Preparation and field emission properties of LIG/CuO composites from laser irradiated copper-containing cork

MA Li'an; HUANG Xu; CHEN Song; WEI Zhaohui; SUN Lei; YE Xiaoyun

doi:10.7498/aps.74.20250378

Abstract

Three-dimensional (3D) graphene materials have excellent electronic emission performance and mechanical stability, showing significant advantages in the field of high current density field emitters. In this study, copper oxide modified three-dimensional graphene composites (LIG/CuO) are prepared in situ by a femtosecond laser one-step method, which realizes the simultaneous regulation of cork carbonization and copper oxidation. Shallow copper-rich precursors are constructed by copper salt infiltration and ascorbic acid reduction. Laser irradiation is used to synchronously induce the carbonization of cellulose into few-layer graphene and the transformation of Cu into CuO, forming a three-dimensional fiber network of microcrystalline graphene coated with CuO nanoparticles (30–80 nm). The structure exhibits excellent field emission performance: the threshold field of preparing pure laser- induced graphene (LIG) is ~2.12 V/μm and the field enhancement factor is ~8223. After optimizing CuO loading, the threshold field of LIG/CuO-5 is reduced to 1.57 V/μm, the field enhancement factor rises up to ~8823, and the ultra-high current density of 22.71 mA/cm² is achieved at 2.89 V/μm. The density functional theory (DFT) calculations show that the electrons at the heterojunction interface transfer from CuO to graphene, which reduces the work function of graphene from 4.833 eV to 4.677 eV, and the band bending of CuO surface synergistically reduces the tunneling barrier. In addition, the local electric field enhancement effect of CuO nanoparticles and the optimized distribution density synergistically increase the effective emission point density. The performance improvement is mainly attributed to three synergistic effects: 1) the three-dimensional porous graphene network provides abundant tip emission sites; 2) the introduction of CuO nanoparticles reduces the work function of the composite material from 4.833 eV to 4.667 eV, effectively reducing the electron escape barrier; 3) the heterojunction interface forms a directional electron migration channel under a positive bias electric field, combined with the excellent conductivity of LIG, which significantly improves the electron tunneling efficiency.

Keywords:

Authors and contacts

1.
School of Materials Science and Engineering, Fujian University of Technology, Fuzhou 350118, China
2.
Zhicheng College, Fuzhou University, Fuzhou 350002, China

Corresponding author: MA Li'an, mlajn@163.com

Funds: Project supported by the Natural Science Foundation of Fujian Province, China (Grant Nos. 2024J01835, 2024J01281) and the Top Young Talents of Eagle Program of Fujian Province, China (Grant No. KY310255).

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References

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Cited By

图 1 激光辐照制备LIG/CuO示意图

Figure 1. Flow diagram of LIG/CuO preparation by laser irradiation.

DownLoad: Full-Size Img PowerPoint

图 2 不同样品的场发射电子显微镜照片　(a1) LIG(截面图); (a2) LIG/CuO-5(截面图); (b1), (b2) LIG; (c1), (c2) LIG/CuAc-5; (d1), (d2) LIG/CuO-2.5; (e1), (e2) LIG/CuO-5; (f1), (f2) LIG/CuO-10; (g) LIG/CuO-5的元素分布图

Figure 2. Field emission electron microscopy images of different samples: (a1) LIG (cross section); (a2) LIG/CuO-5 (cross section); (b1), (b2) LIG; (c1), (c2) LIG/CuAc-5; (d1), (d2) LIG/CuO-2.5; (e1), (e2) LIG/CuO-5; (f1), (f2) LIG/CuO-10; (g) mapping images of LIG/CuO-5.

DownLoad: Full-Size Img PowerPoint

图 3 样品的TEM照片　(a) LIG; (b), (c) LIG/CuO-5

Figure 3. TEM images of samples: (a) LIG; (b), (c) LIG/CuO-5.

DownLoad: Full-Size Img PowerPoint

图 4 样品LIG和LIG/CuO-5的(a) Raman谱图和(b) FTIR谱图

Figure 4. Raman spectra (a) and FTIR spectra (b) of LIG and LIG/CuO-5.

DownLoad: Full-Size Img PowerPoint

图 5 (a) LIG/CuO-5的XPS图谱全谱; (b) C 1s, (c) O 1s, (d) Cu 2p的高分辨XPS光谱

Figure 5. (a) Survey XPS spectrum of the LIG/CuO-5; high-resolution XPS spectra of C 1s (b), O 1s (c) and Cu 2p (d).

DownLoad: Full-Size Img PowerPoint

图 6 (a) 构建的LIG, CuO和LIG/CuO 3D模型和计算得到的功函数; (b) LIG, CuO和 LIG/CuO 的分波态密度(PDOS)图(灰色虚线为费米能级)

Figure 6. (a) LIG, CuO and LIG/CuO 3D models and the calculated work functions; (b) the partial density of states (PDOS) of LIG, CuO and LIG/CuO (the gray dotted line is the Fermi level).

