电化学（中英文） ›› 2021, Vol. 27 ›› Issue (3): 233-256. doi: 10.13208/j.electrochem.201252
张伟艺1, 马宪印1, 邹受忠2,*(
), 蔡文斌1,*()
收稿日期:2021-02-21
修回日期:2021-03-26
出版日期:2021-06-28
发布日期:2021-04-10
通讯作者:
邹受忠,蔡文斌
E-mail:szou@american.edu;wbcai@fudan.edu.cn
Wei-Yi Zhang1, Xian-Yin Ma1, Shou-Zhong Zou2,*(), Wen-Bin Cai1,*()
Received:2021-02-21
Revised:2021-03-26
Published:2021-06-28
Online:2021-04-10
Contact:
Shou-Zhong Zou, Wen-Bin Cai
E-mail:szou@american.edu;wbcai@fudan.edu.cn
摘要：
生物柴油工业的蓬勃发展带来大量副产品丙三醇(甘油),因此如何将甘油转化为高附加值产品具有重要的研究价值。在各种方法中, 电催化氧化由于其条件温和、环境友好和高效率而备受关注。然而,甘油的电氧化非常复杂,涉及许多反应途径和多个电子和质子转移过程,如何合理设计对目标产物具有高选择性的催化剂是很大的挑战。在本文中, 我们主要概述了铂和钯基催化剂上甘油电氧化研究的最新进展。我们首先总结了基于原位和在线谱学研究以及理论计算获得的影响其电催化活性和选择性的因素。然后,选择代表性文献来说明这些因素如何应用于研制高效甘油电氧化催化剂。最后,提出了未来研究中要解决的关键问题。
张伟艺, 马宪印, 邹受忠, 蔡文斌. 铂和钯上丙三醇电氧化研究进展：从反应机理到催化材料[J]. 电化学（中英文）, 2021, 27(3): 233-256.
Wei-Yi Zhang, Xian-Yin Ma, Shou-Zhong Zou, Wen-Bin Cai. Recent Advances in Glycerol Electrooxidation on Pt and Pd: from Reaction Mechanisms to Catalytic Materials[J]. Journal of Electrochemistry, 2021, 27(3): 233-256.
Figure 1
Electro-oxidative valorization of glycerol by means of (A) fuel cell and (B) electrolysis cell. Reproduced with permission[6]. (color on line) Copyright © 2019, The Royal Society of Chemistry.
Figure 2
Plausible reaction pathways with intermediates and products of glycerol oxidation.
Figure 3
Glycerol oxidation mechanism on Pt(111) and Pt(100) electrodes in an acidic solution. Reproduced with permission[24]. Copyright © 2016, American Chemical Society.
Figure 4
Schematic of glycerol electrooxidation mechanism on Pt, PtRu and PtRh in acidic media. Reproduced with permission[34]. (color on line) Copyright © 2016, American Chemical Society.
Figure 5
Reaction pathways proposed for the electrooxidation of glycerol on the bare polycrystalline Pt (Ptp) electrode and after modification by Bi and Pb in alkaline media. Black arrows represent the pathway for the clean Ptp, whereas the green and gray arrows indicate the pathways for the modified electrode. Reproduced with permission[27]. Copyright © 2020, American Chemical Society.
Figure 6
Catalytic routes of glycerol dehydrogenation on Au(111), presented as (A) catalytic cycles and (B) energy landscape. Reproduced with permission[56]. (color on line) Copyright © 2018, American Chemical Society.
Figure 7
Calculated thermodynamically favorable routes. (color on line) Reproduced with permission[57]. Copyright © 2020, American Chemical Society.
Figure 8
Schematic illustration of catalytic surface reactions over the ternary PtRuSn/C catalyst for the electrooxidations of glycerol. Reproduced with permission[62]. Copyright © 2011, Elsevier B.V.
