电化学（中英文） ›› 2021, Vol. 27 ›› Issue (2): 144-156. doi: 10.13208/j.electrochem.201241
所属专题： “理论计算模拟”专题文章； “电催化和燃料电池”专题文章
吴志鹏1,2,3,*(
), 钟传建2,*()
收稿日期:2020-12-31
修回日期:2021-02-21
出版日期:2021-04-28
发布日期:2021-03-12
通讯作者:
吴志鹏,钟传建
E-mail:zpwu@tju.edu.cn;cjzhong@binghamton.edu
Zhi-Peng Wu1,2,3,*(), Chuan-Jian Zhong2,*()
Received:2020-12-31
Revised:2021-02-21
Published:2021-04-28
Online:2021-03-12
Contact:
Zhi-Peng Wu,Chuan-Jian Zhong
E-mail:zpwu@tju.edu.cn;cjzhong@binghamton.edu
摘要：
质子交换膜燃料电池和直接乙醇燃料电池已成为可持续性清洁能源研究的一个聚焦点。在燃料电池中,氧还原反应和乙醇氧化反应是两个重要的反应,其相关高活性、高稳定性并且廉价的催化剂的研发仍然存在很多问题,极大地制约了燃料电池的大规模商业化应用。其中的挑战主要来自于对纳米催化剂结构和反应机理的有限认识。由于实验表征理论计算的结合,对钯基合金纳米材料电催化剂的研究得到了很大的进展。本文从实验和理论计算两个方面出发,重点讨论了应用于氧还原反应和乙醇氧化反应的钯和钯基电催化剂的结构和反应机理方面的近期研究的一些见解。这些见解对未来催化剂的设计与优化有一定的启发意义。
吴志鹏, 钟传建. 钯基氧还原和乙醇氧化反应电催化剂:关于结构和机理研究的一些近期见解[J]. 电化学（中英文）, 2021, 27(2): 144-156.
Zhi-Peng Wu, Chuan-Jian Zhong. Pd-Based Electrocatalysts for Oxygen Reduction and Ethanol Oxidation Reactions: Some Recent Insights into Structures and Mechanisms[J]. Journal of Electrochemistry, 2021, 27(2): 144-156.
Figure 1
(A) A representative transmission electron microscopic (TEM) image (the inset is a representative high-resolution TEM image) of PdCu nanoparticles; (B) A schematic illustration of fcc/bcc phase structure evolution for PdCu nanoparticles[15].
Figure 2
(A) XRD patterns and (B) atomic PDFs for PdCu/C nanoparticles thermochemically treated at different temperatures[15]. (color on line)
Figure 3
RMC models with varying phase structures of PdCu nanoparticle. Yellow and red balls are Cu and Pd atoms, respectively[25]. (color on line)
Figure 4
(A) RDE curves of different PdCu/C catalysts. Insets are the corresponding RMC models featuring different structures; (B) Evolution of the bonding effects, geometric surface area, and retained ORR activity along with the potential cycling numbers for PdCu/400 ℃ catalyst in the in-situ HE-XRD/PEMFC experiment[15, 25]. (color on line)
Figure 5
(A) Energetics of O-O bond cleavage in O2 molecule on fcc and bcc structured PdCu (100) surfaces; (B) Plots of the ORR specific activity and the percentage of fcc structure in the catalyst annealed at different temperatures[15]. (color on line)
Figure 6
(A) Map of the first atomic PDF peak for Pd43Sn57 nanoparticle catalyst in operando experiment; (B) Mass distribution of Pd43Sn57 nanoparticle catalyst in the membrane electrode assemble after 70 min operation; (C) Atomic PDFs of Pd43Sn57 nanoparticle catalyst during in-situ fuel cell operation[28]. (color on line)
Figure 7
(A) Plots of the mass activity and specific activity as a function of chemical composition in PtPd/C alloy catalysts; (B) Variation of OH adsorption energy based on PtPd cluster model with composition; (C) The most stable adsorption configurations of OH on different PtPd alloy cluster models[30]. (color on line)
Figure 8
(A) PEMFC performance curves using PdPtCu and commercial Pt catalysts; (B) Fuel cell stability of PdPtCu catalyst.
Figure 9
The partial reaction network showing the reaction barriers of each elementary step during ethanol oxidation on Pd (100) surface[2]. (color on line)
Figure 10
(A) Cyclic voltammetric curves of Pd/C catalyst in pure 0.5 mol·L-1 KOH solution (blank) and in 0.5 mol·L-1 KOH solution with the addition of 0.5 mol·L-1 acetic acid (0.5 mol·L-1 AA); (B) Normalized peak current on the forward sweep of EOR on Pd/C catalyst in 0.5 mol·L-1 KOH solution with increasing concentrations of pure ethanol, ethanol with acetic acid, and ethanol with acetaldehyde[2]. (color on line)
Figure 11
Cyclic voltammetric curves for different catalysts in 0.5 mol·L-1 KOH solution containing 0.5 mol·L-1 ethanol. (A) Pd/C (a) and PdCo/C (b); (B) Pd/C (a) and PdCu/C (b). Inserts are the corresponding comparisons of mass activities[37]. (color on line)
Figure 12
Cyclic voltammetric curves for different catalysts in 1.0 mol·L-1 NaOH solution with 1.0 mol·L-1 ethanol. (A) Au/C, Pd/C, and Au@Pd/C; (B) Au@Pd/C catalysts with varying Au core particle sizes[33]. (color on line)
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