【摘要】：微生物燃料電池(MFC)是一種利用細(xì)菌的代謝作用,高效處理污水中的有機(jī)物同時(shí)將其直接轉(zhuǎn)化為電能的綠色能源技術(shù)。近年來(lái),MFC的體積逐漸縮小到微納級(jí)別,構(gòu)成了微流體微生物燃料電池(MMFC),其作為一種產(chǎn)電設(shè)備和在線分析檢測(cè)技術(shù),在環(huán)境監(jiān)測(cè)、生物分析以及微小電源技術(shù)方面具有廣闊的應(yīng)用和發(fā)展前景,是微流體能源技術(shù)的研究熱點(diǎn)之一。現(xiàn)階段的MMFC主要是對(duì)大型電池的按比例縮小,受到陽(yáng)極側(cè)生物膜分布有限、電池運(yùn)行成本高昂、電池內(nèi)阻大以及單位成本下產(chǎn)電功率密度低等問題的困擾;與此同時(shí),電池中涉及到的流動(dòng)和傳輸現(xiàn)象并未得到深入研究,特別是在流動(dòng)條件下微小空間內(nèi)生物膜的成膜特性尚未闡釋清楚。針對(duì)以上生物膜分布有限和電池功率低下的問題,本文從工程熱物理學(xué)科中的流體力學(xué)和傳質(zhì)理論出發(fā),立足于微流道內(nèi)陽(yáng)極生物膜的分布調(diào)控,對(duì)MMFC內(nèi)的傳輸機(jī)理和產(chǎn)電特性展開研究。研究?jī)?nèi)容主要包括:(1)構(gòu)建了具有單陽(yáng)極液入口的Y型MMFC,研究了陽(yáng)極液濃度、陰極液濃度、反應(yīng)液流量等運(yùn)行參數(shù)對(duì)電池性能的影響,并對(duì)陽(yáng)極側(cè)沿流動(dòng)方向的生物膜分布進(jìn)行了觀察;(2)構(gòu)建了不同電池構(gòu)型的MMFC,從緩解擴(kuò)散混合區(qū)域影響的角度出發(fā),構(gòu)建了具有漸擴(kuò)流道結(jié)構(gòu)的MMFC,從生物膜分布、陽(yáng)極側(cè)內(nèi)阻、電池產(chǎn)電性能等方面研究了改變流道結(jié)構(gòu)對(duì)電池性能的影響;從減薄陽(yáng)極側(cè)邊界層的角度出發(fā),構(gòu)建了具有多陽(yáng)極液進(jìn)口的MMFC,與單陽(yáng)極液進(jìn)口電池的產(chǎn)電性能進(jìn)行了對(duì)比;通過(guò)控制旁路陽(yáng)極液進(jìn)口的開關(guān)狀態(tài)分析了增加陽(yáng)極進(jìn)口對(duì)電池產(chǎn)電性能的作用機(jī)理;(3)構(gòu)建了新型陽(yáng)極電極和空氣自呼吸式MMFC,基于產(chǎn)電菌附著強(qiáng)化思想,構(gòu)建了一種基于氮摻雜石墨烯氣凝膠的新型三維陽(yáng)極材料,分別從材料化學(xué)和生物化學(xué)的角度對(duì)電極進(jìn)行了表征,并從生物膜附著、陽(yáng)極電荷遷移和電池產(chǎn)電方面進(jìn)行了研究;基于流動(dòng)簡(jiǎn)化思想,構(gòu)建了一種單股流體控制下的空氣自呼吸式微流體MFC,研究了所合成催化劑的物理化學(xué)特性和電催化特性,并分別在連續(xù)流和序批條件下進(jìn)行電池性能測(cè)試。本文主要研究成果如下:1)構(gòu)建了一種基于石墨電極的Y型結(jié)構(gòu)MMFC,電池性能隨著陽(yáng)極入口燃料濃度和陽(yáng)極液體積流量的增加而呈現(xiàn)先增加后下降的趨勢(shì);在入口燃料濃度化學(xué)需氧量為1500 mgL~(-1),陽(yáng)極液流量為10 m L h-1時(shí),輸出的最大面積功率密度為618±4 m Wm~(-2）;對(duì)陽(yáng)極側(cè)表面生物膜形貌的觀察發(fā)現(xiàn):產(chǎn)電菌形成的生物膜厚度沿流動(dòng)方向逐漸減薄,即:流體入口段的生物膜厚度要大于充分發(fā)展段的相應(yīng)厚度;2)構(gòu)建了基于漸擴(kuò)、平行、漸縮的三種微流道結(jié)構(gòu)的MMFC,漸擴(kuò)通道成功避免了擴(kuò)散混合區(qū)的影響,整體上擁有更致密的生物膜分布,同時(shí)基于漸擴(kuò)通道的MMFC在陽(yáng)極側(cè)電荷遷移阻力最低,其產(chǎn)生的最大面積功率密度為2447.7±38.9m Wm~(-2）,是基于漸縮通道的MMFC的5.29倍(462.7±17.5 m Wm~(-2）)和基于平行通道的MMFC的1.24倍(1980.1±27.5 m Wm~(-2）);3)構(gòu)建了基于多陽(yáng)極液進(jìn)口的MMFC(MMFC-MI),生物膜在微通道內(nèi)沿流動(dòng)方向整體呈致密分布,特別是在三個(gè)等間距分布的陽(yáng)極液入口處,生物膜的分布遠(yuǎn)遠(yuǎn)大于單進(jìn)口MMFC;電池在接種完成后旁路進(jìn)口關(guān)閉狀態(tài)下MMFC-MI的最大功率密度是打開狀態(tài)下的85.6%,證實(shí)旁路進(jìn)口的主要作用體現(xiàn)在產(chǎn)電菌富集階段,而在接種完成后陽(yáng)極液強(qiáng)化傳輸?shù)淖饔孟鄬?duì)有限;4)構(gòu)建了一種基于石墨烯氣凝膠(N-GA)的生物陽(yáng)極材料,其三維結(jié)構(gòu)和含氮官能團(tuán)有利于強(qiáng)化產(chǎn)電菌在電極內(nèi)外表面的附著;同時(shí)摻雜氮元素后降低了電子從生物膜表面向電極表面的遷移阻力;基于N-GA生物陽(yáng)極的微型MFC所能達(dá)到的體積功率密度為225±12 Wm~(-3）(正比于腔室體積)和750±40 Wm~(-3）(正比于陽(yáng)極體積);5)構(gòu)建了一種單股流體控制下的空氣自呼吸式MMFC,同時(shí)合成了一種含有豐富官能團(tuán)的氮摻雜石墨烯氣凝膠-活性炭(AC@N-GA)氧還原(ORR)催化劑;該催化劑展現(xiàn)了優(yōu)良的ORR催化性能,電子轉(zhuǎn)移數(shù)達(dá)到3.92,H_2O_2產(chǎn)率只有4.5%,以AC@N-GA為催化劑的MMFC連續(xù)流條件下最大功率密度為1181.4±135.6 Wm~(-3）,序批條件下最大功率密度為690.2±62.3 Wm~(-3）,產(chǎn)電性能是相同條件下國(guó)際報(bào)道MMFC的10倍以上。
