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摘要: 高效析氢催化剂的制备仍是目前亟待解决的重要课题。本研究采用液相浸渍原位还原法制备了Ni(OH)2/Ni/g-C3N4复合催化剂,并与碳纸(CP)组合作为微生物电解电池(MEC)的阴极。采用SEM、TEM、XRD、XPS和电化学分析等技术对所制备的催化剂样品的结构性质和析氢电催化性能进行了分析研究。结果表明,Ni(OH)2/Ni/g-C3N4催化剂在100 A/cm2的电流密度驱动下具有优秀的析氢过电位(1881 mV)、较低的电荷转移电阻(10.86 Ω)和较低的塔费尔斜率(44.3 mV/dec),其电化学活性优于纯g-C3N4催化剂和CP,甚至可与Pt催化剂媲美。
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关键词:
- Ni(OH)2/Ni/g-C3N4 /
- 析氢反应 /
- 微生物电解电池
Abstract: The preparation of efficient catalysts in hydrogen evolution reaction (HER) is an urgent task at present. In this work, Ni(OH)2/Ni/g-C3N4 composite catalyst was prepared through liquid phase impregnation with in-situ reduction, which was used to compose the cathode with carbon paper (CP) for the microbial electrolysis cell (MEC). With the help of SEM, TEM, XRD, XPS and electrochemical analysis techniques, the structure, properties and electrocatalytic performance in hydrogen evolution of the Ni(OH)2/Ni/g-C3N4 composite were investigated. The results indicate that the Ni(OH)2/Ni/g-C3N4 catalyst exhibits excellent electrochemical activity for hydrogen evolution in the MEC. Using the Ni(OH)2/Ni/g-C3N4 catalyst, the current density reaches 100 A/cm2 at a small overpotential of 1881 mV, with a low charge transfer resistance of 10.86 Ω and a low Tafel slope of 44.3 mV/dec, which is much superior to pure g-C3N4 catalyst and CP, and even comparable to the Pt catalyst, suggesting that the Ni(OH)2/Ni/g-C3N4 composite can be a potential candidate of HER catalyst in MEC. -
Figure 1 SEM images of g-C3N4 (a) and Ni(OH)2/Ni/g-C3N4 catalysts (b); TEM image of Ni(OH)2/Ni/g-C3N4 catalyst (c); XRD patterns of g-C3N4 and Ni(OH)2/Ni/g-C3N4 catalysts (d); survey spectrum and XPS spectrum (inset) of O 1s for the Ni(OH)2/Ni/g-C3N4 catalyst (e); XPS spectra of Ni 2p (f), N 1s (g), and C 1s (h) for the Ni(OH)2/Ni/g-C3N4 catalyst; N2 sorption isotherms of g-C3N4 (a) and Ni(OH)2/Ni/g-C3N4 catalysts (i)
Figure 2 LSV curves of Ni(OH)2/Ni/g-C3N4 composite catalysts with different Ni loading ratios (a) and coating amounts (b); Tafel plot (points represent raw data, lines represent fitted data) (c); EIS spectra of bare CP, Ni(OH)2/Ni/g-C3N4 and Pt catalysts (d) (the illustration in Graph (d) is the equivalent circuit used to simulate the HER kinetics process); CP curves (e)
Table 1 Energy efficiencies and hydrogen production in the MEC with different cathodes
Cathode Rcat/% $ {R_{\rm{H}}}_{_2} $/% $ {Q_{\rm{H}}}_{_2} $/
(m3-H2·m−3·d−1)ηw/% ηw+s/% CP 24.77 79.51 0.119 52.41 25.22 Ni(OH)2/Ni/g-C3N4 49.62 249.34 0.3725 104.98 62.18 Pt 37.47 134.47 0.2009 79.27 40.37 -
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