Villarreal Daniel, Sharma Jyoti, Arellano-Jimenez Maria Josefina, Auciello Orlando, de Obaldía Elida
Materials Science and Engineering, University of Texas at Dallas, Richardson, TX 75080, USA.
Materials Science and Engineering and Bioengineering, University of Texas at Dallas, Richardson, TX 75080, USA.
Materials (Basel). 2022 Aug 31;15(17):6003. doi: 10.3390/ma15176003.
This article shows the results of experiments to grow Nitrogen incorporated ultrananocrystalline diamond (N-UNCD) films on commercial natural graphite (NG)/Cu anodes by hot chemical vapor deposition (HFCVD) using a gas mixture of Ar/CH/N/H. The experiments focused on studying the effect of the pressure in the HFCVD chamber, filament-substrate distance, and temperature of the substrate. It was found that a substrate distance of 3.0 cm and a substrate temperature of 575 C were optimal to grow N-UNCD film on the graphite surface as determined by Raman spectroscopy, SEM, and TEM imaging. XPS analysis shows N incorporation through the film. Subsequently, the substrate surface temperature was increased using a heater, while keeping the substrate-filament distance constant at 3.0 cm. In this case, Raman spectra and SEM images of the substrate surface showed a major composition of graphite in the film as the substrate-surface temperature increased. Finally, the process pressure was increased to 10 Torr where it was seen that the growth of N-UNCD film occurred at 2.0 cm at a substrate temperature of 675 C. These results suggest that as the process pressure increases a smaller substrate-filament distance and consequently a higher substrate surface temperature can still enable the N-UNCD film growth by HFCVD. This effect is explained by a mean free path analysis of the main precursors H and CH molecules traveling from the filament to the surface of the substrate The potential impact of the process developed to grow electrically conductive N-UNCD films using the relatively low-cost HFCVD process is that this process can be used to grow N-UNCD films on commercial NG/Cu anodes for Li-ion batteries (LIBs), to enable longer stable capacity energy vs. charge/discharge cycles.
本文展示了通过热化学气相沉积(HFCVD),使用Ar/CH₄/N₂/H₂的混合气体,在商业天然石墨(NG)/铜阳极上生长掺氮超纳米晶金刚石(N-UNCD)薄膜的实验结果。实验着重研究了HFCVD腔室内的压力、灯丝与衬底的距离以及衬底温度的影响。通过拉曼光谱、扫描电子显微镜(SEM)和透射电子显微镜(TEM)成像确定,发现3.0厘米的衬底距离和575℃的衬底温度最适合在石墨表面生长N-UNCD薄膜。X射线光电子能谱(XPS)分析表明氮掺入了整个薄膜。随后,使用加热器提高衬底表面温度,同时将衬底与灯丝的距离保持在3.0厘米不变。在这种情况下,随着衬底表面温度升高,衬底表面的拉曼光谱和SEM图像显示薄膜中石墨占主要成分。最后,将工艺压力提高到10托,发现在675℃的衬底温度下,在2.0厘米处会生长N-UNCD薄膜。这些结果表明,随着工艺压力的增加,较小的衬底与灯丝距离以及相应较高的衬底表面温度仍能通过HFCVD实现N-UNCD薄膜的生长。从灯丝传播到衬底表面的主要前驱体H和CH分子的平均自由程分析解释了这种效应。使用相对低成本的HFCVD工艺来生长导电N-UNCD薄膜这一工艺的潜在影响在于,该工艺可用于在商业NG/铜阳极上生长N-UNCD薄膜,用于锂离子电池(LIB),以实现相对于充放电循环更长的稳定容量能量。