[Abstract]:Microbial fuel cell (MFC) is a green energy technology which uses the metabolism of bacteria to efficiently deal with organic matter in sewage and directly convert it into electrical energy. In recent years, the volume of MFC has gradually reduced to the micro nano scale, which constitutes a microfluidic biofuel battery (MMFC). It is used as an electric equipment and on-line analysis and detection technique. Operation, in the field of environmental monitoring, bioanalysis and micro power supply, has a broad application and development prospect. It is one of the hot topics in the research of micro fluid energy technology. At the present stage, MMFC mainly reduces the proportion of large batteries, is limited by the distribution of the anode side biofilm, the high cost of the electric pool, the large battery internal resistance and the unit cost. At the same time, the flow and transmission phenomena involved in the battery have not been deeply studied. Especially, the film forming characteristics of the biofilm in the micro space under the flow condition have not been explained clearly. In view of the problems of the limited distribution of the biofilm and the low power of the electric pool, this paper from the Engineering Thermo Physics Based on the theory of fluid mechanics and mass transfer in the family, the transmission mechanism and production characteristics in MMFC are studied based on the distribution and regulation of the anode biofilm in the micro channel. The main contents are as follows: (1) the Y type MMFC with the inlet of the single anode liquid is constructed, and the operating parameters such as the concentration of anode liquid, the concentration of cathode liquid, the flow rate of the reaction liquid and so on are studied. The influence of pool performance was observed and the distribution of biofilm distribution along the direction of the anode side was observed. (2) the MMFC of different battery configurations was constructed. From the angle of alleviating the influence of the diffusion mixing region, the MMFC with the gradually diffused channel structure was constructed. The change of the channel junction was studied from the distribution of the biofilm, the internal resistance of the anode side, the battery production performance and so on. The effect of structure on the performance of the battery was constructed. From the angle of the boundary layer of the thin anode side, MMFC was constructed with the multi anode fluid inlet. The electric performance of the single anode liquid imported battery was compared. The mechanism of increasing the anode inlet on the battery production performance was analyzed by controlling the switch state of the anode liquid inlet. (3) a new method was constructed. A new type of three dimensional anode material based on nitrogen doped graphene aerogels was constructed based on the attachment and strengthening idea of a nitrogen doped graphene. The electrode was characterized from the material chemical and biochemical angles, and the electrode was attached to the biofilm, the anode charge migration and the battery production were studied. Based on the flow simplification idea, a kind of air self breathing micro fluid MFC under the control of single strand fluid was constructed. The physical and chemical properties and electrocatalytic properties of the synthesized catalyst were studied. The performance of the battery was tested under continuous and sequence batch conditions. The main results were as follows: 1) a type of Y type based on graphite electrode was constructed. With the increase of the fuel concentration of the anode inlet and the volume flow of the anode liquid, the performance of the cell MMFC