Study on Photoelectrochemical Properties of Colorful Carbon Nitrides Synthesized in Liquid-Phase

doi:10.6023/A20120575

Acta Chimica Sinica ›› 2021, Vol. 79 ›› Issue (4): 506-512.DOI: 10.6023/A20120575 Previous Articles Next Articles

Article

液相合成彩色氮化碳及其光电化学特性研究

何利蓉¹, 唐笑¹^,^*(), 张灵¹, 李艳虹¹, 相国涛¹, 周贤菊¹, 凌发令¹, 姚璐¹, 蒋浩¹

1 重庆邮电大学理学院重庆 400045

投稿日期:2020-12-19 发布日期:2021-03-12
通讯作者: 唐笑
基金资助:
重庆市留学人员创新支持计划重点项目(CX2017023); “成渝地区双城经济圈建设”科技创新项目(KJCX2020028); 国家自然科学基金青年基金(12004061); 重庆市教育委员会科学技术研究重点项目(KJZD-K201800602); 重庆自然科学基金面上项目(cstc2019jcyj-msxmX0525)

Study on Photoelectrochemical Properties of Colorful Carbon Nitrides Synthesized in Liquid-Phase

Lirong He¹, Xiao Tang¹^,^*(), Ling Zhang¹, Yanhong Li¹, Guotao Xiang¹, Xianju Zhou¹, Faling Ling¹, Lu Yao¹, Hao Jiang¹

1 School of Science, Chongqing University of Posts and Telecommunications, Chongqing 400045, China

Received:2020-12-19 Published:2021-03-12
Contact: Xiao Tang
About author:
* E-mail: tangxiao@cqupt.edu.cn
Supported by:
Venture & Innovation Support Program for Chongqing Oversea Returnee(CX2017023); Construction of Double City Economic Circle in Chengdu Chongqing Region Scientific and Technological Innovation Project(KJCX2020028); National Natural Science Foundation of China(12004061); Science and Technology Research Program of Chongqing Municipal Education(KJZD-K201800602); Chongqing Natural Science Foundation(cstc2019jcyj-msxmX0525)

Reducing the band gap value and obtaining an ordered two-dimensional microstructure are crucial to improving the photoelectrochemical performance of carbon nitrides. By adjusting the ratio of urea and citric acid and ripening the precursor at the room temperature, we synthesize the carbon nitride materials with different colors of orange, green and blue. The resultant blue sample has a narrowed band gap of 1.74 eV and the strong absorption to the light in 550~700 nm wavelength range. The photoelectrochemical solar cell is fabricated using the synthesized carbon nitrides as light absorber, TiO₂ as electron transporter and I₃^–/I^– as the redox shuttle in electrolyte. The orange carbon nitride has typical photoelectric conversion performance with J_sc=0.65 mA•cm^–2, V_oc=530 mV and ff=0.64. The blue carbon nitride has obvious enhanced J_sc of 1.03 mA•cm^–2 owing to the obvious enhanced visible light absorption, while the deeply decreased ff of 0.33. The cyclic voltammetry tests demonstrate the electrode reaction properties of the fabricated carbon nitride-based cell under illumination. It turns out that the cell based on the blue carbon nitride has obvious photo-induce pseudocapacitive behavior with an area specific capacitance of 4.9 mF•cm^–2. TEM (Transmission electron microscope), XRD (X-ray diffraction), FTIR (Fourier transform infrared spectroscopy) and XPS (X-ray photoelectron spectroscopy) reveal the microstructure characteristics of the colored carbon nitrides. The orange one is carbon nitride quantum dots with the particle size less than 10 nm. The blue one is a carbon nitride polymer containing graphite domains with oxidized boundaries, forming three-dimensional porous structure constructed by an ordered two-dimensional network. The green one has a mixture microstructure as well as the medium photoelectrochemical properties between the former two, which are both photoelectric conversion and photo-induced charge storage performance.

Key words: carbon nitrides, photoelectric conversion, charge storage, pseudo-capacitance, solar energy

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Lirong He, Xiao Tang, Ling Zhang, Yanhong Li, Guotao Xiang, Xianju Zhou, Faling Ling, Lu Yao, Hao Jiang. Study on Photoelectrochemical Properties of Colorful Carbon Nitrides Synthesized in Liquid-Phase[J]. Acta Chimica Sinica, 2021, 79(4): 506-512.

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Fig. & Tab. 8

Figure 1. (a) Pictures, (b) absorption spectra and (c) transmission spectra of different color samples. Tauc plots and optical band gap values of (d) orange, (e) green and (f) blue samples

Figure 2. TEM images of samples obtained when the mass ratio of citric acid to urea are (a) 1:10 (orange), (b) 1:1 (green) and (c) 1:0.5 (blue)

Figure 3. (a) XRD patterns and (b) FITR spectra of samples obtained when the mass ratio of citric acid to urea are 1:10 (orange), 1:1 (green), and 1:0.5 (blue)

Figure 4. XPS spectra of samples obtained when the mass ratios of citric acid to urea are 1:10 (orange sample), 1:1 (green sample), and 1:0.5 (blue sample): (a) survey spectra; (b) C1s; (c) N1s; (d) O1s

		Orange	Green	Blue
Atomic ratio (%)	C	54.18	55.97	57.35
	N	13.87	12.22	7.11
	O	30.36	29.34	32.7
N/C		0.26	0.22	0.12

Table 1. Atomic percentage of C, N and O of the sample

Figure 5. (a) PL spectra of carbon nitrides with different color (excitation wavelength is 468 nm); (b) J-V curve of the orange carbon nitride (the inset is corresponding photoelectrode); (c) J-V curve of the green carbon nitride (the inset is corresponding photoelectrode); (d) J-V curve of the blue carbon nitride (the inset is corresponding photoelectrode)

Figure 6. Electrochemical properties of the cells assembled with the colorful carbon nitrides are tested under light (100 mW•cm–2) and dark (voltage scanning speed is 50 mV•s–1, constant current density is 0.4 mA•cm–2): (a) CV curve of the cell assemble with the orange carbon nitride under light; (b) CV curve of the cell assemble with the green carbon nitride under light and dark; (c) CV curve of the cell assemble with the blue carbon nitride under light and dark; (d) GCD curve of the cell assemble with the orange carbon nitride under light; (e) GCD curve of the cell assemble with the green carbon nitride under light and dark; (f) GCD curve of the cell assemble with the blue carbon nitride under light and dark

Figure 7. (a) GCD of the cells assemble with the blue carbon nitride tested under illumination with different irradiance; (b) relationship between the corresponding area specific capacitance and irradiance

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液相合成彩色氮化碳及其光电化学特性研究

Study on Photoelectrochemical Properties of Colorful Carbon Nitrides Synthesized in Liquid-Phase

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