本文關(guān)鍵詞：電解水產(chǎn)氫三維電極的構(gòu)建與性能調(diào)控研究　出處：《華南理工大學(xué)》2016年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 三維電極 電催化產(chǎn)氫 二硫化鉬 硫化鈷 石墨烯薄膜

【摘要】：高效穩(wěn)定的電解水產(chǎn)氫催化劑是可再生能源氫能研究的關(guān)鍵,目前廣泛研究的電解水產(chǎn)氫催化劑多為粉末狀,需要添加粘結(jié)劑配成溶液負(fù)載在導(dǎo)電基底上才能參與電解水性能研究。但該過(guò)程不可避免地增大了催化劑與電解質(zhì)溶液的接觸電阻或造成粉末催化劑團(tuán)聚,使得催化劑的電催化活性大打折扣。構(gòu)建電解水三維電極不僅可以有效地解決上述問(wèn)題,還可增大催化劑與電解質(zhì)溶液的接觸面積、增強(qiáng)催化穩(wěn)定性。然而三維電極用作電解水產(chǎn)氫的文獻(xiàn)報(bào)道并不多。近來(lái)研究表明,通過(guò)在三維基底如碳布、碳纖維紙上負(fù)載電解水產(chǎn)氫納米材料或通過(guò)“范德華結(jié)構(gòu)”將二維納米材料進(jìn)行可控組裝可得到高效穩(wěn)定的電解水催化劑。針對(duì)上述現(xiàn)狀,本論文采用不同的方法合成三種不同的電解水產(chǎn)氫三維電極,并對(duì)其產(chǎn)氫催化性能進(jìn)行研究。主要研究?jī)?nèi)容和結(jié)論如下:(1)通過(guò)水熱-電沉積兩步法,在碳纖維上合成了鉑納米顆粒/二硫化鉬納米片/碳纖維三維電極(Pt/MoS2/CFs)。詳細(xì)的電化學(xué)性能表征表明,含鉑量?jī)H為2.03 wt%的Pt/MoS2/CFs催化劑在0.5 mol/L的硫酸電解質(zhì)溶液中顯示了極高的催化活性,其產(chǎn)氫過(guò)電勢(shì)只有5 mV,塔菲爾斜率為53.6 mV/dec。長(zhǎng)時(shí)間的循環(huán)伏安測(cè)試和電流-時(shí)間曲線測(cè)試,顯示催化劑在酸溶液中具有較好的穩(wěn)定性。(2)采用兩步水熱法合成了二硫化鉬納米片/硫化鈷納米線陣列/碳布三維電極(MoS2/CoS2/CC)。本實(shí)驗(yàn)選用碳布為基底,在其表面生長(zhǎng)氫氧化鈷納米線陣列,然后與四硫鉬酸銨水熱反應(yīng)硫化生成硫化鈷納米線陣列,并在硫化鈷上沉積生長(zhǎng)二硫化鉬納米片,同時(shí)實(shí)現(xiàn)對(duì)二硫化鉬的鈷氧摻雜。制備所得的MoS2/CoS2/CC顯示了較低的過(guò)電勢(shì),在-87 mV的電壓下可獲得10 mA/cm2的電流密度,塔菲爾斜率為73.4 mV/dec,催化穩(wěn)定性良好。(3)通過(guò)簡(jiǎn)單的真空抽濾和高溫?zé)Y(jié),研制出一種鈷納米顆粒鑲嵌在層狀氮摻雜石墨烯間的柔性多孔三維電極(Co@NGF)。制備所得的石墨烯薄膜為柔性多孔結(jié)構(gòu),可直接用作電解水產(chǎn)氫電極,在0.5 mol/L的硫酸電解質(zhì)溶液中有較高的電催化產(chǎn)氫活性,過(guò)電勢(shì)僅為14 mV,在-124.6 mV的電壓下可獲得10 mA/cm2的電流密度,塔菲爾斜率為93.9 mV/dec。值得注意的是,本論文首次將Co@NGF電極作為陰極和陽(yáng)極,即組成兩電極體系進(jìn)行電解水產(chǎn)氫測(cè)試,這為全方位的水解催化劑研究開僻了一種新的可能。這種制備技術(shù),亦為水裂解技術(shù)的規(guī)�；峁┝艘环N有效的途徑。本論文采用多種工藝設(shè)計(jì)合成了三種高催化活性的電解水產(chǎn)氫三維電極,為柔性材料在可穿戴電子產(chǎn)品、柔性顯示屏等應(yīng)用上打下堅(jiān)實(shí)基礎(chǔ)。同時(shí),通過(guò)深入研究催化劑組分和結(jié)構(gòu)對(duì)產(chǎn)氫催化活性的影響,為高效穩(wěn)定的電解水產(chǎn)氫催化劑提供重要指導(dǎo)。
[Abstract]:Highly efficient and stable electrolysis hydrogen production catalyst is the key of renewable energy hydrogen research. Currently, the widely researched electrolysis hydrogen catalysts are mostly powdery. It is necessary to add binder and solution to load on the conductive substrate to participate in the research of electrolytic water performance. But this process inevitably increases the contact resistance between catalyst and electrolyte solution, or causes agglomeration of powder catalyst, which makes the electrocatalytic activity of catalyst greatly reduced. The construction of electrolytic water three-dimensional electrode can not only effectively solve the above problems, but also increase the contact area of the catalyst and electrolyte solution, and enhance the catalytic stability. However, there are few reports on the use of three dimensional electrodes for the use of hydrogen in the electrolysis of aquatic products. Recent studies have shown that by electrolysis of hydrogen nanomaterials on three dimensional substrates, such as carbon cloth and carbon fiber paper, or by assembling and assembling two-dimensional nanomaterials by "Fan Dehua structure", efficient and stable electrolysis water catalysts can be obtained. In view of the above situation, three different kinds of electrolysis hydrogen electrode were synthesized by different methods, and the catalytic performance of hydrogen production was studied. The main research contents and