氧化石墨烯生长钨基氧化物酸环境电催化析氢
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国际交流合作项目(BX 2019018);2018年度江苏省研究生培养创新工程项目(KYCX18_1810)


Electrocatalysis of hydrogen evolution reaction for tungsten-based oxides grown on graphene oxide in acidic environment
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International exchange and cooperation projects (BX 2019018); Postgraduate Research & Practice Innovation Program of Jiangsu Provence (KYCX18_1810)

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    摘要:

    为了解决商用铂碳电极在电催化析氢反应(HER)领域生产成本高、催化剂使用周期短等问题,利用磷钨酸提供钨源,以单层氧化石墨烯(GO)作为载体,引入利于电子传输轨道的碳纳米管(CNTs),通过一步水热法和空气中煅烧制备得到WO3-rGO-CNTs纳米异质结电催化剂。利用FT-IR、XRD、XPS、TG、SEM、EDAX、TEM和BET对WO3-rGO-CNTs的化学结构和物理形貌进行了表征。结果表明,在单层GO表面均匀生长WO3晶体,并引入CNTs后,纳米异质结WO3-rGO-CNTs在酸性电解质中表现出优异的HER催化活性。利用线性伏安法(LSV)和循环伏安法(CV)对WO3-rGO-CNTs进行HER测试,当电流密度为10 mA/cm2时,其过电势为218 mV;塔菲尔斜率为130.5 mV/dec。当过电势为-0.5 V vs. RHE时,其阻抗值为8.2 Ω。同时,WO3-rGO-CNTs纳米异质结可以在218 mV(电流密度为10 mA/cm2)过电势下,保持50 h的稳定性和耐久性;其双层电容值为1.2 mF/cm2。电化学数据表明,WO3与GO和CNTs间由于异质结构的存在,产生了协同效应:GO为WO3晶体提供了广阔的金属反应活性位点,而CNTs则提供了利于电子传输的活性轨道。

    Abstract:

    In order to solve the problems of high production cost and short catalytic cycling life of commercial Pt/C electrodes in the field of hydrogen evolution reaction (HER), phosphotungstic acid was used to provide tungsten source, while the single-layer graphene oxide (GO) was used as a carrier and carbon nanotubes (CNTs) with favorable electron transport orbits was adulterated. WO3 crystals was prepared by one-step hydrothermal method and calcination in air. After that, WO3-rGO-CNTs nanoheterostructure was successfully synthesized. The chemical structure and physical morphology of WO3-rGO-CNTs were characterized by FT-IR, XRD, XPS, TG, SEM, EDAX, TEM and BET. The results show that WO3 crystals is uniformly grown on the surface of the single layer of GO with CNTs, the WO3-rGO-CNTs exhibits excellent HER electrocatalytic activities in an acidic electrolyte. Linear Sweep Voltammetry (LSV) and Cyclic Voltammetry (CV) measurements were performed for HER testing with WO3-rGO-CNTs nanoheterostructure. When the current density is 10 mA/cm2, the overpotential is 218 mV and the Tafel slope is 130.5 mV /dec. When the overpotential is -0.5 V vs. RHE, the impedance value is 8.2 Ω. At the same time, WO3-rGO-CNTs nanoheterostructure can maintain long-term stability and durability for up to 50 h under the overpotential of 218 mV (current density is 10 mA/cm2), while its double-layer capacitance value is 1.2 mF/cm2. All of the electrochemical data show that WO3 crystals and GO with CNTs have synergistic effect due to the existence of heterogeneous structure: GO provides a wide range of metal reaction active sites for WO3 crystals, while CNTs provides active orbitals that are conducive to electron transport.

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张凯,蒋平平,曹圣平,蒋国强,张萍波,冷炎.氧化石墨烯生长钨基氧化物酸环境电催化析氢[J].精细化工,2022,39(2):0

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  • 收稿日期:2021-08-04
  • 最后修改日期:2021-09-22
  • 录用日期:2021-10-09
  • 在线发布日期: 2021-12-06
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