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小木蟲論壇-學術科研互動平臺» 學術交流區(qū)» 論文翻譯 » 論文翻譯求助完結子版 » 英譯漢
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Currently, graphene synthesis involves several key factors need to be improved: (i) lengthy high-temperature annealing processes to increase the grain size of the metal catalyst used to form graphene; (ii) utilization of purified and compressed gases to offer a homogenous and controlled delivery of carbon source materials; and (iii) the use of lengthy vacuum operation to avoid the presence of any detrimental reactive oxygen species from air2,4. To overcome these problems, we have designed a thermal CVD process to produce graphene in an ambient-air environment that is completely free of compressed or purified gases and requires minimum processing time. The process is schematically illustrated in Fig. 1a, in which the precursor for graphene growth and a metal catalyst (for example, Ni foil) are placed close together inside the heating zone of a furnace, before heating the quartz tube. The quartz tube is then sealed and the temperature is increased. During the ramping stage, air inside the quartz tube is released through a valve to maintain atmospheric pressure. Once the annealing stage is complete, the sample is removed from the heating zone for rapid cooling. Raman spectra of the samples grown at 800 °C in the ambient-air process indicated the presence of single-to-few layer graphene films covering the surface of the growth substrate (Fig. 1b). In the standard operation, the catalyst is low-cost polycrystalline Ni foil. Graphene growth occurs by thermal reforming of a natural precursor, soybean oil, in a closed ambient-air environment. Unlike conventional CVD methods or conventional natural precursor methods for growing graphene, the technique does not require any purified gases8,9. Moreover, expensive vacuum processing is avoided. The natural precursors substituted for purified gases are cheaper and safer. By restricting the air flow into the quartz tube, the transformation of solid-state carbon into carbon dioxide or other gaseous species is prevented. By controlling the temperature, cooling rate and precursor amount, the process enables the growth of homogenous graphene films of good quality. A comparison of the method with other CVD processes is provided in Supplementary Tables 1 and 2. The parameters observed to control the quality of graphene include temperature, processing time, precursor, substrate and the ambient-air environment. Nickel acted as a good catalyst for the breakdown of precursor material (in this case, the soybean-oil molecules) into smaller building units that are essential for the synthesis of graphene12. To investigate how the transformation occurred in the process, we have analysed the chemical composition of the annealed soybean oils at different temperatures (Supplementary Fig. 1). During the early stages of the annealing process, for instance at 300 °C, the long carbon chains in the soybean oil precursor were thermally dissociated into gaseous carbon building units such as methyl and ethyl species (Supplementary Fig. 1a). Other gaseous species were also generated, including hydrogen, water, hydroxyls and carbon dioxide, as confirmed by mass spectrometry (Supplementary Fig. 1b and c). Traces of heavier hydrocarbons such as propane were also observed. Most of the oil was vapourized by about 425 °C and a rapid mass reduction of the oil was observed by thermogravimetric analysis below 500 °C (Supplementary Fig. 1d). These building units present in the vapour can diffuse through the tube during the heating stage. As the temperature gradually increases to 800 °C, these carbon building units begin to dissociate into carbon atoms and dissolve into the Ni bulk. The sample was annealed for 3 min at 800 °C to promote dissolution of carbon atoms in the Ni substrate. Finally, following the rapid cooling stage, carbon segregates from the bulk and crystallizes on the Ni surface forming graphene12,13. At elevated temperatures, long hydrocarbons in the oil decompose in the presence of O2 to form water vapour. In particular, water vapour can promote the etching of amorphous carbon deposits on the Ni surface14. As such, we did not observe the formation of amorphous carbons in our sample. This also helps maintain the catalytic activity of the Ni surface in breaking down the precursor material15. Moreover, we have conducted a detailed analysis on the consumption of oxygen in the reactor during the growth process (Supplementary Note 1). We found that the precursor amount was critical for the consumption of reactive oxygen species. In the optimal growth condition, a slight carbon excessive environment is used to promote the growth of graphene and deter the formation of amorphous carbon. On the other hand, an over-excessive amount of precursor material led to an oversaturation of deposited carbon in the bulk of Ni, and subsequently, the crystallization of graphite on the Ni surface. This may explain the resulting formation of thick graphene sheets as observed in Supplementary Fig. 2a. Moreover, in the case of an insufficient amount of precursor, oxygen species can be present in the as-grown product in the form of C–O amorphous carbons (Supplementary Fig. 2b), consistent with the aforementioned calculations of oxygen consumption (Supplementary Note 1)16. These experiments indicate the critical role of the thermally dissociated precursor materials (that is, hydrocarbons) in consuming the reactive oxygen species present in the ambient-air environment, which has a profound effect in controlling the quality of the as-grown graphene films.We have also noticed that a slow cooling can promote excessive carbon segregation from the Ni bulk, which may account for the observed formation of a graphite-like film (Supplementary Fig. 2c). Another parameter that significantly influences the growth of graphene in the ambient air environment is the annealing temperature. At an annealing temperature of 500 °C, an incomplete formation of the graphene film was observed (Supplementary Fig. 2d). This may be attributed to an insufficient amount of energy to dissociate and reform the precursor material (that is, hydrocarbon species) required for graphene formation. Conversely, at a higher annealing temperature of 900 °C, thicker graphene sheets were observed (Supplementary Fig. 2e). This may arise from the increased rate of carbon diffusion, segregation and graphitization as a result of the elevated temperature. Importantly, these parameters allow us to obtain graphene films with tuneable average thickness and optical transmission, as characterized by Raman spectroscopy and optical transmission (Supplementary Fig. 3). It is worth mentioning that graphene did not form on other growth substrate materials with significantly lower carbon solubility than Ni, such as the commonly used Cu foil. Moreover, we did not observe graphene formation on graphitic surfaces such as woven carbon cloth (Supplementary Fig. 4). This suggests that the use of Ni (through, for example, carbon solubility, carbon segregation ability, catalytic effect, possibility of formation of oxide in air) and its interaction with the precursor material play a critical role in enabling the growth of graphene films. We also investigated the possibility of transforming other types of renewable oil groups. In particular, we were able to demonstrate the ambient-air growth of similar graphene films from other types of triglyceride (carbon)-containing precursors such as butter (Supplementary Fig. 5). As such, this method is versatile and may be tailored to transform other renewable carbon-containing natural precursors into graphene films. |
