用于氧还原反应的Pt基金属间化合物纳米晶催化剂

doi:10.1016/S1872-2067(21)63991-8

催化学报 ›› 2022, Vol. 43 ›› Issue (6): 1444-1458.DOI: 10.1016/S1872-2067(21)63991-8

用于氧还原反应的Pt基金属间化合物纳米晶催化剂

柏景森^a^,^b^,^†, 杨莉婷^a^,^b^,^†, 金钊^a^,^*(), 葛君杰^a^,^b^,^#(), 邢巍^a^,^b^,^$()

^a中国科学院长春应用化学研究所电分析国家重点实验室, 吉林省低碳化学电源重点实验室, 吉林长春130022
^b中国科学技术大学应用化学与工程学院, 安徽合肥230026

收稿日期:2021-09-30 接受日期:2021-09-30 出版日期:2022-06-18 发布日期:2022-04-14
通讯作者: 金钊,葛君杰,邢巍
作者简介:第一联系人：
^†共同第一作者
基金资助:
国家重点研究发展计划(2017YFB0102905);国家自然科学基金(21875243);国家自然科学基金(21633008);国家自然科学基金(21673221);国家自然科学基金(U1601211);吉林省科技发展项目(20190201270JC);吉林省科技发展项目(20180101030JC)

Advanced Pt-based intermetallic nanocrystals for the oxygen reduction reaction

Jingsen Bai^a^,^b^,^†, Liting Yang^a^,^b^,^†, Zhao Jin^a^,^*(), Junjie Ge^a^,^b^,^#(), Wei Xing^a^,^b^,^$()

^aState Key Laboratory of Electroanalytic Chemistry, Jilin Province Key Laboratory of Low Carbon Chemistry Power, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
^bSchool of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, Anhui, China

Received:2021-09-30 Accepted:2021-09-30 Online:2022-06-18 Published:2022-04-14
Contact: Zhao Jin, Junjie Ge, Wei Xing
About author:First author contact:
† Contributed equally to this work.
Supported by:
National Science and Technology Major Project(2017YFB0102905);National Natural Science Foundation of China(21875243);National Natural Science Foundation of China(21633008);National Natural Science Foundation of China(21673221);National Natural Science Foundation of China(U1601211);Jilin Province Science and Technology Development Program(20190201270JC);Jilin Province Science and Technology Development Program(20180101030JC)

摘要/Abstract

摘要：

质子交换膜燃料电池(PEMFC)是一种具有大规模商业化生产前景的能源技术, 它具有能量密度高、转换效率高、环境友好等优点, 受到人们的广泛关注. 其中, 燃料电池的阴极氧还原反应(ORR)具有较高的反应过电位, 需要贵金属铂催化, 但是铂的成本高昂、资源短缺, 极大地限制了燃料电池的市场化, 因此降低铂负载量, 提高铂基催化剂的活性和稳定性, 是燃料电池商用化的关键. 目前, 通过合金化、形貌控制等方法优化后, 铂基催化剂的质量活性和比活性都得到了极大的提高. 其中, 将铂与其他金属尤其是3d过渡金属合金化已被认为是减少铂负载量并提高ORR催化性能的最有效方法之一. 通过合理设计并精准制备铂基合金、调控铂表面电子结构可以大大提高催化剂的本征活性以及耐久性. 但是, 普通合金化制备的合金一般是无序的, 存在活性位点结构不同, 过渡金属溶解导致稳定下降等问题, 将其有序化形成金属间化合物可有效解决上述问题. 金属间化合物具有长程有序的晶体结构, 原子均有序地占据晶格中的相应格点, 以金属键或离子键相互作用, 能够有效提高活性位点催化活性和防止过渡金属的溶解. 此外, 金属间化合物通过压缩应变调控Pt-Pt键长, 优化铂与氧还原反应中间物种的吸附能, 提高本征催化活性和稳定性.
本文综述了PEMFCs电催化剂的铂基金属间化合物的最新研究进展, 分别从热力学和动力学上理解金属间化合物形成的过程与条件, 为设计金属间化合物奠定理论基础; 从成分、尺寸和形貌等方面分别阐述了近年来铂基金属间化合物的发展, 不仅关注铂基催化剂在的三电极体系下的优异性能, 而且对其在质子交换膜燃料电池的实际应用时的性能表达进行了详细的阐述, 总结了一些提升金属间化合物性能的策略; 同时, 针对目前的发展瓶颈, 总结了Pt基有序金属间纳米晶面临的挑战和未来前景.
本文可以帮助读者更深入地了解铂基金属间化合物纳米晶在ORR领域的最新进展, 对铂基金属间化合物催化剂的合理设计和催化性能改进策略提出更深入的见解, 为促进PEMFC的市场化发展提供一条新思路.

关键词: 氧还原反应, 燃料电池, Pt基催化剂, 金属间化合物, 电催化

Abstract:

Proton exchange membrane fuel cells (PEMFCs) are considered ideal energy-conversion devices because of their environmentally friendly nature and high theoretical energy efficiency. However, cathodic polarization, which is a result of the sluggish oxygen reduction reaction (ORR) kinetics, is a significant source of energy loss and reduces fuel cell efficiency. Further, the need to use Pt in commercial Pt/C cathodes has restricted their large-scale application in fuel cells because of its high cost and poor durability. Thus, improvements in the activity and durability of Pt-based catalyst are required to reduce the amount of Pt required and, thus, costs, while increasing the ORR rate and fuel cell power density and promoting widespread PEMFC commercialization. In recent years, atomically ordered Pt-based intermetallic nanocrystals have received tremendous attention owing to their excellent activity and stability for the ORR. Therefore, in this review, we first introduce the formation of intermetallic compounds from the perspective of thermodynamics and kinetics to lay a theoretical foundation for the design of these compounds. In addition, optimization strategies for Pt-based ordered intermetallic catalysts are summarized in terms of the catalyst composition, size, and morphology. Finally, we conclude with a discussion of the current challenges and future prospects of Pt-based ordered alloys. This review is designed to help readers gain insights into the recent developments in and rational design of Pt-based intermetallic nanocrystals for the ORR and encourage research that will enable the commercialization of PEMFCs.

Key words: Oxygen reduction reaction, Fuel cell, Pt-based catalyst, Intermetallic, Electrocatalysis

柏景森, 杨莉婷, 金钊, 葛君杰, 邢巍. 用于氧还原反应的Pt基金属间化合物纳米晶催化剂[J]. 催化学报, 2022, 43(6): 1444-1458.

Jingsen Bai, Liting Yang, Zhao Jin, Junjie Ge, Wei Xing. Advanced Pt-based intermetallic nanocrystals for the oxygen reduction reaction[J]. Chinese Journal of Catalysis, 2022, 43(6): 1444-1458.

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图/表 7

Fig. 1. (a) Oxygen reduction reaction pathway. (b) Free energy diagram for the four-electron associative ORR on Pt(111). (c) Relationship between the binding free energy of *OOH (ΔGOOH) and that of *O (ΔGO) with respect to ∆GOH on the (111) surfaces of various metals. (d) Curve limiting potential with respect to free energy drawn according to Eqs. 10-13; here, one side of the solid blue line represents strong adsorption, whereas the other side of the solid green line represents weak adsorption. Reprinted from Ref. [21] with permission. Copyright 2018, American Chemical Society.

Fig. 2. Schematic of conditions for the formation of an AmBn intermetallic phase in an A-B binary system at thermodynamic equilibrium. (a) Phase diagram showing the equilibria between disordered solid solution (blue), ordered intermetallic compound (orange), and mixed phases (white) as a function of composition and temperature. At T1 (T1 should be higher than the order-to-disorder transition temperature), a disordered atomic arrangement is preferred over the full range of possible compositions. At T2, an ordered phase appears within a specific range of compositions near the stoichiometric point (marked by a red bar). (b) Diagram showing the Gibbs free energies of the disordered (blue) and ordered (orange) phases as a function of composition at two temperatures: T1 (dashed) and T2 (solid). Reprinted from Ref. [26] with permission. Copyright 2017, John Wiley and Sons.

Fig. 3. (a) Schematic of the core-shell structure formed by acid washing the catalyst. (b) Mass activity of L10-FePt/Pt and commercial Pt/C at the beginning of life (BOL) and after ADT (60 °C). (c) Half-wave potential of L10-FePt/Pt and commercial Pt/C at BOL and after ADT (60 °C). (a-c) Reprinted from Ref. [13] with permission. Copyright 2018, American Chemical Society. (d) High-angle annular dark-field scanning tunneling electron microscopy (HAADF-STEM) image of fully ordered fct-Pt-Fe and hysteresis loops of partially ordered fct-FePt and fully ordered fct-FePt; ORR polarization of fully ordered fct NPs (e), partially ordered fct-Fe NPs (f), and C-fcc-FePt NPs (g) before and after ADT. (d-f) Reprinted from Ref. [33] with permission. Copyright 2015, American Chemical Society. (h,i) Schematic of the synthesis and HAADF-STEM image of L10-FePt/rGO. Reprinted from Ref. [53] with permission. Copyright 2020, American Chemical Society.

