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  本文選題：鎳納米顆粒　切入點：鎳納米棒　出處：《天津工業(yè)大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：直接乙醇燃料電池(DEFC)由于其燃料使用安全、來源豐富、價格低廉、易攜帶和儲存等獨特的優(yōu)越性,越來越引起研究者的關(guān)注,高效低成本催化劑的開發(fā)是直接乙醇燃料電池商業(yè)化必須要解決的問題之一。本論文主要采用非貴金屬制備了氮摻雜碳負載鎳金屬催化劑,系統(tǒng)研究了不同碳源、鎳源、原料配比、氮摻雜的情況下對催化劑性能的影響,設(shè)計了具有形貌和尺寸可控的碳載鎳納米材料,并考察了所制備材料對乙醇的電催化性能。1.通過一步合成法制備了氮摻雜碳包覆納米鎳(NiNC)顆粒催化劑(葡萄糖為碳源,乙酸鎳為鎳源,尿素為氮源)。鎳納米粒子的大小可以通過調(diào)節(jié)原材料的質(zhì)量比來調(diào)控。葡萄糖熱處理后變?yōu)槎嗫谆钚蕴�。添加尿素產(chǎn)生了豐富的氮官能團。在制備的所有的催化劑中,NiNC-4催化劑鎳顆粒平均尺寸最小(2.02 nm),BET比表面積最大(400.7m2g-1)以及含氮總量(7.21 at%)最多。多孔碳結(jié)構(gòu),小的鎳納米尺寸和豐富的官能團使NiNC-4催化劑具有良好的電催化性能。在0.1 mol L-1 NaOH+1 mol L-1 C2H5OH溶液中,NiNC-4催化劑的峰電流密度高達327mAcm-2,并且表現(xiàn)出良好的長期循環(huán)穩(wěn)定性,循環(huán)500圈以后,峰電流密度仍然能保持89%。然后移入新的電解液重復(fù)測試,峰電流密度還能達到初始電流密度的96.8%。NiNC-4催化劑優(yōu)良的電催化性能,來源于多孔碳包覆,豐富的含氮基團和小尺寸鎳納米粒子的協(xié)同作用。2.通過一步合成法制備了尺寸可控的鎳納米棒(蔗糖為碳源,氯化鎳為鎳源,尿素為氮源)。討論了不同鎳前驅(qū)體和不同碳源對納米鎳的微觀形貌影響,表明蔗糖和氯離子是形成鎳納米棒的關(guān)鍵因素。鎳納米棒的大小可以通過反應(yīng)物的比例來控制,并且氮摻雜可以提高乙醇電催化氧化性能。在制備的催化劑中,NiNC'-3催化劑性能最好。相比于NiNC'-l催化劑,NiNC'-3催化劑的電流密度(47.5 mA cm-2)和應(yīng)速率常數(shù)分別是它的5倍和16倍。此外,循環(huán)1500圈以后,NiNC'-3催化劑的電流密度仍能保持80.7%,表明NiNC'-3催化劑有良好的循環(huán)穩(wěn)定性。NiNC'-3催化劑對乙醇高的電催化性能可以歸因于均勻的鎳納米棒以及優(yōu)異的導(dǎo)電性和穩(wěn)定的碳載體。
[Abstract]:Direct ethanol fuel cell (DEFC) has attracted more and more attention due to its unique advantages such as safe use of fuel, abundant sources, low price, easy to carry and store. The development of high efficiency and low cost catalyst is one of the problems that must be solved in the commercialization of direct ethanol fuel cell. In this thesis, the nitrogen-doped carbon-supported nickel metal catalyst was prepared and the different carbon and nickel sources were systematically studied. The effects of the ratio of raw materials and nitrogen doping on the performance of the catalyst were investigated. The carbon supported nickel nanomaterials with controllable morphology and size were designed. The electrocatalytic properties of the prepared materials for ethanol were investigated. 1. The nitrogen-doped carbon coated nano-Ni Ni NNCC catalyst (glucose as carbon source, nickel acetate as nickel source) was prepared by one step synthesis method. Urea is nitrogen source. The size of nickel nanoparticles can be adjusted by adjusting the mass ratio of raw materials. After glucose heat treatment, it becomes porous activated carbon. The addition of urea produces rich nitrogen functional groups. The average size of nickel particles in NiNC-4 catalyst was the smallest (2.02 nm) and the maximum specific surface area of BET was 400.7m2g-1) and the total nitrogen content was 7.21 at.1). In 0.1 mol L-1 NaOH 1 mol L -1 C 2H 5OH solution, the peak current density of NiNC-4 catalyst was 327mAcm-2 and showed good long-term cycling stability. After 500 cycles, the peak current density can still be kept 89%. Then the peak current density can reach 96.8% of the initial current density. NiNC-4 catalyst has excellent electrocatalytic performance, and the peak current density can be obtained from the porous carbon coating. The synergistic effect of rich nitrogen-containing groups and small nickel nanoparticles. (2) Nickel nanorods with controlled size (sucrose as carbon source, nickel chloride as nickel source, nickel chloride as nickel source) were prepared by one-step synthesis method. The effects of different nickel precursors and carbon sources on the microstructure of nickel nanocrystalline were discussed. The results show that sucrose and chloride ions are the key factors in the formation of nickel nanorods. The size of nickel nanorods can be controlled by the ratio of reactants. Nitrogen doping can improve the performance of ethanol electrocatalytic oxidation. The catalytic activity of NiNC- 3 is the best in the prepared catalyst. Compared with NiNC'-l catalyst, the current density of NiNC- 3 catalyst is 47.5 Ma cm-2) and the rate constant is 16 times higher than that of NiNC- 3 catalyst. After 1500 cycles, the current density of the catalyst can be maintained at 80.7, which indicates that the NiNC'-3 catalyst has good cyclic stability. The high electrocatalytic performance of the catalyst for ethanol can be attributed to the uniform nickel nanorods, excellent conductivity and stable carbon support.
【學(xué)位授予單位】：天津工業(yè)大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O643.36;TM911.4

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