Kuei-Hsien Chen

Abstract The present investigation mainly addresses the open circuit voltage (Voc) issue in kesterites based Cu2ZnSn(S,Se)4 solar cells by simply introducing alkali metal fluoride nanolayers (  several nm NaF, or LiF) to lower the work functions of the front İTO\} contacts without conventional hole-blocking ZnO layers. Kelvin probe measurements confirmed that the work function of the front İTO\} decreases from 4.82 to 3.39 and 3.65 eV for NaF and LiF, respectively, resulting in beneficial band alignment for electron collection and/or hole blocking on top electrodes. Moreover, a 10.4% power conversion efficiency ( 11.5% in the cell effective area) \{CZTSSe\} cell with improved Voc of up to 90 mV has been attained. This demonstration may provide a new direction of further boosting the performance of copper chalcogenide based solar cells as well.

The present investigation mainly addresses the open circuit voltage (Voc) issue in kesterite based Cu2ZnSn(S,Se)4 solar cells by simply introducing alkali metal fluoride nanolayers (~ several nm NaF, or LiF) to lower the work functions of the front ITO contacts without conventional hole-blocking ZnO layers. Kelvin probe measurements confirmed that the work function of the front ITO decreases from 4.82 to 3.39 and 3.65 eV for NaF and LiF, respectively, resulting in beneficial band alignment for electron collection and/or hole blocking on top electrodes. Moreover, a 10.4% power conversion efficiency (~ 11.5% in the cell effective area) CZTSSe cell with improved Voc of up to 90 mV has been attained. This demonstration may provide a new direction of further boosting the performance of copper chalcogenide based solar cells as well.

Ascertaining the function of in-plane intrinsic defects and edge atoms is necessary for developing efficient low-dimensional photocatalysts. We report the wireless photocatalytic CO2 reduction to CH4 over reconstructed edge atoms of monolayer 2H-WSe2 artificial leaves. Our first-principles calculations demonstrate that reconstructed and imperfect edge configurations enable CO2 binding to form linear and bent molecules. Experimental results show that the solar-to-fuel quantum efficiency is a reciprocal function of the flake size. It also indicates that the consumed electron rate per edge atom is two orders of magnitude larger than the in-plane intrinsic defects. Further, nanoscale redox mapping at the monolayer WSe2–liquid interface confirms that the edge is the most preferred region for charge transfer. Our results pave the way for designing a new class of monolayer transition metal dichalcogenides with reconstructed edges as a non-precious co-catalyst for wired or wireless hydrogen evolution or CO2 reduction reactions.

Abstract Effects of electronic and atomic structures of V-doped 2D layered SnS2 are studied using X-ray spectroscopy for the development of photocatalytic/photovoltaic applications. Extended X-ray absorption fine structure measurements at V K-edge reveal the presence of VO and VS bonds which form the intercalation of tetrahedral OVS sites in the van der Waals (vdW) gap of SnS2 layers. X-ray absorption near-edge structure (XANES) reveals not only valence state of V dopant in SnS2 is ≈4+ but also the charge transfer (CT) from V to ligands, supported by V Lα,β resonant inelastic X-ray scattering. These results suggest V doping produces extra interlayer covalent interactions and additional conducting channels, which increase the electronic conductivity and CT. This gives rapid transport of photo-excited electrons and effective carrier separation in layered SnS2. Additionally, valence-band photoemission spectra and S K-edge XANES indicate that the density of states near/at valence-band maximum is shifted to lower binding energy in V-doped SnS2 compare to pristine SnS2 and exhibits band gap shrinkage. These findings support first-principles density functional theory calculations of the interstitially tetrahedral OVS site intercalated in the vdW gap, highlighting the CT from V to ligands in V-doped SnS2.

The development of earth-abundant and efficient electrocatalysts for the hydrogen evolution reaction (HER) is one of the keys to success for future green energy systems using hydrogen fuel. Nanostructuring of electrocatalysts is a promising way to enhance their electrocatalytic performance in the HER. In this study, pure pyrite-type beaded stream-like cobalt diselenide (CoSe2) nanoneedles are directly formed on flexible titanium foils through treating a cobalt oxide (Co3O4) nanoneedle array template with selenium vapor. The beaded stream-like CoSe2 nanoneedle electrode can drive the HER at a current density of 20 mA cm−2 with a small overpotential of 125 mV. Moreover, the beaded stream-like CoSe2 nanoneedle electrode remains stable in an acidic electrolyte for 3000 cycles and continuously splits water over a period of 18 hours. The enhanced electrochemical activity is facilitated by the unique three-dimensional hierarchical structure, the highly accessible surface active sites, the improved charge transfer kinetics and the highly attractive force between water and the surface of the nanoneedles that exceeds the surface tension of water.