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過渡金屬化合物氮化鈷和磷化鎳用于光催化水分解制氫應(yīng)用研究

發(fā)布時間:2018-02-08 19:43

  本文關(guān)鍵詞: 光催化制氫 水分解 助催化劑 氮化鈷 磷化鎳 出處:《中國科學(xué)技術(shù)大學(xué)》2017年碩士論文 論文類型:學(xué)位論文


【摘要】:能源短缺問題是目前人類面臨的最重大的問題之一。通過光催化水分解完成太陽能到氫能的轉(zhuǎn)化是解決當(dāng)前能源問題的一條重要途徑。在光催化水分解制氫的過程中,加入適當(dāng)?shù)闹呋瘎┛梢宰鳛榇呋磻?yīng)位點,促進(jìn)催化劑中光生載流子的傳輸和分離,實現(xiàn)光催化劑反應(yīng)活性的提升。貴金屬是一類較高效的光催化水分解助催化劑材料,然而由于貴金屬材料具有低儲量、高成本等缺點,很大程度地制約了它們的大規(guī)模實際應(yīng)用。故而探尋適用于光催化水分解制氫的非貴金屬助催化劑極為重要。近些年來,人們發(fā)現(xiàn)第一周期過渡金屬及其化合物在催化水分解方面表現(xiàn)出很好的性質(zhì)。其中,金屬鎳單質(zhì)和鈷單質(zhì)都能作為高效的催化水分解制氫催化劑,但是其易被氧化的缺點制約了它們的應(yīng)用。本文主要研究了以下兩種既能較好保持金屬單質(zhì)的催化活性,又具有較高穩(wěn)定性的過渡金屬化合物在光催化水分解制氫中的應(yīng)用。1.氮化鈷(Co3N)在光催化水分解制氫效果較好的半導(dǎo)體CdS納米棒表面原位合成Co3N納米顆粒,以Na2S和Na2SO3為犧牲劑,在可見光照射下測量其分解水制氫的效率。實驗結(jié)果得其最大產(chǎn)氫速率可達(dá)到137.33μmolh-1 mg-1左右,產(chǎn)氫量子效率為14.9%左右。通過光致發(fā)光譜和光電流實驗的分析,發(fā)現(xiàn)Co3N助催化劑可以有效地轉(zhuǎn)移光生電子。2.磷化鎳(Ni2P)石墨相氮化碳是非金屬光催化劑,具有無毒、低成本等優(yōu)點,但其因為光生載流子復(fù)合等問題,能量轉(zhuǎn)換效率比較低下。我們通過使用一種簡便的制備方法將其與Ni2P納米顆粒復(fù)合,并測試該復(fù)合催化劑材料的可見光催化水分解制氫的性質(zhì)。實驗結(jié)果顯示復(fù)合了 Ni2P納米顆粒后,體系的產(chǎn)氫效率大大提升。光致發(fā)光譜表明Ni2P作為助催化劑可以有效地抑制光生載流子復(fù)合。
[Abstract]:The problem of energy shortage is one of the most important problems that mankind is facing at present. The conversion of solar energy to hydrogen energy by photocatalytic water decomposition is an important way to solve the current energy problem. In the process of photocatalytic water decomposition to produce hydrogen, The addition of appropriate cocatalyst can be used as the catalytic reaction site to promote the transport and separation of photogenerated carriers in the catalyst, and to enhance the activity of photocatalyst reaction. Precious metals are a kind of efficient photocatalytic catalyst materials for water decomposition. However, due to the disadvantages of low reserves and high cost of precious metal materials, their large-scale practical application is restricted to a great extent. Therefore, it is very important to explore non-noble metal cocatalysts suitable for photocatalytic water decomposition to produce hydrogen. It has been found that transition metals and their compounds exhibit good properties in catalytic water decomposition in the first cycle, in which both nickel and cobalt elements can be used as efficient catalysts for the production of hydrogen by catalytic water decomposition. However, their application is restricted by their easy oxidation. In this paper, the following two kinds of catalysts are studied, which can keep the catalytic activity of metallic elements well. Application of transition metal compounds with high stability in photocatalytic water decomposition to produce hydrogen. 1. Cobalt nitride Co _ 3N) synthesized in situ Co3N nanoparticles on the surface of semiconductor CdS nanorods with better photocatalytic water decomposition to produce hydrogen. Na2S and Na2SO3 were used as sacrificial agents. The experimental results show that the maximum hydrogen production rate can reach about 137.33 渭 molh-1 mg-1 and the quantum efficiency of hydrogen production is about 14.9%. The photoluminescence spectra and photocurrent experiments show that the maximum hydrogen production rate is about 137.33 渭 molh-1 mg-1, and the quantum efficiency of hydrogen production is about 14.9%. It is found that Co3N cocatalyst can effectively transfer photogenerated electrons. The graphite phase carbon nitride is a nonmetallic photocatalyst, which has the advantages of non-toxic and low cost, but it is due to the problems of photogenerated carrier recombination, etc. Energy conversion efficiency is relatively low. We use a simple preparation method to combine it with Ni2P nanoparticles. The properties of the composite catalyst material for hydrogen production by water decomposition under visible light were tested. The experimental results showed that the composite Ni2P nanoparticles were prepared. The photoemission spectra show that Ni2P as a co-catalyst can effectively inhibit photogenerated carrier recombination.
【學(xué)位授予單位】:中國科學(xué)技術(shù)大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:O643.36;TQ116.2

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