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Electrochemical Fabrication of Ultrafine g-C3N4 Quantum Dots as Hydrogen Evolution Reaction Catalyst

YANG Na-na CHEN Zhi-gang ZHAO Zhi-gang CUI Yi

杨娜娜, 陈志刚, 赵志刚, 崔义. 电化学制备超细g-C3N4量子点及其电催化析氢性能[J]. 新型炭材料. doi: 10.1016/S1872-5805(21)60045-8
引用本文: 杨娜娜, 陈志刚, 赵志刚, 崔义. 电化学制备超细g-C3N4量子点及其电催化析氢性能[J]. 新型炭材料. doi: 10.1016/S1872-5805(21)60045-8
YANG Na-na, CHEN Zhi-gang, ZHAO Zhi-gang, CUI Yi. Electrochemical Fabrication of Ultrafine g-C3N4 Quantum Dots as Hydrogen Evolution Reaction Catalyst[J]. NEW CARBON MATERIALS. doi: 10.1016/S1872-5805(21)60045-8
Citation: YANG Na-na, CHEN Zhi-gang, ZHAO Zhi-gang, CUI Yi. Electrochemical Fabrication of Ultrafine g-C3N4 Quantum Dots as Hydrogen Evolution Reaction Catalyst[J]. NEW CARBON MATERIALS. doi: 10.1016/S1872-5805(21)60045-8

电化学制备超细g-C3N4量子点及其电催化析氢性能

doi: 10.1016/S1872-5805(21)60045-8

Electrochemical Fabrication of Ultrafine g-C3N4 Quantum Dots as Hydrogen Evolution Reaction Catalyst

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  • 摘要: 由于其高含量的面内氮元素、优异的化学和热力学稳定性、可调的电子能带结构和环境友好的特点,石墨相结构的氮化碳(g-C3N4)材料作为一种非金属催化剂在光电催化领域已经引起广泛的研究关注。相较于光催化领域能带结构的调控,g-C3N4在电催化领域的设计主要集中在活性位点的构筑和电子转移能力的调节。本文报道了一种三价Al3+离子电化学插层超快制备超细g-C3N4量子点(QDs)的剥离策略,与传统的碱金属离子相比,Al3+带电荷量大、冲击能力强,易于得到粒径和厚度更小的均一量子点材料。相应的透射电镜(TEM),原子力显微镜(AFM)和紫外吸收光谱(UV-vis)表征证实了制备得到的g-C3N4 QDs的平均粒径只有3.5 nm,厚度只有3个C-N原子层(~1 nm),并且富含C/N缺陷。这种超细且富含缺陷的量子点材料在0.5 M H2SO4电解液中具有接近0 V的电催化析氢(HER)启动电位、优异的过电位(η10=208 mV)和较低的塔菲尔斜率(b=52 mV/dec)。这项工作提出的快速制备富含C/N缺陷g-C3N4 QDs的策略也为研究其它二维层状材料的剥离及其在电催化领域的应用提供了一条有趣的研究思路,有利于发掘二维材料更多丰富的物化性质。
  • Figure  1.  (a) Schematic illustration of the electrochemical intercalation of Al3+ cations into the interlayer of bulk g-C3N4 materials. (b) The extraction of Al3+ ions wrapped by oleic acid molecules from the g-C3N4 lattice for the fabrication of the ultrafine g-C3N4 QDs via the sonication process. (c) Typical optical images of bulk g-C3N4 and g-C3N4 QDs

    Figure  2.  (a) XRD patterns of bulk g-C3N4 and g-C3N4 QDs.(b)TEM image of g-C3N4 QDs, with the corresponding SAED pattern in the insert. (c) EDS image of g-C3N4 QDs. (d) Statistic analysis of the lateral dimension of the as-obtained g-C3N4 QDs. (e) HRTEM image of g-C3N4 QDs. (f) AFM image of g-C3N4 QDs. (g) Thickness of g-C3N4 QDs highlighted in line 1 and line 2 in (f).

    Figure  3.  (a) Raman spectrum and (b) UV−vis absorbance spectrum of g-C3N4 and g-C3N4 QDs, with the corresponding band gap inserted in (b).

    Figure  4.  (a) Polarization (LSV) curves and (b) Tafel plots for the as-obtained g-C3N4 QDs, bulk materia and benchmark Pt/C at a scan rate of 5 mV/s in 0.5 M H2SO4 solutions. (c) Comparison of the HER performance obtained from g-C3N4 QDs and other previous reports. (d) Nyquist plots and (e) chronopotentiometry measurements of g-C3N4 QDs and bulk materials.

    Table  1.   the comparison of the merits and demerits of different g-C3N4QDs preparation methods

    MethodsParticle size(nm)Thickness(nm)AdvantagesDisadvantagesReference
    Sonication methodBelow 105–6Simple procedures and facile operationLow yield and long circle[36,37]
    Sonication along with chemical oxidation40.35High yield and high purityHigh cost and complex operation[38,39]
    Hydrothermal method3.32Simple procedures and low costLow yield and long circles[40,41]
    Hydrothermal along with chemical oxidation5-9Below 10High yield and high purityHigh cost and complex operation[42,43]
    Solid-phase method4.31.5–2.5High yieldComplex purification and long circles[44,45]
    Microwave-assisted solvothermal method1-5-Simple procedures, short circles
    and low cost
    Low quantum yield[46,47]
    Quasi-chemical vapor deposition (CVD) method2.4-Closely integratedEnergy-consuming and complex purification[48]
    Electrochemical exfoliation3.51Simple procedures, facile operation, short circles, high yield and high purityNo more experimental exploration for the intercalation mechanismThis work
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  • 收稿日期:  2021-03-09
  • 修回日期:  2021-05-07
  • 网络出版日期:  2021-06-03

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