氧還原反應(yīng)（Oxygen reduction reaction,ORR）催化劑,作為燃料電池的陰極材料,在其電化學(xué)能量轉(zhuǎn)換中起著重要的作用。催化材料決定了氧氣還原反應(yīng)的速率,目前商業(yè)化的催化劑是負(fù)載在碳上的高度分散的鉑（Pt）納米粒子材料。然而,Pt價(jià)格昂貴,且在堿性/酸性溶液中易被腐蝕。過渡金屬碳化物和碳氮化物具有導(dǎo)電性高(104Ω^-1m^-1)、結(jié)構(gòu)容易調(diào)控、化學(xué)穩(wěn)定性好等優(yōu)點(diǎn)。它們的合成方法簡單且環(huán)境友好;同時(shí),用于制備相關(guān)材料的前驅(qū)體在地球上儲量豐富。為了降低成本,實(shí)現(xiàn)可持續(xù)電化學(xué)能量轉(zhuǎn)換,該材料被廣泛地用于取代貴金屬基催化劑。近年來金屬碳化物在燃料電池應(yīng)用方面取得了很大的進(jìn)展,已有報(bào)道相關(guān)材料的功率密度在（14.5-120 mW/cm²）范圍內(nèi)。在此基礎(chǔ)上,本文研究了利用新的合成方法來調(diào)控金屬碳化物和碳氮化物的結(jié)構(gòu)性能,以提高在堿性溶液中的ORR活性。研究內(nèi)容具體如下:第一,研究了碳氮化鈦在氧還原反應(yīng)（ORR）中的催化性能。碳氮化物的合成通常需要在高溫（1200-1800 ^oC）下進(jìn)行,從而... 

【文章來源】：中國科學(xué)院大學(xué)(中國科學(xué)院寧波材料技術(shù)與工程研究所)浙江省

【文章頁數(shù)】：152 頁

【學(xué)位級別】：博士

【文章目錄】：
摘要
Abstract
Chapter 1:Introduction
    1.1 The early proposed catalysts for oxygen reduction reaction
    1.2 Physicochemical properties of carbides relevant for ORR activity
    1.3 Carbides as supports for ORR activity
    1.4 Carbides and non-metal support as ORR electrocatalysts
    1.5 Carbonitride support
    1.6 Methods relevant for tuning physicochemical properties of carbon and carbonitrides support
    1.7 Reference
Chapter 2:Experimental Preparation
    2.1 Main reagent adopted in experiments
    2.2 Instruments
    2.3 Synthetic methods for metal carbides
        2.3.1 Direct element combination
        2.3.2 Carbothermal Synthesis
        2.3.3 Sol-gel synthesis
        2.3.4 Gas phase reaction synthesis
        2.3.5 Solvothermal Synthesis
        2.3.6 Sonochemical synthesis
        2.3.7 Electrochemical synthesis
        2.3.8 Solid State Metal Oxide-Organic Reaction
    2.4 Post-synthesis heat treatment of carbides
    2.5 Reference
Chapter 3:Catalytic Effect of Co@TiC_(0.25)N_(0.75):the Electrocatalyst for Oxygen Reduction Reaction Activity in Alkaline Water
    3.1 Introduction
    3.2 Experimental section
        3.2.1 Electrocatalysts preparation
        3.2.2 Electrocatalysts synthetic mechanism
        3.2.3 Oxygen Reduction Reaction in Alkaline water
    3.3 Result and discussion
        3.3.1 The structural property of the electrocatalyst
        3.3.2 Co distribution on TiC_(0.25)N_(0.75) support
        3.3.3 Discussion of Oxygen Reduction Reaction Performance
        3.3.4 Kinetic modeling
    3.4 Conclusions
    3.5 Reference
Chapter 4:Solid-Solid Separation derived C@CoC_x for High Current Density and Efficient Oxygen Reduction Activity in Alkaline Water
    4.1 Introduction
    4.2 Experimental section
        4.2.1 Catalyst preparation
        4.2.2 Oxygen reduction of alkaline water
    4.3 Result and discussion
        4.3.1 Effect of synthesis design on structural properties of catalyst
        4.3.2 Structural property of the catalysts,surface area and pore distributions
        4.3.3 Oxygen reduction reaction activity and Kinetics modeling
    4.4 Conclusion
    4.5 References
Chapter 5:Single Phase Anti-perovskite Ternary Metal carbides for Oxygen Reduction Reaction on the Surface of Alkaline Water
    5.1 Introduction
    5.2 Experiment
        5.2.1 Anti-perovskite ternary metal carbides preparation
        5.2.2 Characterization
    5.3 Results and discussion
        5.3.1 Physicochemical property of anti-perovskite metal carbides
        5.3.2 Electrochemical performance of anti-perovskite metal carbides
    5.4 Conclusion
    5.5 References
Chapter 6:Summary and Outlook
    6.1 Summary
        6.1.1 Titanium carbonitride as a support for nanoparticles for ORR activity
        6.1.2 Hollow carbon supported CoC_x catalyst for alkaline water oxygen reduction activity
        6.1.3 Modified catalytic property of anti-perovskite metal carbides
    6.2 Outlook
Appendix
Acknowledgement
Author's resume and academic papers and research results published during the course of this degree


【參考文獻(xiàn)】：
期刊論文
[1]氮、硫共摻雜的碳負(fù)載的鈷@碳化鈷:一種高效的非貴金屬氧還原電催化劑（英文）[J]. 申海波,江浩,劉易斯,郝佳瑜,李文章,李潔.  物理化學(xué)學(xué)報(bào). 2017(09)



本文編號：3313145