納米鐵氧化物修飾MFC陽(yáng)極的制備及其提升微生物產(chǎn)電性能的研究
發(fā)布時(shí)間：2018-08-13 19:29
【摘要】：微生物燃料電池(microbial fuel cell, MFC)是一種利用微生物作為催化劑氧化有機(jī)物或無(wú)機(jī)物產(chǎn)生電能的裝置。與其他可再生能源技術(shù)相比,MFC技術(shù)可以從廢水中回收以可生物降解有機(jī)物形式存在的能量,在產(chǎn)電的同時(shí)達(dá)到污水治理的功效,然而當(dāng)前MFC的發(fā)展受到功率輸出低、成本高的限制。陽(yáng)極作為MFC必不可少的組成部分,直接影響產(chǎn)電菌的附著和電子的胞外傳遞,是限制MFC性能提升的關(guān)鍵因素,因此選用和開發(fā)合適的陽(yáng)極材料對(duì)于改善MFC的產(chǎn)電性能、降低MFC的成本起著至關(guān)重要的作用。碳質(zhì)材料因其具有生物相容性好、機(jī)械強(qiáng)度高、導(dǎo)電性好、價(jià)格低廉等優(yōu)勢(shì),已成為目前最受歡迎的MFC陽(yáng)極材料。Shewanella——兼性厭氧,一類重要的異化金屬還原菌(dissimilatory metal-reducing bacteria, DMRB)——在MFC中作為模式產(chǎn)電菌而被頻繁使用。鐵氧化物作為天然電子受體能夠被Shewanella外膜上的細(xì)胞色素C(c-type cytochromes, c-Cyts)識(shí)別而進(jìn)行直接胞外電子傳遞(direct electron transfer, DET),受此啟發(fā)我們利用納米鐵氧化物修飾碳紙電極(carbon paper, CP),以期提高產(chǎn)電菌的胞外電子傳遞(extracellular electron transfer, EET)速率從而改善MFC的產(chǎn)電性能,本文主要結(jié)果如下：(1)利用100℃6h原位水熱法成功制備了一維(1D)α-FeOOH納米線修飾的碳紙電極(NWs/CP),其中納米線的直徑在20-60nm,長(zhǎng)度在650nm～1um。利用循環(huán)伏安法(cyclic voltammetry, CV)和電化學(xué)交流阻抗譜(electrochemical impedance spectroscopy, EIS)研究CP和NWs/CP的電化學(xué)活性。在進(jìn)行42h時(shí)間-電流曲線(i-t)測(cè)試后,CP的電流密度為0.007mA/cm2,而NWs/CP的電流密度比CP提高了71%,達(dá)到了0.012mA/cm2,這是由于α-FeOOH納米線修飾的CP比空白CP更有利于產(chǎn)電菌的附著,且修飾電極的電荷轉(zhuǎn)移電阻減小。i-t測(cè)試結(jié)束后立即進(jìn)行CV掃描,在-0.285V處,NWs/CP的還原峰值電流是CP的20多倍。以上結(jié)果表明原位水熱法制備的修飾電極具有良好的生物相容性以及優(yōu)異的生物電催化活性,因此可以用作MFC陽(yáng)極。(2)利用260℃24h原位水熱法成功制備了二維(2D)a-Fe2O3納米片修飾的碳紙電極(NSs/CP),其中納米片的寬度在5～11μm,厚度在450-800nm。在進(jìn)行20h i-t測(cè)試后,NSs/CP的電流密度為0.0036mA/cm2,約為CP的1.9倍,這可歸因于修飾電極電荷轉(zhuǎn)移電阻的減小。i-t測(cè)試結(jié)束后立即進(jìn)行CV掃描,NSs/CP的CV曲線出現(xiàn)了一對(duì)明顯的氧化還原峰,計(jì)算得出中點(diǎn)電位為-0.233V(vs. SCE),這與文獻(xiàn)報(bào)道的Shewanella外膜上c-Cyts OmcA的中點(diǎn)電位一致(-201mV vs. Ag/AgCl),以上說(shuō)明CP修飾αt-Fe2O3納米片后促進(jìn)了產(chǎn)電菌利用c-Cyts OmcA進(jìn)行DET,從而提高了傳遞效率。我們還通過(guò)控制加水量,制備了寬度分別在400-500nm、180-200nm和60-80nm的α-Fe2O3納米片修飾的CP,電化學(xué)測(cè)試表明當(dāng)納米片的寬度由微米級(jí)減小到納米級(jí)時(shí),更有利于促進(jìn)產(chǎn)電菌EET速率的提升。(3)利用100℃10h水熱輔以通N2保護(hù)情況下500℃2h固相煅燒成功制備了三維(3D)a-Fe2O3介孔納米柱陣列修飾的碳紙電極(NRs-A/CP),其中單個(gè)納米柱的直徑約在70-150nm,長(zhǎng)度約在500-700nm。在進(jìn)行48h i-t測(cè)試后,CP的電流密度為0.00640mA/cm2,而NRs-A/CP的電流密度比CP提高了62.5%,達(dá)到了0.0104mA/cm2,這可歸因于修飾電極電荷轉(zhuǎn)移電阻的減小。EIS測(cè)試結(jié)束后,用新鮮的DM更換半電池中的電解液,CV測(cè)試表明換液對(duì)NRs-A/CP和生物膜之間的電子傳遞影響極小,這可能是由于產(chǎn)電菌與NRs-A/CP的結(jié)合比空白CP更加緊密。
[Abstract]:Microbial fuel cell (MFC) is a device that uses microorganisms as catalysts to oxidize organic or inorganic substances to generate electricity. Compared with other renewable energy technologies, MFC can recover energy in the form of biodegradable organic substances from wastewater, which can produce electricity and achieve the effect of wastewater treatment. However, the development of MFC is limited by low power output and high cost. As an indispensable part of MFC, anode directly affects the attachment of bacteria and the extracellular transmission of electrons. It is the key factor to restrict the performance of MFC. Therefore, the selection and development of appropriate anode materials can improve the performance of MFC and reduce the cost of