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zhaocl鐵桿木蟲 (職業(yè)作家)
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[交流]
關(guān)于贗電容電極材料和Battery-type electrode materials的爭(zhēng)論 已有8人參與
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最近做鈷、鎳等相關(guān)贗電容電極材料的的朋友在投稿時(shí)都會(huì)遇到審稿人提到Battery-type electrode materials，如下： （1）“The as-prepared Ni3(VO4)2 material in this manuscript is termed as a “supercapacitor” electrode material, however, the authors need to carefully check whether Ni3(VO4)2 is a supercapacitor electrode material. The sharp redox peaks in CVs and the flat voltage plateaus in the charge-discharge curves indicate that this material should be a typical battery-type electrode material instead of a pseudocapacitive electrode material. This means that all terms and the calculation of electrochemical performance based on the supercapacitor in this manuscript are unacceptable. More discussion about this issue could be found in literatures, e.g., DOI: 10.1149/2.0201505jes, 10.1021/nn503164x, 10.1126/science.1249625, 10.1126/science.1213003, and B. E. Conway’s book (Electrochemical supercapacitors: scientific fundamentals and technological applications). （2）However, to the best of my knowledge and according to the most recent studies, such system shoudn't be classified as pseudocapacitive material. It's because its electrochemical characteristics is different from a fundamental definition of capacitance (or pseudocapacitance). I'm aware that there is a growing number of reports describing "pseudocapacitive" nature of such oxides as cobalt or nickel but from the fundamental point of view such diffusion controlled faradaic processes charactersistics of aforementioned materials have nothing to do with simple capacitor (or pseudocapacitor)-type storage of electrical charge. Therefore, I suggest to change reported specific capacitances (in F/g) values into specific capacities (in C/g or mAh/g). Also, the energy densities should be calculated using recently suggested methods of evaluation reported in following papers: Thierry Brousse, Daniel Belanger, Jeffrey W. Long, Journal of The Electrochemical Society, 162 A5185-A5189 (2015) * Laheäär, A., Przygocki, P., Abbas, Q., Béguin, Electrochemistry Communications, 60 (2015), 21-25 Further, terms such as " pseudocapacitance", pseudocapacitive" should be used in the manuscript only to distinguish between real pseudocapacitance (such as observed and measured eg. for RuOx or MnOx) and battery-type behaviour such as those reported in the paper. To conclude: the material is of a great potential but as high power battery electrode, rather than capacitive (or pseudocapacitive) material. （3）Materials like Co3O4 should be called as Battery-type electrode, not the Pseudocapacitance according to Journal of the Electrochemical Society, 162 (2015) A5185-A5189. 最近有幾篇文章是徹底妥協(xié)了，如： 1）Physicochemical identity and charge storage properties of battery-type nickel oxide material and its composites with activated carbon. ELECTROCHIMICA ACTA 卷: 194 頁(yè): 480-488 出版年: MAR 10 2016 2) Zhen Li*, et al. A facile enhancement in battery-type of capacitive performance of spinel NiCo2O4 nanostructure via directly tuning thermal decomposition temperature. ELECTROCHIMICA ACTA 卷: 191 頁(yè): 364-374 出版年: FEB 10 2016 3) Erqing Xie*, et al. Construction of hierarchical ZnCo2O4@NixCo2x(OH)6x core/shell nanowire arrays for high-performance supercapacitors. J. Mater. Chem. A, 2016,4, 173-182. 4) Zhongtai Zhang*, et al. Hydroxyl compensation effects on the cycle stability of Nickel-Cobalt layered double hydroxides synthesized via solvothermal method. ELECTROCHIMICA ACTA 卷: 182 頁(yè): 445-451 出版年: NOV 10 2015. 5) High-performance hybrid supercapacitor with 3D hierarchical porous flower-like layered double hydroxide grown on nickel foam as binder-free electrode. Journal of Power Sources, Volume 318, 30 June 2016, Pages 76–85. 