Table 1
Quantitative selectivity of Pt-based electrocatalysts
| Catalyst | Electrolyte | Condition | Selectivity | Ref. |
|---|---|---|---|---|
| Pt9Bi1/C | 2 mol·L-1 glycerol + 0.5 mol·L-1 NaOH | 0.55 V vs. RHE, 4 h, 20 °C | glyceraldehyde 79.6% | [ |
| Pt/C | 0.1 mol·L-1 glycerol + 0.5 mol·L-1 H2SO4 | 1.1 V vs. SHE, 7 h, 60 °C | glyceric acid 57.8% | [ |
| Pt5Ru5/C | dihydroxyacetone 35.0% | |||
| Pt/GNS | 0.5 mol·L-1 glycerol + 0.5 mol·L-1 KOH | 0.2 V vs. SCE, 2 h | glycolate 65.4% | [ |
| PtNi/GNS | 0.1 V vs. SCE, 2 h | glycerate 47.7% | ||
| PtRuNi/GNS | 0.2 V vs. SCE, 2 h | glyceraldehyde 39.2% | ||
| PtRhNi/GNS | -0.4 V vs. SCE, 2 h | oxalate 37.6% | ||
| PtAg skeleton | 0.5 mol·L-1 glycerol + 0.5 mol·L-1 KOH | 0.7 V vs. RHE, 2 h | dihydroxyacetone 82.6% | [ |
| Pt4Au6@Ag | 0.5 mol·L-1 glycerol + 0.5 mol·L-1 KOH | 1.1 V vs. RHE, 2 h | dihydroxyacetone 77.1% | [ |
| PtSb/C | 0.1 mol·L-1 glycerol + 0.5 mol·L-1 H2SO4 | 0.797 V vs. SHE, 10 h, 60 °C | dihydroxyacetone 61.4% | [ |
| Pt2Rh1/C | 0.1 mol·L-1 glycerol + 0.1 mol·L-1 HClO4 | 0.45 V vs. SCE, 8 h, 60 °C | tartronic acid ~40% | [ |
| P-doped Pt/MCNTs | 0.5 mol·L-1 glycerol + 0.5 mol·L-1 KOH | 0.28 V vs. Ag/AgCl, 1 h | tartronate ~52% | [ |
Figure 9
Infrared spectra recorded for glycerol oxidation on Pt/C, Pt3Pd6Bi1/C, and Pt9Bi1/C catalysts in 0.1 mol·L-1 glycerol + 1.0 mol·L-1 NaOH electrolyte (scan rate = 1 mV·s-1, resolution 4 cm-1, T = 293 K). Reproduced with permission[64]. (color on line) Copyright © 2016, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Figure 10
Voltammograms of PtAg skeletons and Pt/C. (A) Cyclic voltammograms (CVs) recorded in 1 mol·L-1 KOH with a scan rate of 50 mV·s-1, (B) linear sweep voltammograms (LSVs) recorded in 0.1 mol·L-1 KOH and 1 mol·L-1 glycerol with a scan rate of 1 mV·s-1 and (C) CVs recorded in 0.1 mol·L-1 KOH + 1 mol·L-1 glycerol with a scan rate of 50 mV·s-1. Both catalysts show a higher current peak in the forward potential scan. Note that the current density of Pt/C was enlarged 5 times. (color on line) Reproduced with permission[81]. Copyright © 2019, American Chemical Society.
Table 2
Quantitative selectivity of Pd-based electro catalysts
| Catalyst | Electrolyte | Condition | Selectivity | Ref. |
|---|---|---|---|---|
| Pd/CNT | 1.0 mol·L-1 glycerol + 6.0 mol·L-1 KOH | 0.2 V vs. SHE, 2 h, 60 °C | tartronate ~60% | [ |
| PdAg3/CNT | oxalate 32% | |||
| Pd/CNT | 1.0 mol·L-1 glycerol + 4.0 mol·L-1 KOH | 0.1 V vs. SHE, 2 h, 60 °C | tartronate 39.5% | [ |
| PdAg3/CNT | oxalate 39.2% | |||
| Pd NCs | 0.5 mol·L-1 glycerol + 0.5 mol·L-1 KOH | -0.4 V vs. SCE, 2 h, ambient temperature. | glyceraldehyde 61.2% | [ |
| Pt@Pd NCs | glycolate ~40% | |||
| PdMn/C | 0.1 mol·L-1 glycerol + 0.1 mol·L-1 NaOH | 0.8 V vs. RHE, 4 h | glycerate ~56% | [ |
| P-doped Pd/CNT | 0.5 mol·L-1 glycerol + 0.5 mol·L-1 KOH | -0.13 V vs. Ag/AgCl, 0.5 h | dihydroxyacetone 90.8% | [ |
| Pd-CNx/G, | 0.5 mol·L-1 glycerol + 0.5 mol·L-1 NaOH | 0 V vs. Hg/HgO, 2 h | glycerate ~32% | [ |
| Pd nanocubes | 0.2 mol·L-1 glycerol + 0.1 mol·L-1 KOH | 0.87 V vs. RHE, 9 h | tartronate 99% | [ |
Figure 11
(A,B) SEM and (C,D) TEM micrographs for a self-supported Pd4Bi sample. Reproduced with permission[107]. Copyright © 2014, American Chemical Society.
Figure 12
Infrared spectra recorded during glycerol oxidation on (A) Pd0.3Au0.7/C, (B) Pd0.5Au0.5/C and (C) Pd0.5Ni0.5/C catalysts in 0.1 mol·L-1 glycerol + 1.0 mol·L-1 NaOH electrolyte at 293 K. Scan rate: 1 mV·s-1, resolution 4 cm-1. Reproduced with permission[110]. Copyright © 2009, Elsevier B.V.
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