硫取代氮增强g-C<sub>3</sub>N<sub>4</sub>光催化产氢性能

引用本文: 王海涛, 余良浪, 江吉周, Arramel, 邹菁. 硫取代氮增强g-C₃N₄光催化产氢性能[J]. 物理化学学报, 2024, 40(5): 230504. doi: 10.3866/PKU.WHXB202305047 shu

Citation: Haitao Wang, Lianglang Yu, Jizhou Jiang, Arramel, Jing Zou. S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity[J]. Acta Physico-Chimica Sinica, 2024, 40(5): 230504. doi: 10.3866/PKU.WHXB202305047 shu

硫取代氮增强g-C₃N₄光催化产氢性能

王海涛 ^{1, †,} ,
余良浪 ^{1, †,} ,
江吉周 ^{1,
,} ,
Arramel ^2, ,
邹菁 ^1,

1.
武汉工程大学, 化学与环境工程学院, 环境生态与生物工程学院, 绿色化工程教育部重点实验室, 磷资源开发利用教育部工程研究中心, 新型催化材料湖北省工程研究中心, 武汉 430205
2.
Nano Center Indonesia, Jalan Raya PUSPIPTEK, South Tangerang, Banten 15314, Indonesia

通讯作者: 江吉周, 027wit@163.com

基金项目:
国家自然科学基金 62004143

湖北省重点研发计划 2022BAA084

湖北省自然科学基金 2021CFB133

国家重点研发计划 2022YFC3902703

磷资源开发利用教育部工程研究中心创新项目 LCX2021003

能量转换与存储材料化学教育部重点实验室开放基金 2021JYBKF05

摘要: 利用取之不尽的太阳能资源进行光催化水裂解制氢是缓解全球能源危机、实现碳中和战略的一项有前景的技术。石墨相氮化碳(g-C₃N₄)因成本低且稳定性高在光催化产氢领域备受关注。然而，纯g-C₃N₄存在表面积小、电子转移慢、光生载流子复合快等缺陷，产氢性能通常不佳。本研究通过直接热解硫酸铵和三聚氰胺混合物，成功实现硫物种对g-C₃N₄氮位点的原位取代，开发出一种高效的硫掺杂g-C₃N₄ (S-g-CN)光催化剂。系列结构和光谱表征证实硫的成功掺杂。密度泛函理论的第一性原理计算表明S活性位对氢的吸附吉布斯自由能近乎为零(~0.26 eV)，揭示S掺杂在优化H活性中间体吸附和解吸过程中起着重要作用。透射电子显微镜和原子力显微镜测试结果表明，S-g-CN具有超薄的纳米片状结构，其片层厚度约为2.5 nm。随后的氮气吸脱附等温线和光电化学性质测试结果表明，S掺杂不仅可显著增大g-C₃N₄比表面积，而且还能有效提高其光生电子-空穴对的转移、分离和氧化还原能力。得益于材料良好的结构特性，S-g-CN的光催化产氢速率高达4923 μmol∙g⁻¹∙h⁻¹，是原始g-C₃N₄的28倍，超越诸多最近报道的其它S掺杂g-C₃N₄光催化剂。而且，S-g-CN的表观量子效率高达3.64%。本研究除了开发一种高效的光催化剂，还将为高性能g-C₃N₄基催化剂的设计提供有益借鉴。

关键词:

理论预测
/ 硫掺杂
/ g-C₃N₄
/ 产氢
/ 光催化

English

S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity

1.
School of Chemistry and Environmental Engineering, School of Environmental Ecology and Biological Engineering, Key Laboratory of Green Chemical Engineering Process of Ministry of Education, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Novel Catalytic Materials of Hubei Engineering Research Center, Wuhan Institute of Technology, Wuhan 430205, China
2.
Nano Center Indonesia, Jalan Raya PUSPIPTEK, South Tangerang, Banten 15314, Indonesia

Corresponding author: Jizhou Jiang, Email: 027wit@163.com

Received Date: 26 May 2023
Accepted Date: 21 June 2023
Revised Date: 21 June 2023
Available Online: 15 May 2024
Fund Project:
the National Natural Science Foundation of China

the Key R&D Program of Hubei Province, China

the Natural Science Foundation of Hubei Province, China

the National Key R&D Program of China

the Innovation Project of Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, China

the Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage (HUST), Ministry of Education, China
^† These authors contributed equally to this work.

Abstract: The use of solar energy as an inexhaustible resource to conduct photocatalytic water splitting in hydrogen (H₂) production can alleviate the worldwide energy crisis and achieve carbon neutrality. However, research in photocatalytic H₂ evolution reaction (HER) is extremely challenging in terms of exploring the current development of an active and durable graphitic carbon nitride (g-C₃N₄)-based photocatalyst. Several parameters of pristine g-C₃N₄ require structural, physical, and chemical improvements, such as optimization of the surface area, electron transfer, and photo-generated carrier recombination, to render the g-C₃N₄ suitable for photocatalysis. In this study, the development of an efficient and robust S-doped g-C₃N₄ (S-g-CN) catalyst was pursued that involves doping nitrogen (N) active sites of g-C₃N₄ with sulfur (S) dopants via one-step calcination of the sulphate and melamine precursors. A combination of structural and spectroscopic fingerprints was established to distinctly determine the realization of S-doping onto the g-C₃N₄ structure. We obtained the optimum Gibbs free energy of adsorbed hydrogen (ΔG_H*) for S-g-CN at the S active sites, which is nearly zero (~0.26 eV), suggesting that the filled S dopants play an essential role in optimizing the adsorption and desorption processes of H-active intermediates. The results of atomic force and transmission electron microscopies (AFM and TEM) demonstrated that the produced S-g-CN catalyst has an ultrathin nanosheet structure with a lamellar thickness of approximately 2.5 nm. A subsequent N₂ sorption isotherms test revealed a substantial increase in the specific surface area after the integration of S dopants into the g-C₃N₄ nanoskeleton. Moreover, the incorporation of S atoms into the g-C₃N₄ significantly increased the carrier concentrations, improving the transfer, separation, as well as the oxidation and reduction abilities of the photo-generated electron-hole pairs. Leveraging the favorable material characteristics of the S-doped two-dimensional nanostructures, the resulting S-g-CN achieved a high H₂ evolution rate of 4923 μmol·g⁻¹·h⁻¹, which is 28 times higher than that of the pristine g-C₃N₄. Additionally, the developed S-g-CN possessed a high apparent quantum efficiency (3.64%) at visible-light irradiation. When compared to the recently reported S-doped g-C₃N₄-based photocatalysts, our optimal S-g-CN catalyst (S-CN_1.0) showed one of the best HER catalytic activities. Our rational design is based on an effective strategy that not only explored a promising HER photocatalyst but also aimed to pave the way for the development of other high-performance g-C₃N₄ based catalysts.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

硫取代氮增强g-C₃N₄光催化产氢性能

通讯作者: 江吉周, 027wit@163.com

English

S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity

Corresponding author: Jizhou Jiang, Email: 027wit@163.com

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通讯作者: 江吉周, 027wit@163.com

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Corresponding author: Jizhou Jiang, Email: 027wit@163.com

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硫取代氮增强g-C₃N₄光催化产氢性能

S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs