电化学（中英文） ›› 2022, Vol. 28 ›› Issue (3): 2108531. doi: 10.13208/j.electrochem.210853
所属专题： “表界面”专题文章； “电催化和燃料电池”专题文章
冯雅辰1,2, 王翔1,2, 王宇琪1,2, 严会娟1,2, 王栋1,2,*(
)
收稿日期:2021-11-24
修回日期:2022-02-05
出版日期:2022-03-28
发布日期:2022-03-08
Ya-Chen Feng1,2, Xiang Wang1,2, Yu-Qi Wang1,2, Hui-Juan Yan1,2, Dong Wang1,2,*()
Received:2021-11-24
Revised:2022-02-05
Published:2022-03-28
Online:2022-03-08
Contact:
*Tel: (86-10)82616935, E-mail: wangd@iccas.ac.cn
摘要：
燃料电池作为一种电化学能量转换系统,具有能量转换效率高、清洁度高等优点。氧还原反应（ORR）是燃料电池中重要的阴极反应。目前,电催化剂仍是制约燃料电池进一步商业化的关键材料之一。ORR反应催化机理的研究对于开发具有良好活性和高选择性的电催化剂具有重要价值。近年来人们通过各种先进的原位表征方法深入研究了ORR催化剂的机理和催化过程。本综述旨在总结用于原位表征技术应用于研究 ORR 反应机制的最新研究进展。我们首先简要介绍各种原位技术在ORR研究中的优势,包括电化学扫描隧道技术、 红外光谱、 拉曼光谱、 X射线吸收光谱、 X射线衍和透射电子显微镜等。然后,从催化剂的角度,总结了各种原位表征技术在催化剂形貌和电子结构演变以及催化过程中反应物和中间体的识别中的应用。最后,展望讨论了该领域原位技术的未来发展。
冯雅辰, 王翔, 王宇琪, 严会娟, 王栋. 电催化氧还原反应的原位表征[J]. 电化学（中英文）, 2022, 28(3): 2108531.
Ya-Chen Feng, Xiang Wang, Yu-Qi Wang, Hui-Juan Yan, Dong Wang. In Situ Characterization of Electrode Structure and Catalytic Processes in the Electrocatalytic Oxygen Reduction Reaction[J]. Journal of Electrochemistry, 2022, 28(3): 2108531.
Figure 1
(A) Potential-dependent Pt L3-edge XAS spectra of Pt NPs on a carbon support. (B) Evolution of the metallic, oxide and the total area of the catalyst as a function of the applied potential. (C) STM image of the as-prepared Pt(111) surface. (D) STM image of the Pt(111) electrode after the 25th sweep in 0.1 mol·L-1 KOH solutions containing Co2+. (A-B) Reproduced from Ref[31]. With permission from the American Chemical Society. (C-D) Reproduced from Ref[21]. With permission from the American Chemical Society. (color on line)
Figure 2
(A) In situ atomic PDFs for Pd30Ni70NPs obtained in a custom-built fuel cell cycled between 0.6 ~ 1.2 V (vs. RHE) at a scan rate of 100 mV·s-1. (B) Trend for the change in composition of Pd30Ni70/C catalyst as a result of Ni-leaching during the potential cycling. (C) Morphologies of Pt-Fe nanocatalysts at additional 5th, 50th, and 150th cycles after the first 130 cycles. (D) The corresponding CV curves at 1st, 5th, 25th, 50th, 100th, and 150th cycles. (A-B) Reproduced from ref[41]. With permission from the American Chemical Society. (C-D) Reproduced from ref[42]. With permission from the American Chemical Society. (color on line)
Figure 3
(A) In situ XANES spectra at the Mn K-edge for the MnO2 at different electrode potentials in 1.0 mol·L-1 KOH. (B) In situ XANES spectra of the Co-PPy-BP cathode and standard Co, Co(OH)2 and CoOOH samples. (A) Reproduced from ref[29]. With permission from the Elsevier. (B) Reproduced from ref[45]. With permission from the Royal Society of Chemistry. (color on line)
Figure 4
(A) SHINERS spectra of the ORR system at a Pt(111) electrode surface in a 0.1 mol·L-1 HClO4 solution saturated with O2.(B) SHINERS spectra of the ORR at a Pt(100) electrode surface in a 0.1 mol·L-1 HClO4 solution. (C) SHINERS spectra of the ORR at a Pt(100) electrode surface in a 0.1 mol·L-1 HClO4 solution. (D) SHINERS spectra of the ORR system at a Pt(111) electrode surface in 0.1 mol·L-1 NaClO4 solution (pH of approximately 10.3) saturated with O2. (E) SHINERS spectra of the ORR at a Pt(100) electrode surface in 0.1 mol·L-1 NaClO4 solution (pH of approximately 10.3) saturated with O2. (F) SHINERS spectra of the ORR at a Pt(100) electrode surface in 0.1 mol·L-1 NaClO4 solution (pH of approximately 10.3) saturated with O2. (G) In situ IR spectra of Pt/C during ORR in 0.1 mol·L-1 HClO4 solution. (H) In situ SHINERS spectra of ORR on dealloyed Pt3Co nanocatalysts in 0.1 mol·L-1 O2-saturated HClO4 solution. (I) In situ SHINERS spectra of the ORR on dealloyed Pt3Co nanocatalysts in O2-saturated 0.1 mol·L-1 NaClO4 + 0.001 mol·L-1 NaOH solutions. (A-F) Reproduced from Ref[46]. With permission from the Nature Energy. (G) Reproduced from Ref[32]. With permission from the Wiley Online Library. (H-I) Reproduced from Ref[38]. With permission from the Wiley Online Library. (color on line)
Figure 5
(A-B) In situ STM images of FePc on Au(111) in O2-saturated 0.1 mol·L-1 HClO4: (A) ORR off; (B) ORR on. (C-D) STM topographic image (C) and cross-section analysis (D) of Mn1Cl at the HOPG/1-octanoic acid interface under ambient conditions; (E) Possible pathways and states of the manganese centre of Mn-porphyrins during their reaction with O2. (A-B) Reproduced from Ref[49]. With permission from the American Chemical Society. (C-E) Reproduced from Ref[50]. With permission from the Nature Chemistry. (color on line)
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