MFC. Carbonaceous materials have become the most popular anode materials for MFC because of their good biocompatibility, high mechanical strength, good electrical conductivity and low cost. Shewanella, facultative anaerobic, a kind of important dissimilatory metal-reducing bacteria (DMRB), is used as a model in MFC. Ferric oxide as a natural electron receptor can be recognized by cytochrome C (c-type cytochromes, c-Cyts) on Shewanella adventitia for direct electron transfer (DET), which inspires us to modify carbon paper electrode (CP) with nano-iron oxide. The main results are as follows: (1) One-dimensional (1D) a-FeOOH nanowires modified carbon paper electrode (NWs/CP) was successfully prepared by in situ hydrothermal method at 100 C for 6 h. The diameter of nanowires was 20-60 nm and the length was 650-1 um. The electrochemical activities of CP and NWs/CP were studied by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). After 42 h time-current curve (i-t) test, the current density of CP was 0.007 mA/cm2, and the current density of NWs/CP was 71% higher than that of CP, reaching 0.012 mA/cm2. This is the result of the test. CV scanning was performed immediately after the I-T test, and the reduction peak current of NWs/CP at -0.285V was more than 20 times that of CP. The results showed that the modified electrode prepared by in-situ hydrothermal method had good biocompatibility. (2) Two-dimensional (2D) a-Fe2O3 nanosheet modified carbon paper electrode (NSs/CP) was successfully prepared by in-situ hydrothermal method a t 260 C for 24 h. The nanosheet was 5-11 micron in width and 450-800 nm in thickness. CV scanning immediately after the I-T test showed a pair of obvious redox peaks in the CV curve of NSs/CP. The calculated neutral potential was - 0.233 V (vs. SCE), which was consistent with the reported neutral potential of c-Cyts OmcA on Shewanella epimembrane (- 201 mV vs. Ag / AgCl). These results indicated that CP modified nanosheets of alpha t-Fe2O3 promoted the use of c-Cyts OmcA for DET and thus improved the transfer efficiency.We also prepared alpha-Fe2O3 nanosheets with widths of 400-500 nm, 180-200 nm and 60-80 nm respectively by controlling the amount of water added.Electrochemical measurements showed that when the width of nanosheets decreased from micron to nanometer (3) Carbon paper electrode (NRs-A/CP) modified by three-dimensional (3D) a-Fe2O3 mesoporous nanocolumn array was successfully prepared by solid-state calcination a t 500 2 h under 100 10 h hydrothermal condition with N2 protection. The diameter of a single nanocolumn was about 70-150 nm and the length was about 500-700 nm. The current density of CP was 0.00640mA/cm2, while that of NRs-A/CP was 62.5% higher than that of CP, which could be attributed to the decrease of charge transfer resistance of modified electrode. After EIS test, fresh DM was used to replace the electrolyte in the half cell. CV test showed that the electrolyte exchange affected the electron transfer between NRs-A/CP and biofilm. This may be due to the combination of NRs-A/CP and CP.
