乙二醇氧化在不同电位区间下的电极负载量的优化

doi:10.13208/j.electrochem.210841

电化学（中英文） ›› 2022, Vol. 28 ›› Issue (2): 2108411. doi: 10.13208/j.electrochem.210841

所属专题： “电催化和燃料电池”专题文章

乙二醇氧化在不同电位区间下的电极负载量的优化

孙圣男¹^,²^,³, 徐梽川¹^,⁴^,⁵^,^*()

1.新加坡南洋理工大学材料科学与工程学院,新加坡,639798
2.新加坡科技研究局材料研究与工程研究院,新加坡,138634
3.北京大学工程科学与新兴技术高精尖创新中心,磁电功能材料与器件北京市重点实验室,北京大学材料科学与工程学院,北京大学工学院,中国北京,100871
4.新加坡-希伯来大学联合研究院,CREATE卓越研究和科技企业园区,新加坡,138602
5.新加坡南洋理工大学能源研究所,交叉研究生院,新加坡,639798

收稿日期:2021-08-04 修回日期:2021-09-04 出版日期:2022-02-28 发布日期:2021-09-22
通讯作者: 徐梽川 E-mail:xuzc@ntu.edu.sg

Mass Loading Optimization for Ethylene Glycol Oxidation at Different Potential Regions

Sheng-Nan Sun¹^,²^,³, Zhi-Chuan Xu¹^,⁴^,⁵^,^*()

1. School of Materials Science and Engineering, Nanyang Technological University, 639798 Singapore
2. Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR), 138634 Singapore
3. Beijing Innovation Center for Engineering Science and Advanced Technology (BIC-ESAT), Beijing Key Laboratory for Magnetoelectric Materials and Devices (BKL-MMD), School of Materials Science and Engineering, College of Engineering, Peking University, Beijing 100871, China
4. Singapore-HUJ Alliance for Research and Enterprise, Campus for Research Excellence and Technological Enterprise (CREATE), NEW-CREATE Phase II, 138602, Singapore
5. Energy Research Institute@NTU, ERI@N, Interdisciplinary Graduate School, Nanyang Technological University, 639798, Singapore

Received:2021-08-04 Revised:2021-09-04 Published:2022-02-28 Online:2021-09-22
Contact: Zhi-Chuan Xu E-mail:xuzc@ntu.edu.sg

摘要/Abstract

摘要：

由于近年来在电化学能源转化、存储及高附加值化学品电合成上的兴趣,设计与制备电催化剂受到越来越多的关注。活性是电催化剂关键参数之一,但观测到的活性会受到催化剂负载量的影响。本工作中,我们采用Co₃O₄/石墨纸（Co₃O₄/GPE）电极作为电极模型,通过循环伏安法和计时电位法展示Co₃O₄的负载量是如何影响乙二醇在碱性溶液（KOH）中氧化的。基于对氧化还原峰和双电层电容的分析可以得出增加催化剂负载量可以增加电化学活性位点数,也可以在低的氧化电位下促进乙二醇氧化,但在高的电位下并没有明显的促进作用。这个结果提供了对有机小分子电催化剂负载量优化的一些思考。

关键词: 负载量, 氧化还原, 双电层电容, 氧化钴, 乙二醇氧化

Abstract:

Designing and fabricating the electrocatalysts is attracting more and more attention in recent years due to a global interest in developing techniques for electrochemical energy conversion and storage, as well as elelectro-synthesis of valuable chemicals. The activity is one of the key performance parameters for electrocatalysts, while the observed activity can be affected by mass loading of electrocatalysts. Here, we take cobalt oxide (Co₃O₄)/graphite paper electrode (Co₃O₄/GPE) as a model electrode to demon-strate how the mass loading of Co₃O₄ catalyst influences ethylene glycol (EG) oxidation in alkaline (KOH) by cyclic votammetry (CV) and chronopentiometry (CP) approaches. Analyses from redox peaks and double layer capacitances reveal that increasing the mass loading provided more electrochemical active sites. Increasing loading made a positive contribution to EG oxidation at the low oxidation potential, while less significant improvement at the high oxidation potential. The results will provide some insight for optimzing the mass loading of electrocatalysts for electrocatalysis of small organic molecules.

Key words: mass loading, redox, double layer capacitance, cobalt oxide, ethylene glycol oxidation

孙圣男, 徐梽川. 乙二醇氧化在不同电位区间下的电极负载量的优化[J]. 电化学（中英文）, 2022, 28(2): 2108411.

Sheng-Nan Sun, Zhi-Chuan Xu. Mass Loading Optimization for Ethylene Glycol Oxidation at Different Potential Regions[J]. Journal of Electrochemistry, 2022, 28(2): 2108411.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.13208/j.electrochem.210841