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2樓2017-02-06 21:25:26
【答案】應助回帖
★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ★ ...
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zsgandy(fjtony163代發(fā)): 金幣+50, 代發(fā) 2017-03-10 03:26:03
zsgandy(fjtony163代發(fā)): 金幣+50, 代發(fā) 2017-03-10 03:26:12
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zsgandy(fjtony163代發(fā)): 金幣+50, 代發(fā) 2017-03-10 03:28:43
fjtony163: 翻譯EPI+1, 代發(fā) 金幣由區(qū)長代發(fā) 2017-03-08 09:17:28
zsgandy(fjtony163代發(fā)): 金幣+50, 代發(fā) 2017-03-09 03:14:47
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zsgandy(fjtony163代發(fā)): 金幣+50, 代發(fā) 2017-03-10 03:26:12
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zsgandy(fjtony163代發(fā)): 金幣+50, 代發(fā) 2017-03-10 03:28:05
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|
Currently, graphene synthesis involves several key factors need to be improved: (i) lengthy high-temperature annealing processes to increase the grain size of the metal catalyst used to form graphene; (ii) utilization of purified and compressed gases to offer a homogenous and controlled delivery of carbon source materials; and (iii) the use of lengthy vacuum operation to avoid the presence of any detrimental reactive oxygen species from air2,4. To overcome these problems, we have designed a thermal CVD process to produce graphene in an ambient-air environment that is completely free of compressed or purified gases and requires minimum processing time. 目前，石墨烯合成涉及多個需要改進的關鍵因素：（i）冗長的高溫退火過程增加用來形成石墨烯的金屬催化劑的晶粒尺寸；（ii）利用純化和壓縮氣體來提供碳源材料的均勻和受控的遞送；以及（iii）使用冗長的真空操作來避免存在來自空氣的任何有害反應性氧物質(zhì)。為了克服這些不足，我們設計了熱CVD工藝來在完全不含壓縮或純化氣體且需要極少加工時間的周圍空氣環(huán)境中制備石墨烯。 The process is schematically illustrated in Fig. 1a, in which the precursor for graphene growth and a metal catalyst (for example, Ni foil) are placed close together inside the heating zone of a furnace, before heating the quartz tube. The quartz tube is then sealed and the temperature is increased. During the ramping stage, air inside the quartz tube is released through a valve to maintain atmospheric pressure. Once the annealing stage is complete, the sample is removed from the heating zone for rapid cooling. Raman spectra of the samples grown at 800 °C in the ambient-air process indicated the presence of single-to-few layer graphene films covering the surface of the growth substrate (Fig. 1b). 這種熱CVD工藝如圖1a示意性顯示，其中將用于石墨烯生長的前體和金屬催化劑（例如，Ni箔）一起靠近設置在爐子的熱區(qū)里面，然后加熱石英管。然后，密封石英管，增加溫度。在升溫階段，通過閥門來釋放石英管里面的空氣，以保持常壓。一旦退火階段完成，從熱區(qū)取出樣品用于快速冷卻。在周圍空氣工藝中在800℃下生長的樣品的拉曼光譜表明存在覆蓋生長襯底的單層石墨烯膜-到-幾層石墨烯膜（圖1b）。 |
3樓2017-02-10 21:24:11
【答案】應助回帖
|
In the standard operation, the catalyst is low-cost polycrystalline Ni foil. Graphene growth occurs by thermal reforming of a natural precursor, soybean oil, in a closed ambient-air environment. Unlike conventional CVD methods or conventional natural precursor methods for growing graphene, the technique does not require any purified gases8,9. Moreover, expensive vacuum processing is avoided. The natural precursors substituted for purified gases are cheaper and safer. By restricting the air flow into the quartz tube, the transformation of solid-state carbon into carbon dioxide or other gaseous species is prevented. By controlling the temperature, cooling rate and precursor amount, the process enables the growth of homogenous graphene films of good quality. A comparison of the method with other CVD processes is provided in Supplementary Tables 1 and 2. 