負(fù)載貴金屬的納米纖維催化劑的制備及應(yīng)用研究
發(fā)布時(shí)間:2018-05-27 21:42
本文選題:靜電紡絲 + 貴金屬負(fù)載; 參考:《吉林大學(xué)》2015年碩士論文
【摘要】:近些年來,生物傳感器越來越受到人們的關(guān)注,這其中對神經(jīng)遞質(zhì)類物質(zhì)的檢測研究尤為熱門,而利用電化學(xué)方法檢測,是現(xiàn)在最常用的方法之一。電化學(xué)傳感器發(fā)展迅猛,不僅成本低廉、響應(yīng)迅速,而且結(jié)果準(zhǔn)確,是目前最好也是最方便的檢測方法,越來越成為電化學(xué)領(lǐng)域研究的熱點(diǎn),這其中找到合適的修飾物來修飾電極以提高測試的準(zhǔn)確性和靈敏度就是關(guān)鍵。另外,除了對已有物質(zhì)的檢測以外,目前人類社會正面臨嚴(yán)重的環(huán)境污染和能源危機(jī),所以尋找新的對人類有益的物質(zhì)也迫在眉睫,F(xiàn)在科學(xué)家們已經(jīng)開始不遺余力的開發(fā)新的清潔能源。氫能源作為最有潛力的新能源之一,已經(jīng)成了科學(xué)家們青睞的研究對象,但目前,氫氣的制備和儲存仍然面臨著很多難以攻克的難題,即使現(xiàn)在已經(jīng)有能夠?qū)嶋H應(yīng)用的儲氫物質(zhì)存在,但釋放其中的氫氣也需要苛刻的條件,所以研發(fā)能在溫和條件下就能讓氫氣釋放的催化劑具有重要的現(xiàn)實(shí)意義。 靜電紡絲因其裝置簡單、成本低廉、發(fā)展較為成熟,已經(jīng)成為制備一維納米纖維最有效的辦法。一維納米纖維在用于電極修飾時(shí)可以增加電子的流動性,提高電化學(xué)傳感器的靈敏度,改善電化學(xué)傳感器的檢測能力;加之納米纖維具有大的比表面積,高的長徑比和孔隙率,在用作催化劑基底時(shí)能夠有效的增加催化位點(diǎn),,提高催化效率,而且在多相催化反應(yīng)中,納米纖維膜的成膜性還為催化劑的回收再利用提供了便捷。 綜上,本論文基于靜電紡絲技術(shù)分別制備了金屬/無機(jī)物和金屬/有機(jī)物復(fù)合納米纖維,并將其應(yīng)用于多巴胺的電化學(xué)檢測和硼烷氨水解制氫的催化中,具體研究成果如下: (1)利用靜電紡絲和焙燒相結(jié)合的技術(shù),成功制備了CeO2/Au復(fù)合納米纖維。由于Au具有良好的導(dǎo)電性、電化學(xué)穩(wěn)定性和生物相容性,納米化的CeO2電子晶界電阻小,電導(dǎo)率高,而且無毒、穩(wěn)定,我們將其復(fù)合作為電極修飾物用作多巴胺的電化學(xué)檢測,得到的檢測限(S/N=3)低達(dá)0.056M,經(jīng)過I-t曲線計(jì)算得到靈敏度為127A·mM1·cm2,同時(shí)在不同掃速的CV曲線中可以看出,整個(gè)過程是受到表面擴(kuò)散速度控制的。該方法為制備多巴胺電化學(xué)傳感器提供了新的途徑。 (2)利用靜電紡絲和微波還原相結(jié)合的技術(shù),成功制備了PAN/Ag/Pd復(fù)合納米纖維,并將其用于催化硼烷氨水解制氫的反應(yīng)中,經(jīng)測試得到的催化轉(zhuǎn)化率值(TOF)達(dá)到了377.2mol H2·h-1·(mol Pd)-1。又經(jīng)過四次同樣的過程循環(huán)測試,仍保持較高催化活性。這是我們首次將金屬/聚合物復(fù)合納米纖維催化劑應(yīng)用在硼烷氨水解制氫的反應(yīng)中,為硼烷氨水解制氫反應(yīng)催化劑的制備提供了新的思路。
[Abstract]:In recent years, more and more attention has been paid to biosensors, in which the detection of neurotransmitters is particularly popular. Electrochemical detection is one of the most commonly used methods. Electrochemical sensors are developing rapidly, not only low cost, rapid response, but also accurate results. It is the best and most convenient detection method at present, and has become a hot spot in the field of electrochemistry. The key is to find the right modifier to modify the electrode to improve the accuracy and sensitivity of the test. In addition, in addition to the detection of existing substances, human society is facing serious environmental pollution and energy crisis at present, so it is urgent to find new substances that are beneficial to human beings. Now scientists are sparing no effort to develop new clean energy sources. Hydrogen energy, as one of the most potential new energy sources, has become a favorite research object of scientists, but at present, the preparation and storage of hydrogen still face many difficult problems. Even though there are some hydrogen storage materials which can be used in practice, the release of hydrogen also requires harsh conditions. Therefore, it is of great practical significance to develop a catalyst that can release hydrogen under mild conditions. Electrostatic spinning has become the most effective method for the preparation of one-dimensional nanofibers because of its simple device, low cost and mature development. One-dimensional nanofibers can increase the mobility of electrons, improve the sensitivity of electrochemical sensors and improve the detection ability of electrochemical sensors when they are used for electrode modification. In addition, nanofibers have large specific surface area, high aspect ratio and porosity. When used as the catalyst substrate, it can effectively increase the catalytic sites and improve the catalytic efficiency. In the heterogeneous catalytic reaction, the film-forming property of the nanofiber membrane also provides a convenient way for the recovery and reuse of the catalyst. In this thesis, metal / inorganic and metal / organic composite nanofibers were prepared based on electrospinning technology, and were applied to the electrochemical detection of dopamine and the catalytic reaction of borane ammonia to produce hydrogen. The results are as follows. 1) CeO2/Au nanofibers were successfully prepared by using the technology of electrostatic spinning and roasting. Due to the good conductivity, electrochemical stability and biocompatibility of au, the nanocrystalline CeO2 has low resistance, high conductivity, nontoxic and stable, so we used it as an electrode modifier for the electrochemical detection of dopamine. The detection limit is as low as 0.056M.The sensitivity is 127A mM1 / cm ~ 2 calculated by I-t curve. It can be seen that the whole process is controlled by the surface diffusion velocity in the CV curves of different sweep speeds. This method provides a new way for the preparation of dopamine electrochemical sensor. (2) PAN/Ag/Pd composite nanofibers were successfully prepared by electrospinning and microwave reduction, and were used to catalyze the hydrolysis of borane to hydrogen in aqueous solution. The measured catalytic conversion value of TOF was up to 377.2mol H 2h -1 / mol PdN 1. After four cycles of the same process, the catalytic activity remained high. This is the first time that the metal / polymer nanofiber catalyst has been used in the hydrolysis of borane to produce hydrogen, which provides a new idea for the preparation of catalyst for the hydrolysis of borane to hydrogen.
【學(xué)位授予單位】:吉林大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2015
【分類號】:O643.36;TQ116.2
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