關(guān)鍵是 Daniel Belanger, Jeffrey W. Long, Journal of The Electrochemical Society, 162 A5185-A5189 (2015)這篇文章很一般，但很多贗電容的文章審稿都要落到這個(gè)人手里，他順便引用幾篇Science上似是而非的文章，要求你必須按照他這篇文章的要求來(lái)修改。 但是Gogotsi et al (Science, 2011, 334, 917) suggesting to create a National or International testing facility for benchmarking electrodes and devices similar to the facilities that exist for benchmarking photovoltaics . “There should be clear rules for reporting the performance of new materials for EES devices. This would help scientists who are not experts in the field, as well as engineers, investors, and the general public, who rely on the data published by the scientists, to assess competing claims.” 不知道大家遇到這個(gè)問(wèn)題該如何處理？ 非常感謝您的交流！ |
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kk2046
木蟲 (正式寫手)
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不錯(cuò)的整理。 個(gè)人覺(jué)得問(wèn)題最大的根源，在于一開始是把redox/faradaic capacitance當(dāng)成一種pseudocapacitance。 然后用一般計(jì)算electric double layer capacitance的計(jì)算法來(lái)操作，但并不符合capacitance的基本原理。 Daniel Belanger, Jeffrey W. Long, Journal of The Electrochemical Society, 162 A5185-A5189 (2015) 這篇文章看起來(lái)很一般，但作者們是領(lǐng)域先驅(qū)，也是真正的電化學(xué)專家（包括Gogotsi, P. Simon等），嘗試撥亂反正。因?yàn)榻赀@領(lǐng)域火熱，許多電化學(xué)基礎(chǔ)不好的科研人員都涌著去做這塊（包括我自己），節(jié)奏太快，很多機(jī)理沒(méi)搞清楚就趕著發(fā)表，人云亦云，就把錯(cuò)誤當(dāng)正宗了。如果是對(duì)的，就不會(huì)近期文章“妥協(xié)”的情況，因?yàn)闆](méi)有道理說(shuō)服編輯和審稿人......目前也沒(méi)有師姐所說(shuō)的爭(zhēng)論之說(shuō)，因?yàn)榇蠹以疽桓C蜂的發(fā)表，之后大牛們出來(lái)指正，然后又一窩蜂的改正。如果師姐有很好的論述，可以嘗試寫篇correspondence去回應(yīng)。 Gogotsi et al (Science, 2011, 334, 917) 提的是另外的問(wèn)題，在PV領(lǐng)域，個(gè)別實(shí)驗(yàn)室的太陽(yáng)能電池，測(cè)量出的Solar Cell Efficiency如果有特出數(shù)值，會(huì)把器件送到其他公共實(shí)驗(yàn)室（比如NREL, Fraunhofer, AIST）根據(jù)國(guó)際標(biāo)準(zhǔn)做審核（certify），得到的數(shù)據(jù)就有公信力。但是電化學(xué)電容器沒(méi)有這種審核，個(gè)別實(shí)驗(yàn)室用個(gè)別的制備方法、實(shí)驗(yàn)、計(jì)算，得到的結(jié)果并不基于同樣的測(cè)試標(biāo)準(zhǔn)，很容易夸大，難以被其他實(shí)驗(yàn)室復(fù)制、實(shí)用價(jià)值低。我個(gè)人曾在PV課題組工作過(guò)，也做過(guò)電化學(xué)電容，非常認(rèn)可Gogotsi論點(diǎn)的必要。 |
3樓2016-04-28 17:02:42
12樓2016-06-20 13:52:53
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2樓2016-04-28 01:48:27
dens314
鐵桿木蟲 (小有名氣)
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4樓2016-04-29 00:21:07
5樓2016-05-02 21:15:43
zhaocl
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However, when taking into account the fundamental definition of capacitance [1], the term pseudocapacitance should be used [16] only for the materials having the electrochemical signatures of the capacitive-type electrodes, i.e. characterized by linear dependencies of charge accumulated within certain ranges of applied potentials and the linear (mirror-like) galvanostatic charge-discharge responses [15]. Having in mind this definition, nickel oxide (undergoing charging-discharging according to a Faradaic mechanism) should be considered more as high-power battery-type rather than pseudocapacitive material. [1] B.E. Conway. Electrochemical Supercapacitors: Scientific Fundamentals and Technological Applications. Springer US (1999) [16] T. Brousse, D. Bélanger, J.W. Long. J. Electrochem. Soc., 162 (2015), pp. A5185–A5189. |
6樓2016-05-02 23:39:05
7樓2016-05-09 10:17:24
zhaocl
鐵桿木蟲 (職業(yè)作家)
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8樓2016-05-09 11:42:21
9樓2016-06-15 16:59:58
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樓主引的幾篇文章中就有我的一篇。 我覺(jué)得你是小看這篇文章了， Daniel Belanger, Jeffrey W. Long, Journal of The Electrochemical Society, 162 A5185-A5189 (2015)， 大牛就是大牛，到現(xiàn)在這篇論文都被引了超過(guò)100次。 可以看看這三個(gè)作者之前的文章，也是很有說(shuō)服力的，早在2011的MRS Bulletin，Asymmetric electrochemical capacitors-Strerching the limits of aqueous electrolytes上，作者就開始嘗試區(qū)別這些機(jī)理，然后從2011-2016這幾年，氧化還原型電極材料的研究徹底陷入一種電容與堿性電池的混亂狀態(tài)，是時(shí)候需要重新梳理了。 |
10樓2016-06-17 22:50:22
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