Citation: Yang Li, Dainan Zhang, Xionghan Feng, Quanjun Xiang. Enhanced photocatalytic hydrogen production activity of highly crystalline carbon nitride synthesized by hydrochloric acid treatment[J]. Chinese Journal of Catalysis, ;2020, 41(1): 21-30. doi: S1872-2067(19)63427-3 shu

Enhanced photocatalytic hydrogen production activity of highly crystalline carbon nitride synthesized by hydrochloric acid treatment

a State Key Laboratory of Electronic Thin Film and Integrated Devices, School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China;
b College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, Sichuan, China

Received Date: 30 April 2019
Revised Date: 27 May 2019

Fund Project: This work was supported by the National Natural Science Foundation of China (51672099, 21403079), Sichuan Science and Technology Program (2019JDRC0027), and Fundamental Research Funds for the Central Universities (2017-QR-25).

Crystalline carbon nitride (CCN) prepared by a molten-salt method is attracting increased attention because of its promising properties and excellent photocatalytic activity. In this work, we further improve the crystallinity of CCN through synthesis by the molten-salt method under the action of aqueous hydrochloric acid (HCl) solution. Our results showed that the crystallinity of the as-prepared samples increased with increasing HCl concentration and reached the maximum value at 0.1 mol L^-1. This can be attributed to the removal of some potassium ions (K⁺) from the terminal amino groups of CCN by the aqueous HCl solution, which results in a release of the polymerization sites. As a result, the crystallinity of the as-prepared samples further increased. Moreover, the obtained 0.1 highly crystalline carbon nitride (0.1HCCN; treated with 0.1 mol L^-1 aqueous HCl solution) exhibited an excellent photocatalytic hydrogen evolution of 683.54 µmol h^-1 g^-1 and a quantum efficiency of 6.6% at 420 nm with triethanolamine as the sacrificial agent. This photocatalytic hydrogen evolution was 2 and 10 times higher than those of CCN and bulk carbon nitride, respectively. The enhanced photocatalytic activity was attributed to the improved crystallinity and intercalation of K⁺ into the xHCCN interlayer. The improved crystallinity can decrease the number of surface defects and hydrogen bonds in the as-prepared sample, thereby increasing the mobility of the photoinduced carriers and reducing the recombination sites of the electron-hole pairs. The K⁺ intercalated into the xHCCN interlayer also promoted the transfer of the photoinduced electrons because these ions can increase the electronic delocalization and extend the π-conjugated systems. This study may provide new insights into the further development of the molten-salt method.
- Crystalline carbon nitride,
- Molten-salt method,
- Photocatalytic hydrogen evolution,
- Potassium ions,
- Aqueous hydrochloric acid solution
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