increases first and then decreases. The maximum area power density of the output is 618 + 4 m Wm~ (-2) at the inlet fuel concentration of 1500 mgL~ (-1) and the anodic liquid flow rate of 10 m L H-1. It is found that the thickness of the biofilm formed by the producing bacteria gradually thins along the flow direction, that is, the thickness of the biofilm in the inlet section of the fluid is greater than the corresponding thickness of the full development section; 2) the MMFC based on the three microfluidic structures, which is based on the gradual expansion, parallel and shrinking, has successfully avoided the influence of the diffusion mixing zone and has a more compact overall. The biofilm distribution, at the same time, is the lowest resistance of MMFC based on the anodic side, the maximum area power density is 2447.7 + 38.9m Wm~ (-2), which is based on the 5.29 times of MMFC of the gradually shrinking channel (462.7 + 17.5 m Wm~ (-2)) and 1.24 times of MMFC (1980.1 + 27.5 m Wm~ (-2)) based on the parallel channel; 3) constructed based on the multi anode fluid. The imported MMFC (MMFC-MI), the biofilm is densely distributed along the flow direction in the microchannel, especially at the three equal spaced anodic fluid entrance, the distribution of the biofilm is far greater than that of the single import MMFC, and the maximum power density of the MMFC-MI is 85.6% under the closed state of the battery after the inoculation is completed. The main role of road inlet is reflected in the enrichment stage of producing electric bacteria, and the effect of enhanced transmission of anodic liquid after inoculation is relatively limited; 4) a biological anode material based on graphene aerogel (N-GA) is constructed. Its three-dimensional structure and nitrogen containing functional groups are beneficial to strengthen the attachment of electric bacteria to the inner and outer surfaces of the electrode; and doping nitrogen elements at the same time. The transfer resistance of electrons from the surface of the biofilm to the surface of the electrode was reduced; the volume power density of the micro MFC based on the N-GA bio anode was 225 + 12 Wm~ (-3) and 750 + 40 Wm~ (-3) (positive ratio to the anode volume); 5), a self breathing MMFC under the control of single strand fluid was constructed, and a synthetic one was synthesized at the same time. A nitrogen doped graphene aerogel - active carbon (AC@N-GA) oxygen reduction (ORR) catalyst, which contains rich functional groups, shows excellent ORR catalytic performance, the number of electron transfer is 3.92, the yield of H_2O_2 is only 4.5%, the maximum power density of MMFC continuous flow with AC@N-GA as catalyst is 1181.4 + 135.6 Wm~ (-3), under the precondition batch condition The maximum power density is 690.2 + 62.3 Wm~ (-3), and the electricity generation performance is 10 times higher than that of the international report MMFC under the same conditions.
【學(xué)位授予單位】：重慶大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2016
【分類號(hào)】：TM911.45

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2 周秀秀;微生物燃料電池陰極催化劑雙核酞菁鈷的結(jié)構(gòu)及性能優(yōu)化[D];華南理工大學(xué);2015年

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4 印霞h，

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