物理化学学报 >> 2024, Vol. 40 >> Issue (8): 2308015.doi: 10.3866/PKU.WHXB202308015

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CoP修饰Ti3C2Tx MXene纳米复合材料作为高效析氢反应电催化剂

孙巍1,†, 王永靖1,†, 项坤1,2,*(), 白赛帅1, 王海涛1, 邹菁1, Arramel3, 江吉周1,*()   

  1. 1 武汉工程大学, 环境生态与生物工程学院, 化学与环境工程学院, 绿色化工过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 光电化学材料与器件教育部重点实验室(江汉大学), 武汉 430205
    3 Nano Center Indonesia, Jalan Raya PUSPIPTEK, South Tangerang, Banten 15314, Indonesia
  • 收稿日期:2023-08-12 修回日期:2023-09-18 录用日期:2023-09-21 发布日期:2023-09-27
  • 通讯作者: Email: xiangkun@wit.edu.cn (项坤)027wit@163.com (江吉周)
  • 作者简介:

    †These authors contributed equally.

  • 基金资助:
    国家自然科学基金(62004143); 国家自然科学基金(22174033); 湖北省重点研发计划(2022BAA084); 光电化学材料与器件教育部重点实验室(江汉大学)开放基金(JDGD-202227); 武汉市知识创新专项项目-曙光计划(2022010801020355)

CoP Decorated on Ti3C2Tx MXene Nanocomposites as Robust Electrocatalyst for Hydrogen Evolution Reaction

Wei Sun1, Yongjing Wang1, Kun Xiang1,2,*(), Saishuai Bai1, Haitao Wang1, Jing Zou1, Arramel3, Jizhou Jiang1,*()   

  1. 1 School of Environmental Ecology and Biological Engineering, School of Chemistry and Environmental 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 Key Laboratory of Optoelectronic Chemical Materials and Devices of Ministry of Education, Jianghan University, Wuhan 430205, China
    3 Nano Center Indonesia, Jalan Raya PUSPIPTEK, South Tangerang, Banten 15314, Indonesia
  • Received:2023-08-12 Revised:2023-09-18 Accepted:2023-09-21 Published:2023-09-27
  • Contact: Email: xiangkun@wit.edu.cn (Kun Xiang)027wit@163.com (Jizhou Jiang)
  • Supported by:
    the National Natural Science Foundation of China(62004143); the National Natural Science Foundation of China(22174033); the Key R & D Program of Hubei Province(2022BAA084); the Opening Project of Key Laboratory of Optoelectronic Chemical Materials and Devices of Ministry of Education, Jianghan University(JDGD-202227); the Knowledge Innovation Program of Wuhan Shuguang Project(2022010801020355)

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摘要：

高效、经济和环保是电化学水分解制氢电催化剂的关键要素。二维(2D) MXene材料因其独特的物理化学性质而受到广泛关注。虽然有许多不同种类的MXene材料，但只有少数具有本征析氢反应(HER)催化活性。然而，MXene材料具有很多优点，如较大的比表面积、高电导率和丰富的表面官能团，因此可以作为与其他物质复合的理想平台。本研究首先通过密度泛函理论(DFT)预测了CoP与Ti3C2Tx MXene (其中Tx =―F和―OH官能团)具有低的氢吸附自由能(ΔGH*)。接着，我们合成了CoP-Ti3C2Tx MXene纳米复合材料，并在0.5 mol∙L−1 H2SO4中测试了其电催化HER性能。该材料在电流密度为10 mA∙cm−2时表现出了低的过电位(135 mV)和Tafel斜率为48 mV∙dec−1。理论计算表明，CoP-Ti3C2Tx MXene纳米复合材料的优异电催化性能源于Ti3C2Tx的高类金属导电性、良好的界面电荷转移、快速的氢吸附/解吸过程以及优化的电子结构。

关键词: Ti3C2Tx MXene, 析氢反应, CoP, 密度泛函理论, 界面电荷转移

Abstract:

Electrocatalysts play a pivotal role in the electrochemical water splitting process to produce hydrogen fuel. The advancement of this technology relies on the development of efficient, cost-effective, and readily available electrocatalysts. Two-dimensional (2D) MXene materials have garnered significant attention due to their unique physicochemical properties, rendering them promising candidates for electrocatalytic applications. While there are numerous types of MXene materials available, only a few possess intrinsic hydrogen evolution reaction (HER) catalytic activity. However, MXene materials can serve as excellent platforms for enhancing catalytic HER activity by combining them with other substances, owing to their large specific surface area, high conductivity, and abundant surface functional groups. In this study, we initially conducted a predictive analysis using density functional theory (DFT) to assess the potential of combining CoP with Ti3C2Tx MXene materials (where Tx represents ―F and ―OH functional groups) in reducing the adsorption free energy of hydrogen (ΔGH*). The results indicated that the CoP-Ti3C2Tx nanocomposites exhibited a ΔGH* value approaching 0, suggesting promising HER performance. Following this theoretical prediction, we synthesized the CoP-Ti3C2Tx MXene nanocomposites. Comprehensive characterization of the synthesized nanocomposites was performed using various techniques, including scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). These analyses confirmed the successful decoration of CoP on the MXene nanosheets and provided insights into the structural and compositional properties of the nanocomposites. Furthermore, we evaluated the electrochemical performance of the CoP-Ti3C2Tx nanocomposites through linear sweep voltammetry and chronoamperometry measurements. The results demonstrated superior catalytic activity and stability for the HER compared to pure Ti3C2Tx and CoP catalysts. Specifically, the as-synthesized CoP-Ti3C2Tx MXene nanocomposites exhibited remarkable electrocatalytic HER kinetics, featuring a low overpotential of 135 mV at a current density of 10 mA∙cm−2 and a small Tafel slope of 48 mV∙dec−1 in a 0.5 mol∙L−1 H2SO4 solution, with the electrocatalyst maintaining stability for up to 50 h. Subsequent theoretical calculations were conducted to elucidate the factors contributing to the exceptional electrocatalytic performance of the CoP-Ti3C2Tx MXene nanocomposites. It was determined that the metallic conductivity of Ti3C2Tx MXene materials, well-structured interface charge transfer, and optimized electronic structure of CoP played significant roles in enhancing catalytic activity. In conclusion, this study underscores the potential of CoP-decorated Ti3C2Tx MXene nanocomposites as promising electrocatalysts for efficient HER in various energy conversion and storage devices. These findings represent a significant contribution to the development of robust and efficient catalysts for hydrogen generation, a critical component of renewable energy applications and sustainable development.

Key words: Ti3C2Tx MXene, Hydrogen evolution reaction, CoP, Density functional theory, Interface charge transfer