DownLoad: Full-Size Img PowerPoint

图 7 (a)样品LIG, LIG/CuAc-5, LIG/CuO-2.5, LIG/CuO-5和LIG/CuO-10的J-E曲线; (b) $\ln(J/E^2) \text{-}1/E $曲线; (c)样品相对应的开启阈值(E_th, 对应电流密度1 mA/cm²)和场增减因子(β)关系曲线; (d)样品LIG和LIG/CuO-5场发射稳定性曲线

Figure 7. (a) J-E plots of LIG, LIG/CuAc-5, LIG/CuO-2.5, LIG/CuO-5 and LIG/CuO-10; (b) $\ln(J/E^2) \text{-}1/E $ plots; (c) relationship plots of E_th (corresponding to a current density of 1 mA/cm²) and β versus the samples; (d) stability plots of LIG and LIG/CuO-5.

DownLoad: Full-Size Img PowerPoint

图 8 LIG/CuO能带结构　(a) 非接触; (b) 接触; (c) 电场作用

Figure 8. LIG/CuO band structure: (a) Non-contact; (b) contact; (c) electric field.

DownLoad: Full-Size Img PowerPoint

map

[1]	Zhang H, Tang J, Yuan J S, Yamauchi Y, Suzuki T T, Shinya N, Nakajima K, Qin L C 2016 Nat. Nanotechnol. 11 273 Google Scholar
[2]	Deka N, Subramanian V 2020 IEEE Trans. Electron Devices 67 3753 Google Scholar
[3]	Xing Y, Zhang Y, Xu N S, Huang H J, Ke Y L, Li B H, Chen J, She J C, Deng S Z 2018 IEEE Trans. Electron Devices 65 1146 Google Scholar
[4]	Cao G, Lee Y Z, Peng R, Liu Z, Rajaram R, Calderon-Colon X, An L, Wang P, Phan T, Sultana S, Lalush D S, Lu J P, Zhou O 2009 Phys. Med. Biol. 54 2323 Google Scholar
[5]	Heer W, Châtelain A, Ugarte D 1995 Science 270 1179 Google Scholar
[6]	郑钦仁, 詹涪至, 折俊艺, 王建宇, 石若立, 孟国栋 2024 73 086101 Google Scholar Zheng Q R, Zhan B Z, Zhe J Y, Wang J Y, Shi R L, Meng G D 2024 Acta Phys. Sin. 73 086101 Google Scholar
[7]	Bhopale S R, Jagtap K K, Phatangare A, Kamble S, Dhole S D, Mathe V L, More M A 2023 Appl. Surf. Sci. 619 156752 Google Scholar
[8]	Guo X, Li Y L, Ding Y Q, Chen Q, Li J S 2019 Mater. Des. 162 293 Google Scholar
[9]	Deng J H, Liu R N, Zhang Y, Zhu W X, Han A L, Cheng G A 2017 J. Alloys Compd. 723 75 Google Scholar
[10]	Huang Y X, Zhao H, Li Z L, Hu L L, Wu Y L, Sun F, Meng S, Zhao J M 2023 Adv. Mater. 35 2208362 Google Scholar
[11]	黄逸轩, 赵继民 2024 光散射学报 36 52 Google Scholar Huang Y X, Zhao J M 2024 J. Light Scat. 36 52 Google Scholar
[12]	Hasaien J, Wu Y L, Shi M Z, Zhai Y N, Wu Q, Liu Z, Zhou Y, Chen X. H, Zhao J M 2025 PNAS 122 e2406464122 Google Scholar
[13]	Jiang L T, Jiang C Y, Tian Y C, Zhao H, Zhang J, Tian Z Y, Fu S H, Liang E J, Wang X C, Jin C Q, Zhao J M 2024 Chin. Phys. Lett. 41 047802 Google Scholar
[14]	Wu L M, Dong Y Z, Zhao J L, Ma D T, Huang W C, Zhang Y, Wang Y Z, Jiang X T, Xiang Y J, Li J Q, Feng Y Q, Xu J L, Zhang H 2019 Adv. Mater. 31 1807981 Google Scholar
[15]	You Z H, Qiu Q M, Chen H Y, Feng Y Y, Wang X, Wang Y X, Ying Y B 2020 Biosens. Bioelectron. 150 111896 Google Scholar
[16]	Zhang J B, Ren M Q, Li Y L, Tour J M 2018 ACS Energy Lett. 3 677 Google Scholar
[17]	Yoon H, Nah J, Kim H, Ko S, Sharifuzzaman M, Barman S C, Xuan X, Kim J Y, Park J Y 2020 Sensor Actuat. B 311 127866 Google Scholar
[18]	Lin J, Peng Z W, Liu Y Y, Zepeda F R, Ye R Q, Samuel E L, Yacaman M J, Yakobson B I, Tour J M 2014 Nat. Commun. 5 5714 Google Scholar
