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n-Type Molybdenium Diselenide-Based Photoelectrochemical Cells: Evidence for Fermi Level Pinning and Comparison of the Efficiency for Conversion of Light to Electricity with Various Solvent/Halogen/Halide Combinations
Interfacial energetics for n-type MoSe2 (Eg = 1.4 eV, direct) and photoelectrochemical conversion of light to electrical energy in the presence of Xn-/X- (X = Cl, Br, I) have been characterized in CH3CN electrolyte solution.Data for MoSe2 in H2O/I3-/I- are included for comparison, along with a comparison of MoSe2-based cells with MoS2- (Eg = 1.7 eV, direct) based cells.Cyclic voltammetry for a set of reversible (at Pt electrodes) redox couples whose formal potential, <*>, spans a range -0.8 to +1.5 V vs.SCE has been employed to establish the interface energetics of MoSe2.For the redox couples having <*> more negative than ca. -0.1 V vs.SCE, we find reversible electrochemistry in the dark at n-type MoSe2.When <*> is somewhat positive of -0.1 V vs.SCE, we find that oxidation of the reduced form of the redox couple can be effected in an uphill sense by irradiation of the n-type MoSe2 with <*>Eg light; the anodic current peak is at more negative potential than at Pt for such situations.The extent to which the photoanodic current peak is more negative than at Pt is a measure of the output photovoltage for a given couple.For <*> more positive than ca. +0.7 V vs.SCE it would appear that this output photovoltage is constant at ca. 0.4 V.For a redox couple such as biferrocene (<*>(BF+/BF) = +0.3 V vs.SCE) we find a photoanodic current onset at ca. -0.2 V vs.SCE; a redox couple with <*> = 1.5 V vs.SCE shows an output photovoltage of 0.43 V under the same conditions.The ability to observe (i) photoeffects for redox reagents spanning a range of <*>‘s that is greater than the direct Eg and (ii) constant photovoltage for a range of <*>‘s evidences an important role for surface states or carrier inversion such that a constant amount of band bending (constant barrier height) is found for a couple having <*> more positive than ca. +0.7 V vs.SCE.Conversion of <*> light to electricity can be sustained in CH3CN solutions of Xn-/X- (X = Cl, Br, I) with an efficiency that is ordered Cl > Br > I where n-type MoSe2 is used as a stable photoanode.In aqueous solution n-type MoSe2 is not a stable anode in the presence of similar concentrations of Br2/Br- or Cl2/Cl-, showing an important role for solvent in thermodynamics for electrode decomposition.In CH3CN, efficiency for conversion of 632.8-nm light to electricity has been found to be up to 7.5percent for Cl2/Cl-, 1.4percent for Br2/Br-, and 0.14percent for I3-/I-.Differences among these redox systems are output voltage and short-circuit current, accounting for the changes in efficiency.In H2O, I3-/I- yields a stable n-type MoSe2-based photoelectrochemical cell with an efficiency for 632.8-nm light a little lower that for the CH3CN/Cl2/Cl- solvent/redox couple system.Data for MoS2-based cells in the CH3CN/Xn-/X- solvent/redox couple systems show that the efficiency again depends on X: Cl > Br >I. …
n-Type Molybdenium Diselenide-Based Photoelectrochemical Cells: Evidence for Fermi Level Pinning and Comparison of the Efficiency for Conversion of Light to Electricity with Various Solvent/Halogen/Halide Combinations
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Reference£º
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion