發(fā)布時(shí)間：2018-02-10 11:05

  本文關(guān)鍵詞： 鈀基納米催化劑 晶體生長(zhǎng) 框架結(jié)構(gòu) 納米片 異質(zhì)結(jié)構(gòu) 氧還原反應(yīng)二氧化碳電還原反應(yīng)　出處：《中國(guó)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】：貴金屬納米材料作為一類重要的催化劑,在很多催化反應(yīng)中都有著廣泛的應(yīng)用前景,例如,它們既可以被用于燃料電池中,也可以被用于CO2電還原反應(yīng)以及光解水反應(yīng)中。然而,貴金屬在地球上的儲(chǔ)量稀少,因此人們開(kāi)始大力發(fā)展具有不同結(jié)構(gòu)的催化劑,這樣不僅可以在一定程度上減少貴金屬的使用,并且往往還因?yàn)榻M分之間的協(xié)同效應(yīng)而表現(xiàn)出更好的催化性能。對(duì)于貴金屬納米催化劑來(lái)說(shuō),它的催化性能與其尺寸、表面結(jié)構(gòu)以及組分密切相關(guān)。因此,為了得到性能更優(yōu)越的催化劑,我們常常通過(guò)調(diào)節(jié)這些參數(shù)來(lái)改善催化劑的性能。對(duì)于鈀基納米催化劑來(lái)說(shuō),大的比表面積、高指數(shù)晶面暴露以及組分之間的協(xié)同效應(yīng)均能有效提高催化劑的催化性能。然而在晶體的生長(zhǎng)過(guò)程中,金屬納米材料趨向形成最小表面積和低表面能晶面。因此,如何獲得理想結(jié)構(gòu)的催化劑也是相關(guān)研究的研究重點(diǎn)。本論文主要工作旨在合成一些鈀基納米材料,并運(yùn)用動(dòng)力學(xué)調(diào)控、晶種生長(zhǎng)法等多種調(diào)控方法,精心設(shè)計(jì)合成了一些納米結(jié)構(gòu),例如,結(jié)構(gòu)開(kāi)放度較高的框架結(jié)構(gòu)、具有協(xié)同效應(yīng)的異質(zhì)結(jié)構(gòu)。一方面,這些特殊結(jié)構(gòu)的合成拓寬了催化劑的設(shè)計(jì)思路,另一方面,它們也在燃料電池、二氧化碳電還原等領(lǐng)域表現(xiàn)出了優(yōu)越的性能。本論文共有四章,各章節(jié)內(nèi)容簡(jiǎn)述如下:在第一章中,我們簡(jiǎn)單介紹了貴金屬納米材料的基本結(jié)構(gòu)特征、性能影響因素、晶體生長(zhǎng)理論以及合成現(xiàn)狀。其中,我們通過(guò)實(shí)例說(shuō)明了幾個(gè)性能影響因素對(duì)貴金屬納米材料的催化性能的影響,以及如何根據(jù)這些影響因素設(shè)計(jì)一些對(duì)于催化反應(yīng)有特殊貢獻(xiàn)的金屬納米晶體,或者根據(jù)一些特殊結(jié)構(gòu)在催化領(lǐng)域的顯著性能來(lái)精心設(shè)計(jì)一些結(jié)構(gòu)。在第二章中,我們首先介紹了框架結(jié)構(gòu)在不同催化體系中的應(yīng)用及其合成方法。然后我們通過(guò)動(dòng)力學(xué)控制,在Pd八面體上選擇性沉積Pt原子并通過(guò)硝酸刻蝕的方法去除Pd晶核成功制備了結(jié)構(gòu)高度開(kāi)放的Pt-Pd雙金屬框架結(jié)構(gòu),詳細(xì)了分析了該框架結(jié)構(gòu)的構(gòu)造以及組成,并探索了該框架結(jié)構(gòu)在燃料電池陰極氧還原反應(yīng)中的電催化性能。在第三章中,我們首先介紹了 CO2電還原發(fā)展現(xiàn)狀及其催化劑發(fā)展現(xiàn)狀,然后我們通過(guò)模板誘導(dǎo)生長(zhǎng)法成功合成了 Pd方形納米片-rGO異質(zhì)結(jié)構(gòu),詳細(xì)分析了該異質(zhì)結(jié)構(gòu)中Pd方形納米片的晶體結(jié)構(gòu),并探究了該異質(zhì)結(jié)構(gòu)在二氧化碳電還原方面的應(yīng)用。在第四章中,我們展望了金屬納米材料應(yīng)用前景,并從催化劑的合成、性能測(cè)試以及催化劑與性能之間的關(guān)系等多個(gè)方面闡述了貴金屬納米催化劑研究中存在的一些機(jī)遇和挑戰(zhàn)。
[Abstract]:As a kind of important catalyst, noble metal nanomaterials have been widely used in many catalytic reactions. For example, they can be used in fuel cells. They can also be used in CO2 electroreduction and photolysis reactions. However, precious metals are scarce on Earth, so people are beginning to develop catalysts with different structures. This not only reduces the use of precious metals to a certain extent, but also tends to exhibit better catalytic performance because of the synergistic effect between components. The surface structure and composition are closely related. Therefore, in order to obtain better catalysts, we often improve the performance of the catalysts by adjusting these parameters. For palladium based nanocatalysts, the specific surface area is large. The high exponent crystal plane exposure and the synergistic effect among the components can effectively improve the catalytic performance of the catalyst. However, in the process of crystal growth, the metal nanomaterials tend to form the minimum surface area and the low surface energy crystal surface. The main purpose of this thesis is to synthesize some palladium based nanomaterials, and to use the kinetic control, seed growth method and other control methods. Some nanostructures have been carefully designed and synthesized, such as frame structures with high structural openness and heterogeneity with synergistic effects. On the one hand, the synthesis of these special structures broadens the design ideas of catalysts, on the other hand, They also show excellent performance in the fields of fuel cell, carbon dioxide electroreduction and so on. In this paper, there are four chapters, and the contents of each chapter are summarized as follows: in the first chapter, we briefly introduce the basic structural characteristics of noble metal nanomaterials. Among them, we illustrate the effect of several performance factors on the catalytic performance of noble metal nanomaterials through examples. And how to design some metal nanocrystals that have a special contribution to the catalytic reaction based on these factors, or elaborate some structures according to the remarkable performance of some special structures in the catalytic field. We first introduced the application of the frame structure in different catalytic systems and its synthesis methods. Selective deposition of Pt atoms on PD octahedron and removal of PD nucleus by nitric acid etching were used to fabricate the highly open Pt-Pd bimetallic frame structure. The structure and composition of the frame structure were analyzed in detail. The electrocatalytic properties of the frame structure in the cathodic oxygen reduction reaction of fuel cells were explored. In chapter 3, we first introduced the development of CO2 electroreduction and the current development of catalysts. Then we successfully synthesized the PD square nanochip -rGO heterostructure by template-induced growth method, and analyzed the crystal structure of the PD square nano-chip in detail. The application of the heterostructure in the electroreduction of carbon dioxide is also discussed. In Chapter 4th, we look forward to the application of metal nanomaterials and the synthesis of catalysts. Some opportunities and challenges in the research of noble metal nanocatalysts were discussed from the aspects of performance test and the relationship between catalyst and performance.
【學(xué)位授予單位】：中國(guó)科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O643.36

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本文編號(hào)：1500371