conclusions are as follows: (1) through the two step process of Hydrothermal Electrodeposition, platinum nanoparticles / molybdenum disulfide nanosheets / carbon fiber three-dimensional electrode (Pt/MoS2/CFs) were synthesized on carbon fiber. The detailed electrochemical characterization showed that the Pt/MoS2/CFs catalyst containing only 2.03 wt% of platinum exhibited very high catalytic activity in sulfuric acid electrolyte of 0.5 mol/L, and its hydrogen generation potential was only 5 mV, and the Tafel slope was 53.6 mV/dec. The long time cyclic voltammetry and current time curve test showed that the catalyst had good stability in the acid solution. (2) a two step hydrothermal method was used to synthesize molybdenum disulfide nanoscale / cobalt sulfide nanowire arrays / carbon cloth three-dimensional electrodes (MoS2/CoS2/CC). In this experiment, carbon dioxide cloth was used as the substrate to grow cobalt hydroxide nanowire arrays on the surface. Then, the cobalt sulfide nanowire arrays were formed by hydrothermal reaction with ammonium molybdate four, and molybdenum sulfide nanosheets were deposited on cobalt sulfide. Meanwhile, cobalt oxide doped molybdenum disulfide was added. The prepared MoS2/CoS2/CC shows a low overpotential. Under the voltage of -87 mV, the current density of 10 mA/cm2 can be obtained. The slope of Tafel is 73.4 mV/dec, and the catalytic stability is good. (3) by simple vacuum filtration and high temperature sintering, developed a flexible porous three-dimensional electrode in layered nitrogen doped graphene between a cobalt nanoparticles embedded (Co@NGF). Graphene films prepared for flexible porous structure, can be directly used as electrolytic hydrogen electrode in sulfuric acid electrolyte solution of 0.5 mol/L in the electro catalytic activity of hydrogen production is high, the potential is 14 mV, the current density obtained at 10 mA/cm2 voltage -124.6 mV, Tafel slope is 93.9 mV/dec. It is worth noting that this is the first time to the Co@NGF electrode as the cathode and the anode, which consists of two electrode system for electrolytic hydrogen test, this research is a full range of hydrolysis catalyst provides a new possibility. This preparation technology also provides an effective way for the scale of water cracking technology. In this paper, three kinds of highly active three-dimensional electrolysis hydrogen hydrogen electrodes were designed and synthesized by various processes, which lay a solid foundation for flexible materials in wearable electronic products, flexible displays and other applications. At the same time, the influence of the catalyst composition and structure on the catalytic activity of hydrogen production is studied, which provides important guidance for the efficient and stable electrolysis hydrogen catalyst.
【學(xué)位授予單位】：華南理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2016
【分類號(hào)】：O643.36;TQ116.2

【相似文獻(xiàn)】

相關(guān)期刊論文 前10條

1 陳武,李凡修,梅平;三維電極方法處理石油工業(yè)廢水COD的實(shí)驗(yàn)研究[J];環(huán)境科學(xué)與技術(shù);2001年S1期

2 曹瑩,周育紅,孫克寧,周德瑞;三維電極在水處理技術(shù)中的應(yīng)用[J];黑龍江電力;2001年02期

3 蔣萌陽(yáng),朱建榮,戴靜波;復(fù)極性三維電極處理印染廢水的能耗分析[J];寧波工程學(xué)院學(xué)報(bào);2005年02期

4 張斌,劉井軍,車玉泉;三維電極法處理印染廢水的實(shí)驗(yàn)研究[J];吉林化工學(xué)院學(xué)報(bào);2005年04期

5 郭玉鳳;王振川;李景印;李敏;王s，

本文編號(hào)：1342927