光沉积Pt复合石墨相氮化碳实现高效光催化产氢

牛凤延; 何齐升; 武世然; 郭晨曦; 雷伟岩; 沈毅

doi:10.13801/j.cnki.fhclxb.20230614.001

光沉积Pt复合石墨相氮化碳实现高效光催化产氢

doi: 10.13801/j.cnki.fhclxb.20230614.001

1.
华北理工大学　材料科学与工程学院，唐山 063210
2.
华北理工大学　矿业与工程学院，唐山 063210

基金项目: 国家自然科学基金 (51772099；51572069)

详细信息

通讯作者:
沈毅，博士，教授，博士生导师，研究方向为光催化材料　E-mail: shenyinfy@163.com

中图分类号: TB333
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出版历程
- 收稿日期: 2023-04-11
- 修回日期: 2023-05-18
- 录用日期: 2023-05-26
- 网络出版日期: 2023-06-14
- 刊出日期: 2024-01-01

Photodeposition Pt composite graphitic carbon nitride realizes efficient photocatalytic hydrogen production

1.
College of Materials Science and Engineering, North China University of Science and Technology, Tangshan 063210, China
2.
College of Mining Engineering, North China University of Science and Technology, Tangshan 063210, China

Funds: National Natural Science Foundation of China (51772099; 51572069)

摘要

摘要: 贵金属作为助催化剂，可以提高石墨相氮化碳(g-C₃N₄)光催化产氢的性能，引起了人们的广泛关注。但是，由于贵金属的不可再生性和高价格，“更少的贵金属，更好的性能”始终是目标。为了实现这一目标，通过光沉积还原法成功制备了一系列不同铂负载量氮化碳复合材料(Pt/CN)，并用于光催化产H₂。结果表明：不同Pt负载量的Pt/CN复合材料都表现出优异的光催化产氢性能。并发现当Pt的负载量为0.5wt%时， Pt/CN复合材料具有最优异的光催化产氢活性，产氢量为409.2 μmol/g，是纯CN (17.8 μmol/g)的23倍，同时证实了Pt和CN二者之间形成了肖特基势垒，使导带的电子快速迁移到Pt上，降低了CN的电子-空穴复合速率。并且Pt作为光催化分解水的活性位点，促进水中的绝大部分氢质子快速吸附到Pt位点，得到电子被还原为H₂，实现了高效光催化产氢。
- 石墨相氮化碳 /
- 光催化产氢 /
- 铂 /
- 光沉积 /
- 复合比
Abstract: Noble-metal, as co-catalysts, can improve the photocatalytic hydrogen production performance of graphitic carbon nitride (g-C₃N₄). It has been paid extensive attention, however, due to the non-renewability and high expense of noble-metal, "less noble-metal, better performance" is always the goal. To achieve this goal, composite CN with different Pt loadings (Pt/CN) was successfully prepared by photoreduction deposition and used for photocatalytic hydrogen production. The results show that Pt/CN with different Pt loadings can improved photocatalytic hydrogen production performance than CN. It is found that Pt/CN loaded with 0.5wt%Pt have the best photocatalytic hydrogen production activity, with a hydrogen production rate of 409.2 μmol/g, which is 23 times higher than that of CN (17.8 μmol/g). At the same time, it is confirmed that a Schottky barrier is formed between Pt and CN, which makes the electrons of the conduction band migrate rapidly to Pt, which reduces the electron-hole recombination rate of CN. Moreover, Pt is used as the active site of photocatalytic water splitting, which promotes the rapid adsorption of most of the hydrogen protons in the water to the Pt site, and the electrons are reduced to hydrogen, realizing efficient photocatalytic hydrogen production.
- graphitic carbon nitride /
- photocatalytic hydrogen production /
- Pt /
- photodeposition /
- compound rad

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图 1 石墨相氮化碳(CN) (a) 和Pt/CN (b) 的制备

Figure 1. Synthesis of graphitic carbon nitride (CN) (a) and Pt/CN (b)

g-C₃N₄—Graphitic carbon nitride (CN)

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图 2 不同Pt负载量下Pt/CN的XRD图谱(a)和FTIR图谱(b)

Figure 2. XRD patterns (a) and FTIR spectra (b) of Pt/CN under different Pt doping amounts

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图 3 0.5wt%Pt/CN 样品的TEM图像((a), (b))、EDS能谱(插表为ZAF法无标定量分析) (c)、Mapping ((d)~(g))

Figure 3. TEM images ((a), (b)), EDS energy spectrum (Insert table is Zahl absorption fluorescence method (ZAF) standardless quantitative analysis) (c), mapping ((d)-(g)) of 0.5wt%Pt/CN sample

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图 4 CN (a)和0.5wt%Pt/CN复合材料(b)的氮气吸附-脱附曲线及孔径分布图(c)

Figure 4. Nitrogen adsorption-desorption curve of CN (a) and 0.5wt%Pt/CN composites (b) and pore size distribution (c)

STP—Standard temperature and pressure

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图 5 不同Pt负载量下Pt/CN的UV-vis DRS (a)、Tauc-plot图(b)、PL光谱(c)、EIS (d)、瞬时光响应电流图(e)

Figure 5. UV-vis DRS (a), Tauc-plot (b), PL spectra (c), EIS (d), transient photocurrent density (e) of Pt/CN under different Pt doping amounts

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图 6 (a)不同Pt负载量下Pt/CN的光解水产H₂曲线；(b) 0.5wt%Pt/CN的循环光催化测试；反应前后0.5wt%Pt/CN的XRD图谱(c)和FTIR图谱(d)

Figure 6. (a) Photolyzed aquatic H₂ curves of Pt/CN under different Pt doping amounts; (b) Cycling photocatalytic test of 0.5wt%Pt/CN; XRD patterns (c) and FTIR spectra (d) of 0.5wt%Pt/CN before and after reaction

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图 7 Pt/CN 复合光催化产氢过程

Figure 7. Pt/CN composite photocatalytic hydrogen production process

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