在標準操作中，催化劑是低成本多晶Ni箔。通過在密封周圍空氣環(huán)境中天然前體大豆油的熱重整來開始石墨烯生長。與用于生長石墨烯的常規(guī)CVD方法或常規(guī)天然前體方法不同，這種技術部需要任何純化的氣體。此外，避免了昂貴的真空加工。取代純化氣體的天然前體更便宜且更安全。通過限制進入石英管的空氣流動，阻止固態(tài)碳轉變成二氧化碳或其它氣體物質(zhì)。通過控制溫度、冷卻速率和前體量，該熱CVD工藝實現(xiàn)生長具有良好質(zhì)量的均勻的石墨烯膜。在補充的表1和表2中，比較了該方法與其它CVD工藝。 The parameters observed to control the quality of graphene include temperature, processing time, precursor, substrate and the ambient-air environment. Nickel acted as a good catalyst for the breakdown of precursor material (in this case, the soybean-oil molecules) into smaller building units that are essential for the synthesis of graphene12. 觀察到控制石墨烯質(zhì)量的參數(shù)包括溫度、加工時間、前體、襯底和周圍空氣環(huán)境。鎳用作用于將前體材料（在這種情況下，大豆油分子）分解成對石墨烯的合成而言所必要的構成單元。 To investigate how the transformation occurred in the process, we have analysed the chemical composition of the annealed soybean oils at different temperatures (Supplementary Fig. 1). During the early stages of the annealing process, for instance at 300 °C, the long carbon chains in the soybean oil precursor were thermally dissociated into gaseous carbon building units such as methyl and ethyl species (Supplementary Fig. 1a). Other gaseous species were also generated, including hydrogen, water, hydroxyls and carbon dioxide, as confirmed by mass spectrometry (Supplementary Fig. 1b and c). Traces of heavier hydrocarbons such as propane were also observed. Most of the oil was vapourized by about 425 °C and a rapid mass reduction of the oil was observed by thermogravimetric analysis below 500 °C (Supplementary Fig. 1d). These building units present in the vapour can diffuse through the tube during the heating stage. As the temperature gradually increases to 800 °C, these carbon building units begin to dissociate into carbon atoms and dissolve into the Ni bulk. The sample was annealed for 3 min at 800 °C to promote dissolution of carbon atoms in the Ni substrate. Finally, following the rapid cooling stage, carbon segregates from the bulk and crystallizes on the Ni surface forming graphene12,13. 為了研究在這個工藝中轉變是如何進行的，我們分析了在不同溫度下的退火的大豆油的化學組成（補充圖1）。在退火過程的早期階段，例如在300℃下，大豆油前體的長碳鏈熱解離成氣態(tài)碳構成單元例如甲基和乙基物質(zhì)（補充圖1a）。還產(chǎn)生其他氣態(tài)物質(zhì)，包括氫氣、水、羥基和二氧化碳，如通過質(zhì)譜所確認（補充圖1b和1c）。還觀察到痕量的更重的烴，例如丙烷。大多數(shù)的油到約425℃時蒸發(fā)，通過熱重分析在500℃以下觀察到油的快速的質(zhì)量下降（補充圖1d）。在加熱階段過程中，在蒸氣中存在的構成單元可擴散通過管。隨著溫度逐漸增加到800℃，這些碳構成單元開始解離成碳原子，并溶解進入Ni本體。將樣品在800℃下退火3分鐘，以促進碳原子在Ni襯底中的溶解。最后，在快速冷卻階段之后，碳從本體分離，且在Ni表面上結晶，這形成石墨烯。 |
4樓2017-02-10 21:48:37
【答案】應助回帖
|
At elevated temperatures, long hydrocarbons in the oil decompose in the presence of O2 to form water vapour. In particular, water vapour can promote the etching of amorphous carbon deposits on the Ni surface14. As such, we did not observe the formation of amorphous carbons in our sample. This also helps maintain the catalytic activity of the Ni surface in breaking down the precursor material15. Moreover, we have conducted a detailed analysis on the consumption of oxygen in the reactor during the growth process (Supplementary Note 1). We found that the precursor amount was critical for the consumption of reactive oxygen species. In the optimal growth condition, a slight carbon excessive environment is used to promote the growth of graphene and deter the formation of amorphous carbon. On the other hand, an over-excessive amount of precursor material led to an oversaturation of deposited carbon in the bulk of Ni, and subsequently, the crystallization of graphite on the Ni surface. This may explain the resulting formation of thick graphene sheets as observed in Supplementary Fig. 2a. 在升高的溫度下，油中的長烴在O2的存在下分解，以形成水蒸汽。具體地，水蒸汽可促進沉積在Ni表面上的無定形碳的蝕刻。這樣，在我們的樣品中，我們沒有觀察到形成無定形碳。這也有助于保持Ni表面在分解前體材料時的催化活性。此外，我們還對生長過程指南反應器中氧氣的消耗進行了詳細的分析（補充注釋1）。我們發(fā)現(xiàn)前體量對于反應性氧物質(zhì)的消耗是關鍵的。在優(yōu)化的生長條件下，使用稍微碳過量的環(huán)境來促進石墨烯的生長，且阻止形成無定形碳。另一方面，過度過量的前體材料導致Ni本體中沉積的碳的過飽和，且隨后導致在Ni表面上石墨的結晶。這可解釋導致形成如補充圖2a中所觀察到的較厚的石墨烯片。 明天繼續(xù)吧！ |
