Enhancing and stabilizing α-Fe2O3 photoanode towards neutral water oxidation: Introducing a dual-functional NiCoAl layered double hydroxide overlayer

Enhancing and stabilizing α-Fe2O3 photoanode towards neutral water oxidation: Introducing a dual-functional NiCoAl layered double hydroxide overlayer
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增强和稳定α-Fe2O3光阳极对中性水的氧化:引入双功能NiCoAl层状双氢氧化物覆盖层

DOI:
10.1016/j.jcat.2018.01.011
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发表时间:
2018-03
影响因子:
7.3
通讯作者:
Zhixian Chang
Zhixian Chang
中科院分区:
化学1区
文献类型:
--
作者:
Guang Wang;Baoyun Wang;Caihong Su;Deliang Li;Ling Zhang;Ruifeng Chong;Zhixian Chang

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Hematite (α-Fe2O3) is a promising candidate as photoanode for photoelectrochemical (PEC) water splitting. However, it still suffers from low efficiency and serious hydrolysis in neutral pH electrolyte. Herein, NiCoAl layered double hydroxides (NiCoAl-LDH) is successfullyin situconstructed onto hematite (α-Fe2O3) nanoarrays. The resulting NiCoAl-LDH/α-Fe2O3photoanode exhibits an onset potential as low as 0.55 Vvs.reversible hydrogen electrode (RHE) and a significantly enhanced photocurrent density of 2.56 mA cm−2at 1.23 Vvs.RHE for PEC water oxidation in neutral electrolyte, which isca.13, 2 and 1.4 times as high as that of α-Fe2O3, NiAl-LDH/α-Fe2O3and CoAl-LDH/α-Fe2O3. Comprehensive electrochemical and structural analysis reveal the synergistic effect of Ni and Co should be responsible for the enhanced PEC performance. Ni and Co could cause local structure distortion of MO6(M = Ni or Co) in NiCoAl-LDH, which (1) improve the conductivity of MAl-LDH, thus enhance the separation and the transfer of photogenerated charges and (2) slightly change the chemical environment of Co and Ni and facilitate the formation of low-valent oxidation states, thus lower the energy barrier of Co2+or Ni2+to high oxidation states and accelerate the kinetics of water oxidation. The versatile skeleton and interlayered anions as well as the thicker decoration of NiCoAl-LDH enable NiCoAl-LDH/α-Fe2O3to possess excellent stability in neutral electrolyte. This work reveals the partial substitution of Co (or Ni) with Ni (or Co) in MAl-LDH could produce more efficient materials toward high PEC water splitting and will stimulate further development on ternary LDHs as excellent cocatalysts for other electrode in neutral electrolyte.
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