https://electrochem.xmu.edu.cn/CN/Y2022/V28/I2/2108411

图/表 4

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参考文献 17

[1]	Wu T Z, Sun S N, Song J J, Xi S B, Du Y H, Chen B, Sasangka W A, Liao H B, Gan C L, Scherer G G, Zeng L, Wang H J, Li H, Grimaud A, Xu Z J. Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation[J]. Nat. Catal., 2019, 2(9):763-772. doi: 10.1038/s41929-019-0325-4 URL
[2]	Lü C D, Zhong L X, Liu H J, Fang Z W, Yan C S, Chen M X, Kong Y, Lee C, Liu D B, Li S Z, Liu J W, Li S, Chen G, Yan Q Y, Yu G H. Selective electrocatalytic synjournal of urea with nitrate and carbon dioxide[J]. Nat. Sustain., 2021, 4(10):868-876. doi: 10.1038/s41893-021-00741-3 URL
[3]	Anantharaj S, Kundu S. Do the evaluation parameters reflect intrinsic activity of electrocatalysts in electrochemical water splitting?[J]. ACS Energy Lett., 2019, 4(6):1260-1264. doi: 10.1021/acsenergylett.9b00686
[4]	Yu L, Sun S, Li H Y, Xu Z J. Effects of catalyst mass loading on electrocatalytic activity: an example of oxygen evolution reaction[J]. Fundamental Research, 2021, 1(4):448-452. doi: 10.1016/j.fmre.2021.06.006 URL
[5]	Sun S N, Li H Y, Xu Z C J. Impact of surface area in evaluation of catalyst activity[J]. Joule, 2018, 2(6):1024-1027. doi: 10.1016/j.joule.2018.05.003 URL
[6]	Chong L, Wen J G, Kubal J, Sen F G, Zou J X, Greeley J, Chan M, Barkholtz H, Ding W J, Liu D J. Ultralow-loading platinum-cobalt fuel cell catalysts derived from imidazolate frameworks[J]. Science, 2018, 362(6420):1276-1281. doi: 10.1126/science.aau0630 pmid: 30409809
[7]	Sun S N, Sun Y M, Zhou Y, Xi S B, Ren X, Huang B C, Liao H B, Wang L Y P, Du Y H, Xu Z C. Shifting oxygen charge towards octahedral metal: a way to promote water oxidation on cobalt spinel oxides[J]. Angew. Chem. Int. Ed., 2019, 58(18):6042-6047. doi: 10.1002/anie.v58.18 URL
[8]	Suntivich J, May K J, Gasteiger H A, Goodenough J B, Shao-Horn Y. A perovskite oxide optimized for oxygen evolution catalysis from molecular orbital principle[J]. Science, 2011, 334(6061):1383-1385. doi: 10.1126/science.1212858 pmid: 22033519
[9]	Wei C, Xu Z C J. The possible implications of magnetic field effect on understanding the reactant of water splitting[J]. Chinese J. Catal., 2021, 43(1):148-157. doi: 10.1016/S1872-2067(21)63821-4 URL
[10]	Sun S N, Sun L B, Xi S B, Du Y H, Prathap MUA, Wang Z L, Zhang Q C, Fisher A, Xu Z C J. Electrochemical oxidation of C3 saturated alcohols on Co₃O₄ in alkaline[J]. Electrochim. Acta, 2017, 228:183-194. doi: 10.1016/j.electacta.2017.01.086 URL
[11]	Xie R C, Batchelor-McAuley C, Rauwel E, Rauwel P, Compton R G. Electrochemical characterisation of Co@Co(OH)₂ core-shell nanoparticles and their aggregation in solution[J]. ChemElectroChem, 2020, 7(20):4259-4268. doi: 10.1002/celc.v7.20 URL
[12]	Xiao Z H, Huang Y C, Dong C L, Xie C, Liu Z J, Du S Q, Chen W, Yan D F, Tao L, Shu Z W, Zhang G H, Duan H G, Wang Y Y, Zou Y Q, Chen R, Wang S Y. Operando identification of the dynamic behavior of oxygen vacancy-rich Co₃O₄ for oxygen evolution reaction[J]. J. Am. Chem. Soc., 2020, 142(28):12087-12095. doi: 10.1021/jacs.0c00257 URL
[13]	Augustyn V, Come J, Lowe M A, Kim J W, Taberna P L, Tolbert S H, Abruña H D, Simon P, Dunn B. High-rate electrochemical energy storage through Li⁺ intercalation pseudocapacitance[J]. Nat. Mater., 2013, 12(6):518-522. doi: 10.1038/nmat3601 URL
[14]	Dai C, Chan C W I, Barrow W, Smith A, Song P, Potier F, Wadhawan J D, Fisher A C, Lawrence N S. A route to unbuffered pH monitoring: a novel electrochemical approach[J]. Electrochim. Acta, 2016, 190:879-886. doi: 10.1016/j.electacta.2016.01.004 URL
[15]	Li Z, Gadipelli S, Li H, Howard C A, Brett D J L, Shearing P R, Guo Z, Parkin I P, Li F. Tuning the interlayer spacing of graphene laminate films for efficient pore utilization towards compact capacitive energy storage[J]. Nat. Energy, 2020, 5(2):160-168. doi: 10.1038/s41560-020-0560-6 URL
[16]	Da Silva L M, De Faria L A, Boodts J F C. Determination of the morphology factor of oxide layers[J]. Electrochim. Acta, 2001, 47(3):395-403. doi: 10.1016/S0013-4686(01)00738-1 URL
[17]	Bard, A J, Faulkner L R. Electrochemical methods fundamentals and applications (Second edition)[M]. John Wiley & Sons, Inc., 2001: 102.

乙二醇氧化在不同电位区间下的电极负载量的优化

Mass Loading Optimization for Ethylene Glycol Oxidation at Different Potential Regions

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