Citation: Rongchen Shen, Lei Hao, Qing Chen, Qiaoqing Zheng, Peng Zhang, Xin Li. P-Doped g-C₃N₄ Nanosheets with Highly Dispersed Co_0.2Ni_1.6Fe_0.2P Cocatalyst for Efficient Photocatalytic Hydrogen Evolution[J]. Acta Physico-Chimica Sinica, ;2022, 38(7): 211001. doi: 10.3866/PKU.WHXB202110014 shu

P-Doped g-C₃N₄ Nanosheets with Highly Dispersed Co_0.2Ni_1.6Fe_0.2P Cocatalyst for Efficient Photocatalytic Hydrogen Evolution

Rongchen Shen ¹ ,
Lei Hao ¹ ,
Qing Chen ² ,
Qiaoqing Zheng ² ,
Peng Zhang ³ ,
Xin Li ^1,,

1.
Institute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization, Ministry of Agriculture and Rural Affairs, South China Agricultural University, Guangzhou 510642, China
2.
College of Materials and Energy, South China Agricultural University, Guangzhou 510642, China
3.
State Center for International Cooperation on Designer Low-Carbon & Environmental Materials (CDLCEM), School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China

Corresponding author: Xin Li, xinli@scau.edu.cn; xinliscau@126.com
Received Date: 12 October 2021
Revised Date: 3 November 2021
Accepted Date: 3 November 2021
Available Online: 8 November 2021
Fund Project: the National Natural Science Foundation of China 21975084the National Natural Science Foundation of China 51672089Special Funding on Applied Science and Technology in Guangdong, China 2017B020238005

Throughout the twentieth century, temperatures climbed rapidly as the use of fossil fuels proliferated and greenhouse gas levels soared. Thus, the need to develop environmentally friendly energy sources to replace traditional fossil fuels is urgent. Clean and highly efficient, hydrogen is considered the most promising energy source to replace traditional fossil fuels. The production of hydrogen by photocatalytic water splitting is environmentally friendly, and is considered the most promising method for producing hydrogen energy. Enhancing the separation efficiency of photogenerated electron-hole pairs has been identified as a key milestone for constructing high-efficiency photocatalysts. However, the construction of efficient and stable hydrogen-evolution photocatalysts with highly dispersed cocatalysts remains a challenge. Here, we succeeded, for the first time, in fabricating P-doped CNS (PCNS) with a highly dispersed non-noble trimetallic transition metal phosphide Co_0.2Ni_1.6Fe_0.2P cocatalyst (PCNS-CoNiFeP), by a one-step in situ high-temperature phosphating method. Remarkably, the CoNiFeP in PCNS-CoNiFeP demonstrated no aggregation and high dispersibility compared with CoNiFeP prepared by the traditional hydroxide-precursor phosphating method (PCNS-CoNiFeP-OH). X-ray diffraction, X-ray photoelectron spectroscopy, element mapping images, and high-resolution transmission electron microscopy results demonstrate that PCNS-CoNiFeP was successfully synthesized. The UV-Vis absorption results indicate a slight increase in absorbance for PCNS-CoNiFeP in the 200–800 nm wavelength region compared with that of PCNS. Photoluminescence spectroscopy, electrochemical impedance spectroscopy, and photocurrent results demonstrated that CoNiFeP cocatalysts could effectively promote the separation of photogenerated electron-hole pairs and accelerate the migration of carriers. The linear sweep voltammetry results also demonstrate that the CoNiFeP cocatalyst loading could significantly decrease the overpotential of CNS. Therefore, the maximum hydrogen evolution rate of PCNS-CoNiFeP was 1200 μmol·h^-1·g^-1, which was approximately four times higher than that of pure CNS-Pt (320 μmol·h^-1·g^-1) when using TEOA solution as a sacrificial agent. The apparent quantum efficiency of PCNS-CoNiFeP was 1.4% at 420 nm. The PCNS-CoNiFeP also exhibited good stability during the photocatalytic reaction. In addition, the TEM results indicate that CoNiFeP with a size of 6–8 nm are highly dispersed on the PCNS surface. The highly dispersed CoNiFeP demonstrated better charge-separation capacity and higher intrinsic electrocatalytic hydrogen-evolution activity than the aggregated CoNiFeP. Thus, the hydrogen evolution rate of aggregated CoNiFeP-PCNs (300 μmol·h^-1·g^-1) was much lower than that of PCNS-CoNiFeP. Furthermore, P doping of CNS could improve electric conductivity and charge transport. It is expected that loading highly dispersed CoNiFeP and P doping could be extended to promote photocatalytic hydrogen production using various photocatalysts.
- Trimetallic phosphide,
- Photocatalytic hydrogen evolution,
- Non-noble metal cocatalyst,
- P doping,
- Graphitic carbon nitride
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

P-Doped g-C3N4 Nanosheets with Highly Dispersed Co0.2Ni1.6Fe0.2P Cocatalyst for Efficient Photocatalytic Hydrogen Evolution

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通讯作者: 陈斌, bchen63@163.com

P-Doped g-C₃N₄ Nanosheets with Highly Dispersed Co_0.2Ni_1.6Fe_0.2P Cocatalyst for Efficient Photocatalytic Hydrogen Evolution