5樓2017-02-10 22:01:46
【答案】應助回帖
★ ★ ★ ★ ★
愛與雨下: 金幣+5 2017-02-14 07:28:19
愛與雨下: 金幣+5 2017-02-14 07:28:19
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Moreover, in the case of an insufficient amount of precursor, oxygen species can be present in the as-grown product in the form of C–O amorphous carbons (Supplementary Fig. 2b), consistent with the aforementioned calculations of oxygen consumption (Supplementary Note 1)16. These experiments indicate the critical role of the thermally dissociated precursor materials (that is, hydrocarbons) in consuming the reactive oxygen species present in the ambient-air environment, which has a profound effect in controlling the quality of the as-grown graphene films.We have also noticed that a slow cooling can promote excessive carbon segregation from the Ni bulk, which may account for the observed formation of a graphite-like film (Supplementary Fig. 2c). 此外，在不充分的前體的量的情況下，氧物質(zhì)可以C-O無定形碳的形式存在于剛生長的產(chǎn)物中（補充圖2b），這與上文提及的氧消耗的計算一致（補充注釋）。這些實驗表明了在消耗周圍空氣環(huán)境中存在的反應性氧物質(zhì)時熱解離前體材料（即，烴）的關鍵作用，這對控制剛生長的石墨烯膜的質(zhì)量具有深遠的影響。我們還注意到緩慢的冷卻可促進來自Ni本體的過量的碳分離，這可解釋觀察到的石墨狀膜的形成（補充圖2c）。 Another parameter that significantly influences the growth of graphene in the ambient air environment is the annealing temperature. At an annealing temperature of 500 °C, an incomplete formation of the graphene film was observed (Supplementary Fig. 2d). This may be attributed to an insufficient amount of energy to dissociate and reform the precursor material (that is, hydrocarbon species) required for graphene formation. Conversely, at a higher annealing temperature of 900 °C, thicker graphene sheets were observed (Supplementary Fig. 2e). This may arise from the increased rate of carbon diffusion, segregation and graphitization as a result of the elevated temperature. Importantly, these parameters allow us to obtain graphene films with tuneable average thickness and optical transmission, as characterized by Raman spectroscopy and optical transmission (Supplementary Fig. 3). 顯著影響周圍空氣環(huán)境中石墨烯生長的另一參數(shù)是退火溫度。在500℃的退火溫度下，觀察到不完全的石墨烯膜形成（補充圖2d）。這可歸因于用于石墨烯形成所需的不足的解離和重整前體材料（即，烴物質(zhì)）的能量。相反，在900℃的更高退火溫度下，觀察到更厚的石墨烯片（補充圖2e）。這可起因于因升高溫度導致的碳擴散、分離和石墨化的增加的速率。重要地是，這些參數(shù)允許我們獲得具有可調(diào)節(jié)的平均厚度和光學透射率的石墨烯膜，如通過拉曼光譜和光學透射率所表征（補充圖3）。 It is worth mentioning that graphene did not form on other growth substrate materials with significantly lower carbon solubility than Ni, such as the commonly used Cu foil. Moreover, we did not observe graphene formation on graphitic surfaces such as woven carbon cloth (Supplementary Fig. 4). This suggests that the use of Ni (through, for example, carbon solubility, carbon segregation ability, catalytic effect, possibility of formation of oxide in air) and its interaction with the precursor material play a critical role in enabling the growth of graphene films. We also investigated the possibility of transforming other types of renewable oil groups. In particular, we were able to demonstrate the ambient-air growth of similar graphene films from other types of triglyceride (carbon)-containing precursors such as butter (Supplementary Fig. 5). As such, this method is versatile and may be tailored to transform other renewable carbon-containing natural precursors into graphene films. 值得一提的是，在具有比Ni顯著更低的碳溶解度的其它生長襯底材料例如常用的Cu箔上，不形成石墨烯。此外，我們在石墨化表面上例如紡織碳布上沒有觀察到石墨烯形成（補充圖4）。這表明使用Ni（通過，例如碳溶解度，碳分離能力，催化效果，空氣中形成氧化物的可能性）及其與前體材料的相互作用在實現(xiàn)石墨烯膜生長時起著關鍵作用。我們還研究了轉換其它類型的可再生油基團的可能性。具體地，我們能證明從其它類型的含有甘油三酸酯（碳）的前體例如黃油的相似石墨烯膜的周圍空氣生長（補充圖5）。這樣，這種方法是通用的，且可調(diào)節(jié)來將其它可再生的含碳天然前體轉換成石墨烯膜。 |
6樓2017-02-10 23:05:24
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