【學(xué)位授予單位】：東南大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TM911.45
[Abstract]:Microbial fuel cell (MFC) is a device that uses microorganisms as catalysts to oxidize organic or inorganic substances to generate electricity. Compared with other renewable energy technologies, MFC can recover energy in the form of biodegradable organic substances from wastewater, which can produce electricity and achieve the effect of wastewater treatment. However, the development of MFC is limited by low power output and high cost. As an indispensable part of MFC, anode directly affects the attachment of bacteria and the extracellular transmission of electrons. It is the key factor to restrict the performance of MFC. Therefore, the selection and development of appropriate anode materials can improve the performance of MFC and reduce the cost of MFC. Carbonaceous materials have become the most popular anode materials for MFC because of their good biocompatibility, high mechanical strength, good electrical conductivity and low cost. Shewanella, facultative anaerobic, a kind of important dissimilatory metal-reducing bacteria (DMRB), is used as a model in MFC. Ferric oxide as a natural electron receptor can be recognized by cytochrome C (c-type cytochromes, c-Cyts) on Shewanella adventitia for direct electron transfer (DET), which inspires us to modify carbon paper electrode (CP) with nano-iron oxide. The main results are as follows: (1) One-dimensional (1D) a-FeOOH nanowires modified carbon paper electrode (NWs/CP) was successfully prepared by in situ hydrothermal method at 100 C for 6 h. The diameter of nanowires was 20-60 nm and the length was 650-1 um. The electrochemical activities of CP and NWs/CP were studied by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). After 42 h time-current curve (i-t) test, the current density of CP was 0.007 mA/cm2, and the current density of NWs/CP was 71% higher than that of CP, reaching 0.012 mA/cm2. This is the result of the test. CV scanning was performed immediately after the I-T test, and the reduction peak current of NWs/CP at -0.285V was more than 20 times that of CP. The results showed that the modified electrode prepared by in-situ hydrothermal method had good biocompatibility. (2) Two-dimensional (2D) a-Fe2O3 nanosheet modified carbon paper electrode (NSs/CP) was successfully prepared by in-situ hydrothermal method a t 260 C for 24 h. The nanosheet was 5-11 micron in width and 450-800 nm in thickness. CV scanning immediately after the I-T test showed a pair of obvious redox peaks in the CV curve of NSs/CP. The calculated neutral potential was - 0.233 V (vs. SCE), which was consistent with the reported neutral potential of c-Cyts OmcA on Shewanella epimembrane (- 201 mV vs. Ag / AgCl). These results indicated that CP modified nanosheets of alpha t-Fe2O3 promoted the use of c-Cyts OmcA for DET and thus improved the transfer efficiency.We also prepared alpha-Fe2O3 nanosheets with widths of 400-500 nm, 180-200 nm and 60-80 nm respectively by controlling the amount of water added.Electrochemical measurements showed that when the width of nanosheets decreased from micron to nanometer (3) Carbon paper electrode (NRs-A/CP) modified by three-dimensional (3D) a-Fe2O3 mesoporous nanocolumn array was successfully prepared by solid-state calcination a t 500 2 h under 100 10 h hydrothermal condition with N2 protection. The diameter of a single nanocolumn was about 70-150 nm and the length was about 500-700 nm. The current density of CP was 0.00640mA/cm2, while that of NRs-A/CP was 62.5% higher than that of CP, which could be attributed to the decrease of charge transfer resistance of modified electrode. After EIS test, fresh DM was used to replace the electrolyte in the half cell. CV test showed that the electrolyte exchange affected the electron transfer between NRs-A/CP and biofilm. This may be due to the combination of NRs-A/CP and CP.
【學(xué)位授予單位】：東南大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TM911.45
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