Fig. 4. (a) Schematic of L10-CoPt/Pt NPs with a Pt shell (blue, Co; white, Pt). (b,c) Enlarged STEM image of L10-CoPt/Pt NPs with Pt shell (blue, Co; red, Pt). (d) SA and MA of commercial Pt/C, etched A1-CoPt, and L10-CoPt/Pt measured at 0.9 V vs. RHE. (e) ORR polarization curves of L10-CoPt/Pt NPs from BOL to end of life (EOL). (f) MA of L10-CoPt/Pt NPs measured at BOL and EOL in a fuel cell. (a-f) Reprinted from Ref. [55] with permission. Copyright ORR polarization curves of Pt3Co with different Co contents in the Co-metal-organic framework (g) and Pt/40Co-nanocrystals sintered at different temperatures in O2-saturated 0.1 mol/L HClO4 at room temperature at a rotation speed of 900 rpm (h). (i) Potential cycling stability tests of Pt/40Co-NC-900 at 0.6-1.0 V at a scan rate of 50 mV/s. (j) STEM-electron energy loss spectroscopy images of Pt3Co nanoparticle. (g-j) Reprinted from Ref. [56] with permission. Copyright 2019, Elsevier.

Fig. 5. HAADF-STEM images of cubic (a), concave (b), and defect-rich cubic (c) intermetallic Pt3Sn. (a-c) Reprinted from Ref. [67] with permission. Copyright 2016, John Wiley and Sons. (d) Schematic illustration of the structural change of the FePtAu NPs upon annealing. Reprinted from Ref. [72] with permission. Copyright 2012 American Chemical Society. (e) Schematic of L10-Pt-Ni-Co synthesis (acac = acetylacetonate). (f) Linear sweep voltammetry curves of commercial Pt/C, C-A1-PtNi0.8Co0.2, and C-L10-PtNi0.8Co0.2. (g) Mass activities of commercial Pt/C, C-A1-PtNi0.8Co0.2, and C-L10-PtNi0.8Co0.2 at 0.9 V. (e-g) Reprinted from Ref. [76] with permission. Copyright 2019, John Wiley and Sons. (h) Image of L10-W-PtCo. (i) Mass activities of L10-W-PtCo/C and P/C before and after ADT. (j) Pt-Pt bond lengths and oxygen adsorption energies of the studied catalysts. (h-j) Reprinted from Ref. [77] with permission. Copyright 2019 John Wiley and Sons.

Fig. 6. (a) Formation of ordered fct Pt-Fe NPs and N-doped carbon shells. Reprinted from Ref. [35] with permission. Copyright 2015, American Chemical Society. (b) HAADF images of sub-Pt3Co-MC. (c) HAADF-STEM of Pt3Co NPs. (d) Model of ordered Pt3Co NPs. (b-d) Reprinted from Ref. [80] with permission. Copyright 2021, PNAS. (e) HAADF-STEM image of L10-PtZn NP. (f) ORR polarization curves of L10-PtZn/Pt-C. (g) H2-O2 fuel cell polarization curves of L10-PtZn. (e-g) Reprinted from Ref. [84] with permission. Copyright 2020, John Wiley and Sons.

Fig. 7. (a) STEM-ADF image of Pt3Co NWs/C. (b) HAADF-STEM image of Pt3Co NWs/C. (c) ORR-specific activities and mass activities of Pt/C and PtxCoy. (a-c) Reprinted from Ref. [56] with permission. Copyright 2015 American Chemical Society. (d) Synthesis of D-Pt3Co NWs and O-Pt3Co NWs. (e) Transmission electron microscopy (TEM) and high-resolution (HR)TEM images of O-Pt3Co NWs. (f) ORR polarization curves and MAs of different catalysts. (d-f) Reprinted from Ref. [86] with permission. Copyright 2019, American Chemical Society. (g) Schematic of PtPb nanoplate; (h) SAs and MAs of different catalysts [66]. (i) Schematic of Meso-PtNi. (j) ORR polarization curves before and after the ADT of Pt/C, Meso-PtNi_1, and Meso-PtNi_2. (g-j) Reprinted from Ref. [87] with permission. Copyright 2016 John Wiley and Sons.

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用于氧还原反应的Pt基金属间化合物纳米晶催化剂

Advanced Pt-based intermetallic nanocrystals for the oxygen reduction reaction

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