ( E _onset = 0.965 V _RHE , E _1/2 = 0.883 V _RHE). 在ORR耐久性测试中，恒电位测试10 000 s后其电流保持率（92.3%）仍高于40% Pt/C（86.7%），其循环伏安法（CV）和线性扫描伏安法（ LSV) 曲线在 500 次循环后表现出出色的稳定性。此外，pCN@NHCS-Fe/Pt-280在加入甲醇后迅速恢复到初始值的79.1%，而40% Pt/C只能恢复到72.3%，表明抗酒精氧化能力优越。此外，作为PEMFC阴极催化剂的pCN@NHCS-Fe/Pt-280在H _{2 -空气电池测试中的最大功率密度（518.7 mW cm}^–2 ）也高于Pt/C（515.3 mW cm ^–2 ),而其功率密度低于Pt/C在H ₂ –O ₂由于高电流密度下的高温影响，在不同压力下进行电池测试。该工作为多结构（HCSs、MOFs、CNTs等）电催化剂的设计提供了有价值的思路，并为开发低Pt负载的ORR催化剂提供了可行的策略。

更新日期：2023-01-23

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