[19]	Chyan Y, Ye R Q, Li Y L, Singh S P, Arnusch C J, Tour J M 2018 ACS Nano 12 2176 Google Scholar
[20]	Le T S D, Park S B, An J N, Lee P S, Kim Y J 2019 Adv. Funct. Mater. 29 1902771 Google Scholar
[21]	Wu W B, Liang R X, Lu L S, Wang W T, Ran X, Yue D D 2020 Surf. Coat. Technol. 393 125744 Google Scholar
[22]	Cheng J F, Lin Z X, Wu D, Liu C L, Cao Z 2022 J. Hazard. Mater. 436 129150.Google Scholar
[23]	Ryu C, Do H M, In J B 2024 Appl. Surf. Sci. 643 158696 Google Scholar
[24]	Rodrigues J, Zanoni J, Gaspar G, Fernandes A J S, Carvalho A F, Santos N F, Monteiro T, Costa F M 2019 Nanoscale Adv. 1 3252 Google Scholar
[25]	Lal A, Porat H, Hirsch L O, Cahan R, Borenstein A 2024 Appl. Surf. Sci. 643 158660 Google Scholar
[26]	Ma L A, Chen Y B, Ye X Y, Sun L, Wei Z H, Huang L, Chen H X, Wang Q T, Chen E G 2021 Ceram. Int. 47 27487 Google Scholar
[27]	Huang X, Chen S, Pan J, Wei Z H, Ye X Y, Wang Q T, Ma L A 2024 Ceram. Int. 50 24205 Google Scholar
[28]	Perdew J P, Burke K, Wang Y 1996 Phys. Rev. B Condens. Matter 54 16533 Google Scholar
[29]	Sun Z L, Shao Z G, Wang C L, Yang L 2016 Carbon 110 313 Google Scholar
[30]	Zhang H W, Sun Y S, Li Q W, Wan C X 2022 ACS Sustainable Chem. Eng. 10 11501 Google Scholar
[31]	Raveendran K, Ganesh A, Khilar K C 1996 Fuel 75 987 Google Scholar
[32]	Babinszki B, Sebestyén Z, Jakab E, Kőhalmi L, Bozi J, Várhegyi G, Wang L, Skreiberg Ø, Czégéy Z 2021 Bioresour. Technol. 338 125567 Google Scholar
[33]	Sugioka K, Cheng Y 2014 Light Sci. Appl. 3 e149 Google Scholar
[34]	Chen L F, Yu H, Zhong J S, Wu J, Su W T 2018 J. Alloys Compd. 749 60 Google Scholar
[35]	Keiluweit M, Nico P S, Johnson M G, Kleber M 2010 Environ. Sci. Technol. 44 1247 Google Scholar
[36]	Yu S J, Wang L Z, Li Q H, Zhang Y G, Zhou H 2022 Mater. Today Sustain. 19 100209 Google Scholar
[37]	Miao M, Zuo S L, Zhao Y Y, Wang Y F, Xia H A, Tan C, Gao H 2018 Carbon 140 504 Google Scholar
[38]	Wu J B, Lin M L, Cong X, Liu H N, Tan P H 2018 Chem. Soc. Rev. 47 1822 Google Scholar
[39]	Arulkumar E, Shree S S, Thanikaikarasan S 2024 J. Mater Sci. Mater. EL 35 198 Google Scholar
[40]	杨孟骐, 姬宇航, 梁琦, 王长昊, 张跃飞, 张铭, 王波, 王如志 2020 69 167805 Google Scholar Yang M Q, Ji Y H, Liang Q, Wang C H, Zhang Y F, Zhang M, Wang B, Wang R Z 2020 Acta Phys. Sin. 69 167805 Google Scholar
[41]	Zhang Y H, Ding H, Liu C X, Zhang J C, Wang C B, Guo W H, Ji Q Y, Zhao J Y, Zi Y Y 2024 Diamond Relat. Mater. 144 110972 Google Scholar
[42]	Chu Y L, Young S J, Cai D Y, Chu T T 2021 IEEE J. Electron. Devi. 9 1076 Google Scholar
[43]	Meng G D, Zhan F Z, She J Y, Xie J N, Zheng Q R, Cheng Y H, Yin Z Y 2023 Nanoscale 15 15994 Google Scholar
[44]	Fan L N, Chen W, Zhou K, Zheng H, Zheng P, Zheng L, Zhang Y 2023 ACS Appl. Electron. Mater. 5 123 Google Scholar

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